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 Chapter 1
 Introduction

 Atmospheric deposition takes place via two pathways: wet deposition and dry deposition.  Wet
 deposition is the result of precipitation events (rain, snow, etc.) which remove particles and
 gases from the atmosphere. Dry deposition is the transfer of particles and gases to the
 landscape through a number of atmospheric processes in the absence of precipitation. Wet
 deposition rates of acidic species across the United States have been well documented over the
 last 10 to 15 years; however, comparable information is unavailable for dry deposition rates.
 This lack of information on dry deposition increases the uncertainty in estimates of
 interregional, national, and international transport and confounds efforts to determine the
 overall impact of atmospheric deposition.

 The direct measurement of dry deposition is not straightforward, but a number of investigations
 have shown that it can be reasonably inferred by coupling air concentration data with routine
 meteorological measurements (Shieh etal., 1979; Hicks etal., 1985; Meyers and Yuen, 1987;
 Wesely and Lesht, 1988). Shieh et al.  (1979) have shown that submicron particle and sulfur
 dioxide (SO2) deposition rates for the eastern United States were strongly dependent on
 windspeed, solar radiation, and the condition and type of ground cover. For example, rapidly
 growing  vegetation and forests were found to generally experience higher deposition rates than
 senescent vegetation, short grass, or snow. This approach has been expanded (Wesely, 1988) to
 calculate deposition rates for various additional atmospheric species using site-specific
meteorological  data.
In 1986, the U.S. Environmental Protection Agency (EPA) contracted with Environmental
Science & Engineering, Inc. (ESE) [currently known as QST Environmental Inc. (QST)] to
establish and operate the National Dry Deposition Network (NDDN).  The objective of the
NDDN was to obtain field data at approximately 50 sites throughout the United States to
establish patterns and trends of dry deposition.  The approach adopted by the NDDN was to
estimate dry deposition using measured air pollutant concentrations and modeled deposition
velocities (Vds) estimated from meteorological, land use, and site characteristic data. The
model currently used for dry deposition calculations is a multi-layer version of the Big Leaf
Model developed by Meyers et al. (1991).
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Passage of the Clean Air Act Amendments (CAAA) in 1990 required implementation of a
national network to monitor the status and trends of 1) air emissions, pollutant deposition, and
air quality; 2) determine the effects of emissions on water quality, forests, and other sensitive
ecosystems; and 3) assess the effectiveness of emission reduction requirements through
operation of a long-term monitoring program.  In response to these requirements of the CAAA,
the EPA, in coordination with the National Oceanic and Atmospheric Administration (NOAA),
created the Clean Air Status and Trends Network (CASTNet). CASTNet became operational
in mid-1991, and the NDDN program was incorporated into CASTNet at that time. To
increase spatial representation of CASTNet for the  western United States, EPA and the NPS
agreed to share responsibilities in the operation of 19  NPS monitoring sites for the
measurement of dry deposition.

This report summarizes results of NDDN and CASTNet monitoring activities from 1987
through 1995.  Concentration and deposition data for atmospheric sulfur and nitrogen species
are presented and discussed as grand averages for the entire  time period as well as annual
averages for 1989, 1992,  and 1994.  Annual and seasonal averages for each year are discussed
regionally. Relative contribution of gases versus aerosols are evaluated. Wet deposition data
for 21 CASTNet and 38 National Atmospheric Deposition Program (NADP) sites are presented
and then used, along with dry deposition calculations, to estimate total depositions of sulfur and
nitrogen.  The relative magnitude of wet and dry deposition  are discussed.  Ozone (O3)
concentrations and exposure statistics are illustrated for 1989, 1992, and 1994 and analyzed for
the entire monitoring record.
Data and results from the visibility and mountain acid deposition programs are briefly
discussed. The mobile system for the direct measurement of dry deposition is described along
with field studies in which the system was successfully utilized. Initial results of the comparison
between filter packs and annular denuders is also given.

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 Chapter 2
 Network Description and Methods

 2.1  Network Description
 Figure 2-1 shows the locations of current and historical CASTNet Deposition Network (CDN)
 sites. Forty-five primarily rural eastern sites and three western sites are currently operational
 (sites with 100 series designations). Two of the eastern sites are collocated for assessment of
 network precision. Eighty-one percent of the network was installed and collecting data as of
 July 1989. The remaining nine sites came online between July 1990 and July 1995. Eleven sites
 were discontinued from October 1988 through December 1993, mostly due to less than ideal
 siting conditions.  Table 2-1 lists all of the CASTNet sites, their locations, and dates of
 operation. In December 1995, the number of CDN sites was reduced to 15 due to funding
 limitations, with 13 sites in the eastern United States and 2 sites in the western United States. In
 June 1996, funding was restored, and most of the original sites were reactivated, returning the
 network to its original configuration. The number of sites in the network is summarized by year
 hi Table 2-2.

 In 1994, the EPA and National Park Service (NFS) began a collaborative effort to expand dry
 deposition measurements  in the western United States [primarily at National Parks (NP) and
 Monuments]. EPA agreed to provide operating protocols, assistance with equipment
 installation, data management, and reporting, while NPS agreed to support field operations,
 laboratory analysis, and quality assurance (QA). As of May 1997, 19 NPS sites were installed
and operational (sites with 400 series designations). During this period, one eastern and three
western CASTNet sites were operationally turned over to the NPS.
As part of routine network operations, data are collected at a site hi Egbert, Ontario, Canada to
determine if measurement biases exist between the United States and Canadian dry deposition
systems. This site is currently occupied by two Canadian trends monitoring networks [Canadian
Acid Deposition Monitoring Network (CAPMoN) and Acid Precipitation hi Ontario Study
(APIOS)].

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Wet deposition samples are collected at 18 eastern and 3 western CDN sites and 1 network
intercomparison site [NADP/National Trends Network (NTN), CAPMoN, CASTNet] at Scotia
Range, PA.

2.1.1  Site Selection
The current network is designed to support investigation of relationships between emissions and
atmospheric concentrations/depositions. Assessments of sensitivity to O3 and acid deposition
have shown that large areas of potentially sensitive terrestrial and aquatic ecosystems exist in
the eastern United States and that limited areas of sensitive ecosystems exist hi the western
United States. These findings, coupled with the expected changes in emissions of sulfur oxides
(SOJ and nitrogen oxides (NOX), underlie the distribution  of sites in the network. Each of the
eastern United States monitoring sites was selected by considering:
       1.   Regional representativeness,
       2.   Long-term availability, and
       3.   Accessibility.

For the western United States, the limited number of sites  and higher diversity of the region
precluded determination of spatial patterns. Therefore, site selection focused primarily on
locations where specific research issues could be addressed and where natural resources were at
risk (e.g., national parks). These locations included calibrated watersheds, in which dry
deposition information was needed to close geochemical cycles for sulfur, nitrogen, and
alkalinity.

Regional representativeness refers to the overall similarity of the site to a characteristic area
[typically 80 by 80 kilometers (km)]  surrounding the site.  This implies that concentrations
must also be representative. Thus, major sources of SOX and/or NOX were avoided to reduce
the likelihood of locally perturbed concentration fields.  In addition, land use near the site
matches, as much as possible, the dominant regional land use to make appropriate use of
meteorological data in Vd calculations. Finally, monitoring sites needed to be available for
extended periods (10 to 15 years) in order to assess dry deposition trends.
Site-specific criteria relate to conditions in the immediate vicinity of a prospective monitoring
site. Specifically, they concern local features that may perturb air quality and meteorological

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observations.  Local sources of air contaminants and local features that may influence
windspeed, wind direction, etc. are the focus of these criteria.  A list of site-specific criteria
that are used during the site-selection process is shown in Table 2-3.

An iterative procedure for selecting dry deposition monitoring sites was followed. The major
steps include:
       1.   Identification of general areas for inclusion in the network;
       2.   Review of emission inventory, population, and land-use data to identify areas that
           are regionally representative;
       3.   Visits to the areas identified in Step 2 to identify and document candidate sites; and
       4.   Selection of measurement sites by the EPA Project Officer.

By design, the network attempts to capture anticipated gradients hi atmospheric pollutants
(especially SO2).  Thus, the northeastern sites are closely spaced around emission sources in the
Ohio River valley and more distantly spaced throughout New England and the Atlantic coast
states.  Network spacing is still greater hi the southeast and west, where emission densities (and
expected gradients) are considerably lower than hi  the northeast.
2.1.2 Subregions
For presentation purposes, sites in the eastern United States have been grouped into six
subregions (see Figure 2-2).  Subregional designations, with numbers of sites hi parentheses,
are as follows:  northeast (11), upper northeast (3), midwest (9), upper midwest (3), south
central (11), and southern periphery (3).  Besides geographic location, site groupings were
based on terrain and general spatial patterns of atmospheric concentration data. The
categorization of sites also divides the Appalachian Mountains into three convenient geographic
ranges.  The northern Appalachians, including the Adirondack Mountains of New York, the
Green Mountains of Vermont, and the White Mountains of New Hampshire fall within the
upper northeast subregion. The central Appalachians, including the Catskill Mountains of New
York, and the Allegheny Mountains of West Virginia, fall within the northeast subregion.
Finally, the southern Appalachians, including the Great Smoky Mountains of North Carolina
and Tennessee and the Blue Ridge Mountains of Virginia, fail within the south central
subregion. Each of these subregions thus includes sites in mountainous areas, both for the

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purpose of monitoring deposition in sensitive areas and to elucidate variability of deposition in
complex terrain.

Sites in the upper northeast subregion are exclusively rural-forested, while those in the
northeast subregion exhibit a range of characteristics.  Six northeastern sites are rural-forested,
two are rural-agricultural (106 and 128), and three are near or within the Washington-
Baltimore-Philadelphia-New York City conurbation (104, 116, and 144). The upper midwest
sites are rural-agricultural or rural-forested (149). The midwest sites are rural-agricultural,
except for Site 146 (suburban Chicago), which is urban-agricultural.  Although rural in
character, three sites (122,  140, and 157) are influenced, to a greater or lesser extent, by SO?
emissions from nearby point sources with annual emissions hi excess of 1,000 tons per year
(tpy)-

The south-central sites are either rural-forested or rural-agricultural but exhibit a wide range of
terrain characteristics. Three sites are located above 1,000 m and form a line extending from
northern Virginia to southwestern North Carolina.  Site 118 (currently NFS Site 418) is situated
on a ridge of the eastern Blue Ridge Mountains, and Sites 120 and 126 occupy the spine of the
Appalachian Mountains.  Due to the unique exposure of these sites, they have been placed in a
separate terrain category (i.e., mountaintop).  Two sites (121 and 137) are located in hollows
or valleys, and the other six sites hi the subregion are in rolling terrain.  The distribution of
sites in this subregion provides an opportunity to investigate relationships among terrain
characteristics, atmospheric concentrations, and dry deposition (see Section 3.0). Finally, all
three of the southern periphery sites are rural-forested hi flat or rolling terrain.
Despite apparent similarities hi land use and terrain, the western sites are not homogeneous in
character. For this reason, no attempt was made to group western sites. Site 161 (Gothic, CO)
occupies a mountain valley within the central Rocky Mountains. Site 162 is located on the
foothills of the High Uintas, the most prominent east-west mountain range in North America.
Sites 163 and 164 are located  in semi-arid rangeland near the northern extreme of the Great
Basin. Sites 165 and 169 represent the transition from the western Great Plains to the Rocky
Mountains.  Sites 167 and 174 are located in the arid southwest; Site 167 is hi the Sonoran
Desert, while Site 174 is on the extensive and forested Kaibab Plateau. Site 168 (near the
Canadian border) alone represents the western boreal forest. Thus, although these sites ,are

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collectively termed the western part of the network, they represent a wide range of
environments.

Site locations and descriptive information are provided in Table 2-4. Terrain and land-use
information refers to a 10-km radius around the site and is presented to convey a sense of the
setting within which each site operates.  Site numbers are used for identification purposes only
and do not correlate with order of installation or operation.

2.2 Methods
This section provides a brief overview of the CDN methods. Step-by-step protocols and
additional details on these activities can be found in the CDN Field Operations Manual,
Laboratory Operations Manual, and Data Management Manual (ESE, 1990a, 1990b, 1991a).

2.2.1 Field Operations
Ambient measurements for O3, SO2, particulate sulfate (SO^), particulate nitrate (NO3), nitric
acid (HNO3), particulate ammonium (NHJ), and meteorological variables required for dry
deposition calculations are performed at each CDN site.  Meteorological variables and O3
concentrations are recorded continuously and reported as hourly averages consisting of a
minimum of nine valid 5-minute averages. Atmospheric  sampling for sulfur and nitrogen
species is integrated over weekly collection periods using a 3-stage filter pack (Figure 2-3). In
this approach, particles and selected gases are collected by passing air at a controlled flow  rate
through a sequence of Teflon®, nylon, and Whatman filters. The Teflon® filter removes
particulate SO|~, NO3, and NHJ,  and the nylon filter is used to remove HNO3. The Whatman
filter is a cellulose filter base that is impregnated by potassium carbonate (K2CO3) and is used
for removal of SO2. In practice, a fraction (usually <20 percent) of ambient SO2 is captured on
the nylon filter. The nylon filter SO2 and Whatman filter SO2 are therefore summed to provide
weekly average concentrations. The nylon filter HNO3 is converted to NO3 and added to the
Teflon® filter NO3 to provide weekly total NO3 concentrations.
Filter packs are prepared and shipped to the field weekly and exchanged at each site every
Tuesday.  Blank filter packs are collected monthly to evaluate passive collection of particles
and gases as well as contamination during shipment and handling. At 21 sites located more than

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50 km from NADP/NTN sites (Figure 2-4), wet deposition samples are collected weekly
(according to NADP/NTN protocols) and shipped to QST for chemical analysis.

Filter pack sampling and O3 measurements are performed at 10 m using a tilt-down aluminum
tower (Aluma, Inc.). Filter pack flow is maintained at 1.50 liters per minute (Lpm) at eastern
sites and 3.00 Lpm at western sites, for standard conditions of 25 degrees Celsius (°C) and
760 millimeters of mercury (mmHg) with a mass flow controller (MFC). Wet deposition
samples are collected in precleaned polyethylene buckets using an Andersen Model APS
precipitation sampler. Buckets are placed on the sampler on Tuesday and removed, whether or
not rainfall has occurred, the following Tuesday.  Buckets are weighed in the field, decanted to
a 1-liter (L) polyethylene bottle, sealed, and shipped to QST for chemical analysis.
Precipitation amount (depth) is also monitored at wet deposition sites. Figure 2-5 depicts a
typical CDN site configuration.

O3 is measured via ultraviolet (UV) absorbance with a Thermo-Environmental Model 49-103
analyzer operating on the 0- to 500-part per billion (ppb) range.  Ambient air is drawn from the
10-m air quality tower through a 3/8-inch TFE Teflon® sampling line.  Teflon® filters housed at
the tower inlet and the analyzer inlet prevents particle deposition within the system. Periodic
checks indicate that online losses through the inlet system are consistently less than 3 percent.
Zero, precision (60 ppb), and span (400 ppb) checks of the  O3 analyzer are performed every
third day using an internal O3  generator.

In addition, various observations are periodically made at the CDN sites to support model
calculations of dry deposition.  Site operators record surface conditions (e.g., dew, frost, snow)
and vegetation status weekly. Vegetation status and land-use information are used to define the
distribution and condition of plant species around each site that could influence deposition rates
for gases (especially SOj) and particles.  Vegetation data are obtained to track  evolution of the
dominant plant canopy, from leaf emergence (or germination) to senescence (or harvesting).
Once a year, site operators also provide information on major plant species and land-use
classifications within 1.0 km of the site. Additional land-use data was obtained by digitization
and analysis of aerial photographs obtained from the U.S. Geological Survey (USGS) National
Cartographic Information Center in Reston, VA. Photographs were interpreted according to
procedures described by Anderson et al.  (1978).
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Leaf area index (LAI) measurements were taken at all CDN sites during the summers of 1991
and 1992.  LAI is the one-sided leaf area of the plant canopy per unit area of ground at full leaf
emergence and has been shown to play an important role in atmosphere-canopy exchange
processes (McMillen, 1990).  LAI is measured using an LAI-2000 Plant Canopy Analyzer
manufactured by Li-Cor (Lincoln, NE). The LAI-2000 makes indirect (i.e., nondestructive)
estimates of LAI from simultaneous measurements of light interception by the plant canopy at
five angles of inclination (Li-Cor, 1989). Initial development and testing of the LAI-2000 by
the manufacturer focused on a variety of agricultural crops, such as soybeans and wheat, and
similar approaches have been used to measure LAI of forest canopies (Pierce and Running,
1988; Chason et al.,  1990).

All field equipment is subjected to quarterly inspections and multipoint calibrations, using
standards traceable to the National Institute of Standards and Technology (NIST). In addition,
independent equipment audits were performed annually by Ogden Environmental and Energy
Services, Inc. (Ogden), and randomly by EPA or its designee. Results of field calibrations are
used to assess sensor accuracy and flag, adjust, or invalidate field data. Precision and accuracy
criteria for CDN field measurements are shown hi Table 2-5.
2.2.2 Laboratory Operations
Filter pack samples are loaded, shipped, received, extracted, and analyzed by QST personnel at
the Gainesville, FL laboratory. Filter packs contain three types of filters in sequence:  a
Teflon® filter for collection of aerosols, a nylon filter for collection of HNO3, and dual K2CO3-
impregnated cellulose filters for collection of SO2.

Following receipt from the field, exposed filters and blanks are extracted and then analyzed for
SO2; and NO3' by micromembrane-suppressed ion chromatography (1C). Teflon® filter extracts
are also analyzed for NHJ by the automated indophenol method using a Technicon II or
TRAACS-800 Autoanalyzer system. All analyses are completed within 72 hours of filter
extraction.  Figure 2-6 depicts the sequence of laboratory operations for filter pack sample
analyses.

Wet deposition samples are filtered and then analyzed for pH, conductivity, acidity, sodium
(Na+), potassium (K+), NHJ, calcium (Ca2+), magnesium (Mg2+), chloride (Cl'), nitrite

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NOj, and SO*'. Analysis of NHJ and anions is as described previously for filter pack samples.
Analysis of Na+, Mg2+, and Ca2+ is performed with a Perkin-Elmer P-2 inductively coupled
argon plasma (ICAP) emission spectrometer.  Acidity is determined via titration to
approximately pH 8.3, and K+ was analyzed via atomic emission through first quarter 1995 and
subsequently via ICAP. Table 2-6 lists the analytes per sample plus the QC solutions for
periods of record.  Figure 2-7 depicts the sequence of laboratory operations for wet deposition
sample analyses.

Results of all valid analyses are stored in the laboratory data management system [Chemistry
Laboratory Analysis and Scheduling System (CLASS™)]. Atmospheric concentrations are
calculated (based on volume of air sampled) following validation of hourly flow data.
Atmospheric concentrations of particulate  SO2', NO^, and NHJ are calculated based on the
analysis of Teflon® filter extracts; HNO3 is calculated based on the NOj found in nylon filter
extracts; and SO2 is calculated based on the sum of SO^ found hi nylon and cellulose filter
extracts.

2.2.3 Data Management
The Data Management Center (DMC) activities consists of four major operations:  data
acquisition,  data validation, model operation, and transmittal to EPA. These activities are
described briefly hi this section. Details on data management and operation of the Multi-Layer
Dry Deposition model are provided in the CASTNet Data Management Manual, the paper by
Clarke and Edgerton (1993), and in Section 3.1.2.

The data acquisition process stresses multiple levels of redundancy to minimize data loss. The
primary mode of data acquisition from the field is via telephone modem. Each site is
automatically polled by the DMC between 2:00 and 5:00 a.m. every day using an IBM-
compatible PC and software developed by Odessa Engineering, Inc.  The polling software
permits recovery of hourly data and status files, power failure logs, and automated calibration
results from the previous 7 days. The program also maintains synchronization of the network
by checking the clock within each data acquisition system (DAS) and correcting the tune if it
deviates from expectation by more than 5  minutes. If daily polling results  hi incomplete data
capture from any site, then diskettes of data from the primary and backup DAS  are read into
the database management system. If the database is still incomplete,  missing data are entered

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manually either from site printouts or recovered from data cartridges. Each datum is
automatically given a source flag that is used to trace its mode of entry into the system (i.e.,
modem, cartridge, or manual entry).

At each site, an Odessa DSM-3260 interfaced with a Turbo XT PC (compatible with an
IBM XT) comprises the primary DAS. The DAS collects and processes data from the station
sensors and instruments; averages, flags, and stores the data; transmits data upon command;
and generates standard reports. Activation of the zero/span/precision sequence of the O3
analyzer is also controlled by the DAS. The DAS records hourly averages in a 16K internal
random-access memory (RAM) and on a 128K external data cartridge. The 16K internal RAM
and the 128K cartridge hold approximately 7 and 90 days of hourly data, respectively. Sixteen
channels of data can be input into the DSM-3260. Currently, 12 input channels are assigned for
precipitation, vector-averaged wind direction and windspeed, temperature, delta temperature
(lapse rate), relative humidity, O3 (two channels), solar radiation, filter pack flow rate, scalar-  .
averaged windspeed, and wetness. For the Mountain Acid Deposition Program (MADPro), one
channel is used to collect cloud presence data. Cloud presence is defined as a 5-minute period
with an average liquid water content of at least 0.05 gram per cubic meter (g/m3). Standard
deviation of wind direction (sigma.theta) is calculated as 15-minute averages of 1-second
readings. Four consecutive 15-minute averages are then averaged to produce hourly values.

The onsite PC serves as a terminal for communicating with the DAS and allows the site
operator to:
      1.   Review hourly averages and instantaneous values,
      2.   Review the status  of initialization functions and control outputs, and
      3.   Download data for transmittal to QST.

Data are downloaded from the data cartridge to a floppy disk that is mailed to QST.  A backup
copy of the data is retained onsite. In addition, a dot-matrix printer provides a hard copy of
hourly data and site operator interactions with the DAS. Printouts are sent to QST the first
Tuesday of every month.
An Odessa DSM-3260L is used as the backup DAS. The 3260L is equipped with a 128K RAM
cartridge, which can store approximately 3 months of hourly averages from eight input
                                          11

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channels. The channels recorded on the backup DAS are windspeed, wind direction, relative
humidity, solar radiation, O3, temperature, delta temperature, filter pack flow, and sigma theta.

In summary, the continuous data are transmitted from CDN sites to the DMC via:
       1.   Daily dial-up of each site by modem,
      2.   A disk with hourly averages from the DSM-3260,
      3.   Hard-copy printouts from the PC XT, and
      4.   A backup disk with hourly averages from the DSM-3260L.

The CDN database management system (DBMS) consists of a custom version of Odessa
Engineering's Environmental Aide software. The Environmental Aide system consists of two
programs, ENVICOM and ENVAID, which reside on a Local Area Network (LAN) in the
DMC.

ENVICOM is a communications and data transmittal package that contains configuration
parameters for up to 100 remote stations. The primary function of ENVICOM is to poll each
site daily and incorporate the previous day's hourly averages into the raw database. When
ENVICOM calls a DAS, it instructs the unit to transmit the data 1 hour at a time for all
parameters. Check sums are embedded  in each string to verify error-free transfer.  If errors are
detected, data will be replaced with a missing code. At each poll, ENVICOM attempts to
replace missing values for the past week with valid information.

Data retrieved through ENVTCOM are entered directly into the raw database and stored in
binary data and status files. ENVICOM is also used to ingest cartridge data that have been
transferred to disk. Information that has been recorded on the disk, but is missing in the
ENVICOM database, will automatically be inserted, replacing only missing periods.

ENVAID consists of data management software that provides capabilities to edit the data and
status files, run simple statistical analyses, and manually enter missing data. When the data
have been reviewed and validated, a third program, REPORTS, is used to present  the data in
readable summaries. REPORTS is also used to convert the edited binary database into ASCII
format, which is copied to a high-density disk for database transmittal.
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 The process of data validation begins within hours after the stations are polled. Daily
 summaries are generated as data are collected from the sites. Field operations personnel then
 review these reports daily and detect potential problems with minimal delay. Site Status Report
 Forms (SSRFs) and operator logsheets are reviewed weekly to verify the validity of the data
 received. When data for 1 month have been collected from all means available, those data are
 considered to be validated at Level I.

 Level II validation involves a more detailed screening of the data.  SSRFs, operator logsheets,
 calibration data, and audit results are all reviewed for each site. This is the most labor-intensive
 step since defensible decisions need to be made. In addition, data are screened using the
 automated program VCHECK, which identifies potential problems such as values greater than
 the expected range and invalid combinations of status flags, values, and spikes. All review and
 editing activities which take place in the DMC are documented. When a monthly data set for a
 site is reviewed, the data analyst records recommended changes along with reasons on a
 Change Documentation Review  Form (CDRF). The data management supervisor reviews these
 changes, consulting the QST Work Assignment Manager as necessary, and passes approved
 changes along to the data management personnel. The times and dates of all changes are
 recorded on the CDRF entry form by the person who makes the changes.

When all documentation has been reviewed and the database has been edited to the satisfaction
of the data management supervisor, the  project QA supervisor reviews approximately
 10 percent of the database for traceability. Upon completion of the QA review, the data
management supervisor, project QA supervisor, and work assignment manager deem the
database as validated at Level II.

Data generated from filter pack samplers, precipitation samplers, and cloudwater samplers is
managed by CLASS™. Figure 2-8 depicts the flow of data management activities that are
handled by CLASS™.

Attainment of Level I validation for discrete data consists of meeting the following criteria:
      1.    Data are determined to be reasonable based on the analyst's evaluation of the data
           batch QC sample results.
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      2.   Data transfer by electronic or manual entry into CLASS™ is completed properly as
           evaluated by the Laboratory Operations Manager.
      3.   The appropriate analytical batches are processed through an automated QC
           checking routine performed by CLASS™ and determined to be acceptable.  For each
           analytical batch, an alarm flag will be generated if any of the following occurs.
           a.   Insufficient QC data are run for the batch.
           b.   Correlation coefficient of standard curve is less than 0.995.
           c.   The 95-percent confidence limit of the Y-intercept exceeds the limit of
                quantitation.
           d.   Sample response exceeds the maximum standard response in the standard
                curve (i.e., the sample must be diluted to bring the response within the range
                of the curve).
           e.   Continuing verification samples (CVSs) exceed the recovery limits.
           f.   Reference samples exceed accuracy acceptance limit.

A batch with one (or more) flags can be accepted only if written justification is provided by the
Laboratory Operations Manager.

To calculate atmospheric concentrations from filter pack samples, filter pack flow data are
merged with laboratory data. Atmospheric concentrations are calculated only if valid hourly
averages for filter pack flow represent at least 75 percent of the sampling period and analytical
data meet all QC criteria.  Filter pack samples with greater than 75 percent but less than
90 percent valid flow data will be flagged to indicate uncertainty in concentration calculations.

For wet deposition samples, a second laboratory data validation check involves three
interparameter consistency checks:
       1.   Percent difference of cations versus anions,
       2.   Percent difference of predicted-versus-measured conductivity, and
       3.   pH-versus-conductivity relationship of the  sample compared to the expected
            relationship when rainfall is assumed to be controlled by sulfuric acid.
The evaluation of these interparameter consistency checks provides a method for determining
whether the analysis should be repeated or verified.

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 CLASS™ has been programmed to calculate cations, anions, and predicted conductivity.
 Percent ionic and conductivity difference values are calculated by the following equation:

             Percent difference = 200 x —	—
                                                                                   (2-1)
       The criterion for re-analysis is:
       a.   Percent ionic difference of cations (Value 1) versus anions (Value 2):
                If pH <4.8, then criterion = ±15 percent
                If pH >4.8, then criterion = ±30 percent
       b.   Percent conductivity difference for predicted (Value 1) versus measured (Value 2)
           conductivity:
                If conductance < 10, then criterion  = ±30 percent
                If conductance > 10, then criterion  = ±10 percent

Figure 2-9 shows the flow of data through the entire data management system.

Attainment of Level II validation requires that:
       1.   All Level I data meeting QC criteria are reviewed and evaluated as acceptable by
           the Laboratory Operations Manager.
      2.   A review and evaluation of any alarm flags is completed by the Laboratory
           Operations Manager.
      3.   Written justification for acceptance of data that did not meet QC criteria is
           approved by the QA Supervisor.
      4.   SSRFs and Precipitation Sample Report Forms (PSRFs) are reviewed.
      5.   As received from the DMC, valid flow data are processed and checked before
           calculation of atmospheric concentrations.
      6.   Atmospheric concentrations are calculated as follows:
         Volume in m3 = tatal samPle time t*r) * average flow x 60
                                      1,000
(2-2)
  Atmospheric
 Concentration = J»g °f analytelfilter x analyte dependent constant (if necessary)
                                     volume
   in pgfm*
(2-3)
                                           15

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  Constant
                         molecular weight of analyte in air
           molecular weight of corresponding element (e.g., S or N) in solution
(2-4)
           Note: m3 = cubic meter.
                 fig = microgram.

      7.   The CDN transfer file and flag counts are submitted to and confirmed by the data
           management staff.

Within 120 days after the end of a quarter, the Level II database is submitted in ASCII format
on a high-density S^-inch diskette along with hardcopy printouts and a quarterly data report.
Every file submitted to EPA is accompanied by a QC report, which lists parameter averages by
site and aggregated counts of status flags. The quarterly data report summarizes network
activities in the period and presents results of all field and laboratory QC checks. Results of
traceability audits by the project QA supervisor are also presented.

2.2.4 Quality Assurance
The CDN QA program is a comprehensive program that addresses all major aspects of project
operations. Tables 2-7 and 2-8 list the routine QA audits performed at CDN sites and the QST
laboratory, respectively.

2.2.4.1 Field Data Audits
Level n Database Audit
Since transmission errors have been shown to be extremely rare, this audit focuses on
documentation, validation, and manual entry operations.

Field data are validated hi monthly batches, and approximately 5 percent of these monthly
validation batches is selected at random for audit purposes. Another 5 percent is selected that
involve a high degree of data entry and manipulation. Since there are typically 165 batches
(three monthly batches for 55 sites), 17 batches are selected. Each monthly data batch is
accompanied by a CDRF, which documents all changes made to the database during the
validation process. Each transaction documented on the CDRF of the selected batch is verified
                                           16

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 by review of the corresponding Level II database as well as review of all calibration
 information.

 Corresponding portions of the database are also reviewed to detect undocumented or
 inadvertent changes that would not appear on the CDRF. This is accomplished by ensuring that
 all data source flags are correlated with CDRF entries. Data source flags indicate the mode of
 entry of each datum into the database. Any numeric value or status flag manually entered or
 modified is prefixed with an "m" source flag. All errors and cases of confusing documentation
 are discussed with the DMC manager and staff. A review of completeness, discrepancies
 found, and resulting corrective actions are reported.

 QC Failure Audit
 This audit  includes a review of all reported problems with sensors and equipment at the sites
 and the actions taken to solve such problems. Calibration result summaries, external audit spot
 reports, and mail-out audit results are reviewed as well. Calibration results and problem reports
 for the site-months audited during the Level II database audit are cross-referenced with the
 CDRFs and the database to ensure that the validation process includes required updates.

 Field Calibrator Audit
 The QA supervisor observes field calibration and conducts a systems audit of the monitoring
 site.

Field Calibration Data Audit
Calibration files of the Level II audit sites are reviewed for completeness of the calibration
information, manual entry, transcription errors, and standard operating procedures (SOPs).
Certification results are also reviewed, and transfer sensor serial numbers are cross-referenced
with the transfer sensor serial numbers on the calibration forms.
2.2.4.2 Laboratory Data and Operations Audits
The laboratory component of the QA audit addresses data obtained from filter packs collected
at all CDN sites and wet deposition samples collected at selected sites. Six types of QA checks
are performed to evaluate the following:
       1.   Traceability of data from analytical instruments to CLASS™,
                                           17

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      2.   Validity of filter pack flow calculations used to determine atmospheric
           concentrations,
      3.   Status of filter media acceptance tests and chain-of-custody audits,
      4.   Accuracy of precipitation field data including review of rain gauge charts,
      5.   Compliance with overall data requirements for the project, and
      6.   Life history audits.
The procedure for each of these checks is outlined as follows:
       1.   Laboratory Recalculation Audit:
           a.   The audit for filter pack analytes is conducted by randomly selecting
                20 percent of all data batches analyzed for the quarter. Calibration curves for
                selected batches are regenerated from raw analytical data (MAXIMA) and
                compared with CLASS™ printouts.
           b.   Concentrations of filter pack analytes determined by 1C are recalculated using
                the raw data from MAXIMA for analyte response and calibration curves
                (generated in Step a), then compared with CLASS™ concentrations.
           c.   The concentration of NHJ hi wet deposition samples and Teflon® filter
                extracts,  analyzed by TRAACS, is audited by recalculating the coefficients of
                the quadratic regression equation, followed by recalculation of every tenth
                sample in the batch.
           d.   The audit for wet deposition analytes is conducted by selecting between 20
                and 40 percent of batches  analyzed for the quarter. The percent selected
                depended on the number of batches run per analyte grouping, but in all cases
                at least one batch is selected.
           e.   Concentrations of wet deposition analytes determined by 1C are recalculated
                using the procedures outlined in Steps a and b.
           f.   The pH and conductivity data are audited by proofing the manual entry of
                data into CLASS™ and by reviewing QC data.
           g.   Wet deposition data for  K+ are audited by regenerating the linear calibration
                curve and determining the correlation coefficients.
           h.   Wet deposition Na+, Ca2+, and Mg2+  data (analyzed by ICAP) are audited by
                regenerating the linear calibration curves and recalculating correlation
                coefficients for all analytes.
                                            18

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      i.   Wet deposition data for acidity are audited by proofing the manual entry of
          data into the CLASS™ system and recalculating acidity on every tenth sample.
 2.    Flow Verification Audit:
      a.   The on/off dates and times for all filter packs in the chemistry database are
          compared to data recorded by site operators on SSRFs.
      b.   For all site-weeks, valid hours, total available hours, and average flow values
          are redetermined from Level n validation flow data obtained from the DMC
          and compared with corresponding values in the chemistry database.
      c.   Total sample volume and atmospheric concentration [micrograms per cubic
          meter (/ig/m3)] of each analyte are calculated and compared for all filter pack
          samples with the data in the final chemistry report for the quarter.
 3.    Filter Acceptance and Chain-of-Custody Audits:
      a.   All acceptance test data for Teflon®, nylon, and Whatman filters are reviewed
          to ensure that only batches of filters which met the acceptance criteria are
          used for sample collection.
     b.   Field logsheets for selected sites for the entire quarter are reviewed  to
          determine completeness of the shipping and receiving dates for filter packs.
4.   Precipitation Field Data Audits:
     a.   Data reported on the PSRFs are compared to data in the chemistry database
          for  all wet deposition sites.
     b.   Precipitation amounts  from the RG charts are recalculated for 20 percent of
          all samples.  Collector efficiencies are recalculated when differences are
          discovered in the precipitation amounts. Audit samples are selected from those
          samples with collector efficiencies of either < 80 percent or > 120 percent.
     c.   Weekly precipitation amounts are recalculated from the RG charts for the
          entire quarter for one wet deposition site and compared to corresponding
          values on the PSRFs.
5.   QC Chart Audits:
     QC charts are reviewed to ensure that all batches and all analytes meet the
     established data quality criteria, or that appropriate corrective actions are
     implemented.
                                     19

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      6.   Life History Audits:
           The life history audit traces samples from a selected week within the quarter from
           media testing and preparation through chemical analysis to inclusion into the
           validated database. The format for this audit may vary from quarter to quarter. For
           example, it may not be necessary to audit each component of sample analysis every
           quarter.

2.2.4.3 External Audits
External QA was provided by Ogden. Ogden performed annual field, laboratory, and DMC
audits. Two types of external QA reports were prepared by Ogden. Spot reports providing
rapid feedback on sensor and system performance were submitted to QST within 72 hours of a
site audit. Monthly audit reports from Ogden contained audit data from each site, details of
problems encountered, and descriptions of recommended solutions.

2.2.4.4 Precision and Accuracy Objectives
Three separate measures of precision are produced for CDN data.  The primary assessment of
overall precision is made using collocated (i.e., duplicate) sets of equipment at selected sites.
Direct field measurements and laboratory measurements are compared the same way.  In
addition, all laboratory measurements require two assessments of analytical precision:  one to
assess sample-to-sample precision within a single analytical data batch, and one to assess batch-
to-batch precision.  Batch-to-batch precision is estimated only for filter pack analyses.
Precipitation samples undergo a series of analytical procedures for analysis of numerous
parameters and are therefore not suitable for batch-to-batch replication.

The overall precision of meteorological variables and O3 is assessed quarterly by calculating the
difference between simultaneous measurements (i.e., hourly averages) taken by separate
instruments at collocated sites. Collocated sites are selected to be representative of the
observed range of pollutant concentrations and environmental conditions that exist within the
network. The precision objectives for the CDN for field measurements are listed in Table 2-5.
The overall precision of atmospheric concentration and wet deposition data is assessed
quarterly by calculating the relative percent difference (RPD) of values for simultaneous
samples at collocated sites. Precision objectives for these variables are listed in Table 2-9.
                                            20

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The precision objectives listed in Tables 2-5 and 2-9 have been estimated from instrument
specifications, EPA data, and QST experience with similar measurements. Approximately
10 percent of CDN sites were collocated in the past. Currently, only 5 percent of the network
is collocated as adequate results on network precision were obtained during the earlier years.
The current 5 percent collocation level provides sufficient information to assess whether
precision estimates continue to meet CASTNet objectives.

Analytical precision within sample batches is assessed by calculating the RPD and percent
recovery of CVSs run hi that batch. CVSs are independently produced standards, which
approximate the midpoint of the analytical range for an analyte and are run after every tenth
environmental sample. Precision within a batch is also assessed by replicating 5 percent of the
samples within a run. Samples to be replicated are selected randomly.

Analytical precision from batch to batch for dry deposition anions and NHJ is estimated by
analyzing selected samples in two separate batches. Five percent of each batch is  selected at
random and rerun hi a subsequent batch.  Although no precision objectives have been
established for this analysis, comparisons provide a means of estimating the batch-to-batch
analytical precision.

The accuracy of field measurements is determined by challenging instruments with standards
that are traceable to the NIST.  Continuing accuracy is verified during quarterly calibration by
QST personnel and annual audits by an independent QA auditor. Accuracy objectives for field
measurements are listed in Table 2-5.
The accuracy of laboratory measurements is determined by analyzing an independently
prepared reference sample in each batch and calculating the percent recovery relative to the
target (theoretical) value. The percent recovery must meet or exceed the acceptance criteria
listed hi Table 2-9. If possible, the reference should be traceable to NIST, be obtained directly
from NIST (when available), or ordered from other laboratories. Unknown reference samples
containing SOJ" and NO^ on filter media are also provided by the EPA Project QA Officer.
Unknown reference samples provided by EPA are extracted using CDN procedures and
analyzed at the beginning and end of each 1C run.
                                           21

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2.2.4.5 Precision and Accuracy Results
Field Data
Precision statistics generated via collocated sampling efforts from 1987 through 1995 are
presented in Table 2-10. The operational time periods for each collocated site that correspond
to the precision values in Table 2-10 are presented in Table 2-11. Precision estimates hi RPD
for all meteorological parameters for all collocated sites ranged from -20.67 to 87.82 percent.
Both of these values are for delta temperature and appear high due to differences at the low end
of the Centigrade scale (0.13 versus 0.16°C, and 0.04 versus 0.02°C, respectively). The
absolute RPDs for each parameter averaged for all collocated sites are presented in Table 2-12.
Except for an RPD of 20.95 percent for delta temperature, all other RPDs are well within
CASTNet criteria, ranging from 0.63 to 9.91 (wetness). Table 2-13 presents results of
collocated sampling for the two sites collocated during 1994 as an example of results from a
typical sampling year.

Results of the external performance audits conducted by Ogden are used as an estimate of
accuracy. Table 2-14 lists by site the external audit results performed during 1994. Summary
statistics of the external audit results for 1994 are presented in Table 2-15. Of 430 sensors
audited, only 2.8 percent (12 sensors) failed to meet CASTNet accuracy criteria, and
2.6 percent (11 sensors) were within warning limits.

Except for the delta temperature and wetness sensors, the precision of the field instrumentation,
as assessed by collocated sampling, is excellent. Results for delta temperature appear highly
variable as the precision estimate of RPD magnifies the small differences at the low end of the
Centigrade scale. If the precision acceptance criteria of ±0.25°C (see Table 2-5) is directly
applied to the differences between the collocated instrument values, then all collocated delta
temperature sensors fall within the acceptance limits. Results for the wetness sensors, on the
other hand, appear relatively variable due to the fact that the sensors are difficult to align with
high precision within one hour of one another.

Accuracy of the field instrumentation as assessed by external audits is also excellent, indicating
that the continuous O3 and meteorological data are of the highest quality.
                                            22

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Laboratory Data
Filter Pack Samples
Precision results by site via collocated sampling for filter pack data from 1987 through 1995
are presented in Table 2-16 (see Table 2-11 for the corresponding operational time periods for
each collocated site). Precision estimates in RPD for all analytes for all collocated sites ranged
from -3.86 percent for SO2 to 10.59 percent for NO3. The absolute RPDs for each analyte
averaged over all collocated sites (Table 2-17) ranged from 1.56 percent for SO^ to
3.65 percent for NO3". Table 2-18 presents results of collocated sampling for the two sites
collocated during 1994 as an example of results from a typical sampling year, and Figures 2-10
and 2-11 display these results as scatterplots for SOJ", SO2, NO3, and HNO3.
Precision estimates obtained from analysis of CVS and replicate samples for 1994 (typical
project year) and for the 1987 through 1995 period (total average project precision) are
presented in Tables 2-19 and 2-20, respectively.  Precision for the CVS samples is calculated as
percent recoveries whereas precision for the  replicate sampling is calculated as RPDs. Percent
recoveries for both 1994 and the entire period for all analytes were within -1.54 percent of 100,
and the RPDs for the replicate analyses for both time periods were between 1.21 percent for
SOf (Teflon® filter) and 8.24 percent for NO3 (Whatman filter) hi batch-to-batch replicates,
and between 0.58 percent for SC# (Teflon® filter) and 3.73 percent for NO3 (Whatman filter)
for in-run replicates. As might be expected, in-run replicates exhibited greater precision than
batch-to-batch replicates. Replicate analysis results also yielded the highest standard deviations.
This is due to analysis of samples with low-level concentrations near the detection limits where
small differences hi replicate versus original values are amplified. Since samples to be
replicated are chosen randomly (i.e., "blind"), inclusion of low concentration samples could
not be avoided.
Accuracy of the filter pack sample analyses is estimated by calculating the percent recoveries of
NIST reference solutions. Accuracy estimates for 1994 and the 1987 to 1995 period are also
presented in Tables 2-19 and 2-20, respectively. Percent recoveries for both time periods
ranged from 98.47 percent for NO3" (Whatman filter) to 100.68 percent for SO|- (nylon filter).
In general, the precision and accuracy of the laboratory data are extremely high. The only
notable exceptions where precision criteria were not met occurred for NO3 species during
estimation of precision via collocated sampling.  The NO3, HNO3, and total-NO3 precision
                                           23

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values for 1987 through 1995 for collocated Site 107/207 (Table 2-16) were out of the
acceptance criteria of ±5 percent with values of 10.59, 7.90, and 8.38, respectively. It should
be noted, however, that this site was collocated for only 18 months and was one of the first
sites to be configured as such. The only other collocated site to exceed acceptance criteria was
Site 153/253 for NOj (7.61 RPD), another pioneer collocated site. Besides the fact that these
sites exhibit two of the lowest average NOj concentrations in the east with respect to other
eastern collocated sites, the high RPDs may also be reflective of configurational problems at
the sites rather than poor precision.

Precipitation Samples
Precision results by site via collocated sampling for wet deposition data from 1989 through
1995 (wet deposition sampling did not begin until 1989) are presented in Table 2-21 (see
Table 2-22 for the corresponding operational time periods for each collocated site). Precision
estimates in RPD for all analytes for both collocated sites ranged from -18.32 percent for
ammonia (NH3) to 9.82 percent for NHJ. The absolute RPDs for each analyte averaged over
all collocated sites (Table 2-23) ranged from 0.30 percent for SO|" to 14.07 percent for NHJ.
Table 2-24 presents results of collocated sampling for the two sites collocated during 1994 as
an example of results from a typical sampling year.

Precision estimates obtained from analysis of CVS and replicate samples for 1994 and for the
1989 through  1995 period are presented in Tables 2-25 and 2-26, respectively.  Percent
recoveries of CVS samples for both 1994 and the 1989 through 1995 period for all analytes
were within ±4.83 percent of 100, and the  RPDs for the replicate analyses for both time
periods were between 0.22 and 5.15 percent.  Unlike filter pack analyses, replicate analysis
results did not necessarily exhibit higher standard deviations. Precipitation samples are
replicated in sequence (i.e.,  replicate analyzed immediately after original sample)  whereas filter
pack replicates are analyzed at the end of a  batch. There can be a difference of up to 3 hours
between analysis of the original and replicate sample as well as up to 60 samples in between the
replicate and original sample.  The higher RPDs and standard deviations of the filter pack
samples may simply be reflective of instrument drift and slight changes in the 1C column
integrity.
                                           24

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Accuracy of the precipitation sample analyses is estimated by calculating the percent recoveries
of NIST reference solutions. Accuracy estimates for 1994 and the 1989 to 1995 period are also
presented in Tables 2-25 and 2-26, respectively. Percent recoveries for both time periods
ranged from 95.84 percent for Na+ to 105.35 percent for pH.  Unknown reference samples
prepared by High Purity Standards are also analyzed along with the CDN precipitation samples
as an extra internal check. The percent recoveries of these samples are also  presented in
Tables 2-25 and 2-26.
                                          25

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Chapter 3
Results and Discussion

3.1 Overview
Air quality measurements collected since the commencement of the NDDN in 1987 through the
year 1995 are presented and analyzed in this chapter. The scope of the analysis has been
limited generally to graphical and tabular presentation and straightforward statistical analyses,
which do not account for the year-to-year variations in meteorology or for quantified modeled
uncertainties. More detailed and interpretative studies will be presented elsewhere.

The results from Chapter 2 demonstrate conclusively that the observed changes in
concentrations shown in the figures and tables in this chapter are real and not the result of
modifications to field and analytical protocols or of data imprecision or inaccuracy. The few
changes in sampling and analytical procedures have been assessed and have been shown to
have had a positive or neutral effect on data quality. The CASTNet QA/QC program has
demonstrated the accuracy and precision of the measurements. Concentration reductions are the
result of changes in emissions and of meteorological fluctuations, not of changes in the
network.

Concentrations measured on the CASTNet filter packs  are presented first. Concentration data
are given in terms of annual and quarterly averages,  summer (June through August) and winter
(December through February) levels and various scattergrams and time series. Linear
regressions of annual, summer and winter values versus year are shown to ascertain any
statistically significant trends in concentrations.

The multilayer model (MLM) used to calculate deposition velocities from meteorological
measurements and various land-use data is described. Example calculations hi terms of time
series of weekly average deposition velocities are presented for several sites.
Dry depositions (fluxes) are calculated as the product of weekly average deposition velocities
and concentrations. Annual average depositions and time series of weekly deposition rates are
presented. Depositions are compared to concentrations. The deposition data are analyzed for
trends.
                                           26

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Precipitation chemistry and precipitation rates are measured at 21 CASTNet sites (18 eastern).
Pollutant concentrations in precipitation and wet deposition rates are calculated. These data are
combined with data from certain NADP sites located near CASTNet sites to assemble tables
and maps of annual, seasonal, and quarterly average depositions and concentrations. These data
are analyzed for trends.

Dry and wet deposition data are combined to estimate total deposition of sulfur and nitrogen
species. Annual and seasonal averages are presented by year and by region. Total deposition
rates are analyzed for trends.

O3 measurements are then presented and discussed. The O3 data are used to provide estimates
of various exposure statistics and to assess compliance with current and proposed air quality
standards. The data are also used to analyze the effects of terrain and other site characteristics
on O3 concentrations.

The MADPro is then discussed. Concentrations in rain, cloudwater, and ambient air are
compared.

Data from the CASTNet Visibility Network are presented. The section begins with a
description of the network, instrumentation, and operations. An initial analysis of the visibility-
related air quality measurements is presented. The year 1994 was selected for the analyses and
presentations. Annual concentrations of fine particles and their chemical constituents are
shown, and seasonal variability is also discussed. Time series of 24-hour average fine particle
concentrations and the chemical constituents are presented. Relationships between fine particle
concentrations and SOf" concentrations and between atmospheric light scattering coefficient
(Bscat) and fine particles and SO^ are discussed. Finally, photographs of scenic vistas at the
Arendtsville site are contrasted for high and low SO^ days.

Chapter 3 also provides example results from other studies sponsored by CASTNet. Brief
descriptions are given of the mobile monitoring system used to measure directly dry deposition
fluxes and comparisons between denuder and filter pack measurements.
                                           27

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3.2 Air Chemistry and Dry Deposition
The emphasis of CASTNet has been the measurement of ambient concentrations of sulfur
species (SO2 and SO4'), nitrogen species (HNO3, NO3, and total NO3), NHJ, and O3, which is a
product of the photochemical reactions among NOX and reactive organics. Precursor emissions
are transported by the wind, mixed by atmospheric turbulence, undergo dry and wet
deposition, and are transformed to other species by chemical processes. A simple, linear model
of the change in SO2 and SOl~ concentrations is shown in Equations 3-1 and 3-2.
dC2        dC2
	 = -u  	
  dt
                                                                             (3-1)
    dt
             _*--£-(£; —1
              dx     dz   z dt
                                                                             (3-2)
The two equations represent the various atmospheric processes that produce changes in SQ2 and
SO^. SO2 is represented by C2 and SO^ by C4 in the two equations. The first two terms
represent advection and turbulent mixing. The terms kD2C2 and kD4C4 represent the dry
deposition of the gas SO2 and aerosol SO4". The two terms kw2C2 and kw4C4 represent the
scavenging of SO2 and SO4" by precipitation. The term kjC2 represents the conversion of SO2
into SO4". It represents a loss of SO2 in Equation 3-1 and a gain of SO4" in Equation 3-2. The Q
term represents emissions. The concentration terms are three-dimensional. The other
parameters are a function of both space and time. The production of HNO3 and NO3 from NOX
emissions can be represented by similar, but more complicated (i.e., with nonlinear chemical
reactions), equations.
Equations 3-1 and 3-2 provide a simple framework in which to consider the results presented in
this chapter. For example, SO2 and SO4~ are lowered by dry deposition processes (the third
terms in the two equations) and by precipitation scavenging (the fourth terms). The terms kD2
and kD4 are related to deposition velocities (discussed in Section 3.2.2) and vary with space and
time (e.g., seasonally and diurnally). The production of SOI' from SO2 is simulated as a linear
transformation process. In reality, the transformation processes are nonlinear and are controlled
by complex photochemical processes. Sophisticated models like the Regional Acid Deposition
                                          28

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Model (RADM) (Dennis et al., 1993) simulate the highly nonlinear chemical transformations.
However, the k, term captures the essence of the production of SO|" in that SO^ is produced
directly from SO2 and the transformation varies with space and time (e.g., higher
transformation associated with summertime photochemical processes).

Concentrations are measured directly throughout the eastern and western networks. Dry
depositions are estimated as the product of concentrations and modeled dry deposition
velocities. Concentrations and dry depositions are discussed hi detail in this section of the
report. Wet deposition is measured at 21 CASTNet sites. Wet depositions are discussed hi
Section 3.3. The CASTNet wet deposition measurements are combined with wet deposition
data from NADP to provide geographic coverage of the eastern subregions. The dry and wet
deposition data are summed hi Section 3.4 to obtain information on total deposition. O3
concentrations are discussed separately in Section 3.5.

3.2.1  Concentrations
3.2.1.1 Six-Year and Annual Average  Concentrations
Sulfate
Figure 3-1 shows annual average SO^ concentrations  averaged over the 6-year period 1989 to
1994.  This period was selected because of its extensive and relatively complete data record.
Figure 3-2 shows SO2 emissions (EPA,  1996) for the  same period. The map of concentrations
represents a regional-average, 6-year exposure to SO^ that is produced by the SO2 emissions,
remembering that the CASTNet measurements were taken to characterize regional, rural
conditions. The monitoring sites were situated to avoid individual point sources and groups of
sources and to represent regional air quality.

Six-year average concentrations above 6.0 /ug/m3 were observed from southwestern Indiana to
northern Alabama across central Pennsylvania, reflecting the geographic distribution of large
emitters along the Ohio river. The highest value of 6.7 /ug/m3 was measured at several sites.
Most of the eastern portion of CASTNet measured concentrations above 4.0 /ug/m3, with a
sharp decrease in New York and New England.

The measurements at the western sites ranged from 1.4 to 0.7 /*g/m3.
                                          29

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 To assess variability in annual averages, maps of annual SOI concentrations for the years 1989,
 1992, and 1994 are presented in Figures 3-3 through 3-5. Similar concentration patterns were
 observed in the 3 years with the highest measured values in 1989. Only a few values above
 6.0 //g/m3 were measured in 1992. A larger region and more sites with values above 6.0
 are shown on the 1994 map. A discussion of geographic averages and trends in SQ% is
 provided later in Section 3.2.5.
Sulfur Dioxide
Average SO2 concentrations from 1989 to 1994 are given hi Figure 3-6. A broad area of values
above 10 A*g/m3 extends from southern Illinois to western New York, again reflecting the
distribution of SO2 sources in Figure 3-2. Annual averages for 1989, 1992, and 1994 are given
in Figures 3-7, 3-8, and 3-9, respectively. Fairly similar patterns of higher SO2 levels were
observed from year-to-year, although the number of sites with high levels and the magnitude of
the peak observations decreased from 1989 to 1994.

Nitrate
Figure 3-10 shows the 1989 to 1994 average NO3 levels for the CASTNet. Figure 3-11 shows
NOX emissions for the same period. Six-year average NO3~ concentrations are more variable
spatially than SQ% with the highest levels measured hi the Midwest. The pattern of observed
NO3 is not as well correlated with the distribution of NOX emissions as was SO2 and SO|". For
example, NOX emissions in the Southeast are about the same magnitude as in the Midwest, yet
NO3" levels  are significantly lower. In short, the highest NO3 were observed in the agricultural
area of the  Midwest. This suggests two potential mechanisms for NOj formation, including the
gas-phase reaction between  HNO3 and NH3 and gas-particle reaction of HNO3 with soil
particles. Although both reactions are likely in agricultural areas, the apparent spatial
correlation  between NHJ and NOi levels (see Section 3.2.1.4) provides evidence that the first
mechanism may be more important.
Six-year average NO^ concentrations show little variability across the western sites. Measured
averages are all below 0.6
                                          30

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 Annual average NO3- values for 1989, 1992, and 1994 are illustrated in Figures 3-12 through
 3-14, respectively.  Nitrate values show extensive geographic variability but little yearly
 change.

 Ammonium
 Six-year average NHJ concentrations are shown in Figure 3-15. In general, higher
 concentrations were detected at agricultural sites, rather than forested sites. Measured NHJ
 concentrations are less than or equal to 0.5 Aig/m3 throughout the western network.

 Annual average levels of NHJ for 1989, 1992, and 1994 are given in Figures 3-16 through
 3-18, respectively. The annual patterns are similar, and higher concentrations were generally
 measured in 1989.
 Nitric Acid
 HNO3 concentrations averaged from 1989 to 1994 are shown in Figure 3-19. In general, the
 data show little spatial variability except in the northern and southern extremes of CASTNet
 and in the Appalachians. The effects of complex terrain on site exposure, local photochemistry,
 and dry deposition could explain some of the spatial variability. This topic is explored later in
 this chapter. Concentrations observed across the western sites range from 0.9 to 0.3 ftg/m3.

 Annual HNO3 levels for 1989, 1992, and 1994 are given in Figures 3-20, 3-21, and 3-22,
 respectively.  The concentration patterns are similar from year to year and to the 6-year
 average distribution.  Lower concentrations were measured in 1992. The highest annual
 average was routinely measured in southeastern Pennsylvania.

 Total Nitrate
 The 6-year composite map for total NO3' is shown in Figure 3-23. The data show considerable
 spatial variability among the sites in the eastern network. Total NO3 levels are influenced by
 complex terrain effects at the higher elevation sites and by the availability of paniculate NO3 hi
agricultural areas. The higher values were observed in the Midwest and eastern Pennsylvania.
Values at western sites range from  1.2 to 0.5 /wg/m3. Annual maps of total NO3- for 1989, 1992,
and 1994 are shown hi Figures 3-24 through 3-26, respectively. Annual patterns are similar
from year to year. The highest values were measured hi 1989.

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Summary of Annual Averages
As discussed earlier, one of the objectives of the CASTNet is to detect trends in air quality
measures in response to changes in emissions. Tables 3-1, 3-2, arid 3-3 list annual average
concentrations for six air quality parameters (two each table) for the years 1987 through 1995.
Annual levels are provided for each CASTNet subregion and for all eastern and western sites
combined. A site had to have data for 26 weeks during a year to be included in this table.

The data for the eastern sites combined show a 23-percent reduction in SOJ" and a 43-percent
reduction in SO2 between 1989 and 1995 annual concentrations. These values do not account
for the variations hi concentrations between 1989 and 1995. Changes in sulfur species are more
pronounced in the four northern subregions and smaller, but still substantial, hi the  two
southern subregions. There is no apparent trend in the data from the western sites. The eastern
data indicate about 70 percent of ambient sulfur is hi the form of SO2. Throughout the western
network SO2 represents about 55 percent of the  ambient sulfur.

As shown in Table 3-3, HNO3 and total NOj concentrations averaged over the eastern sites
show little change over the monitoring period, with perhaps a 5-percent reduction hi total  N0§>
HNO3 concentrations show a downward trend in three of the subregions.
 Concentrations averaged over the western network are all less than 1.0 /^g/m3. There is sorne
evidence of a reduction in total NOi with a decrease to 0.69 /ug/m3 from the 1989 average of
0.85 /J.g/m?. Nitric acid contributes about 65 percent of ambient nitrogen throughout the
network.
3.2.1.2 Quarterly Average Concentrations
Time series of quarterly average concentrations of SO2 and SOJ" are given in Figures 3-27 and
3-28, respectively, for Sites 109 (Woodstock, NH) and 120 (Horton Station, VA). Despite
large concentration differences, seasonal patterns are similar between sites and between years.
SO2 levels are the highest hi the whiter and fall and drop off markedly in spring and summer.
Sulfate values rise during the spring, peak in summer and reach minimum levels hi fall and
whiter. SO2 emissions are typically high hi the whiter and summer, reflecting heating and air
conditioning demands. The photochemical production of SOJ" hi summer corresponds to a tune
with high emissions. With little photochemical activity hi the cold months SO2 emissions
produce the highest ambient SO2 concentrations.
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 3.2.1.3  Summer and Winter Averages
 To illustrate further seasonal behavior, Figures 3-29 through 3-40 present time series of
 summer (June through August) and winter (December through February) averages for the six
 filter pack measurements (i.e., SO|% SO2, NO;, NH}, HNO3, total NO;) for five eastern and
 three western sites. Figures 3-29 through 3-34 show the summer and winter averages for the
 eastern sites. Similarly,  Figures 3-35 through 3-40 show the summer and winter averages for
 the western sites. The 1989 winter averages represent the period December 1988 through
 February 1989 and so forth for subsequent years.

 Summer SOf concentrations show considerable year-to-year variability (i.e., typically
 20 percent or more) throughout the eastern network. Summer SO^ at the western sites is less
 variable and fairly low in concentration. Whiter SO|- shows little annual change throughout the
 east and is typically less than 3.0 or 4.0 Mg/m3. Whiter SC# in the west is typically less than
 1.0 Mg/m3.  During four of the seven years,  SO^ levels are higher in the winter than the
 summer at Site 168 (Glacier NP).

 Winter SO2 levels are about a factor of 2.0 higher than  summer levels and exhibit considerable
 annual variability among the eastern sites. The Woodstock, NH site (109) and the Sumatra, FL
 site were exceptions and measured very low SO2 concentrations with almost no year-to-year
 change.  With the exception of Glacier NP, MT, SO2 levels were higher in the whiter at the
 western sites.

 The year-to-year variations in measured summer and whiter average SO^ and SO2
 concentrations are consistent with regional (e.g., RADM) modeling studies which simulate 20-
 or 30-percent changes from year to year. Even point source modeling studies, assuming
 constant  emissions, result hi 20- to 30-percent variability at a model receptor location over a
 5-year simulation period because  of fluctuations hi meteorological conditions.

 Ammonium and HNO3 concentrations are generally higher in the summer throughout
 CASTNet. Woodstock,  NH, and Sumatra, FL, are exceptions hi that there is little difference
between summer and whiter levels. Similarly, HNO3 measured at Glacier NP, MT, shows
 little summer-whiter variability.
                                          33

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Total NOs levels do not vary much between winter and summer at the eastern sites.  Observed
summer total NO^ concentrations are higher in summer in Arizona and Wyoming, but lower at
Glacier NP, MT.
3.2.1.4 Ammonium Versus Sulfate
Data for the CDN sites suggest regional variability in aerosol speciation as well as
concentration. This is illustrated in Figure 3-41, which shows the relationship between NHJ
and SO2' (molar basis) for each CDN site using annual average concentrations for 1991 as an
example.  Similar relationships were observed for other years. Solid and dashed lines are also
plotted in this figure to depict 1:1 and 2:1 ratios of NHJ to SO2,', respectively. The 2:1 line
represents completely neutralized SO2;', and the 1 : 1 line represents 50-percent neutralization of
SO2)', assuming that only NHJ  and SO2; are present in the aerosol phase. Other aerosol species
are undoubtedly present and, therefore, ratios represent only approximate levels of
neutralization.

Results show that the majority of eastern sites fall between the 50-percent and 100-percent
neutralization lines and that the western sites scatter around the 100-percent neutralization line.
Inspection of Figure 3-41 also  shows a small number of eastern sites on or above the
100-percent neutralization line and a small number of sites only slightly above the 50-percent
neutralization line. The highest NHJiSO2,' ratios all correspond to agricultural sites in the
midwest and upper midwest. The lowest ratios of NHJ iSO2,', in contrast, all correspond to sites
in predominately  forested areas of the southeast and northeast.
Although filter pack data cannot be used to quantify aerosol acidity, these results suggest broad
qualitative differences in aerosol acidity. For agricultural sites in general, there appears to be
sufficient NHJ to completely neutralize SO2.'. For forested sites at significant distances from
agricultural activity, observed SO2' must be balanced by other cations in addition to NHJ. The
metal cations Na+, K+, Ca2+, and Mg2+ were measured in CDN filter pack samples during
1989 (ESE, 1990c).  Results showed that Na+, K+, Ca2+, and Mg2+ were minor aerosol
constituents at all sites except those in the midwest or near the coast (Sites 104, 116, and 156).
On the whole, these data show that aerosol composition varies from region to region and
suggest that aerosol acidity may be greater at predominantly forested sites then at
predominantly agricultural sites.
                                           34

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 3.2.1.5  Trend Analysis
 The 1970 Clean Air Act (CAA), the Amendments of 1977, and the 1990 Amendments have
 produced reductions in SO2 and NOX emissions over the last two decades Specifically, the 1990
 Act called for a 10-million tons per year reduction in SO2 emissions relative to 1980 emissions.
 EPA (1997) has estimated that SO2 emissions were actually reduced by 13 percent in 1995 as
 the result of CAA requirements. EPA has also calculated a 22-percent reduction in nationwide
 SO2 emissions over the period 1989 to 1995, a 25-percent reduction in SO2  emissions in the
 eastern United States over the same period, and a 24-percent reduction in electric utility SO2
 emissions. Without taking into account year-to-year variability, CASTNet data from the eastern
 sites show a 43-percent reduction in SO2 concentrations, a 23-percent reduction in SO^ levels,
 and a 38-percent reduction in ambient sulfur between 1989 and 1995 (Table 3-1). Figures 3-42
 and 3-43 show the measured percent reduction in annual concentrations of SO2 and SOI',
 respectively,  from 1989 through 1995. Reductions are provided for individual sites and for
 subregional averages. The highest percent reductions for both SO2 and SOft were observed for
 the upper midwest and upper northeast subregions. Reductions were observed for all
 subregions.

 CASTNet has measured significant reductions in concentrations of sulfur species.  Are those
 reductions related to changes  in SO2 emissions or natural meteorological variability, or both?
 Although detailed statistical analyses are beyond the scope of this project, a few analyses have
been performed to address the question. EPA (1997) has started detailed analyses of the
 relationships between emission changes and air quality and has developed nonlinear statistical
models to detect trends in ambient sulfur and nitrogen species.

The initial statistical analyses presented herein are simple linear regressions. Although they do
not differentiate between emission changes and meteorological fluctuations,  linear regressions
can assess the statistical significance of the observed trends, whatever their cause. Figure 3-44
shows  linear regressions based on annual average SO2 concentrations versus year for the entire
eastern network. The figure shows statistically significant reductions in SO2 averages at better
than 95-percent confidence (p^O.05). Similarly, linear regressions for annual SQfc levels are
shown in Figure 3-45. The results show statistically significant reductions in SO£ since 1989.
                                           35

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Linear regressions were also calculated for the six eastern subregions and for the western data.
Calculations were made for annual, summer, and winter average concentrations of SO2 and
804" (see Tables 3-4 and 3-5). The reductions in annual SO2 are considered statistically
significant for all six eastern subregions. The annual data for the western network did not show
a statistically significant trend. The regressions based on the summer average SO2
concentrations show statistically significant reductions for five subregions, all except the
southern periphery and the west. The reductions in winter SO2 are considered statistically
significant for four of the seven subregions.

For SOf, me reductions are considered significant for all seven subregions on an annual basis.
The summer regressions show statistically significant reductions for five subregions and
inconclusive results for northeast and midwest, although the p-values for these two regions are
only slightly above 0.05,  the value indicative of results at the 95-percent confidence level. The
reductions in winter are considered statistically significant for two subregions.

Linear regressions were also performed on annual average HNO3, NOj, and total NOj
concentrations collected from 1987 through  1995. The results for all eastern sites combined are
shown in Figures 3-46, 3-47, and 3-48. The results show a slight reduction in HNO3 levels
which is considered statistically significant. No  significant trends  are shown for NO3" and for
total NOj.

3.2.1.6 SURE Data
The analysis of trends for SO^" concentrations can be extended by incorporating measurements
taken in 1977 and 1978 during the Sulfate Regional Experiment (SURE) (Mueller etal., 1983).
Schreffler and Barnes (1996) recently used the SURE data and measurements from the Acid-
MODES/OEN Network (Heisler et al., 1992) to demonstrate a statistically significant reduction
in SOI' over the period 1978 to  1989.
Table 3-6, which was adapted from the Schreffler and Barnes (1996) paper, shows 1978 annual
average SOI" concentrations taken from the SURE Class I Network. The table also lists the five
CASTNet sites that are located nearest the SURE stations. Figure 3-49 shows linear regression
plots for Sites 144, 114, 140, 133, and 120 using the SURE and CASTNet data. The analysis
shows average percent reductions in annual SOI' °ver me period 1978 to 1995 from 35 to
                                           36

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 50 percent. The results are statistically significant at the 99-percent confidence level for all five
 sites.

 3.2.1.7  Summary of Trends in Concentrations
 The CASTNet measurements show statistically significant reductions in SO2, SO|% and HNO3
 concentrations averaged over all eastern sites. SO2 concentrations show significant reductions in
 summer and whiter seasons, even though concentrations are much higher in winter. The
 downward trends have been measured consistently across the eastern network, except for the
 subregion called the southern periphery. The sites hi this region are less influenced by source
 groups and, hence,  less influenced by change in SO2 emissions. No trend is evident hi the
 western data.
The downward trend in SO|" has been observed consistently across all eastern sites. The decline
in summer average SOf levels explains the decline in annual averages. Sulfate peaks hi the
summer because of active photochemical reactions that transform SO2 into SO|". Extending the
trend analysis by including the 1978 SURE measurements reinforces the demonstration of a
significant downward trend in
The reduction in HNO3 concentrations results from the decline in summer averages. The
downward trend is observed hi all of the subregions, except for the southern periphery and the
west. No trends are observed hi annual concentrations of NOj and total NO3 averaged over the
eastern and western networks.

3.2.2 Calculation of Deposition Velocities
CASTNet was designed to use meteorological measurements and information on land use,
vegetation, and surface conditions to calculate dry deposition velocities for each filter pack
measurement and O3. The meteorological and O3 data are recorded continuously and archived
as hourly averages. The filter pack measurements give weekly concentrations.  Site operators
survey major plant species and land use within 1 km of each monitoring station. They also
record the presence of dew, frost and snow. Weekly vegetation information is also recorded.
The LAI was surveyed at each site during periods of maximum leaf out during the summers of
1991 and 1992.
                                          37

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3.2.2.1 Deposition Model
The network design was based on the assumption that dry deposition or flux could be estimated
as the linear product of ambient concentration (C) and Vd:
                                                                                   (3-3)
where the overbars indicate an average over a suitable time period (Chamberlain and
Chadwick, 1953).
The influence of meteorological conditions, vegetation, and chemistry is simulated by Vd.  Dry
deposition processes are modeled as resistances to deposition (Hicks et al.,  1985):
                                                                                   (3-4)
R,, the aerodynamic resistance, is inversely proportional to the atmosphere's ability to transfer
material downward from the planetary boundary layer to the surface layer by turbulent
processes. Rb is the boundary layer resistance to vertical transport (molecular diffusion) through
a shallow (approximately  1 millimeter) nonturbulent layer of air in direct contact with the
surface.  Rb depends on the aerodynamics of the surface and the diffusivity of the pollutant
being deposited. R,., the canopy or surface uptake resistance, contains several terms
(represented as parallel resistances) that account for the direct uptake/absorption of the
pollutant by leaves, soil, other biological receptors within  and below the canopy, and other
surfaces such as rock and water. R. contains parameterizations for vegetation type and density*
solar radiation penetration of the canopy and wetness  of the surface. Rc is difficult to treat
theoretically, and the system of equations for estimating R,, is normally empirically adjusted
based on direct  observation of dry fluxes. Figure 3-50 illustrates the resistance model of dry
deposition.
For pollutant species with low solubility or reactivity, such as O3 and SO2, the controlling
component of RC is the stomatal resistance, which has large diurnal and seasonal variability.
For highly reactive species such as HNO3, R,. is generally small, regardless of season of canopy
type, and R, and Rb control Vd.  Deposition of the particle species 804"  and NOj is primarily
governed by turbulent processes and is represented in the model as a function of R^
                                            38

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 Using this physical and mathematical framework, two dry deposition models (Big Leaf and
 MLM) have been used to calculate dry deposition for CASTNet. Both models were developed
 by NOAA Atmospheric Transport and Diffusion Division, Oak Ridge, TN. The Big Leaf
 model (Hicks et al., 1985) treats the vegetation canopy as a one-dimensional surface. Big Leaf
 model results, aggregated to seasonal and annual averages for 1991, have been reported by
 Clarke and Edgerton (1993). The MLM is a variation of the Big Leaf model wherein similar
 calculations are applied through a 20-layer canopy in which model parameters are modified by
 the redistribution of heat, momentum, and pollutants (see Figure 3-50). The MLM also
 accounts for water stress on the vegetation and deposition to snow surfaces. Additionally,
 several parameters (e.g., soil resistance) have been modified in the MLM from those used in
 the Big Leaf model. While the MLM is a significant technical improvement over the Big  Leaf
 model,  seasonal and annual fluxes calculated by the two models do not differ greatly. Dry
 deposition calculations for the CASTNet sites  (and the results reported here) are currently made
 using a version of the MLM (Meyers et al., 1991).

 The MLM requires the following input data: wind speed, wind direction, sigma theta,
 temperature, relative humidity, solar radiation, surface wetness, LAI, vegetative species,  and
 percent green leaf-out.

 The meteorological variables used to determine Ra, Rb, and Rc are obtained from the 10-m
 meteorological tower at each of the sites, normally located in a clearing over grass or another
 low vegetative surface. Data on vegetative species and percent green leafout are obtained  from
 site surveys and observations by the  site operator. LAI measurements were taken during 1991
 and 1992 at times of summer maximum. LAI values that are used in the MLM are extrapolated
 from the 1991 and 1992 measurements using percent leafout observations. The resistance  terms
 (Ra, Rb, and RJ are calculated for each chemical species and major vegetation/surface type
every hour. The Vd for a site is then calculated as the area-weighted Vd over vegetation types
within 1.0 km of the site. Hourly Vd values are then averaged over a week and multiplied by
the weekly integrated concentrations to produce weekly fluxes of HNO3, SO^, NO^, NHJ and
SO2. O3 flux is calculated using hourly O3 measurements and hourly Vd values. Weekly flux
calculations are considered valid if more than 70 percent of hourly Vd values are available for
                                          39

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that week. Weekly values were aggregated to seasonal averages if 10 of 13 weeks are valid.
Seasonal averages are aggregated to annual only if all four seasons are valid.

3.2.2.2 Model Uncertainties
Uncertainties in MLM calculations can be considered in the context of the model formulation,
input errors, and representativeness. The MLM itself is an imperfect representation of the large
number of complex atmospheric processes that the model simulates. Consequently, the MLM
calculations will never be able to match perfectly observed deposition velocities. Instrument
errors  and incomplete or inaccurate characterization of other input data (e.g., percent green
leafout or LAI) produce uncertainties in model calculations. Extrapolation of deposition
velocities calculated for specific  CASTNet sites to larger regions may result in additional
uncertainties.
Some MLM uncertainties are discussed briefly in this section to provide context to the
calculated deposition velocities.  EPA investigators (Clarke et al, 1997) are currently
evaluating the MLM in considerable detail. Results of these evaluations, sensitivity studies and
statistical studies will be published elsewhere.

The MLM formulation is based on the assumption that covariance between C and Vd is zero
over the appropriate sampling time (i.e., the right-hand term in the following equation is zero):
                    Flm=Vd*C+v'd*c'
(3-5)
 where the overbar indicates a weekly or hourly average.

 The first term on the right-hand side is the product of the weekly average Vd and C (i.e.,
 weekly flux, as calculated in the CASTNet). The second term on the right-hand side represents
 the covariance (correlation) between hourly concentrations and hourly deposition velocities.
 This term was assumed to be small, and thus ignored, in the formulation of the dry deposition
 model. Depending on its sign, the correlation may increase or decrease flux. There is evidence
 that the correlation between Vd and C may be large and positive under certain conditions.
 Meyers and Yuen (1987), using fall and winter data for a forested site near Oak Ridge, TN,
 found that the product of weekly average  SO2 and weekly average Vd provided a reasonable

                                            40

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 estimate of flux relative to that calculated using hourly concentration and hourly Vd. In
 contrast, Matt and Meyers (1993) suggest the correlation term could be as large as 40 percent
 for SO2 during the summer months at the same site. The MLM may, therefore, underestimate
 annual SO2 fluxes at Oak Ridge by about 20 percent, considering the whiter and summer results
 together.
 The potential effect of the covariance term on the CASTNet dry deposition calculations
 specifically was assessed through an analysis of CASTNet data collected over a 21-month
 period from 1987 to 1989 when the network collected weekly integrated filter packs for
 separate daytime and nighttime periods. Fluxes were calculated as:
     Fluxl  = Vd (day) * C (day) + Vd (night) * C (night)
               Flux2 = V (week) * C (week)
(3-6)
(3-7)
The ratio Flux2/Fluxl was calculated for each week of available data, and averages and
standard deviations were calculated by species and month (see Clarke and Edgerton, 1993, for
additional details). For SO2 and HNO3, calculating flux by Equation 3-7 (CASTNet approach)
resulted in underestimation of the flux relative to Equation 3-6. The underestimate, averaged
over the network, is about 5 to 15 percent (winter-summer range) for SO2 and 5 to 20 percent
for HNO3.
As part of CASTNet, EPA has sponsored a program to measure directly dry deposition fluxes
at selected sites (see Section 3.9 of this report).  Field studies have been completed in eight
locations since 1994. The data from these field studies provide a mechanism for the direct
evaluation of the MLM simulations.  Perhaps the most comprehensive databases for evaluating
the MLM are available from field experiments at Bondville, IL (Site 130) during the summer
and fall of 1994, at Sand Mountain, AL (Site 152) during the late spring of 1995, and at
Keysburg, KY (near Nashville) during the summer and fall of 1995. An example evaluation is
shown in Figure 3-51 which provides a comparison of MLM simulations and field
measurements of Vd for O3 at Bondville and Keysburg. The comparison shows that MLM
underestimates Vd. In general, the MLM tended to underestimate Vd, especially during foliated,
summertime conditions.
                                          41

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Apart from the uncertainties discussed previously, there can be significant spatial variability in
dry deposition. The Vd reported for the CASTNet are areal averages representative of a 1-km
radius surrounding the CASTNet site. Dry deposition may vary spatially due to variability in
concentration and Vd. To minimize these effects, site-selection criteria emphasized uniform
terrain and vegetation, as well as large distances from sources of pollutants. These siting
criteria, however, cannot always be achieved.
Data from a site in southwestern North Carolina provide an interesting example of spatial
variability in both concentration and Vd. The Coweeta, NC site (Site 137) is located in a valley
about 300 m below and within 1,000 m of a satellite site, specifically located to study the
effects of terrain on dry deposition. Concentration measurements for SO^, SO2) and HNO3
from the ridge site between June and December 1991 average 1.3, 2.6, and 2.5 times higher,
respectively, than for the valley site. It is believed that these differences are primarily due to
deposition under a shallow boundary layer characteristic of the valley site. Deposition velocity
for the ridge-top site averaged 1.1,  1.2, and 1.7 times higher for SO;;', SO2, and HNO3,
respectively, than at the valley site, reflecting the higher levels of turbulence  normally observed
at higher elevations. Using the product of concentration ratios and Vd ratios as a first
approximation of flux ratios, fluxes are about 1.4, 2.9, and 4.4 times higher at  the ridge site for
SOJ", SO2, and HNO3, respectively. Although this may be an extreme example, it shows that
the scale of representativeness of a site may be quite short, especially in areas of complex
terrain.
A concept of MLM uncertainty is evolving based on the comparisons of modeled Vd for O3 and
SO2 with the direct measurements, other studies reported hi the literature, and the various
uncertainty analyses. The MLM results tend to underestimate observed deposition velocities for
SO2 and O3, especially daytime values during the periods of plant growth. The uncertainty is
higher for periods of rapid plant growth. The results for HNO3 and aerosols suggest that the
uncertainty is higher because of the variability in windspeed and sigma theta.

Extrapolation of deposition velocities calculated for a specific CASTNet site to other locations
should be done with caution, especially in areas of complex terrain.
                                           42

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3.2.2.3 Modeled Deposition Velocities
Annual average deposition velocities for SO2 and HNO3 are given by subregion in Table 3-7,
and for O3 and aerosols (SO^, NO^, and NHJ) in Table 3-8. Vd for SO2 is typically about
0.32 centimeters/second (cm/sec). The variability among subregions and from year-to-year is
about 15 to 20 percent. The deposition velocity for HNO3 averages about 1.7 cm/sec for the
eastern sites and about 2.3 cm/sec for the western network.  The annual and subregional
variability is about 50 percent. The Vd for O3 averages about 0.17 cm/sec throughout the
eastern network and about 0.12 cm/sec in the west.  The deposition velocity for particles is
about 0.1 cm/sec for the eastern sites and about 0.16 cm/sec for the west.

The weekly variability of SO2 Vd is shown for four sites for 1994 in Figure 3-52.  The four
sites represent a range in land-use characteristics hi West Virginia, Virginia, Ohio, and Illinois.
The West Virginia site is hi forested, complex terrain.  The Virginia site is a forested
mountaintop site. The site at Oxford, Ohio is located at Miami University, 50 km northwest of
Cincinnati.  The site is characterized as  rolling, agricultural. The Illinois site is a flat terrain
site hi the corn belt.  The deposition velocities hi Figure 3-52 show about a factor of 2,0
increase from the whiter to the 3-month period of June to August. The mountaintop site shows
the highest values which are slightly higher than the two rolling terrain sites.  The flat terrain
site experiences the lowest deposition velocities.

The deposition velocities for HNO3 shown in Figure 3-53 show somewhat less of a whiter-
summer contrast than for SO2. The weekly variability is greater; and the mountaintop site
experiences the highest velocities although only during the fall are the values significantly
higher than the Ohio site. Again, the flat terrain site in Illinois experiences the lowest
deposition velocities.

Figure 3-54 illustrates deposition velocities for particles for the four sites.  The data suggest
peak velocities hi the late spring and fall. The highest values are simulated for the rolling
agricultural site  hi Ohio and the lowest values for the complex  terrain site hi West Virginia.
Weekly variability is as high as a factor of 2.0.
The O3 deposition velocities (Figure 3-55) show a strong summertime peak with more than a
400-percent increase over winter values. The flat terrain site hi Illinois shows the lowest
                                           43

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values.  There is little weekly variability other than the sharp gradients in the spring and fall.
The distributions are virtually flat from November through March,

3.2.3 Dry Deposition Patterns and Trends
3.2.3.1 Annual Depositions
Sulfur Species
Table 3-9 presents annual dry depositions in kilograms per hectacre (kg/ha) of SO2 and SOJ", all
expressed as sulfur (S), averaged by subregion for the years 1987 through 1995. The highest
depositions were measured in the northeast and midwest subregions; the lowest were measured
at the upper northeast sites. The data for the eastern sites combined show a 29-percent
reduction in deposition of SO2 (as S) from 1989 through 1995, and only a (3-percent reduction
in deposition of SO^'. These percentage reductions in depositions are lower than comparable
reductions in concentrations that were discussed in Section 3.2.1.1. The calculated reduction in
total sulfur is 27 percent. The eastern data indicate about 85 percent of sulfur deposition is in
the form of SO2. Changes in sulfur depositions are more pronounced in three (northeast, upper
northeast, and upper midwest) of the six eastern subregions although still significant in the
other three subregions.  Despite the low average in 1995, there is no apparent trend in the data
from the western sites. Throughout the western network, SO2 deposition represents about 65 to
70 percent of total sulfur deposition.

To  illustrate variability in annual dry depositions, maps of annual fluxes of total sulfur for the
years 1989, 1992,  and 1994 are presented in Figures 3-56 through 3-58. The distribution of
sulfur deposition is similar from year to year with an area above 6.0 kg/ha, extending from
southwestern Indiana across central New York. The map of sulfur depositions corresponds well
with the maps of SO^ and SO2 concentrations discussed in Section 3.2.1 and reflects the
distribution of SO2 sources shown in Figure 3-2. Peak depositions are estimated for eastern
Ohio and western Pennsylvania. Sharp gradients are observed across northern New England
and the upper Midwest. Values above 3.0 kg/ha are observed as far south as Georgia Station
(Site 159), but decrease to about 1.0 kg/ha on the Florida panhandle.

Average sulfur depositions for the western sites are less than 1.0 kg/ha, except for Chiricahua,
located in southeastern Arizona.
                                           44

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 Nitrogen Species
 Table 3-10 lists annual dry deposition rates of HNO3 and NO3. The HNO3 and NO3- fluxes are
 expressed as nitrogen.  The highest regional average HNO3 depositions were measured hi the
 northeast and midwest subregions in 1994. The highest depositions of NO3 are consistently
 measured in the midwest.  Total nitrogen deposition, on a regional average basis, is highest in
 the northeast.  The data averaged over all eastern sites show an increase of about 17 percent hi
 HNO3 and total NO3 depositions with no change hi deposition of NO3.

 Figures 3-59 through 3-61 show maps of annual average dry depositions of total  nitrogen for
 1989, 1992, and 1994.  Most of the sites hi the eastern network, except along its periphery,
 show depositions above 2.0 kg/ha for all 3 years.  Depositions for sites  along the  Appalachian
 chain are also less than 2.0 kg/ha, showing the influence of complex terrain on atmospheric
 nitrogen species. In general, patterns are similar from year to year, although hi  1994 the areal
 coverage of depositions in excess of 4.0 kg/ha is considerably greater than hi the two previous
 years. The data for the eastern sites hi Table 3-10 show an increase hi nitrogen deposition over
 the period of record.

 The maximum value shown throughout the western network over the 3 years is 1.4 kg/ha.
 About half of the sites showed depositions less than 1.0 kg/ha.  The lowest value was observed
 at Glacier NP.

Ammonium
Annual average dry depositions of NHJ by year and by subregion are shown in Table 3-11.
The midwestern subregion shows the highest annual NHJ depositions, followed by the
northeast subregion , and then the south-central subregion.  The other three subregions hi the
eastern network show much lower depositions. Averaged data from the western sites show
NHJ depositions all less than 0.13 kg/ha.

Figure 3-62  shows annual average NHJ fluxes for 1992 as  an example year. Three areas with
depositions above 0.5 kg/ha are shown on the map:  Indiana and Ohio,  eastern Tennessee and
North Carolina, and the mid-Atlantic states.  The highest depositions are shown for midwestern
monitors and one site (Arendtsville) in southeastern Pennsylvania.
                                          45

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3.2.3.2 Weekly Depositions
Sulfur Dioxide
Five sites were selected from five eastern subregions to illustrate weekly distributions of
deposition rates: Vicennes, IN (Site 140), Cowetta, NC (Site 137), Arendtsville, PA (Site 128),
Perkinstown, WI (Site 134), and Woodstock, NH (Site 109). Figures 3-63 through 3-67 show
time series of weekly SO2 concentrations, deposition velocities, and depositions for 1995 for
these five sites.  All five figures show the annual cycle of deposition velocities, gradually rising
from about 0.2 cm/sec in the winter to between 0.4 and 0.5 cm/sec in the middle of the
summer. The curves of SO2 Vd show little weekly variability superimposed on the annual
cycle.  Higher SO2 concentrations are observed in the cold months with significantly higher
concentrations at the sites  near major sources.  For example, the Indiana monitor measured
weekly SO2 levels  as high as 40 Atg/m3; whereas the New Hampshire monitor measured
concentrations typically at levels around 1 Aig/m3 with higher concentrations in the 2 to 4 //g/m3
range.  The range  in SO2 concentrations is as high as a factor of 6.0 as compared to the roughly
factor of 2.0 change in deposition velocities. The distributions of depositions shown in the five
figures follow more closely the patterns of concentrations, rather than deposition velocity.

To investigate the  relationship between SO2 concentrations and depositions Figure 3-68 gives a
scattergram of weekly concentrations and depositions for 1995 for the five sites combined.  The
data show a good relationship, with a correlation coefficient of 0.87.  Despite  the complexity of
dry deposition processes, the relationships are fairly consistent from site to site, suggesting that
the variability in deposition is largely driven by variability in concentration. The relationship is
stronger for lower concentrations, as shown in Figures 3-69 and 3-70.  Figure 3-69 shows a
scattergram for SO2 concentrations (as S) less than or equal to 2.0 Atg/m3.   Figure 3-70 provides
a scatter diagram for SO2  levels (as S) greater than 2.0 Aig/m3.  Evidently, the  efficiency of the
deposition processes decreases somewhat as SO2 concentrations increase.
Sulfate
Figures 3-71 through 3-75 show time series of weekly average 804" deposition velocities,
concentrations and depositions for 1995 for the same five sites. The distributions of deposition
velocities do not show a strong annual cycle like SO2, except perhaps for a general tendency
for higher values in spring and early summer. The aerosol deposition velocities are more
related to changes in meteorological conditions, rather than changes in vegetation. Because of
                                           46

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 enhanced atmospheric photochemistry in the warmer months, SO£ concentrations and
 depositions peak in the summer. SO^ concentrations are higher at the Indiana and Pennsylvania
 monitors and much lower at the Woodstock, NH site.

 Figure 3-76 provides a scattergram of weekly SO% concentrations versus depositions for 1995.
 Again, there is a consistent relationship between concentrations and depositions across all five
 stations.
Nitric Acid
Time series of HNO3 deposition velocities, concentrations, and depositions (fluxes) for 1995 for
the same five sites are given in Figures 3-77 through 3-81. The curves for deposition are
dissimilar among the five sites. Only the Vincennes site shows an annual cycle with maximum
velocities in the summer.  However,. the weekly variability is also considerable.  The North
Carolina site shows the highest HNO3 Vd in the spring.  No seasonal or annual cycles are
apparent hi the data from the other three sites.  Concentrations are generally higher hi the
warm months with a few exceptionally high values in the whiter.  Depositions generally follow
concentrations although there seems to be more of an influence of deposition velocity on
depositions than for SO2 and
Figure 3-82 shows a scattergram of HNO3 depositions versus concentrations for 1995 data
aggregated from the five sites. The data again show a good linear relationship (correlation
coefficient) across the five sites and for an order of magnitude range in both concentrations and
depositions,

3.2. 3. 3 Trend Analysis
As an initial test of trends hi dry deposition, linear regressions (deposition versus year) were
calculated for depositions of SO2, SO^, total dry sulfur, HNO3, NO3, and total NO3 from 1989
through 1995 for all the eastern sites combined. The results are shown hi Figures 3-83 through
3-88, respectively.  Downward trends are indicated for the sulfur species although the trend
lines are not considered statistically significant. The downward slopes for SO2 and total sulfur
are greater than for SO|', consistent with the results for concentrations. The reductions hi
depositions of sulfur species are lower than the corresponding reductions in concentrations.
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The slopes for the regression lines for HNO3 and total NOj are slightly positive; the slope, for
NC>3 aerosol deposition is 0.0.  These results are not considered statistically significant.

Depositions of sulfur and nitrogen species measured throughout/the, western network exhibit no
trends.

3.3 Wet Deposition
The purpose of wet deposition monitoring within CASTNet is to facilitate the comparison of
dry deposition rates with wet deposition rates and to calculate total deposition. Therefore, wet
deposition monitoring was initiated at those CDN sites that are 50 km or further from the
nearest NADP monitoring site. Figure 2-4 shows the location of the CDN wet deposition sites.
Except where noted, the following sections discuss results generated by data collected at CDN
sites and those NADP sites that correspond to CDN dry deposition only sites. Data from the
two networks were combined since, in most cases, the small number of CDN wet deposition
sites does not allow for meaningful analysis or conclusions on a regional basis.

3.3.1 Concentrations in Precipitation
3.3.1.1 Annual Average Concentrations
Sulfate
To assess variability in annual averages, maps of annual SOJ" concentrations for the years 1990,
1992, and 1994 are presented in Figures 3-89 through 3-91. Similar concentration patterns
were noted for these 3 years, with highest concentrations (3.0 mg/L or above) appearing in
southern Illinois, eastern Michigan,  Ohio, south-central Pennsylvania, and central We.st
Virginia.  The lowest concentrations were exhibited during 1994.
Nitrate
Figures 3-92 through 3-94 show the annual NOi concentrations for 1990, 1992, and 1994,
respectively. These figures show that the highest concentrations (above 2.5 mg/L) were
observed at only two sites in 1990 (Sites 124 and 128).  A high concentration region was
evident in 1992 and included sites in the upper midwest (Site 134), midwest (Sites 114, 115,
123, and 157), and one site in the northeast region (Site 128). This area receded to three sites
hi the Ohio-Michigan region hi 1994.  The overall 1994 concentrations were the lowest of the
3 years.
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pH
The lowest annual pH values (less than or equal to pH 4.2) occurred at sites in New York,
Pennsylvania, West Virginia, and Virginia in 1990 (Figure 3-95). Only two of these sites
(Sites 119 and 128) maintained the low pH levels in  1992 with Site 114 mimicking them in
1994 (Figures 3-96 and 3-97). In general, the lowest pH values in the network were detected
in western New York,  Ohio, Pennsylvania, and West Virginia. Except for Sites 114 and 119, a
steady rise in pH values can be detected from 1990 to  1994. Sites 114 and 119 also did not
exhibit lower SO2,' and NOj concentrations over this period. The pH values of the western sites
were approximately 0.5 pH units higher than the eastern sites.

Ammonium
During 1990, 1992, and 1994, concentrations above 0.5 mg/L occurred primarily in
agricultural areas (Figures 3-98, 3-99, and 3-100,  respectively). NH"J concentrations were less
than or equal to 0.5 mg/L for the western sites. There  was a decrease in NH^ values for most
of the sites in the higher concentration area between  1990 and 1994 with the highest
concentrations occurring in 1992.

Chloride
Annual concentrations for 1992 and 1994 only are shown in Figures 3-101 and 3-102. These
annual maps show, as would be expected, that sites on or near the coast detected higher Cl"
levels with respect to inland sites.  Among inland sites,  those sites paralleling the East Coast
exhibited generally higher Cl' levels than sites further inland. Chloride concentrations at the
western sites mirrored concentrations at the inland eastern sites. Declines in Cl" concentrations
were exhibited by individual sites but not by an area  or a region.

Cations
A higher concentration area of Ca2+ was noticeable in the midwest and upper midwest for 1994
(Figure 3-103). This high concentration area was also apparent in other years (not shown) and
seems to be correlated with agricultural sites as with  NH1;. Concentrations from the western
sites were similar to concentrations at the midwestern agricultural sites. Of the four cations,
Ca2+ exhibited the highest concentrations.
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Figures 3-104 through 3-106 show annual concentrations for 1994 for Na+, Mg2+, and K+,
respectively. Sodium concentrations followed the same pattern as for Cl"; sites with the highest
concentrations were detected on the  coast and sites paralleling the eastern seaboard exhibited
concentrations between the coastal sites and those further inland (Figure 3-104).

There were no noticeable areas of high concentration for Mg2+ and K+. With the exception of
the coastal and Atlantic seaboard sites for Na+, concentrations for all three cations were
measured on the same order of magnitude. Concentrations at the western sites were similar to
those for the eastern sites.
3.3.1.2 Quarterly Average Concentrations
Time series of quarterly average concentrations of SO2; are presented in Figures 3-107 through
3-109 for Sites  114 (Deer Creek State Park, OH),  126 (Cranberry, NC), and 128 (Arendtsville,
PA), respectively. A very pronounced seasonal pattern was evident for all three sites with SO^
concentrations peaking during second and third quarters and dropping off during the fourth and
first quarters. This seasonal fluctuation was either non-existent or not as strong for sites in the
periphery of the network. The western sites showed seasonal fluctuation with same pattern as
the eastern sites. Figures 3-110  and 3-111 show quarterly SO2; concentrations at Sites 161
(Gothic, CO) and 167 (Chiricahua, AZ), respectively.
Nitrate values at the three eastern sites (114, 126, and 128) also peaked primarily during
second and third quarters. However, the pattern was not as pronounced as that for SO2,",
especially for Site 114. This site had some peaks occurring during the fourth and first quarters.
The two western sites showed strong NO^ peaks during the same quarters as the eastern sites.
Figures 3-112 and 3-113 illustrate the NOj seasonally for Sites 126 and 167, respectively.
Sites 126 and 128 displayed strong seasonally for NH 4 with peaks occurring during the warm
quarters, but Site 114 exhibited some peaks during the fourth quarter as well. In the west, NH^
peaked during the second and third quarters at Sites 161 and 167.

At the three eastern sites (114, 126, and 128), pH values peaked (lower acidity) during the
fourth and first quarters and dipped during second and third quarters (Figures 3-114 through
3-116, respectively). This pattern is consistent with the observation that SO2; and NOj values
                                           50

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peaked during the summer months, resulting in precipitation with lower pHs with respect to the
winter months. The western sites did not exhibit seasonality for pH, perhaps due to lower
concentrations of SO^" and NO^ with respect to eastern sites.

There were no noticeable patterns for the rest of the analytes, except for Cl~ for the western
sites. Site 161 exhibited Cl peaks mostly during the third quarter (Figure 3-117), and Site 167
exhibited peaks during the second quarter (Figure 3-118).
3.3.1.3 Summer and Winter Averages
Seasonal behavior is also demonstrated by time series of summer (June through August) and
whiter (December through February) averages of analytes. Figures 3-119 and 3-120 illustrate
the summer and whiter averages of SOft for seven eastern sites. Both figures show that the
summer averages were generally more variable from year to year than the winter averages.
Sites 126 and 180 clearly had higher summer concentrations of SO|-. Site 114 average values
also illustrated the same difference, except for 1991 when winter SO^ values approximated
typical summer values. The peripheral sites, 134 and 156, showed more variability in SO^
concentrations during the summer, but demonstrated only a relatively small difference in
summer versus whiter concentrations with respect to Sites 114, 126, and 180.  Site 125 summer
averages showed great variability from year to year but an inconsistent pattern with respect to
winter averages.
Figure 3-121 (summer and whiter average concentrations for Sites 161 and 167) shows greater
year-to-year variability among summer concentrations and lower concentrations during the
whiter with one exception (the whiter 1990 value for Site 167).

The difference between summer versus whiter NOj concentrations is illustrated hi
Figures 3-122 and 3-123. Both figures show that NOj concentrations were higher and more
variable from year to year during the summer. Figure 3-124 demonstrates the same correlations
for Sites 161  and 167 for summer versus whiter NH^ concentrations.
3.3.1.4 pH versus Sulfate and Nitrate
To briefly investigate the association between pH, SO^", and NOj, 1994 concentrations of
and NOj from eastern CDN sites only were regressed against hydrogen ion (H+) concentrations
                                          51

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in Figures 3-125 and 3-126, respectively.  An r2 value of 0.79 for SO2r versus H+
concentrations indicates a relatively strong association between SQ^: and pH values. Nitrate,
however, does not appear to be as strongly correlated with pH and/or H+ concentrations
(r2 = 0.48). These results indicate that SO% concentrations werevmore critical in affecting the
pH of precipitation at the eastern CDN sites.
3.3.1.5 Trends Analysis
Trends in precipitation concentrations were evaluated by performing linear regressions on
annual, summer and winter averages on a subregional and regional basis (east and west) for
SOI' a*14* NOs (Tables 3-12 and 3-13). Reductions in annual SO|" concentrations were
considered significant only for the upper northeast and southern periphery subregions,.
Although the eastern region as a whole did not exhibit a significant trend, the p^value of 0.07
was very close to the significance level of 0.05, indicating a downward trend.  Two subregions,,,
the upper midwest and south-central, also showed downward correlations with p-values, of Q.,Q9
for both.  The western region did not show any trends.  Annual regression plots of SO2; for
each subregion and region are presented in Figures 3-127 through 3-134.
The regressions based on the summer average SO2; concentrations did not show any significant
reductions whereas the whiter concentrations showed significant reductions for three, subregiQns
and the eastern region as a whole.

There were no significant trends in annual and summer data for NO^. Winter concentrations
exhibited significant reductions for three subregions (upper northeast, northeast, and south-
central).  The eastern region showed a downward trend that is not considered statistically
significant with a p-value of 0.07.

Annual average precipitation concentrations by analyte for CDN sites only from 1990 through
1994 are presented for reference purposes in Tables 3-14 through 3-22. The last four columns
of these tables also present the 5-year mean, the standard deviation of the mean, the coefficient
of variation (CV), and the percent difference (%D).
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 3.3.2  Wet Deposition Patterns and Trends
 Annual average depositions by analyte for 1990 through 1994, 5-year mean averages, standard
 deviations of the 5-year mean averages, CVs, and %Ds for the CDN wet deposition sites are
 presented for reference purposes in Tables 3-23 through 3-31. Tables 3-32 and 3-33 present
 the same information for  SOi' as sulfur (S) and for NO; as nitrogen (N), respectively.

 3.3.2.1 Annual and Period Average Depositions
 Deposition values for the more significant analytes such as SO2,-, NO;, and pH as hydrogen ion
 are presented as annual averages for the years 1990, 1992, and 1994. Depositions of NH"J and
 Cl- are presented as period averages (i.e., 1990 to 1994) and depositions of Ca2+,  K+, Na+, and
 Mg2+ are presented in the table formats described above (Tables 3-27 through 3-30).

 Sulfate
 The combined CDN/NADP annual average deposition rates for SO2,- are presented in
 Figures 3-135, 3-136, and 3-137 for 1990, 1992, and 1994, respectively. Figure 3-135 shows
that the high SO2,- deposition area (25 kg/ha or above) through Ohio, West Virginia, and
 Pennsylvania continues west into Indiana and central Illinois, south through Kentucky into
 eastern Tennessee and reaches northward to include Maryland, New Jersey, and southern
New York. The highest deposition occurred in northwestern Pennsylvania with a value of
43.4 kg/ha. Figure 3-136 illustrates that this relatively large high SOf deposition area shrunk in
 1992 and covered Ohio, Pennsylvania, West Virginia, and southern New York, and included
the high elevation site (126) in North Carolina.  This same general area, but slightly larger, is
depicted in Figure 3-137 for 1994 with high SO2,' deposition also measured in eastern
Tennessee.

Nitrate
The year-to-year variations of NO; values for 1990, 1992, and 1994 are shown hi
Figures 3-138, 3-139, and 3-140, respectively. The highest NO; depositions occurred in
northern Pennsylvania and southern New York for all three years.  Sites in New Jersey and
West Virginia also exhibited high deposition in  1994. High NO; depositions did not extend as
far west or south as did high SO2,' depositions. This is especially noticeable for 1990.
                                          53

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pH as Hydrogen Ion
Hydrogen ion (H+) depositions for the CDN/NADP sites for 1990, 1992, and 1994 are
presented in Figures 3-141, 3-142, and 3-143, respectively. The highest H+ depositions in 1990
occurred over Ohio, West Virginia, Pennsylvania, southern New York, and one site in eastern
Tennessee. Depositions for H+ hi Ohio and southwestern New York showed a steady decrease
from 1990 to 1994, whereas H+ depositions hi West Virginia and Pennsylvania  dipped in 1992
but rose slightly hi 1994. The highest H+ depositions for all 3 years were measured in
northwestern Pennsylvania. The Catskill-New York site did not exhibit any change hi H+
deposition over the 3 years, and H+ deposition at the eastern Tennessee site rose back to 1990
levels after a decline hi 1992.

Regionally, the midwest experienced the greatest reduction (32.0 percent) in H+ deposition
between  1990 and  1994, and the northeast had the smallest (13.4 percent). The northeast region
also had the highest regional average H* depositions  hi 1990 (0.67 kg/ha) and hi 1994
(0.58 kg/ha). All regions declined hi regional H+ depositions, except for the southern
periphery.  The three sites hi this group exhibited a 14.8-percent increase hi average H+
deposition.

Ammonium
The highest NH 4 depositions were measured over the midwestern region with an extension into
Pennsylvania as depicted hi Figure 3-144.  The relatively high CVs in Table 3-26 are indicative
of an up  and down pattern over the years in NH 4 depositions for many of the CDN sites rather
than a steady downward trend.

Chloride
Figure 3-145 shows that Cl" depositions are greatest at the  coastal sites and decline steadily as
one moves away from the coasts. The southern periphery sites and those south-central sites
paralleling the Gulf Coast as well as sites paralleling  the East Coast all exhibited higher Cl~
depositions than sites further inland.
Cations
Tables 3-27 through 3-30 present the yearly deposition averages and accompanying statistics
for Ca2+, Na+, Mg2+, and K+, respectively for CDN sites only. In general, deposition values

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for Ca2+, Na+, and Mg2+ declined for most CDN sites from 1990 to 1994.  High CV values
indicate an up and down pattern at most sites. At all but four sites, K+ depositions increased
from 1990 to 1994.
3.3.2.2 Summer and Winter Averages
Depositions, like concentrations, also exhibited seasonality. SO2,', NOj, and NH1J depositions
were higher in the warmer months than in the colder months. Figures 3-146 and 3-147 show
this seasonality (summer versus winter) for SO^ at eastern Sites 114, 134, 156, and 180, and
western Sites 161 and 167, respectively. Deposition values for SO2,' also showed greater
variability from year to year in the summer months than during the winter months.

Figure 3-148 shows the same summer versus winter difference for NOj for the same eastern
sites, except for the NOj deposition value in 1991 at Site 114. Summer versus winter values for
NH"J are plotted in Figure 3-149 for the same four eastern sites, and in Figure 3-150 for the
western sites.
3.3.2.3 Depositions and Concentrations
For the most part, wet depositions and concentrations follow the same pattern. This was
illustrated with the summer and winter averages and is further exemplified in Figures 3-151
through 3-155. Figures 3-151 and 3-152 show average quarterly SO|- concentrations and
depositions plotted together for Sites 126 and 128, respectively. At both sites, SOl~
concentrations and depositions peaked during second and third quarters. The difference in
magnitude between the peaks and valleys in deposition values is much greater than in the
concentrations.
The same relationship is seen for NO^ hi Figures 3-153 and 3-154, and for NH^ at Site 126
only in Figure 3-155.

On occasion (e.g., second quarter 1991 in Figures 3-152 and 3-154), depositions either
decreased when concentrations increased, or they did not increase as greatly as concentrations
did. Other scenarios include instances of relatively large drops in deposition with respect to
rather small decreases in concentration (e.g., fourth quarter 1989 hi Figure 3-154). Such cases
                                           55

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provide opportunities for further investigation into the effects of meteorological parameters on
deposition rates.

3.3.2.4 Trends Analysis
The trend analyses presented in this section are based on linear regressions of deposition versus
year conducted on the combined CDN/NADP database. Regressions were calculated for S0|~
as S and NOj as N for all eastern sites combined and for each subregion for 1989 through
1995. The results are summarized hi Table 3-34.

Significant downward trends were indicated for the sulfur species for the eastern region, and
for the upper northeast, northeast, midwest, and south-central subregions,  No significant
reductions were indicated for nitrogen. However, the eastern and western regions and the
upper northeast subregion exhibited downward trends with p-values close to significance (0.07,
0.07, and 0.08, respectively).  Figures 3-156, 3-157, and 3-158 illustrate the results of
regression analyses for sulfur for the eastern region, and the upper northeast and south-central
subregions, respectively. Figures 3-159 and 3-160 show the strong downward trends of
nitrogen depositions for the eastern and western regions, respectively, even though the results
are not considered statistically significant.

3.4 Total Deposition of Sulfur and Nitrogen Species
Dry and wet depositions of sulfur and nitrogen species are summed, analyzed, and presented  in
this section. The analyses generally follow those used to present the concentration, dry
deposition, and wet deposition measurements discussed hi previous sections.

Figure 3-161 shows annual average total sulfur depositions averaged over the 6-year period
1989 to 1994. Six-year  average depositions above 10 kg/ha were observed across most of the
eastern network. Depositions above 15 kg/ha were observed at sites located in and downwind
of the major source region of SO2 emissions, Depositions drop off significantly along the
peripheries of the network.

Depositions at the western sites are at or below 3 kg/ha with the Chiricahua site (107) showing
depositions about three  times higher than the other western sites.
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 The variability in annual depositions are illustrated in the maps of annual averages shown in
 Figures 3-162 through 3-164 for 1989,  1992, and 1994, respectively. Similar patterns of
 depositions were observed in the 3 years with the highest values occurring in 1989. The
 geographic coverage of higher (above 15 kg/ha) depositions is smallest in 1992. The area with
 depositions above 15 kg/ha increased into New Jersey and Maryland in 1994.

 The percentages of total deposition that are in the form of dry deposition are given in
 Figure 3-165  for the 6-year average and in Figure 3-166 for 1994. The patterns are similar in
 the two figures. The higher percentages of dry deposition occur along the Ohio River into
 New York State and also in the mid-Atlantic states. An area of relatively lower percentages
 exists along the Appalachians into central Pennsylvania. This area could reflect the higher
 precipitation that occurs hi the mountains. Other regions with lower percentages occur in
 regions with low ambient concentrations (e.g., New England and the upper midwest). Lower
 percentages are also observed hi the deep South, a region with high  rainfall.

 Table 3-35 provides subregional averages of total sulfur deposition by year and also
 percentages of dry deposition. The calculated total depositions show about a 32-percent
 reduction hi sulfur deposition for all of the eastern sites combined. The downward trend is
 shown consistently for every subregion. Even the western sites show a downward trend.
 Figure 3-167 shows a linear regression for the eastern sites combined. The regression plot
 verifies a statistically significant reduction hi total sulfur deposition.

 Figure 3-168 shows 6-year average rates of total deposition of nitrogen species. Most of the
 eastern network has values above 5 kg/ha. Two deposition values above 8 kg/ha were
 observed. Depositions drop off along the peripheries of the network. Depositions of nitrogen
 species hi the  western network are 2.0 kg/ha or less. Again, the Arizona site  monitor
 experienced the highest deposition rate.

 Annual average total nitrogen depositions are shown hi Figures 3-169 through 3-171 for 1989,
 1992, and 1994. The patterns of depositions are similar from year to year, with most of the
 eastern sites observing values above 5 kg/ha. In 1989, the highest levels occurred hi Ohio,
West Virginia, and Pennsylvania. In 1992, one value above 8.0 kg/ha was observed hi
                                           57

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New York. In 1994, the area of peaks shifted to northern Virginia, eastern Pennsylvania, and
New Jersey.

Percentages of dry deposition are given in Figure 3-172 for the 6-year averages and in
Figure 3-173 for the year 1994. The percentages calculated for most of the eastern sites are
above 40 percent. Again, an area of lower values exists along the Appalachian chain. A sharp
gradient is observed over New England. The percentages for dry nitrogen deposition are higher
in the South than for the corresponding percentage for dry  SOI deposition. The percentages for
the western sites are at or above 40 percent.

Table 3-36 lists total nitrogen deposition by subregion and by year and also shows the
percentages of dry deposition. The calculated total depositions rates of nitrogen species exhibit
no trend for eastern sites combined. The table shows a small reduction of the northeast and
upper northeast subregions. However, the linear regression analysis of total nitrogen deposition
versus year, shown in Figure 3-174, shows no significant trend.
3.5 Ozone Concentrations
The CASTNet O3 network was designed, in part, to provide information on the distribution of
O3 across rural areas of the United States. As discussed in Chapter 2.0, the siting criteria used
to locate sites in the network and the attention given to physically locating sites to provide the
greatest regional representativeness possible allow the O3 measurements to give at least a
qualitative analysis of geographic patterns throughout the eastern United States. The data
provide estimates of exposure statistics and allow gauging compliance with national air quality
standards. The data also allow the analysis of the effects of terrain and other site characteristics
on O3 concentrations.

O3 concentrations are regulated by the National Ambient Air Quality Standard (NAAQS) of
0.12 part per million (ppm) hourly average. In practice, O3 levels of 125 ppb or greater are
counted as exceedances of the current NAAQS. A violation of the NAAQS occurs when the
fourth highest hourly concentration measured in any  3-year period equals or exceeds 125 ppb.

In November 1996, EPA proposed eliminating the one-hour primary standard and replacing it
with an 8-hour standard. The proposed eight-hour standard was set at 0.08 ppm. The 0.08-ppm
                                            58

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level was proposed in November 1996 in terms of the third highest daily maximum 8-hour
concentration, averaged over 3 years. In July 1997, EPA promulgated a new standard in terms
of the fourth highest daily 8-hour concentration. A violation of the new NAAQS would occur
when the 3-year average of the fourth highest, daily, running 8-hour averages exceeds 84 ppb.

EPA had also proposed a revised secondary standard — either identical to the proposed primary
standard or establishing a "seasonal SUM06" secondary standard. The SUM06 standard is
expressed as the sum of hourly O3 concentrations summed over 12 hours per day (8:00 a.m. to
8:00 p.m.) during the 3-month period when O3 concentrations are at their highest. The
numerical value of the standard is 25 parts per million hours (ppm-hr). Although EPA did not
promulgate the SUM06 standard, SUM06 provides a measure of the exposure of vegetation and
crops to O3 during the growing season.

W126 is another measure proposed by Lefohn and Runeckles (1987) for examining O3 damage
to forests and crops.  W126 is an S-shaped function that weights O3 concentrations in a manner
that emphasizes high values (i.e., > 80 ppb) and de-emphasizes low values (i.e., < 30 ppb),
based on the expectation that the higher concentrations are more harmful to crops. Another
measure of overall exposure is simply the annual average concentration.

The CASTNet O3 database was used to calculate the measures discussed above for each
monitoring site and each year since 1987.  Running eight-hour concentrations were calculated
for  each hour of the day.  SUM06 and W126 statistics were based on rolling 3-month averages.

3.5.1 Annual Averages
Annual averages by site and arranged by subregion are listed in Table 3-37. Annual
concentrations measured throughout the eastern network ranged from around 20 ppb to about
50 ppb.  The highest annual averages occur at mountaintop sites (e.g., 118, 120, and 126) along
the  Blue Ridge and Appalachian Mountains, while the lowest annual averages were recorded at
sites in steep valleys (e.g., Sites 119 and 121) and in suburban areas (e.g., Sites 116 and  146).
Although there is considerable geographic variability in annual averages, there is little year-to-
year variability at individual stations. Unlike SO2 and SO|", there is no discernible trend in
annual averages. The lower annual averages were  recorded at monitors situated far away from
major source regions and at stations significantly influenced by local nighttime sinks  (discussed
                                          59

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later).  The higher annual averages were observed hi 1995 and 1988, while lower averages;
were recorded in 1992.

Data for the western sites show annual averages ranging from 21 ppb in Montana to 52 ppb in
southeastern Wyoming. The annual averages typically exceed 40 ppb, except for Glacier NP,
MT (Site 168) and Reynolds Creek, ID (Site 163). These two sites are situated at the two
lowest elevations hi the western network. In general, the annual averages measured at the
western sites are higher than those recorded in the east. The relatively high annual
concentrations at the western sites are consistent with the high annual levels at the mountaintop
eastern sites.

3.5.2  Hourly Concentrations
Table 3-38 shows the peak hourly O3 concentrations by site and subregion for each year the site
was operational. Table 3-39 shows the frequency of hourly concentrations  above 125 ppb by
site, subregion, and year. The data hi these two tables allow a compliance  analysis with respect
to the current  1-hour NAAQS. During the summer of 1988, several sites measured
concentrations above 125 ppb, and several sites showed violations of the NAAQS. The
summer of 1988 was unusually hot and dry in most of the eastern United States  and resulted in
a season of very high O3 levels. Figure 3-175 shows the number of values greater than
124 ppb at each site for 1988 and for all other years combined, separated by a diagonal.

After 1988, the monitors with three or more exceedances and with violations of the NAAQS
were limited to locations  hi the Washington - New York corridor (i.e., the Maryland, New
Jersey, and West Point, New York sites).  Other sites recorded between one and three
exceedances of the  1-hour standard, but no violations, from 1989 through  1995. In general,
these were rural-agricultural sites located approximately 50 to 75 km from a major urban
center.

Peak hourly concentrations measured throughout the western network were generally much
lower that the eastern measurements, although one hourly measurement hi southern Arizona
exceeded 125 ppb.  No violations of the current NAAQS were recorded at the western sites.
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 3.5.3  Eight-Hour Concentrations
 Running 8-hour O3 concentrations were calculated for every day throughout the sampling
 record. Daily peaks were selected from the running 8-hour values.  Figures 3-176 through
 3-178 show the fourth highest, daily 8-hour concentration for each site for the years 1993
 through 1995. Figure 3-179 provides averages of the fourth highest values for each site. A
 violation of the proposed NAAQS would occur if a value in Figure 3-179 equals or exceeds
 85 ppb. The 3-year averages show that 15 eastern sites would have recorded a violation of the
 proposed primary standard for the 1993 to 1995 period. Figure 3-180 shows the maximum and
 minimum number of days in any year from the monitoring record with levels above 80 ppb. A
 site with a minimum  of 4 days or more would have experienced a violation for every 3-year
 period in the data record. The fourth highest 8-hour concentration for each site by subregion
 are shown for 1988 to 1991 in Figure 3-181 and for 1992 to  1995 in Figure 3-182. Sites with
 3-year averages above 85 ppb would have experienced a violation of the proposed NAAQS.

 Concentrations above the proposed primary standard were measured in the midwest and
 northeast subregions with a few high values in the south-central subregion.  None of the
 western sites recorded annual maximum running 8-hour O3 concentrations above 85 ppb.
 Values ranged from 43 to 72 ppb.

 3.5.4 SUM06
 The measure SUM06 has been proposed as a secondary standard to protect human welfare and
 the environment.  Table 3-40 lists maximum SUM06 by site, subregion, and year.  The table
 also shows the 3-month period in which the maximum SUM06 was recorded for each year. A
 majority of sites show SUM06 values consistently above 25 ppm-hr, the proposed numerical
 limit. The peak SUM06 values were most often recorded in June through August, although
 occasionally high SUM06 levels were earlier in the year, March through May.

 Figure 3-183 illustrates peak SUM06 levels for 1995. Values above 25 ppm-hr were observed
 across most of the Midwest and Mid-Atlantic states, from Illinois to New  Jersey. Most of the
southeastern sites recorded values above 25. No values above 25 ppm-hr were measured in
Wisconsin, Michigan, New England, and along the southern edge of the network on the Florida
                                         61

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panhandle and in Arkansas. Three sites in the core of the network (i.e., Cedar Creek, WV;
Prince Edward, VA; and Beaufort, NC) recorded values less than 25 ppm-hr in 1995.

Four SUM06 values above 25 ppm-hr were recorded in the western network since 1991.

3.5.5 W126
Table 3-41 lists maximum W126 by site, subregion, and year. Twenty-five ppm-hr was chosen
as a numerical measure for W126 for the purpose of comparison to SUM06 levels. The highest
W126 values were recorded in 1988.  The highest level (51.8 ppm-hr) recorded throughout
CASTNet was in June through August 1988 at Site 122 (Oxford, OH). Many high values were
also recorded in 1991.

Figure 3-184 shows the geographic distribution of W126 values measured in 1995. As
compared to SUM06, the geographic extent of elevated W126 values is considerably smaller.
Values above 25 ppm-hr were restricted to most of the Midwest, the Mid-Atlantic stations, and
the two sites in  Georgia and Alabama. Measurements throughout the western network were all
below 20 ppm-hr.

3.5.6 Geographic Variability
Tables 3-42 and 3-43 summarize O3 concentrations and the SUM06 and W126 measures for
1995 and  1992  for 12 sites that cover a variety of terrain settings and locations.  The year 1995
was selected because it is the most recent year available from the CASTNet database and
because it was a relatively high O3 year. The year 1992 was selected because it was a low Oj
year. During 1995, the fourth highest, daily 8-hour concentration exceeded 85 ppb at half the
sites. The 1993 to 1995 averages (Figure 3-179) of the fourth highest, daily 8-hour levels
exceeded  85 ppb at the same six sites. The SUM06 levels exceeded 25 ppm-hr at all, but the
two remote  sites in Maine and Wisconsin and also the Prince Edward, VA site. Peak 1-hbur
levels exceeded 125 ppb at the two suburban sites in Maryland and New Jersey. In 1992, the
fourth highest,  daily 8-hour concentrations exceeded 85 ppb at only three sites. SUM06 was
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 at all the sites, except for the two suburban sites on the east coast and the Cranberry, NC site.
 Only one peak hourly concentration was above 125 ppb.

 The highest annual concentrations were observed at the three mountaintop sites (118, 120, and
 126) along the Appalachian chain. The highest hourly and 8-hour levels were measured at the
 two suburban sites.  These two sites had the two lowest annual averages. Eight-hour
 concentrations are high (above 85 ppb) throughout the midwest and northeast. High SUM06
 values are extensive, although there is significant yearly variability.

 The geographic differences can be explained by several factors:  the proximity of monitors to
 source regions; terrain and atmospheric boundary layer effects; and day-night differences in
 photochemistry, scavenging and dry deposition. Differences in diurnal cycles illustrate the
 influence of some of these factors. Hourly average O3 concentrations  for a site in rolling terrain
 (Prince Edward, VA), a site in complex terrain (Parsons, WV), a mountaintop site (Big
 Meadows, VA), and a suburban site (Beltsville, MD) are shown for several annual averaging
 periods in Figure 3-185. The rolling terrain site exhibits moderate day/night variability, with
 nighttime values about 50 to 60 percent of daytime peaks. The  daytime levels reach a broad
 peak between the hours of 1200 through  1700. Hourly values for the complex terrain site
 indicate more day/night variability. Daytime values are about twice nighttime values.  The
 duration of the daytime peak is shorter. The mountaintop site shows a fiat diurnal pattern.
 There is little variability from hour to hour. The suburban site shows the lowest values in the
morning near sunrise with daily peaks three to four times early morning levels.

Mountaintop sites are situated typically at elevations above the tops of nocturnal boundary
layers that affect valley sites or sites located in rolling or flat terrain. Mountaintop sites are
generally in contact with reservoirs of O3 that have been observed to exist in the planetary
boundary layer at night above ground-based inversions.  Because mountaintop sites are
typically above ground-based inversions, O3 is not depleted by deposition processes or by
scavenging by low-level emissions.  Consequently, concentrations are relatively constant
throughout the day and are high on an annual basis. Suburban  sites are influenced by nearby
sources and nighttime sinks. Therefore, suburban sites show more day/night change, have low
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values in early morning, and are relatively lower on an annual basis because of low nighttime
levels. Nighttime O3 is depleted by fresh nitric oxide (NO) emissions which are trapped under
a ground-based inversion and by dry deposition. Rural rolling terrain and complex terrain sites
are subject to the effects of nighttime inversions and deposition losses but most likely not by
locally-produced, fresh NO emissions. Hence, nighttime and early morning O3 levels are low,
but there is less day/night change than at the suburban sites. Annual concentrations generally
fall between those measured at mountaintop and suburban sites.

3.6 Mountain Cloud Deposition Program
The MADPro is a multi-year study of the deposition of air pollution to high-elevation forests
(i.e.,  above cloud base) in the eastern United States.  Clouds can be the primary pathway
(approximately 60 percent) for deposition of pollutants to high elevation ecosystems compared
with rainfall and dry deposition (approximately 20 percent each) (Murthy and Aneja,  1990;
Li and Aneja, 1992). Not only are substantial volumes of cloudwater deposited on surfaces, but
higher concentrations of pollutants are found in cloudwater than in precipitation (Mohnen,
1990). This can lead to high fluxes of acidity, sulfur, and nitrogen from cloud droplet
interception by forest canopies (Lovett et al, 1982; Waldman et al, 1982). High elevation fir
and red spruce forests from Maine to North Carolina have shown progressive decline over the
past years (Mohnen, 1990; Vong, 1989), evidenced as visible injury, increased mortality, and<
decreased radial growth (McLaughlin, 1985; Hornbeck and Smith,  1985; Johnson and
Siccama, 1983). A consistent body of evidence supports the conclusion that acidic cloudwater
is one of the causal factors leading to this recent decline in mountain forests in the United States
(Falconer and Falconer, 1980; Mclaughlin etal., 1990, 1991; Eagar and Adams, 1992).

MADPro exists to update and extend the largest previous work on cloud chemistry in the
 eastern United States -- the Mountain Cloud Chemistry Project (MCCP), also sponsored by the
 EPA. MCCP was in operation from 1986 to 1989 and was implemented by the Forest
 Response Program of the National Acid Precipitation Assessment Program (NAPAP). The data
 collected by the MCCP have been used hi the NAPAP Integrated Assessment to evaluate the
 role  of airborne chemicals in the changing condition of forests.  Other notable mountain cloud
 research has been performed in Canada and Europe (see Vong, 1991; Schemenauer, 1988).
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 The objectives of the MADPro are to measure cloud chemistry, estimate cloud and total
 deposition, and define source regions which impact high elevation ecosystems in the eastern
 United States. Further objectives are to relate atmospheric deposition to effects on high
 elevation forests and to effects on surface water, as well as soil effects such as nitrogen
 saturation. Since 1994, MADPro has been in operation, using a few high elevation monitoring
 sites (see Figure 3-186) to gather the requisite data to meet these objectives. Annual reports that
 include technical details and data analyses of the MADPro results have been prepared for EPA.

 3.6.1  MADPro Sites and Automated Cloudwater Collection System
 Three automated cloudwater collection sites have been in operation through the warm seasons
 of 1994, 1995, and 1996 (see Table 3-44):  Whitetop Mountain, Mt. Rogers National
 Recreational Area, VA; Whiteface Mountain, Adirondack State Park, NY; and Clingman's
 Dome, Great Smoky Mountain National Park, TN. A fourth site  in the Catskill Mountains of
 New York was added in 1995 for a manual sampling program. The automated systems were
 functionally similar, but some components were variable due to logistics and contingencies.
 For a detailed description of the cloudwater collection system, see Baumgardner etal, 1997. A
 generalized system, depicted hi Figure 3-187, includes  an automated cloud collector for
 collection and storage of hourly cloudwater samples, a  particle volume monitor (PVM) for
 determination of continuous liquid water content of clouds (Gerber, 1984), a meteorological
 station for measurement of a suite of parameters necessary for estimating deposition fluxes
 onto vegetation, a filter pack system to collect weekly measurements of airborne gases and
particles and a wet deposition system consisting of a wet/dry collector and rain gauge.
Continuous gas monitors were operated at some sites for determination of other atmospheric
pollutants of interest (e.g., O3, SO2). Also, a DAS collects and stores the electronic information
from the various monitors and  sensors.

The cloud collector and PVM are interfaced with the DAS, windspeed, rainfall and temperature
sensors so that when the liquid water content of a cloud exceeds 0.05 g/m3, windspeed is  higher
than 2.5 meters per second (m/sec), ambient air temperature is above freezing [practically,
 > 2 degrees Fahrenheit (°F)], and there is no rainfall, then the cloud collector is activated and
projected out of its protective housing.
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3.6.2 Total Deposition at Whitetop Mountain, VA
One of the objectives of the MADPro is to obtain measurements of cloud chemistry,
precipitation chemistry,  and filter pack (dry deposition) chemistry which can be used to model
acidic deposition for these three pathways. The methodology for modeling these high elevation
deposition fluxes is under development. Average monthly concentrations of SO^ and NO"3
found in dry air (filter pack analyses; expressed in //g/m3 dry air) and in samples of rainwater
and cloudwater (laboratory analyses of samples; expressed as mg/L water) are shown in
Figures 3-188 and 3-189, respectively, for the 3 years of this study (1994 to 1996). Average
monthly concentrations of H+ found in cloudwater and rainwater samples for the same period
are shown in Figure 3-190.  While a direct comparison will await calculation of deposition
values,  these figures uphold the previous statement that cloudwater can be the primary pathway
for deposition of pollution to high elevation ecosystems. In all three cases over 3 years, the
mean concentrations of cloudwater samples are higher (sometimes much higher) than those of
the rainwater samples.

3.7 Visibility Network
The purpose of the CASTNet Visibility Network is to measure visibility and related parameters
for the purpose of defining status and trends. The measurements are expected to undergo
appropriate levels  of QA and QC. The data are to be delivered in computerized formats and
through various technical reports.

Visibility monitoring includes three measurement types as defined by the Interagency
Monitoring of Protected Visual Environments (IMPROVE) program:
       1.   Scene:   Visual characteristics of a scene are monitored to document scene-
                     specific visibility.
      2.   Optical:  Optical properties of the atmosphere are monitored for a scene-
                     independent measure of air quality.
       3.   Aerosol:  Aerosol characteristics (concentration, composition, and size) are
                     determined to relate atmospheric optical properties with various species.
 IMPROVE protocols are the basis for optical and scene monitoring and for instrument
 specifications, siting criteria, sample frequency, QA, and analytical techniques. Primary scene
 and optical monitoring techniques include automated cameras and nephelometers, respectively.
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 Aerosols are measured using an annular denuder system (ADS) and three single-stage filter
 packs. The locations of visibility sites are shown in Figure 3-191.

 Each of the ten sites is equipped with an aerosol sampling system. Through November 1995,
 three sites were equipped with scene monitoring equipment (i.e., cameras), and four sites were
 equipped with optical monitoring equipment (i.e., nephelometers).

 3.7.1  Site-Selection Process
 Site survey reports were prepared to present suitability and  representativeness information for
 four new CASTNet visibility monitoring sites in north-central Louisiana, southwestern
 Kentucky, southern Indiana, and eastern Ohio.  Six existing dry deposition sites were upgraded
 to complete the ten station visibility network. The surveys addressed the siting of:  (1) a particle
 sampler for quantification of SO^, NO3, organic carbon, and trace and crustal elements; (2) a
 slide camera for documentation of vista conditions; and (3) an ambient temperature
 nephelometer  for quantification of particle scattering. CDN siting criteria were used to evaluate
 site suitability for particulate and nephelometer measurements.  Eastern Fine Particle and
 Visibility Network (EFPVN) siting criteria (Air Resource Specialists, Inc., 1994) were used to
 evaluate site suitability for camera operation. The information necessary for site evaluation was
 divided into five categories: representativeness,  suitability, logistics, administration, and
 identification.

 Survey reports were prepared for each  candidate area surveyed and delivered to EPA for
 review. The reports were intended to be used by EPA as the basis for approval or disapproval
 of a site or recommendations for further study.  These reports provided a descriptive summary
 of the results of the presurvey evaluations and field surveys.

 Once a site was selected for inclusion in the network, a complete documentation package was
prepared that clearly and fully presents the survey findings.  This package includes the site
 summary, color photographs, maps, and graphics.
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3.7.2 Instrumentation
3.7.2.1 Optical
Optec NGN-2 nephelometers are operated according to the following protocol:
      •    2-minute integrated average of the ambient scattering coefficient and associated
           status code are collected at 5-minute intervals.
      •    Particle free zero air scattering measurements and associated status codes are
           collected at 30-hour intervals.
      •    Manual zero air and span (using SUVA 134a refrigerant gas) scattering
           measurements and associated status codes are performed at operator-initiated
           intervals (every 2 weeks).

3.7.2.2 Scene
Scene monitoring was performed by 35mm automatic camera systems taking three photographs,
a day at 0900, 1200, and 1500 hours local standard time. Kodachrome ASA 64 color slide film
was used for its fine grain and excellent color reproduction qualities.

Site operators visited each site a minimum of once every 10 days to change film and service the
camera system.  Operators then sent the exposed film and completed log sheets to Air Resource
Specialists, Inc. for processing.

3.7.2.3 Aerosol
The aerosol sampling system includes three independent flow channels, which are operated at
 10,  16.7, and 10 Lpm, equipped with mass flow controllers and located in a weather-proof
enclosure at  10 meters (m)  above ground level. The channel for aerosol SO*" and NOj includes
a 2.5-micrometer (//m) cyclone followed by a single base impregnated annular denuder tube,
followed by a single-stage (Teflon®, nylon) filter pack. The trace/crustal elements and carbon
channels include a 2.5-//m cyclone followed  by a single-stage filter pack.  Trace/crustal
 element samples are collected on Teflon® filters, while carbon samples are collected on
 precombusted quartz fiber filters. Figures 3-192 and 3-193 depict the annular denuder and
 Teflo® and quartz assemblies, respectively. Figure 3-194 shows the combined aerosol sampling
 system.
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 Advantages of this aerosol system include the following:
            The 10-m sampling height provides some protection from surface activity and near-
            surface concentration gradients.
       •    Mass flow controllers and logging of flows (as hourly averages) permit accurate
            determination of sample volumes.
       •    Independent flow systems protect each channel from problems associated with other
            channels.
            The overall system has the flexibility to meet a variety of monitoring requirements.

 3.7.3  Operations
 The visibility monitoring network ranged from ten sites in 1993 to nine in 1995 (see
 Table 3-45). Aerosol samples (24-hour integrated) were collected at all sites, and Optec
 NGN-2 open-air integrating nephelometers were operated at four sites:  Site 510 (Connecticut
 Hill, NY), Site 528 (Arendtsville, PA), Site 572 (Quaker City, OH), and Site 570 (Sikes, LA).
 Visual scene photographs were taken three times daily at three sites: Site 510 (Connecticut
 Hill, NY), Site 528 (Arendtsville, PA), and Site 572 (Quaker City, OH). Aerosol samples are
 also collected at Site 518 (Shenandoah National Park, VA) on a 14-day schedule to develop
 comparability data (inter-network precision) with the IMPROVE network. Duplicate aerosol
 samples are collected at Site 572 (Quaker City, OH) on a 12-day schedule to document intra-
 network sampling precision.

 After each sampling event, filters are shipped to the QST Laboratory, where they are logged in
 and distributed to analytical laboratories. Through 1995, QST analyzed SO|- and NO3- on nylon
 filters; Desert Research Institute (DRI) analyzed organic and elemental carbon on quartz filters;
 and the University of California at Davis (UCD) analyzed mass, absorbance, and trace/crustal
 elements on Teflo® filters.

 3.7.4 Measurement Period/History
 The Work Plan for visibility monitoring was completed in October 1992. Site surveys and
 report submittals for the four new installations were completed between February 1993 and
June 1993. Optec NGN-2 open-air integrating nephelometers were operational at Site 510
 (Connecticut Hill, NY, on June 28, 1993), Site 528 (Arendtsville, PA, on June 26,  1993),
Site 570 (Sikes, LA, on June 10,  1993) and Site 572 (Quaker City, OH, on July 23, 1993).

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Through 1995, automated camera systems were operational at Sites 510, 528, and 572 at the
same time as the nephelometers. The collection of aerosol samples began in October 1993 at all
10 sites on a 3-day schedule through July 1994.  The schedule changed to a 6-day collection
period in August 1994 and continued through November 1995. Site 557 (Alhambra, IL)
collected aerosol samples from October 1993 through March 1994. Site 557 was discontinued
on March 30, 1994.

Site 518 (Shenandoah National Park, VA) was installed to develop comparability data (inter-
network precision) with the IMPROVE network.  Site 518 collected aerosol samples on a 3-day
schedule from October 1993 through July 1994. The schedule changed to once every  12 days
in August 1994 and continued through December 1994.  From January through November
1995, Site 518 collected aerosol samples every other Saturday only.

Duplicate aerosol samples were collected at Site 572 (Quaker City, OH) on a 3-day schedule
from February through July 1994 to document intra-network sampling precision. Duplicate
samples were collected on a 6-day schedule from August 1994 through January 1995.  From
February through November 1995, duplicate samples were collected on a 12-day schedule.

All visibility network operations stopped on November 14, 1995, at the request of EPA.  The
network was then reactivated in July 1996.

3.7.5  Quality Assurance
The QA program for the visibility monitoring network is very similar to the CDN QA program
described in Sections 2.2.4.1 and 2.2.4.2. The main difference between the two programs is
that the laboratory operations and  data audits for the visibility QA program also address the
activities of the two subcontractor laboratories. The subcontractor laboratories respectively
perform carbon analyses via Thermal Optical Reflectance  (TOR) on the quartz filters, and
mass, trace element, and absorbance analyses via gravimetry, proton induced X-ray emission
 (PIXE), and light induced proton microscopy (LIPM) methods on the Teflo® filters. Analysis of
 the nylon filters via 1C is performed at QST. Table 3-46 summarizes the results of collocated
 samples from 1994 for all three filters. Figures 3-195 through 3-198 show the collocated results
 for some of the analytes as regression plots.
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 As evident from the results presented in Table 3-46, the trace elements analyzed via PIXE do
 not exhibit the same levels of precision. In some cases, such as magnesium and zirconium, the
 high median absolute percent differences (APDs) were most likely due to the small number of
 collocated samples (1 and 2, respectively). Other cases of high median APDs were probably
 due to differences in very low concentrations (arsenic, rubidium, strontium, and zirconium). A
 closer inspection of field and laboratory methods is needed to provide explanations for the rest
 of the elements exhibiting higher median APDs.

 The median APDs for elemental and organic carbon are relatively high as well with values of
 24.0  and 19.35, respectively. In the case of elemental carbon the high APDs are, again, most
 likely due to differences in low concentrations. The value for organic carbon, albeit on the high
 end,  was within project criteria of ±20 percent for carbon analysis.

 One possibility for all the analytes that exhibited higher median APDs may be that  some
 elements, for whatever reasons, may not have deposited evenly on the filters of the collocated
 filter  packs.  This is a situation,  as mentioned above, that requires further research.

 3.7.6 Data Analysis
 This section presents an initial analysis of the visibility-related air quality measurements.  The
 year 1994 was selected for the analyses and presentations. More extensive analyses are beyond
 the scope of this report.  Emphasis is given to aerosols  that affect atmospheric visual quality.
 Aerosols are composed of fine and coarse liquid and solid particles in the atmosphere.  Fine
 particles (i.e., less than 2.5 ^m in diameter) scatter light and degrade the visual quality of a
vista.   Fine particles consist of different chemical species like sulfates, nitrates, organic and
 elemental carbon and soil dust. Annual concentrations of fine particles and their chemical
constituents are presented. Seasonal variability is also discussed. Time series of 24-hour
average fine particle concentrations and the chemical constituents are presented. Relationships
between fine particle concentrations and SO|- concentrations and between Bscat and fine particles
and SOf are also discussed. Finally, photographs of scenic vistas at the Arendtsville site are
contrasted for high and low SOI' days.
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3,7.6.1 Annual Averages
Figures 3-199 through 3-203 show 1994 annual average concentrations (<2.5 ^m) of fine
particles, SOl% NO^, organic carbon, and elemental carbon, respectively, measured throughout
the CASTNet visibility network. Fine particle concentrations range from 8.4 /ug/m3 in New
York to 13.6 /zg/m3 in eastern Ohio. The NAAQS for PM25 recently proposed by EPA
(62 Federal Register 38421) has a numerical limit of 15.0 ^g/m3 for annual averages. Sulfate
contributes about half the mass of the  fine particle concentrations. Annual (fine) SO^
concentrations range from 3.5 Mg/m3 in southern Illinois to about 7.0 ytig/m3 hi Ohio.  Total
SOl' measured at the same Ohio monitor was 7.2 ,ug/m3 hi 1994 (see Figure 3-5).  Comparing
Figures 3-200 and 3-5 demonstrates that smaller SOt" aerosols contribute more than 85 percent
of the mass of total SO^. On a percentage basis, organic carbon is the second most dominant
contributor to fine particle mass. Organic carbon is second to SC% at  eight of the nine sites
with complete annual data. Nitrate aerosol is second to SO*" only at the Bondville site hi
Illinois. Elemental carbon is consistently fourth on a mass basis. Other trace concentrations
(from the Teflo® filters) contribute minute amounts to mass loadings.
3.7.6.2 Summer and Winter Averages
Summer average concentrations of the same five air quality parameters are shown in
Figures 3-204 through 3-208. Winter averages are shown hi Figures 3-209 through 3-213.
Fine particle and SO^ concentrations are highest in summer.  In fact, summer SOft
concentrations are typically three times higher than whiter levels. In summer, SO|' contributes
an even higher fraction of fine particle mass. Fine NO; aerosol levels are higher hi whiter than
hi summer. Organic carbon values are somewhat higher in summer with more interstation
variability and less seasonal variability. Results for elemental carbon measurements are the
opposite of organics with some sites showing higher concentrations hi the whiter.

3.7.6.3  Monthly and 24-Hour Concentrations
Time series of monthly average SO^ and NO; concentrations for all sites are shown hi
Figures 3-214 and 3-215.  These data show the highest SO£ concentrations occur hi June
through July, probably contributing significantly to  visibility degradation (discussed later). NO;
 concentrations peak hi the four cold months of December through March. Bar charts that
 illustrate tune series of 24-hour concentrations of fine mass,  SO*", NO;, organics, and elemental
 carbon measured hi the summer are given hi Figures 3-216 through 3-218 for three sites
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 (Arendtsville, PA - Site 528; Livonia, IN - Site 573; and Sikes, LA - Site 570). The method
 for illustrating concentrations of the five chemical species is shown in the legend.  For
 example, concentrations of fine mass are shown by a "star" (*).  The bar charts show the
 magnitude of the concentrations and the percentage contribution to fine mass loadings. For
 example, the peak 24-hour fine mass value observed at Arendtsville during the summer of 1994
 was 38.6 yug/m3 on July 31,  1994. On that day, SO$- contributed 24.1 ^g/m3, about 62 percent
 of the particle mass. Concentrations of other species were all less than 2.4 /ug/m3.  During the
 summer, 24-hour concentrations varied by more than an order of magnitude with a majority of
 values above 20.0 //g/m3 at the Arendtsville site.  Fine particle concentrations were lower at the
 Livonia monitor.  However, several values above 20 //g/m3 were observed. Again, SO|- was
 the major contributor to fine mass loading. Fine particle concentrations were even lower at the
 Sikes, LA site with most observed concentrations below 10 ^g/m3. Both SO|- and organic
 carbon contributed significantly to fine mass loadings; although for the very highest fine
 particle concentrations, SO^' was the major contributor.

 Bar charts for winter measurements are shown in Figures 3-219 through 3-221.  Measurements
 at Arendtsville show much lower fine particle concentrations, with most values less than
 10 /ig/m3.  The contribution of SO^ has decreased, and the percentage contributions of organic
 carbon and NOs aerosol are significant and exceed SOf on several days. The Indiana data show
 fine particle concentrations are lower in winter. Twenty-four average values are typically below
 15 /zg/m3with three concentrations above 20 Aig/m3.  NOj  aerosols and organic carbon are
 significant contributors to wintertime fine mass. The Sikes, LA fine mass concentrations in
 winter are typically less than 10 ^g/m3. SO|- and organic carbon are the principal contributors
 to fine mass with NOj being important on 2 days.
3. 7. 6.4 Relationships Among Optical and Chemical Species Data
A scattergram of 24-hour fine mass and SOJ- concentrations for all visibility monitoring sites is
given in Figure 3-222. The data show a strong relationship between fine particles and SO|- with
a correlation of 0.86. There are a few fine particle concentrations hi the 20 to 30 /zg/m3 range
that correspond to relatively low SO|- values. However, at the high concentration end for both
fine mass and SO^, there is a very strong relationship. This graph demonstrates that SO^" is a
major contributor to atmospheric fine mass loading.
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Nephelometers were operated continuously at four sites (510, 528, 572, and 570) in 1994.
Nephelometers measure the Bscat, which is a component of overall light extinction and a
measure of visual quality.  Scatter diagrams of Bscat values and concentrations of fine particles
and SO^ were prepared to gain an understanding of the relationship between light scattering
and aerosol concentration and composition. Figures 3-223 through 3-226 show scattergrams
between 24-hour average Bscat and fine mass for the four monitoring sites that operated
nephelometers. Figures 3-227 through 3-230 scattergrams for Bscat and SC£. The Bscat
measurements are reasonably well correlated with both fine mass and SO|- at the New York and
Pennsylvania sites. The Ohio site shows correlations of close to 0.5 for both fine mass and
SOl\ The Sikes,  LA site shows the poorest correlation. The Sikes monitor is frequently
influenced by high humidity, which affects the Bscat measurements and confounds the
correlation analysis. In any event, atmospheric optical properties as measured by light
scattering are strongly  influenced by fine aerosols, whose major component is SO^, at the three
sites in eastern Ohio, Pennsylvania, and southwestern New York.  This three-state  region is
downwind of the  major SO2 source region along the Ohio River.  No conclusions can be made
regarding the Sikes data.

3.7.6.5 Photographic Visual Quality
As a preliminary  analysis of the relationship between visual quality and particle concentrations
and composition, the record of 24-hour particle levels and photographs taken at Arendtsville in
1994 were examined.  Two days were selected for presentation. November 10, 1994 had low
fine mass and SOi" levels.  The fine mass value was 1.4 Mg/m3; and the SO^ value was
 1.5 A*g/m3.  Figure 3-231 shows a photograph of the scenic view from the Arendtsville
monitoring site.  The visibility is quite good. The visual information content (contrast, color,
line, and texture) of the scene is also good. Note the excellent view of the mountains in the
background of the photograph.  Contrast is evidenced by the image of the silo in the left side of
the figure and by the peak on the right side.  Good texture is shown in the  details of the Valley
 in the "middle" of the picture.  Note the red bam on the right side.  Obviously, the fine
 visibility and visual information content resulted from the very low particle and SO^
 concentrations. Afternoon Bscat values were low. Measured levels were about 0.02.
 Figure 3-232 shows a photograph of the same view on July 31, 1994. The 24-hour fine mass
 concentration was 38.6 //g/m3, and the SOS" level was 24.1 ^g/m3. The visual quality and
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 visual information content is poor as evidenced by the significant haze in the photograph. Bscat
 levels averaged over 0.3. The relationship between high fine mass and SO|- levels and poor
 visibility is obvious in this example.
 3.7.6.6 Summary
 An initial analysis of 1994 visibility-related measurements showed a strong relationship
 between atmospheric light scattering, visual quality, and fine particle concentrations.  Fine
 particle levels peaked in the summer and were highly correlated with atmospheric fine SC#. In
 the winter, NO3 and organic carbon contributed to fine mass loadings. Light scattering (Bscat)
 increased as concentrations of fine particles and SO^ increased. Photographs of scenic vistas
 showed excellent visual quality and content during periods of low fine particle and SO^
 concentrations and poor visual quality (e.g., dense haze) during periods of elevated fine mass
 and
3.8  Other Studies
3.8.1 Mobile Dry Deposition Program
EPA is sponsoring as part of CASTNet a study to measure directly dry deposition fluxes to
better understand deposition processes and to evaluate and improve the MLM and other
models. A mobile system for measuring directly dry depositions of O3, SO2, and HNO3 was
designed, built, and deployed at several sites since early 1994. The system, instrumentation,
and sampling protocol are summarized in this section, along with a brief description of the
several field studies.
Figure 3-233 provides a schematic of the measurement system components and instruments.
Table 3-47 lists the measurements and methods of the system. Fluxes of O3, SO2, and CO2 are
measured by eddy correlation using fast response pollutant analyzers. The analyzers include a
chemiluminescent O3 instrument with a 4-hertz (Hz) sampling rate, a modified Meloy flame
photometric SO2 sensor with a 1-Hz sampling rate, and a LICOR 6262 sensor that measures
H2O and CO2 at 5 Hz by differential absorption of infrared radiation. A sonic anemometer is
used to measure the three components of wind for the eddy correlation calculations.

Nitric acid  is measured at 1 and 8 m above ground level to provide a vertical gradient. HNO3
is sampled over a 2-hour period using two filter packs. The HNO3 gradient is converted to flux

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by applying a heat exchange coefficient calculated from the sonic wind and temperature
gradient measurements. An energy budget is also calculated for the purpose of evaluating the
quality of the flux measurements (Finkelstein etal, 1995). The energy budget is characterized
by heat flux, latent heat flux, soil heat flux, soil storage, and net radiation.

Meteorological data are also collected continuously hi a standard CDN configuration to provide
input to the MLM. In addition, LAI and information on vegetation are collected weekly.

The DAS calculates eddy correlation fluxes of O3, SO2, CO2, and H2O, temperature, virtual
temperature, and the three components of the wind in real time and outputs  30-minute averages
continuously. Raw data files (10-Hz data for nine measures) are saved for 10 or more half-hour
periods each day. The measurements undergo QA as  described by Finkelstein et al. (1995).
Post field processing includes converting units, removing suspect values,  and MLM
calculations of deposition velocities.

Initial site deployment took place over the winter of 1994 at an agricultural  research station
operated by North Carolina State University in Raleigh, NC.  The terrain was gently rolling
pasture land.  Mixed grasses comprised the vegetation type.  This installation served as a test
and shake down period for the instrumentation.

In April 1994, the system was moved to Beaufort, NC, and deployed in a pasture on Open
Ground Farms, near Site 142. Fluxes were measured above mixed grasses.  The terrain was
very flat with a fetch of over  5 km. The system remained deployed until July  1994, when it was
returned to the QST Environmental office in Research Triangle Park, NC.  Equipment
modifications continued through the operation at Beaufort to improve flux measurement
technique.

 In August 1994, the system was moved to Bondville, IL, near Site 130. The terrain was flat
 with extensive fetch. Measurements were above corn plants approximately  8 feet tall.  Fluxes of
 O3, SO2, CO2, and water vapor were measured as well as heat flux parameters as the corn
 senesced.  Nitric acid gradient sampling was also performed. Equipment remained operating
 during harvest,  and flux measurements were continued above the bare field until the system
 was removed hi October 1994.
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 From December 1994 through February 1995, the system was again deployed at North
 Carolina State University in Raleigh, NC, with limited operation. During this time, O3 flux
 measurements were performed above grass and sometimes snow.

 From April through May, 1995, the system was deployed at Sand Mountain, AL, several
 kilometers from Site 152. The terrain was gently rolling with grass vegetation. Cattle were
 grazing the pasture. Fluxes of O3, SO2, CO2, and water vapor were measured.  Heat flux, soil
 and plant conditions were also monitored.  Fluxes of HNO3 were determined by the gradient
 sampling method.

 From June through October 1995, the system was deployed in a soybean field near Allenville,
 KY. The terrain was gently rolling. The equipment was installed 3 days after the beans were
 planted. Crop development was documented during the entire life cycle of the beans. LAI and
 porometer measurements were taken to characterize plant activity. Fluxes of O3, SO2, CO2, and
 water vapor were taken as the beans developed and were harvested. Heat flux and soil
 conditions were also monitored. Empirical soil moisture samples were also collected to develop
 a calibration curve for the continuous soil moisture probes used in routine operation.  Data
 collected during this field effort were made available as part of the Southeastern Consortium
 Intermediate Oxidant Network (SCION) oxidant study summer intensive program conducted
 near Nashville.

 From April 1996 through May 1996, limited site operation commenced at Duke Experimental
 Forest in Chapel Hill, NC. Within the 2-km fetch, the terrain was mostly flat with planted pine
vegetation. The main objective of this experiment was flux measurement comparison for
precision purposes. Three sonic anemometers and fast O3 analyzers, with two CO2/water vapor
 analyzers, were deployed at the same height above the forest canopy.  Applied Technology
Incorporated (ATI) and Gill sonic anemometers were compared. After the precision flux
measurements were taken, flux profiles above the canopy were measured with the three
 systems.  Personnel from Duke University performed water vapor flux and plant physiology
measurements during the same time period. During system operation, another experiment
 involving CO2 enrichment, conducted by Brookhaven National Laboratory, proceeded.
Experience with logistical difficulties while operating the flux measurement equipment above a
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forest canopy was gained during this field effort, which proved to be very valuable for future
installation situations.

From July 15, 1996, through August 15, 1996, the system was deployed in another bean field
near Plymouth, NC. The terrain was flat. This effort was part of the Nitrous Oxidant precursor
measurement technique and Validation Assessment program (NOVA,  1996) hosted by North
Carolina State University. The experiment was attended by various flux measurement groups,
including Argonne National Laboratory, National Aeronautics and Space Administration
(NASA), University of Maryland, NCS, NOAA, and the National Center for Atmospheric
Research (NCAR) as a technique comparison study.  All parameters were measured as a
routine complete system operation.  An additional experiment designed to measure particle flux
with a laser particle counter was also conducted.

From August 1996 through October 1996, the system was deployed at Rutgers University
Marine Research Field Station in Tuckerton, NJ. The surface of interest during this effort was
the estuary water. Equipment was installed on an existing tower previously used for
communication by the U.S. Coast Guard. During high  tide, water was present at the base of the
tower. At low tide, the marsh grass was exposed. Fluxes of O3, SO2, CO2, and water vapor
were measured combined with HNO3 gradient samples. A fiber optic data link was employed to
transmit the sensor and analyzer output from the tower to the computers located seven hundred
feet away in the equipment trailer. Some of the methods for operation pioneered at the earlier
experiment in Duke Forest were refined for improved operation under extremely harsh
conditions encountered in the marine environment.

Planned operation for  1997 will include measurements  above a deciduous forest canopy.
Approximately 70 percent of the sensitive ecosystems are forested, making it an important
environment for deposition study. It is anticipated that more complex terrain will also be
involved during future site operation.  Instrument development and modification continue to
improve operation and reliability, including operation of a new design fast O3 analyzer.
An EPA investigation (Clarke, 1997) is using the data collected from the mobile monitoring
system to better understand deposition processes and to evaluate and refine the MLM. Results
from these studies will be published elsewhere.
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 3.8.2 Comparison of Filter Pack and Annular Denuder Samplers
 CASTNet uses a three-stage filter pack sampler to measure concentrations of acid gases and
 aerosols. Because of various concerns expressed in the literature about the efficacy of filter
 pack sampling, EPA is sponsoring a study to compare measurements taken with filter pack
 samplers to measurements taken with annular denuders and also with SO2 and HNO3 continuous
 analyzers. The study is also addressing the utility of using cyclones for removing large particles
 from the air sampling stream as a means of improving the measurements.

 The study so far includes 10 months of collocated collection of weekly denuder and filter pack
 samples at 11 CASTNet sites (Figure 3-234). At two sites (133 and 147), cyclones were also
 tested. At three separate sites, continuous analyzers are operated to measure low-level (i.e.,
 low concentrations) of SO2 and NOX. A NOX analyzer is operated with  three channels to
 separate NOX,  HNO3, and NOj. Preliminary results have been reported by ESE (1997). The
 study will continue through August 1997 with a final report scheduled  in November.

 The results to date show a high correlation between SO|- measurements from the filter pack and
 annular denuder system. HNO3 measurements on the filter packs are higher than the denuder
values  (e.g., 11 to 12 percent higher at Site 133). SO2 concentrations measured by the filter
pack and annular denuder system show very little difference (Figure 3-235). These results are
considered preliminary and may change with a more complete analysis of the data.
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Chapter 4
Summary

4.1 CASTNet Operations
EPA initiated regional measurements of acid gases and aerosols and supporting meteorological
data in 1986 through the NDDN.  Field measurements began in 1987, and more than
80 percent of the network was operational in 1989. NDDN was incorporated into CASTNet in
1991. Chapter 2 summarizes the history of the network. Currently, CASTNet operates
45 eastern sites and 3 western sites and 21 sites that measure precipitation chemistry.

The CASTNet sites were selected to characterize regionally representative air quality.  Major
sources of SOX and NOX were avoided to reduce the likelihood of measured concentrations
being influenced by individual plumes or groups of sources. In addition, the land use near each
station was selected to match, as much as possible, the predominating regional land use in
order to make use of the meteorological data to model representative deposition velocities and
fluxes.

QST has developed a substantive infrastructure involving field operations, laboratory
operations, and data management. The QST infrastructure has resulted in an efficient system
that covers the process of taking the measurements through delivering the data to EPA.

CASTNet is served by a strong QA/QC program. EPA established rigorous goals for  the
accuracy and precision of the field and laboratory data. The CASTNet data largely meet the
stated precision and accuracy objectives. In short, the CASTNet data constitute an exceptional
database for the purpose of discerning status and trends in air quality and of supporting other
scientific activities.

The results from the QA/QC program demonstrate conclusively that the observed changes in
concentrations and depositions discussed in this report are real and not the result of network
modifications or of data imprecision or inaccuracy.  Concentration and deposition changes are
the result of changes hi emissions and of meteorological fluctuations, not of changes in the
network.
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 4.2 Concentrations
 Concentrations of pollutant gases and aerosols are presented and discussed for various
 averaging periods. Annual averages of SO2 and SO^ reflect the geographic distribution of
 sources of SO2. Peak concentrations are observed in and downwind of the major source
 regions.  Sharp concentration gradients are observed along the peripheries of the network. SO2
 concentrations are highest in the winter, whereas SO|- levels are highest in summer, reflecting
 significant photochemical activity in the summer months. Weekly average concentrations show
 significant week-to-week variability superimposed on the seasonal cycles.

 The pattern of annual NO3  levels is not as well correlated with the geographic distribution of
 NOX emissions as was SO2  and SO|-. Evidently,  the agricultural use of NH3 influences NO3
 aerosol formation as much  as the distribution of NOX sources. Annual HNO3 concentrations are
 lower along the Appalachian chain, reflecting loss processes induced by the presence of
 complex terrain. Annual levels of total NOj are lower generally in the southeast despite the
 fact that NOX emissions are about the same as  in the midwest, the  area with the highest
 observed NO3  levels. HNO3 concentrations are  higher in the summer throughout CASTNet.
 Total NO3 levels show little seasonal variability.

 CDN data show regional variability in aerosol speciation and acidity as well as concentration.
 The relationship between NH^ and SOJ" (molar basis) based on annual values for 1991 give an
 indication of the amount of neutralization of the  acidic SO£ aerosol. On the whole, the data
 suggest that aerosol acidity  is greater at forested sites than at agricultural sites. Ammonium is
 the predominant neutralizing cation with metal cations playing an insignificant role except at a
 few midwestern sites and sites near the coast.
The CASTNet measurements show statistically significant reductions in annual SO2, SO^, and
HNO3 concentrations averaged over all eastern sites. The data for the eastern sites combined
show a 23-percent reduction in SO|  and a 43-percent reduction in SO2 between 1989 and 1995
annual concentrations. These decreases do not account for the year-to-year variations in
concentrations between 1989 and 1995 and may not appear as large when the variations are
taken into account. Changes in sulfur species are more pronounced in the four northern
subregions and smaller, but still substantial, in the two southern subregions. There is no
apparent trend in the data from the western sites. The eastern data indicate about 70 percent of
ambient sulfur is in the form of SO2.
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SO2 concentrations show significant reductions in summer and winter seasons, even though
concentrations are much higher in winter and concentrations are more directly related to
emissions in the colder months.
The trend in summer average SOf" levels explains the decline in annual averages. Extending the
trend analysis by including the 1978 SURE measurements reinforces the demonstration of a
significant downward trend in SQ%~.

The slight reduction in HNO3 concentrations results from the decline in summer averages.  The
downward trend is observed in all of the subregions, except for the southern periphery and the
west. No trends are observed in annual concentrations of NO3 aerosol and total NOj.

The trend analyses presented herein are based on straightforward linear regressions. They do
not attempt to explain the causes of the downward trends. However, the percent reductions in
sulfur species are larger than can be explained by typical yearly meteorological variability. The
logical conclusion is a  significant relationship between the downward trend in concentrations
and the reported reductions in SOX emissions. In any event, EPA investigators  are pursuing
advanced statistical models of the trends in concentrations which will be published elsewhere.

4.3 Dry Depositions
The MLM was used to simulate deposition velocities of gases and aerosols using CDN
meteorological, land use, and vegetation data as input. Hourly deposition velocities were
calculated from the measurements and data.  Except for O3, the hourly deposition velocities
were averaged to obtain weekly average deposition velocities. Estimates of the uncertainties in
the simulated deposition velocities suggest the MLM results tend to underestimate observed
deposition velocities for SO2 and O3, especially daytime  values during periods Of plant growth.
The results for HNO3 and aerosols suggest the uncertainty is higher. Extrapolation of
deposition velocities from a specific CASTNet site to other locations should be done With
caution, especially in areas of complex terrain.

Weekly average concentrations were combined with weekly deposition velocities to calculate
weekly average dry depositions (fluxes).  The deposition data were then averaged to obtain
annual and seasonal averages. Maps of annual fluxes of total sulfur are discussed in Chapter 3.
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The distributions of annual dry sulfur depositions are similar from year to year and correspond
well with the maps of SO2 and SO^ concentrations and reflect the distribution of SOX sources.
Annual fluxes of total nitrogen show a fairly uniform pattern of depositions above 2.0 kg/ha (as
N) from year to year. Lower depositions were calculated for the CDN sites in the Appalachian
chain, similar to the results for HNO3 concentrations.

Time series of weekly fluxes show considerable site-by-site and weekly variability.  The
seasonal cycles of fluxes of individual species are similar to the seasonal behavior of
concentrations.  Scattergrams and correlation statistics show a strong relationship between
concentrations and depositions of SO2, SO|% and HNO3 measured in 1995.

Linear regressions were calculated for annual depositions of SO2, SO^, total sulfur, HNO3,
NO3,  and total NOj (as N) from 1989 through  1995 for all the eastern sites combined.
Downward trends are indicated for the sulfur species although the trend lines are not
considered statistically significant. The downward slopes for SO2 and total sulfur are greater
than for SOf,  consistent with the results for concentrations. The data show a 29-percent
reduction in deposition of SO2 (as S) and only a 6-percent reduction in deposition of SO|"
aerosol. These percentage reductions in depositions are lower than the comparable reductions
in concentrations.

The linear regressions show  no significant trends in depositions of the nitrogen species.
Depositions of sulfur and nitrogen species calculated for the western sites exhibit no trends.
4.4 Concentrations in Precipitation
Concentrations of anions and cations were measured in precipitation samples collected at
CASTNet sites and those NADP sites approximately collocated with CDN sites that do not
collect precipitation samples. The CDN and NADP data were combined to form one
concentration and wet deposition database. Geographic patterns of concentrations (in
precipitation) of SO*', NO3, and pH show some yearly variability while, at the same time,
reflect the distribution of major sources of SOX and NOX in the eastern United States. Summer
average concentrations of SOl  and NO3 in precipitation are higher and more variable than
corresponding winter values. Correlation analyses show a strong relationship between pH and
   l' levels and a reasonable relationship between pH and NO3. Annual  SOf concentrations
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exhibited statistically significant downward trends for the upper northeast and southern
periphery subregions. Although the eastern region did not exhibit a statistically significant
reduction, a downward trend is indicated by the data and analyses.

4,5  Wet Depositions
Wet deposition rates were calculated from the combined CASTNet and NADP database.
Patterns of wet SO^ depositions suggest an overall reduction in depositions between 1990 and
1994. In general, wet depositions decreased at a faster rate than concentrations.

Linear regressions of annual wet depositions of SO^' (as S) show statistically significant
downward trends for all the eastern sites combined.  The results show an overall decrease in
wet SO!" deposition of approximately 35 percent over the period 1989 to 1995.

No significant trends were indicated for wet NO| depositions. However,  the measurements still
show a reduction of about 20 percent for the eastern data combined over the 7-year period even
though the results are not considered statistically significant.

4.6 Total Deposition
Dry and  wet depositions were summed to obtain total depositions of sulfur and nitrogen
species.  Patterns of annual total depositions of sulfur again reflect the distribution of SOX
sources and the prevailing winds across the eastern United States. The percentages of total
deposition that are in the form of dry deposition show significant geographic variability. The
range in percentages varies from 14 to 60 percent. Dry deposition is a more significant
contributor hi and near the major source region. In areas with heavy precipitation, wet
deposition is much more important.  The estimates of dry deposition percentages are probably
low given the uncertainties in modeled deposition velocities.

The percentages of total nitrogen that occur as dry deposition are significant. Most of the sites
show a contribution of 40 percent or more. Again, the percentages are relatively lower in areas
of high terrain and areas with heavy rainfall. The  percentages are also lower at the remote
sites.
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 The total deposition data show statistically significant reductions in annual deposition of sulfur
 over the period 1989 through 1995. The downward trends are considered significant throughout
 the eastern network, except for the upper midwestern sites. No trend is apparent in the western
 data.

 Estimates of total deposition of nitrogen species exhibit no trend.

 4.7 Ozone
 The CDN O3 data provide estimates of exposure statistics and allow gauging compliance with
 the NAAQS for O3. During the summer of 1988, several sites measured concentrations above
 the 1-hour standard of 125 ppb. After 1988, violations of the NAAQS were limited to sites in
 the Washington-New York corridor. Concentrations above the new 8-hour standard of 85 ppb
 (3-year average of the fourth highest, daily running 8-hour average in each year) were
 measured throughout the midwest and northeast subregions.

 The measure SUM06 had been suggested as a secondary standard for O3. A majority of CDN
 sites show SUM06 values consistently above 25 ppm-hr, the proposed numerical limit.
 Another proposed measure W126 shows more geographic variability with fewer sites
 measuring values above 25 ppm-hr.

 The  O3 measurements show significant geographic differences which are influenced by a
variety of atmospheric processes (e.g., boundary layer effects, day-night differences in
photochemistry, and scavenging and dry deposition).  For example, mountaintop sites show
little diurnal variability and experience high exposure because of the locations of these sites
above ground-based inversions and their isolation from deposition processes and scavenging by
nighttime NOX emissions. On the other hand, suburban sites show large diurnal variability,
high short-term concentrations, and lower exposure statistics.
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4*8 Synopsis of CASTNet Measurements
A synopsis of CASTNet measurements for the 7-year period (1989 to 1995) is given in
Table 4-1. The table provides means and coefficients of variation for six air quality measures.
Overall means and CDN subregional and seasonal averages are provided. Results are given for
ambient concentrations, deposition velocities, dry deposition fluxes, and wet depositions.
Certain calculated ratios are also provided. The averages were calculated from annual (or
seasonal) averages for the group of CDN sites operating in each of the 7 years (seasons). The
dry and wet fluxes are given in terms of sulfur and nitrogen. Annual fluxes are given in units of
kg/ha per year. Seasonal fluxes  are given in units of kg/ha per season. The sum of four
seasonal fluxes equals the annual flux. The coefficients of variation represent Combined annual
(seasonal) - geographic variability.

The data hi Table 4-1 reinforce the discussions in Sections 4.2 through 4.7. The precursor gas
SO2 shows generally more variability than the reaction products like SO^ aerosol and the gas
HNO3, One exception is the annual coefficient of variation for NO3 aerosol, which is explained
by the fact that NO3 formation is influenced by NOX emissions and NH3 usage. Cdrieelitratidns
arid dry depositions are more variable than deposition velocities. Dry fluxes are fribre* variable
than wet fluxes.

Extremes in the measurements were generally observed in the summer and whiter, while values
more typical of CASTNet averages were observed in spring and fall. Peak concentratiofis and
dry depositions of SO^, O3, and HNO3 were observed in summer. Peak concentrations arid dry
depositions of SO2  were observed  in winter. Maximum values of wet deposition of siilfiif 2nd
nitrogen were observed hi summer and minimum values in winter.

The ratios hi Table 4-1  show the importance of SO2 and HNO3 hi contributing to the" dry
deposition of sulfur and nitrogen, respectively. The ratios show the importance of the
contribution of dry deposition processes to total deposition of sulfur arid nitrogen, especially
considering that dry deposition fluxes represent lower bound estimates.
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 4.9 Mountain Cloud Deposition Program
 MADPro is a component of CASTNet designed to study over several years the deposition of air
 pollutants to high elevation forests.  MADPro objectives are to measure cloud chemistry,
 determine total deposition, and define source regions which impact high elevation ecosystems
 in the eastern United States. MADPro has been in operation since 1994 at a few high elevation
 sites. The results to date show that cloudwater can be the primary pathway for deposition of
 pollution. MADPro results have been presented in annual reports for 1994, 1995, and 1996.
 Work has begun on modeling the various deposition pathways at these high elevation sites.

 4.10  Visual Air Quality
 An initial analysis of visual air quality measurements taken in 1994 was discussed.  The data
 show a strong relationship between atmospheric light scattering, visual quality,  and fine particle
 concentrations. Fine particle levels peaked in the summer and were highly correlated with fine
 atmospheric SO^. In the winter, NO^ and organic carbon contributed to fine mass loadings.
 Annual averages of fine mass concentrations are below the proposed NAAQS of 15 ,ug/m3.
 Light scattering increased as concentrations of fine particles and SO^- increased. Photographs
 of scenic vistas showed excellent visual  quality and content during periods of low fine particle
 and SO^ concentrations  and poor visual quality during periods of high concentrations.

 4.11  Other Studies
 EPA is sponsoring a series of field studies to measure directly dry deposition fluxes over a
 variety of land use and terrain settings to better understand deposition processes and to evaluate
 and improve the MLM and other models. Fluxes of SO2 and O3 are measured by eddy
 correlation.  HNO3 flux  is estimated by measuring the vertical gradient of HNO3
concentrations. The flux measurement system is supported by meteorological measurements
and a DAS.  The mobile system has  been used since 1994 to collect data at several  sites. The
resulting extensive database is being used by EPA investigators to evaluate and improve MLM.
The results will be published elsewhere.
CASTNet includes an intercomparison study between annular denuders and filter packs.  The
results to date show a high correlation between SO|- measurements using the two measurement
systems and similar results for SO2. HNO3 measurements on the filter packs are higher than the
denuder values. These results are considered preliminary while awaiting additional analyses.
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4.12  Data Completeness
This section provides an overview of the data completeness rules used for the various analyses
presented in this report.

4.12.1 Filter Pack Concentrations
The percent completeness statistics for filter pack concentration data for all CDN sites for years
1987 through 1995 are presented in Table 4-2. To be included in the 6-year average maps
(1989 to 1994), sites were required to have data for 5 of the 6 years with a 75-percent
completeness. In most cases, completeness exceeded 90 percent. This same requirement was
used in creating the single year plots for 1989, 1992, and 1994 (Figures 3-1 through 3-26).

Requirements for the sites used in the quarterly plots (Figures 3-27 and 3-28) were 70-perceiit
completeness per quarter. A 70-percent completeness rule was also used in selecting the sites
for the summer versus winter plots (Figures 3-29 through 3-40).
For Figures 3-42 and 3-43, the completeness requirement was 70 percent annually from 1989
through 1995. The only exceptions to this rule were Sites 151, with a 67-percent completion
rate in 1992, and Sites 114, 115, 123, and 135 with 69-, 56-, 69-, and 67-percent completeness
rates, respectively, in 1995. These lower completion rates were due to the shutdowii during the
fourth quarter.
Although a 50-percent completeness rate
3-3, there are only a handful of sites that
listed by year, are:
       1987 - Site 120  58 percent
       1988 - Site 109  50 percent
              Site 128  50 percent
       1989 - Site 111  58 percent
              Site 161  63 percent
              Site 162  67 percent
              Site 163  58 percent
              Site 164  58 percent
              Site 167  65 percent
              Site 169  63 percent
(i.e., 26 weeks) is specified on Tables 3-1 through
fall below a 70-percent completion rate. These sites,

                1992  - Site 151     67 percent
                1993  - Site 103/104 69 percelit
                       Site 164     6? percent
                1994  - Site 145     60 percent
                       Site 175     58 percent
                1995  - Site 114     69 percent
                       Site 115     56 percent
                       Site 123     69 percent
                       Site 135     67 percent
                       Site 138     67 percent
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The data used to produce these tables were also used to generate the regression plots in
Figures 3-44 through 3-48.

4.12.2  Filter Pack Deposition Velocities and Fluxes
Completeness percentages for all CDN sites by region for calculation of deposition velocities
and fluxes for the years 1987 through 1995 are presented in Table 4-3. The rules used for
calculation of Vd were as follows:
      1.    Seasonal averages — For calculation of seasonal averages by site, a season was
            required to have at least 8 non-missing weeks (62-percent completion rate) to be
            valid.  If a season had less than 8 non-missing weeks, the seasonal Vd was set to
            missing. For seasons with 8 or more non-missing weeks, the non-missing values
            were averaged by season.
      2.    Annual averages — For calculation of annual averages by site, a year was
            required to have at least 3 non-missing seasonal averages to be valid. If a year had
            less than 3 non-missing seasons,  the annual Vd was set to missing. For years with
            4 non-missing seasons, the seasonal Vds were averaged. For years with 3 non-
            missing seasons, the non-missing seasonal Vds were averaged.
      3.    Regional statistics — For calculation of regional statistics, the  site averages for the
            period in question (e.g., annual,  seasonal) were averaged.
The rules used for calculation of fluxes were as follows:
      1.    Seasonal sums — For calculation of seasonal sums by site, a season was required
            to have at least 8 non-missing weeks to be valid. If a season had less than 8 non-
            missing weeks, the seasonal flux was set to missing. For seasons with 8 or more
            non-missing weeks, the non-missing values were averaged by season and then
            multiplied by 13.
      2.    Annual sums — For calculation of annual sums by site, a year was required to
            have at least 3 non-missing seasonal sums to be valid. If a year had less than 3
            non-missing seasons, the annual flux was set to missing. For years with 4 non-
            missing seasons, the seasonal fluxes were summed. For years with 3 non-missing
            seasons, the non-missing seasonal fluxes were averaged and then multiplied by 4.
      3.    Regional statistics — For calculation of regional statistics, the site values  for the
            period in question (e.g., annual, seasonal) were averaged.
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These above rules were followed to produce Tables 3-7 through 3-11, Figures 3-52 through
3-62, and Figures 3-83 through 3-88. The five sites used in Figures 3-63 through 3-83 all apply
to this rule except for Site 137. Table 4-3 shows this site with two missing seasons in 1995.
However, since these figures are plotted on a weekly basis for 1995, and inclusion of a high
elevation site was desired for these comparisons, the site was used as the annual completeness
rate of 73 percent (using number of weeks with deposition values in 1995) was sufficient to
illustrate the desired comparisons between concentrations, Vds, and  fluxes.

4.12.3 Precipitation Concentrations and Depositions
Quarterly completeness percentages for all CDN wet deposition sites from 1989 through 1995
are presented in Table 4-4. All CDN precipitation sites plotted on the maps in Figures 3-89
through 3-106 and 3-135 through 3-145 had annual completeness rates of 85 percent or greater.
The sites used (Sites 114, 126, 128, 161, and 167) for the quarterly time series plots in
Figures 3-107 through 3-118 and 3-151 through 3-155 were required to have quarterly
completeness of 8 out of 13 weeks, or 62 percent, in order for a quarterly average to be
plotted. As shown in Table 4-4, however, rates this low were the exception for these sites. The
seasonal plots in Figures 3-119 through 3-124 and 3-146 through 3-150 also required the
selected sites to have 62-percent completeness for the season. The only instances completeness
rates were this low for a season occurred for winter 1995 during the shutdown period. For a
precipitation site to be included hi the regression analyses (Figures 3-127 through 3-134 and
3-156 through 3-160), a site was required to have an annual completeness rate of 70 percent.

4.12.4 Rolling 8-hour Ozone Concentrations
Annual fourth-highest daily maximum 8-hour O3 concentrations were calculated for all
available CASTNet data according to the data handling conventions and computational
standards  outlined in Appendix I of 40 CFR Part 50.  Methods and calculations are summarized
below.

The months comprising the O3 season vary by state (40 CFR Part 50). All available records for
each site/year/season were selected and processed. Completeness was determined by comparing
the number of valid records to the total possible days for each site/season. These values are
presented in Table 4-5.
                                          90

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Averages were calculated for each available consecutive 8-hour block of ozone monitoring
data. Averages, in ppb, were assigned to the beginning hour of each period. Blocks with fewer
than 6 valid hours were considered valid only if, after substituting 0.001 ppb for missing
values, the average exceeded the standard. Values were truncated to three decimal places.

Daily maxima were calculated for all days with 18 or more valid hours. Days with fewer than
18 valid hours, but a maximum exceeding the standard were also  considered valid.

The fourth-highest annual daily maximum value was selected for all sites with at least
75 percent of O3 season days having valid daily maximum values. In addition, years with fewer
than 75 percent valid hours but  fourth-highest values exceeding the standard were considered
valid.

Data completeness criteria were first applied to establish the validity of the period for each site.
Guidance includes exclusions for sites with less than 75-percent complete annual O3 season
data; these exclusions require overview by a Regional EPA Administrator and were not applied
for this analysis. Criteria are, in general, 75-percent completeness for each year and 90-percent
completeness for the period.  Fourth-highest annual daily maxima were averaged for each site
meeting completeness criteria. Values were rounded to two decimal places, with thousands of 5
and greater rounding up.  Rounded values of 0.09 (ppb) and greater were flagged as exceeding
the primary standard.
                                           91

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Chapter 5
Conclusions and Recommendations

5.1 Conclusions
CASTNet data precision and accuracy meet the EPA objectives. GASTNet data constitute all
exceptional database for understanding regional air quality and for supporting other scientific
activities.

CASTNet measurements collected over the period 1989 to 1995 are able to detect trends in
concentrations of acid gases and aerosols. Although the following results do not account for
variations in meteorology from year to year, concentration data still show statistically
significant reductions in annual SO2, SC£, and HNO3 levels, the eastern data show a
23-percent reduction in SO|" and a 43-percent reduction in SO2 between 1989 and 1995.
Extending the trend analysis by including the 1978 SURE measurements reinforces the
demonstration of a significant downward trend in SO|". The eastern data indicate about
70 percent of ambient sulfur is in the form of SO2.

The percent reductions in sulfur species are larger than can be explained by mete§f6l6gieai
variability. There is an apparent relationship between reductions in concentrations arid reported
reductions in emissions.

Concentration data show a slight decline in HNO3 levels.  No trends are observed in annual
concentrations of NOi aerosol and total NO3. HNO3 contributes about 65 percent of athbient
nitrogen throughout the network.

Data collected in the western network exhibit no trends.

 Estimates of the uncertainties in deposition velocities suggest the MLM results tend to
 underestimate observed Vd (and consequently fluxes) for SO2 and O3.  The uncertainty in Vd for
 HNQ3 and aerosols is higher.  Calculated dry depositions consequently represent lower bound
 estimates and do not account for quantified modeled uncertainties.

-------
Calculated annual fluxes show downward trends for the sulfur species although the trend lines
are not considered statistically significant. The eastern data show a 29-percent reduction in
deposition of SO2 (as S) and only a 6-percent reduction in deposition of SO^'. The calculated
reduction in total sulfur deposition is 27 percent. The eastern data indicate about 85 percent of
sulfur deposition is in the form of SO2.

No trends are apparent for the eastern nitrogen fluxes or in the depositions calculated for the
western sites.
Concentrations in precipitation of SO^, NOj, and pH show extensive spatial variability.
Precipitation concentrations of annual SO^ measured between 1989 and 1995 show significant
reduction for two subregions. Although the regression results for all eastern CDN and NADP
sites combined are not significant, a downward trend is indicated. Linear regressions of annual
     concentrations observed in precipitation show no significant trends.
Sulfate wet depositions (combined CDN/NADP database) averaged over the eastern sites show
a 35-percent reduction over the period 1989 to 1995. The results are considered statistically
significant.

Nitrate wet depositions show about a 20-percent reduction over the 7-year period although the
results are not considered statistically significant.

Estimates of total deposition show significant reductions in annual sulfur deposition for the
eastern sites combined over the period 1989 to 1995. No trend is evident in total depositions of
nitrogen.

O3 data show that 8-hour concentrations above the proposed primary NAAQS were measured
throughout most of the eastern network.

A majority of sites show SUM06 values consistently above 25 ppm-hr, the proposed numerical
limit.
                                           93

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The O3 measurements show significant geographic differences which are influenced by terrain
effects, atmospheric boundary layer scavenging and photochemistry.
The results to date from the MADPro show that cloudwater can be the primary pathway for
deposition of pollutants at high elevation sites.

Visual an: quality data show a strong relationship between light scattering, visual quality, and
fine particle concentrations.  Fine particles peaked in summer and were correlated with fine
  £ levels.
Light scattering increased as concentrations of fine particles and SOf increased. Photographs of
scenic vistas showed excellent visual quality and content during periods of low fine mass and
SO!' levels and the opposite during periods of high concentrations.

Annual concentrations of fine particles (<2.5 pan in diameter) are below the proposed NAAQS
of 15
5.2  Recommendations
CASTNet should be operated with minimum disruptions to continue the appropriate database
and allow for various analyses, including status and trends.

The number of CDN sites and site locations should be reviewed to optimize site locations for
improvement hi the several displays and analyses.

The MLM should continue to be evaluated and improved to reduce the uncertainties and
improve the precision hi the estimates of dry deposition. Model acceptance criteria should be
developed.

The mobile dry deposition field studies should continue until the MLM is fully evaluated and
flux calculations are representative of a wide variety of land use and terrain settings.
 Advanced statistical analyses need to be performed on the CASTNet data to elucidate the
 apparent trends and decipher trends not apparent from the simple linear regressions.

                                           94

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 Statistical analyses should investigate trends at individual sites as well as subregional averages
 in order to better understand the response to changes in emissions and meteorological
 fluctuations.

 RADM simulations should be performed as diagnostic tools to better explain the effects of
 photochemistry and precipitation scavenging on dry and wet deposition.

 The visual air quality data collected throughout the visibility network should be analyzed more
 thoroughly, including the use of absorbance data analyzed from the Teflon® filters. The
 absorbance data combined with the light scattering data provide an estimate of total light
 extinction.

 The visibility network should be continued and perhaps expanded to detect trends in visibility-
 related air quality parameters.

 MADPro data should continue to be analyzed to model the cloudwater pathway of deposition at
 high altitude locations.

 CASTNet has produced an exceptional database that satisfies many of the requirements of the
 CAAA of 1990.  The network will help assess compliance with the proposed NAAQS for O3
and fine particles and gauge progress toward attainment. It will continue to measure
improvements  hi air quality and depositions associated with CAA-mandated reductions in SOX,
NOX, and VOC emissions over the next 10 years.
                                          95

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                                       References
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       Classification System for Use with Remote Sensor Data. U.S. Geological Survey Circular 671.
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Air Resource Specialists, Inc. 1994. Site Selection for Optical Monitoring Equipment (IMPROVE
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Baumgardner, R.E., Kronmiller, K.G., Anderson, J.B., Bowser, J.J., and Edgerton, E.S.  1997.
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Clarke, J.F., and Edgerton,  E.S. 1993. Dry Deposition Flux Calculations for the National Dry
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Clarke, J.F., Ellestad, T.G., Finkelstein, P.L., Edgerton, E.S, and Bowser, J. 1995. Design and
       implementation of a  transportable system for direct measurement of dry deposition fluxes.
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Clarke, J.F., Edgerton, E.S., and Martin, B.E. 1997. Dry Deposition Calculations for the Clean Air
       Status and Trends Network. Atmos. Environ.  31:3667.

Dennis, R.L., McHenry, J.N., Barchet, W.R.; etal.  1993. Correcting RADM's sulfate
       underprediction: Discovery and correction of model errors and testing the corrections through
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Eager, C., and Adams, M.B., (Ed.)  1992. Ecology and Decline of Red Spruce in the Eastern United
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Environmental Science & Engineering, Inc. (ESE).  1990a.  National Dry Deposition Network (NDDN)
       Field Operations Manual.  Prepared for U.S. Environmental Protection Agency (EPA).
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Environmental Science & Engineering, Inc. (ESE).  1990b. National Dry Deposition Network (NDDN)
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                                             96

-------
                                     References (continued)
Environmental Science & Engineering, Inc. (ESE). 1991a. National Dry Deposition Network (NDDN)
       Data Management Manual. Prepared for U.S. Environmental Protection Agency (EPA).
       Contract No. 68-D2-4451.  Gainesville, FL.

Environmental Science & Engineering, Inc. (ESE). 1997. Comparison of CASTNet Filter Pack and
       Annular Denuder Samplers - Interim Data Report (October 1996 - February 1997). Draft
       Report. Prepared for U.S. Environmental Protection Agency (EPA). Contract No. 68-D2-
       4451.  Gainesville, FL.

Falconer, R.E. and P.D. Falconer. 1980. Determination of cloudwater acidity at a mountain
       observatory in the Adirondack Mountains of New York State. Journal of Geophysical
       Research 85C:7465-7470.

Gerber, H.  1984.  Liquid water content of fogs and hazes from visible light scattering. Journal of
       Climatology and Applied Meteorology 23:1247-1252.

Heisler, S. etal. 1990. Acid Model Operational Diagnostic Evaluation Study (Acid MODES) and
       Operational Evaluation Network (OEN). ENSR. Glastonbury, CT 06033.

Hicks, B.B., Baldocchi, D.D., Hosker, R,P., Jr., Hutchison, B.A., McMillen, R.T., and Satterfield,
       L.C.  1985. On the Use of Monitored Air Concentrations to Infer Dry Deposition (1985).
       NOAA Technical Memorandum ERLARL-141. 66pp.

Hornbeck, J.W., and R.B. Smith.  1985. Documentation of red spruce decline.  Canadian Journal of
       Forest Research, pp. 1199-1201.

Hosker, R.P., Jr. and Womack, J.D.  1986. Simple Meteorological and Chemical Filter Pack
       Monitoring System for Estimating Dry Deposition of Gaseous Pollutants,  in: Proceedings of
       the 5th Annual National Symposium on Recent Advances in the Measurement of Air Pollutants,
       Raleigh, NC, 14-16 May 1985, EPA/600/8-85/029 (available from NTIS, Springfield, VA),
       pp. 23-29.

James, K.O.W. 1993.  1991 Quality Assurance Report, NADP/NTN Deposition Monitoring.  Office of
       Atmospheric Chemistry.  Illinois State Water Survey.  Champaign, IL.

Lefohn, A.S. and Runeckles, V.C.  1987. Establishing a Standard to Protect Vegetation-Ozone
       Exposure/Dose Considerations.  Atmos. Environ. 21:561-568.

Lefohn, A.S., Laurence, J.A., and Kohut, RJ.  1988.  A Comparison of Indices that Describe the
       Relation Between Exposure to Ozone and reduction in the Yield of Agricultural Crops.
       Atmos. Environ. 22:1229-1240.

Li, Z. and V.P. Aneja.  1992.  Regional analysis of cloud chemistry at high elevations in the eastern
       United States. Atmos. Environ. 26A:2001-2017.
                                            97

-------
                                     References (continued)
Li-Cor, Inc. 1989.  LAI-2000 Plant Canopy Analyzer-Technical Information. LI-COR, Inc., 4421
       Superior Street, Lincoln, NE.

Lindberg, S.E., Silsbee, D., Schaefer, D.A., Owens, J.G., and Petty, W. 1988. A Comparison of
       Atmospheric Exposure Conditions at Low- and High-Elevation Forests in Southern Appalachian
       Mountain Range, pp. 321-344. In: M.H. Unsworth and D. Fowler, eds.  Acid deposition at
       High Elevation Sites, NATO ASI Series C:Vol.252, Klumer Publ., Boston.

McLaughlin, S.B.,  C.P. Anderson, N.T. Edwards, W.K. Roy and P.A. Layton. 1990. Seasonal
       patterns of photosynthesis and respiration of red spruce saplings from two exevations in
       declining Southern Appalachian Stands. Canadian Journal of Forest Research 20:485-495.

McLaughlin, S.B.,  C.P. Anderson, P.J. Hanson, M.G. Tjoelker and W.K. Roy. 1991. Increased park
       respiration and calcium deficiency of red spruce in relation to acidic deposition at high
       elevation Southern Appalachian Mountain sites. Canadian Journal of Forest Research
       21:1234-1244.

McMillen, R.T.  1990.  Estimating the Spatial Variability of Trace Gas Deposition  Velocities.  NOAA
       Tech. Memo. ERL ARL-181, 37 pp.

Meyers, T.P. and Yuen, T.S. 1987.  An Assessment of Averaging Strategies Associated with
       Day/Night Sampling of Dry-Deposition Fluxes of SO2 and O3.  /. Geophysic Res.
       92: 6705-6712.

Meyers, T.P., Hicks, B.B., Hosker, R.P., Womack, J.D., and Satterfield, L.C. 1991.  Dry deposition
       inferential measurement technique-II seasonal and annual deposition rates of sulfur and nitrate,
       Atmos. Environ. 25A(10): 2361-2370.

Mohnen, V.A. and J.A. Kadlecek. 1989. Cloud chemistry research at Whiteface Mountain.
       Tellus 41B:79-91.

Mohnen, V.A. and R.J. Vong.  1993. A climatology of cloud chemistry for the eastern United States
       derived from the Mountain Cloud Chemistry Project. Environ. Reviews 1:38-54,

Mueller, P. and Hidy, G.  1983.  The Sulfate Regional Experiment: Report of Findings, Vols. 1 and 2.
       EPRI. Palo Alto, CA. EPRIEA-1901.

Pierce, L.L. and Running, S.W.  1988.  Rapid Estimation of Coniferous Forest Leaf Area Index Using
       a Portable Integrating Radiometer.  Ecology 69(6): 1762-1767.

Saxena, V.K., R.E. Stogner, A.H. Hendler, T.P. DeFelice, RJ.-Y. Yeh and N.-H. Lin, 1989.
       Monitoring the  chemical climate of the Mt. Mitchell State Park for evaluation of its impact on
       forest decline.  Tellus 41B:92-109.
                                             98

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                                      References (continued)
 Schemenauer, R.S. and C. Winston, 1988.  The 1986 Chemistry of High Elevation Fog (CHEF)
        project.  81st Annual Meeting of the Air Pollution Control Association, 19-24 June  Dallas
        88-129.6:1-16.

 Schemenauer, R.S. 1986. Acidic deposition to forests: the 1985 Chemistry of High Elevation Fog
        (CHEF) project. Atmosphere-Ocean 24:303-328.

 Schemenauer, R.S., P.H. Schuepp,  S. Kermasha and P. Cereceda.  1988. Measurements of the
        properties of high elevation fog in Quebec, Canada. In:  Acid Deposition at High Elevation
        Sites, M.H. Unsworth and D. Fowler (Eds.), Kluwer Academic Publishing Dordrecht
        pp. 359-374.

 Shreffler, J.H. and Barnes, Jr., H.M. 1996. Estimation of Trends in Atmospheric Concentrations of
        Sulfate in the Northeastern United States. JAWMA 46:621-630.

 Sheih, C.M., Wesely,  M.L., and Hicks, B.B.  1979.  Estimated Dry Deposition Velocities of Sulfur
        Over the Eastern United States and Surrounding Waters.  Atmos. Environ. 13:1361-1368.

 U.S. Environmental Protection Agency (EPA). 1996. National Air Pollutant Emission Trends
        1990-1995. EPA-454/R-96-007. OAQPS, RTP, North Carolina 27711.

 U.S. Environmental Protection Agency (EPA). 1997. Examination ofCASTNet: Data, Results, Costs,
        and Implications  (Draft). ORD, Washington, DC 20460.

Vong, R.J., J.T. Sigmon and S.F. Mueller.  1991.  Cloud water deposition to Appalachian forests.
       Environ. Sci. Technol.  25:1014-1021.

Wesely, M.L. and Lesht, B.M. 1988. Comparison of RADM Dry Deposition Algorithm with a
       Site-Specific Method for Inferring Dry Deposition.  Water, Air, and Soil Pollution
       44: 273-293.
                                            99

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Table 2-1. Locations and Operational Dates of CDN Sites
Site
No.
Site Name
                             Latitude      Longitude
Operational
  Date(s)
Currently Active Sites

106       PSU, PA
107       Parsons, WV
108       Prince Edward, VA
109       Woodstock, NH
110       Connecticut Hill, NY
111       Speedwell, TN
112       Kane Experimental Forest, PA
113       M.K. Goddard State Park, PA
114       Deer Creek State Park, OH
115       Ann Arbor, MI
116       Beltsville, MD
117       Laurel Hill State Park, PA
119       Cedar Creek State Park, WV
120       Horton Station, VA
122       Oxford, OH
123       Lykens, OH
124       Unionville, MI
125       Candor, NC
126       Cranberry, NC
127       Edgar Evins State Park, TN
128       Arendtsville, PA
130       Bondville, IL
13If      Mackville, KY
132       Rowland, ME
133       Salamonie Reservoir, IN
134       Perkinstown, WI
135f      Ashland, ME
136       Crockett, KY
137       Coweeta, NC
138       Stockton, IL
139       Blackwater NWR, MD
140       Vincennes, IN
142       Beaufort, NC
144       Washington's Crossing, NJ
145       Lye Brook, VT
147       Abington, CT
149       Wellston, MI
150       Caddo Valley, AR
151       Coffeeville, MS
152       Sand Mountain, AL
40.73
39.09
37.17
43.94
42.40
36.47
41.60
41.43
39.63
42.60
39.03
40.00
38.88
37.33
39.53
40.92
43.61
35.26
36.11
36.04
39.92
40.05
37.70
45.22
40.82
45.21
46.61
37.92
35.05
42.29
38.35
38.70
34.88
40.31
43.04
41.86
44.22
34.18
34.00
34.29
77.93
79.67
78.31
71.70
76.65
83.83
78.77
80.15
83.26
83.92
76.82
79.17
80.85
80.55
84.72
83.00
83.36
79.84
82.04
85.73
77.31
88.37
85.05
68.71
85.66
90.60
68.41
83.06
83.43
90.00
76.11
87.49
76.60
74.88
73.06
72.00
85.82
93.10
89.80
85.97
01/06/87
01/14/88
11/01/87
12/31/88
09/14/87
06/30/89
12/31/88
01/08/88
09/30/88
06/30/88
12/31/88
12/10/87
11/09/87
06/03/87
08/18/87
09/30/88
06/30/88
09/30/90
12/31/88
03/22/88
06/30/88
02/09/88
07/31/90
12/01/92
06/30/88
09/30/88
12/31/88
08/24/93
11/03/87
01/01/94
07/01/95
08/05/87
01/08/94
12/31/88
01/01/94
01/15/94
06/30/88
09/30/88
12/31/88
12/31/88
 p/castnet/wa24/anrpt-2v

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 Table 2-1. Locations and Operational Dates of CDN Sites (Continued, Page 2 of 3)
Site
No.
153
156
157
161
165
169
175
181
MADPro
300
301
302
303
Site Name
Georgia Station, GA
Sumatra, FL
Alhambra, IL
Gothic, CO
Pinedale, WY
Centennial, WY
Claryville, NY
Egbert, Ontario
Sites
Whiteface Mountain, NY
Hunter Mountain, NY
Whitetop Mountain, VA
Clingman's Dome, TN
Latitude
(°)
33.18
30.11
38.87
38.96
42.93
41.31
42.20
44.23

44.23
41.10
36.38
35.34
Longitude
(°)
84.41
84.99
89.62
106.99
109.79
106.15
74.25
79.78

73.59
74.14
81.36
83.29
Operational
Date(s)
06/30/88
12/31/88
06/30/88
06/30/89
12/31/88
06/30/89
01/15/94
11/01/89

Seasonal
Seasonal
Seasonal
Seasonal
NPS Deposition Sites

401       Big Bend NP, TX
402       Sequoia, CA
403       Joshua Tree NM, CA
404       Yosemite NP, CA
405       Mesa Verde NP, CO
406       Rocky Mountain NP, CO
407       Canyonlands NP, UT
408       Yellowstone NP, WY
409       Mount Rainier NP, WA
410       Lassen Volcanoes NP, CA
411       Great Basin NP, NV
412       Death Valley NM, CA
413       Voyageurs NP, MN
414       Pinnacles NM, CA
415       Northern Cascades NP, WA
418       Big Meadows, VA*
467       Chiricahua NM, AZ*
468       Glacier NP, MT*
474       Grand Canyon NP, AZ*

Visibility Sites

510       Connecticut Hill, NY
513       M.K. Goddard, PA
518       Shenandoah Mountain Park, VA**
29.31
36.50
34.07
36.43
37.20
40.28
38.46
44.39
46.76
40.54
39.01
36.51
48.41
36.49
48.54
38.52
32.01
48.51
36.06
103.18
118.70
116.39
118.76
108.49
105.55
109.82
110.39
122.12
121.57
114.22
116.85
92.83
121.16
121.45
78.44
109.39
113.99
112.18
07/18/95
02/25/97
02/16/95
09/25/95
01/10/95
09/27/94
01/24/95
06/26/96
08/29/95
07/25/95
05/16/95
02/20/95
06/13/96
05/16/95
02/14/96
06/30/88
07/01/89
01/01/89
07/01/89
42.40
41.43
38.52
76.65
80.15
78.44
09/20/93
09/17/93
10/18/93
p/castnet/wa24/anrpt-2v

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Table 2-1.  Locations and Operational Dates of CDN Sites (Continued, Page 3 of 3)
Site
No.
528
530
570
571
572
573
Special
180
182
183
Site Name
Arendtsville, PA
Bondville, IL
Sikes, LA
Cadiz, KY
Quaker City, OH
Livonia, IN
Study Sites
Scotia Range, PA (wet deposition only)
Coweeta, NC (ridge)
Woodstock, NH (ridge)
Latitude
(°)
39.92
40.05
32.07
36.78
39.94
38.58

40.79
35.05
43.95
Longitude
(°)
77.31
88.37
92.46
87.85
81.34
86.26

77.92
83.44
71.70
Operational
Date(s)
09/16/93
09/24/93
06/10/93
09/16/93
07/24/93
12/31/88

10/01/93
06/27/91-09/30/92
08/11/91-09/30/92
Discontinued Sites
101
102
103
104
105
121
129
146
162
163
164
Research Triangle Park, NC
Oak Ridge, TN
West Point-A, NY
West Point-B, NY
Whiteface Mountain, NY
Lilley Cornett Woods, KY
Perryville, KY
Argonne, IL
Uinta, UT
Reynolds Creek, ID
Saval Ranch, NV
35.91
35.96
41.35
41.35
44.39
37.13
37.68
41.70
40.55
43.21
41.29
78.88
84.29
74.05
74.05
73.86
82.99
84.97
88.00
110.32
116.75
115.86
01/01/87-01/01/90
01/01/87-01/01/89
01/01/87-10/01/88
01/01/87-10/01/93
01/01/87-04/01/93
01/19/88-12/31/93
08/11/87-07/01/90
07/01/87-04/01/93
07/01/89-10/01/93
06/30/89-10/01/93
06/30/89-10/01/93
 *Former EPA CASTNet site.
 fCurrent collocated site.
 """Collocated with IMPROVE aerosol sampler.

 Source:  QST.
 p/castnet/wa24/ampt-2v
                                                                                                   .

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Table 2-2.  Deployment History of the CDN
Year
1988
1989
1990
1991
1992
1993
1994
1995
1996

Eastern
16
41
41
41
41
42
46
45
13
No. of Sites*
Western
0
2
9
9
9
9
6
6
2

Total
16
43
50
50
50
51
52
51
15
"Indicates number of sites in operation as of January 1.




Source: QST.
p/castnet/wa24/anrpt-2v

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Table 2-3.  Site-Selection Criteria for CDN Sites
Potential Interferant
Minimum Acceptable
   Distance (km)
SO2 or NOX Pt. Source > 100 tpy
SO2 or NOX Pt. Source > 1,000 tpy
Major Industrial Complex
Town, population 1,000 - 10,000
Town, population 10,000 - 25,000
City,  population 15,000-50,000
City,  population > 50,000
Major highway, airport, railway
Secondary road, heavily traveled
Secondary road, lightly traveled
Feedlot operations
Intensive agricultural activities
Limited agricultural activities
Parking lot or large paved area
Building with fuel combustion
Sewage treatment plant
Forced main vent or lift station
Tree line
Complex terrain
         20
         40
         10
          5
         10
         20
         40
          2
          0,5
          0.2
          0.5
          0.5
          0.1
          0.2
          0.2
          1.0
          0.2
          0.1
        variable
Note:  km — kilometer.
Source:  QST.
p/c*stnet/wa24/ampt-2v

-------
 Table 2-4.  CDN Site Listing
Site
No.
104
105

106
107
108

109
110
111
112

113
114

115
116
117

118
119
120
121

122
123
124
125
126
127

128
129
130
131
132
133
134
135
136
137
138
139
140
142
144

145
146

147
149
150
151
152
Site Name
West Point, NY
Whiteface
Mountain, NY
PSU, PA
Parsons, WV
Prince Edward,
VA
Woodstock, NH
Connecticut Hill,
NY
Speedwell, TN
Kane Experimental
Forest, PA
M.K. Goddard, PA
Deer Creek State
Park, OH
Ann Arbor, MI
Beltsville, MD
Laurel Hill State
Park, PA
Big Meadows, VA
Cedar Creek State
Park, WV
Horton Station, VA
Lilley Cornett
Woods, KY
Oxford, OH
Lykens, OH
Unionville, MI
Candor, NC
Cranberry, NC
Edgar Evins State
Park, TN
Arendtsville, PA
Perryville, KY
Bondville, IL
Mackville, KY
Howland, ME
Salamonie, IN
Perkinstown, WI
Ashland, ME
Crockett, KY
Coweeta, NC
Stockton, IL
Blackwater NWR, MD
Vincennes, IN
Beaufort, NC
Washington's
Crossing, NJ
Lye Brook, VT
• Argonne National
Laboratory, IL
Abington, CT
Wellston, MI
Caddo Valley, AR
Coffeeville, MS
Sand Mountain, AL
Initial
Reporting
Date
01/06/87
01/06/87

01/06/87
01/14/88

11/01/87
12/31/88
09/14/87
07/01/89
12/31/88

01/08/88
09/30/88

06/30/88
12/31/88
12/10/87

06/30/88
11/09/87
06/03/87
01/19/88

08/18/87
09/30/88
06/30/88
09/30/90
12/31/88
03/22/88

06/30/88
06/88
02/09/88
07/31/90
12/01/92
06/30/88
09/30/88
12/31/88
08/24/93
11/03/87
01/01/94
07/01/95
08/05/87
01/08/94
12/31/88

01/01/94
07/01/87

01/15/94
06/30/88
09/30/88
12/31/88
12/31/88
Latitude
41.35
44.39

40.73
39.09

37.17
43.94
42.40
36.47
41.60

41.43
39.63

42.42
39.03
40.00 •

38.52
38.88
37.33
37.08

39.53
40.92
43.61
35.26
36.11
36.04

39.92
37.68
40.05
37.70
45.22
40.82
45.21
46.61
37.92
35.06
42.29
38.35
38.74
34.88
40.30

43.04
41.70

41.86
44.22
34.18
34.00
34.29
Elevation
Longitude (m)
74.05
73.86

77.95
79.66

78.31
71.70
76.65
83.83
78.77

80.15
83.26

83.90
76.82
79.25

78.44
80.85
80.55
82.99

84.72
83.00
83.36
79.84
82.04
85.73

77.31
84.97
88.37
85.05
68.71
85.66
90.60
68.41
83.06
83.43
90.00
76.11
• 87.49
76.60
74.87

73.06
87.99

72.00
85.82
93.10
89.80
85.97
203
570

378
510

146 .
258
515
361
622

384
265

267
46
615

1,073
234
920
335

284
303
201
198
1,219
302

269
279
212
353
69
249
472
235
455
686
274
—sea level
134
— sea level
58

730
229

209
295
71
134
352
Primary
Land
Use
Forested
Forested

Agricultural
Forested

Forested
Forested
Forested
Agricultural
Forested

Forested
Agricultural

Forested
Urban-Agric.
Forested

Forested
Forested
Forested
Forested

Agricultural
Agricultural
Agricultural
Forested
Forested
Forested

Agricultural
Agricultural
Agricultural
Agricultural
Forested
Agricultural
Agricultural
Agricultural
Agricultural
Forested
Agricultural
Wetland
Agricultural
Agricultural
Agric.-Urban

Forested
Urban-Agric.

Urban-Agric.
Forested
Forested
Forested
Agricultural
Terrain
Complex
Complex

Rolling
Complex

Rolling
Complex
Rolling
Rolling
Rolling

Rolling
Rolling

Flat
Flat
Complex

Mountaintop
Complex
Mountaintop
Complex

Rolling
Flat
Flat
Rolling
Mountaintop
Rolling

Rolling
Rolling
Flat
Rolling
Rolling
Flat
Rolling
Flat
Flat and Open
Complex
Rolling and Open
Coastal Plain
Rolling
Flat and Open
Rolling

Complex
Flat

Complex
Flat
Rolling
Rolling
Rolling
p/casmet/wa24/anrpt-2v

-------
Table 2-4. Continued, Page 2 of 2
Site
No.
153

156
157
161
162
163
164
165
167
168

169
174
175
181
Site Name
Georgia Station,
GA
Sumatra, FL
Alhambra, IL
Gothic, CO
Uinta, UT
Reynolds Creek, ID
Saval Ranch, NV
Pinedale, WY
Chiricahua, AZ
Glacier National
Park, MT
Centennial, WY
Grand Canyon, AZ
Claryville, NY
Egbert, Ontario
Initial
Reporting
Date
06/30/88

12/31/88
06/30/88
07/01/89
07/01/89
07/01/89
07/01/89
12/31/88
07/01/89
12/31/88

07/01/89
07/01/89
01/15/94
11/01/89
Latitude
33.18

30.11
38.87
38.96
40.55
43.21
41.29
42.93
32.01
48.51

41.31
36.06
42.20
44.23
Longitude
84.41

84.99
89.62
106.99
110.32
116.75
115.86
109.79
109.39
114.00

106.15
112.18
74.25
79.76
Elevation
(m)
270

14
164
2,926
2,500
1,198
1,873
2,388
1,570
963

2,579
2,073
825
251
Primary
Land
Use
Agricultural

Forested
Agricultural
Range
Range
Range
Range
Range
Range
Forested

Range
Forested
Forested
Agricultural
Terrain
Rolling

Flat
Flat
Complex
Complex
Rolling
Rolling
Rolling
Complex
Complex

Complex
Complex
Complex
Rolling
Source:  QST.
p/casmet/wa24/anrpt-2v

-------
 Table 2-5. Precision and Accuracy Objectives of CDN Field Measurements
Measurement
Parameter
Windspeed
Wind Direction
Sigma Theta
Relative Humidity
Solar Radiation
Precipitation
Ambient Temperature
Delta Temperature
03
Filter Pack Flow
Surface Wetness
Objectives*
Method
Anemometer
Wind Vane
Wind Vane
Hygrometer
Pyranometer
Rain Gauge
Platinum RTD
Platinum RTD
UV Absorbance
Mass Flow Controller
Conductivity Bridge
Precision
.+0.5 m/sec
±5°
±10%
±10% (of
full scale)
±10% (of
reading
taken at
local noon)
±10% (of
reading)
±0.5°C
±0.25°C
±10% (of
reading)
±0.15 L/min
Undefined
Accuracy
the greater of
±0.2 m/sec or
±5%
±5°
Undefined
±10% (of
full scale)
±10%
±0.05 inch*
±0.25 °C
±0.25°C
±10%
±10%
Undefined
Note:    m/sec = meters per second.
          RTD = resistance-temperature device.

 'Precision criteria apply to collocated instruments, and accuracy criteria apply to calibration of
 instruments.
fFor target value of 0.50 inch.

Source:  QST.
p/castnet/wa24/anrpt-2v

-------
Table 2-6.  Chemical Analysis of Samples Plus QC Solutions (Periods of Record)
   Sample Medium
       Analyte(s)
Period of Record
Teflon® filter extract

Teflon® filter extract

Teflon® filter extract

Nylon filter extract

Whatman filter extract

Precipitation samples



Fine particulate filters

Coarse particulate filters
SOI; NO;

NHJ

Na+, K+, Ca2+, Mg2+

SOI, NO;

SO2,', NO;

pH, conductivity, acidity,
C1-, NO;, NO;, SOI;
NHJ, Na+, K+, Ca2+, Mg2+

Tare/final mass

Tare/final mass
 1/87 - present

 6/88 - present

 6/88 - 9/89

 1/87 - present

 1/87 - present

 1/89 - present



 1/89 - 12/89

 1/89 - 12/89
Note:    Precipitation and particulate filters collected at selected sites, other analyses performed for
         all CDN sites.

Source:  QST.
p/casmet/wa24/ampt-2v

-------
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-------
Table 2-9.  Precision and Accuracy Objectives for CDN Laboratory Data
Objectives*
Analyte
pH*
Conductivity
Acidity
NHJ
Na+
K+
Mg2+
Ca2+
CI-
NQ;
NO;
so2-
Medium
W
W
W
W/F
W/F
W/F
W/F
W/F
W
W
W/F
W/F
Precision
Method (RPD)
Electrometric
Electrometric
Titrimetric
Automated colorimetry
ICP-AE
Flame atomic emission
ICP-AE
ICP-AE
1C
1C
1C
1C
12
10
15
10
10
10
10
10
5
5
5
5
Accuracy
88-
90-
85-
90-
90-
90-
90-
90-
95-
95-
95-
95-
112
110
115
110
110
110
110
no
105
105
105
105
Note:        W = wet deposition samples.
             F = filter pack samples.
             1C = ion chromatography.
        ICP-AE = inductively coupled plasma - atomic emission.
          RPD = relative percent difference.

*Precision and accuracy criteria represent ±0.05 pH unit.

Source: QST.
 p/castnet/wa24/ampt-2v

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-------
 Table 2-11.  Operational Dates for Collocated Filter Pack Monitoring Sites
Site
107/207
114/214
128/228
131/231
153/253
156/256
157/257
163/263
167/267
Beginning
Date
04/01/89
10/01/90
10/01/90
01/01/93
04/01/89
10/01/90
04/01/89
10/01/90
01/01/90
Ending
Date
09/30/90
09/30/92
06/30/95
09/30/95
09/30/90
03/31/93
09/30/90
12/31/92
09/30/92
 Source: QST.
p/castnet/wa24/anrpt-2v

-------
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-------
Table 2-14.  Summary Results of External QA Performance Audits of Monitoring Sites for 1994
Site
No.
107
108
109
110
111
114
115
118
119
120
122
123
124
125
126
127
130
131
132
133
134
135
137
138
140
142
144
145
149
150
151
152
153
156
157
161
165

167
168
169
174
Audit
Date
05/03/94
05/08/94
06/25/94
06/20/94
12/01/94
04/22/94
04/25/94
05/09/94
05/05/94
05/06/94
04/21/94
04/23/94
04/26/94
05/07/94
12/06/94
12/03/94
11/14/94
11/30/94
06/28/94
11/16/94
11/10/94
06/26/94
12/05/94
11/12/94
11/17/94
05/11/94
06/17/94
06/23/94
04/27/94
03/28/94
03/26/94
03/24/94
03/23/94
04/02/94
11/19/94
10/12/94
10/09/94

10/16/94
10/06/94
10/10/94
10/14/94
T
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
ii
|T
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P

P
P
P
P
Delta
T
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
I
:•:•&
P
P
P
P
RH
*
fr
p


p
p
11
F
p
p
p
m
P*
p
p
p
p
ii
P
p
p
p
p
p
!i
H
fr
p
p
p
m
P,
p
ii
fr
p

p
p
p
p
SR
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
i
P
P
P
P
P
P
P
P
P
P
P
P

P
P
i
p
Rain- Wind-
fall speed
P
P
P
P
P
P
P
P
P
P
1
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
1
P
P

P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P

P
P
P
P
Wind
Direc-
tion
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P

P
P
P
P
Filter
Pack
O3 Flow
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
NA
P
P
P
P
P
P
P
P
P

P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
i|
T
p
p
p
p
p
p
p
p
p
p
p
p
p
p
p

p
p
p
p
Wet-
ness
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P
P

P
P
P
P
p/castnet/wa24/anrpt-2v
-------
 Table 2-14. Continued, Page 2 of 2

Site
No.
175
231

Audit
Date
06/30/94
11/30/94

Delta
T T
•Iff! #&
•m*.- ;fx-
m <&•
1 P


RH
P
P


SR
P
P

Rain-
fall
P
P

Wind-
speed
P
P
Wind
Direc-
tion
P
P


03
NA
P
Filter
Pack
Flow
P
P

Wet-
ness
P
P
 Failures                  22122       1020       0

  Total Failures           12

 Warnings                 109       00       0       0      0       1       0

  Total Warnings          11
 Note:          | = fail.
              NA = not applicable.
                P = pass.
              RH = relative humidity.
              SR = solar radiation.
                T = temperature.
              HIH warning.

 Source:  QST.
p/castnet/wa24/ampt-2v
-------
Table 2-15.  Summary Statistics of External QA Performance Audits of Monitoring Sites for 1994
                                First
                               Quarter
Second
Quarter
 Third
Quarter
Fourth
Quarter
Total
Number of Sites Audited            5

Number of Sensors Audited        50

Number of Sensor Failures          0

Number of Sensor Warnings        1

Percent Failure                   0.0

Percent Warning                  2.0
  20

  200

   5

   7

  2.5

  3.5
   0

   0

   0

   0

   0

   0
   18

  180

   7

   3

  3.9

  1.7
 43

 430

 12

 11

 2.7

 2.6
Source: QST.
p/castnet/wa24/anipt-2v
-------
 Table 2-16.  Summary Statistics for Collocated Filter Pack Data for All Years, 1987 through 1995
Site
107





114





128





131





153





156





157






MeanX*
Mean Y*
N
RPD
Median AD
Median APD
MeanX*
Mean Y*
N
RPD
Median AD
Median APD
MeanX*
MeanY*
N
RPD
Median AD
Median APD
MeanX*
MeanY*
N
RPD
Median AD
Median APD
MeanX*
Mean Y*
N
RPD
Median AD
Median APD
MeanX*
MeanY*
N
RPD
Median AD
Median APD
MeanX*
MeanY*
N
RPD
Median AD
Median APD
SOf
7.58
7.65
77.00
-0.90
0.11
2.03
6.34
6.14
96.00
3.19
0.23
4.67
5.95
6.02
231.00
1.03
0.14
2.63
6.68
6.46
129.00
3.26
0.30
5.77
6.56
6.56
68.00
0.09
0.19
4.12
3.90
3.79
114.00
2.76
0.13
3.50
6.94
6.87
79.00
0.98
0.10
1.30
NO;
0.65
0.58
77.00
10.59
0.07
16.46
1.64
1.59
96.00
3.03
0.10
7.80
1.54
1.59
231.00
-3.42
0.09
8.18
1.01
0.99
129.00
2.72
0.05
6.99
0.43
0.40
68.00
7.61
0.04
14.95
0.48
0.48
114.00
-1.22
0.03
9.36
2.56
2.50
79.00
2.34
0.09
4.80
NHJ
1.83
1.84
77.00
-0.83
0.04
2.45
2.41
2.35
96.00
2.72
0.08
3.93
2.26
2.26
230.00
-0.04
0.05
2.63
2.24
2.15
128.00
4.02
0.11
5.60
1.87
1.82
67.00
2.54
0.07
5.11
0.83
0.81
111.00
2.03
0.03
3.85
2.83
2.77
79.00
1.96
0.04
1.94
HN03
2.09
1.93
79.00
7.90
0.15
6.50
2.91
2.91
72.00
-0.13
0.12
4.68
3.47
3.46
231.00
0.24
0.30
9.58
3.03
2.93
131.00
3.44
0.14
5.77
2.25
2.29
70.00
-1.86
0.11
6.21
1.01
1.03
88.00
-2.66
0.06
6.40
2.48
2.40
81.00
3.36
0.11
4.49
SO2
12.34
11.94
79.0
3.26
0.46
4.46
12.71
12.54
72.00
1.38
0.45
4.86
14.43
14.44
231.00
-0.03
0.49
4.09
9.81
9.48
131.00
3.37
0.41
4.92
7.83
7.90
70.00
-0.81
0.25
4.30
2.23
2.31
89.00
-3.86
0.14
7.12
12.65
12.28
81.00
2.95
0.32
2.67
Total
NO;
2.68
2.47
77.00
8.38
0.22
8.62
4.53
4.48
72.00
1.15
0.19
4.91
4.95
5.00
231.00
-0.91
0.29
6.08
4.01
3.88
129.00
3.26
0.18
5.20
2.66
2.67
68.00
-0.54
0.13
6.30
1.48
1.50
87.00
-1.79
0.08
5.88
4.99
4.85
79.00
2.94
0.15
2.94
p/castnet/wa24/anrpt-2v
-------
Table 2-16. Continued, Page 2 of 2
Site
163





167






MeanX*
MeanY*
N
RPD
Median AD
Median APD
MeanX*
MeanY*
N
RPD
Median AD
Median APD
sol-
0.70
0.69
114.00
1.10
0.02
2.60
1.43
1.44
172.00
-0.77
0.02
1.63
NO;
0.59
0.59
114.00
-0.46
0.02
5.22
0.29
0.29
172.00
-1.46
0.02
6.33
NHJ
0.37
0.37
113.00
-0.99
0.01
2.88
0.47
0.47
172.00
-0.78
0.01
2.01
HNO3
0,37
0.36
113.00
1.30
0.01
4.58
0.64
0.64
146.00
0.47
0.02
3.32
S0?
0.29
0.29
113.00
0.03
0.02
7.10
1.98
2.01
146.00
-1.49
0.05
3.37
Total
NO;
0.95
0.95
113.00
0.15
0.02
3,39
0.93
0.93
146.00
-0.15
0.03
2.93
Note:      median AD — median absolute difference.
         median APD = median absolute percent difference.
        mean X and Y = mean value for primary and collocated sensors, respectively.
                 RPD = relative percent difference.

* Values in /*g/m3.

Source:  QST.
 p/cistnet/wa24/anrpt-2v
-------
  Table 2-17.
Network Precision Values for Filter Pack Data as Estimated from Collocated Sampling Results
Presented as Absolute RPDs, Averaged Over All Years, All Sites
 sol
    NO;
NHJ
                                      HNO,
                                                                         SO,
                                                   Total NO;
  1.56
   3.65
                                     1.77
                                       2.3.7
                                                                         1.91
                                                                           2.14
 Source: QST.
p/castnet/wa24/anrpt-2v
-------
Table 2-18. Summary Statistics for Collocated Filter Pack Data for 1994
Site
128 Mean X*
MeanY*
N
RPD
Median AD
Median APD
131 Mean X*
MeanY*
N
RPD
Median AD
Median APD
SOJ
5.88
5.82
50.00
1.16
0.16
2.72
6.59
6.43
43.00
2.55
0.29
4.65
N0i
1.22
1.29
50.00
-5.04
0.15
17.04
0.99
0.95
43.00
3.83
0.04
6.19
NHJ
2.11
2.10
50.00
0.40
0.07
3.66
2.14
2.05
43.00
4.16
0.09
4.51
HNO3
4,18
3.69
50.00
12.60
0.46
12.83
2.94
2.86
44.00
2.86
0.14
5.56
SO2
15.61
14.94
50.00
4.40
0.50
3.56
9.89
9.59
44.00
3.05
0.36
3.93
Total NOj
5.34
4.91
50.00
8.28
0.40
8.73
3.90
3.78
43.00
3.06
0.18
4.83
Note:      median AD = median absolute difference.
         median APD = median absolute percent difference.
        mean X and Y = mean value for primary and collocated sensors, respectively.
                 RPD = relative percent difference.

* Values in /ig/m3.

Source:  QST.
p/castnet/wa24/ampt-2v
-------











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-------
 Table 2-21.  Summary Statistics for Collocated Wet Deposition Data for All Years, 1989 to 1995
Parameter
Site 128
Ca2+
H+
Mg2+
Na+
NHJ
NOj
Rain
SO|
Site 157
Ca+
H+
Mg2+
Na+
NH+
NO;
Rain
SO?
MeanX*

13.50
70.13
3.53
6.39
33.68
46.66
1.80
87.17

15.69
37.80
3.52
3.90
31.50
29.02
1.89
56.33
MeanY*

13.61
75.80
3.86
7.30
40.48
49.60
1.76
87.08

16.68
36.59
3.72
3.99
28.55
30.57
1.97
.56.05
N

107
100
107
107
107
107
124
107

85
80
85
85
85
85
110
85
RPD

-0.79
-7.77
-8.95
-13.41
-18.32
-6.11
1.87
0.11

-6.16
3.24
-5.47
-2.23
9.82
-5.20
-4.06
0.50
Median AD

1.70
4.50
0.33
0.41
2.22
2.27
0.08
4.38

1.80
3.75
0.63
0.48
2.78
1.56
0.10'
3.96
Median APD

25.09
9.00
16.83
13.30
11.31
7.77
6.40
8.21

19.14
13.75
20.11
19.20
11.20
9.22
7.73
7.86
* Values in /tg/m3.




Source:  QST.
p/castnet/wa24/anrpt-2v
-------
Table 2-22. Operational Dates of Collocated Wet Deposition Monitoring Sites
Site
  ; inning
 Date
Ending
  Date
157/257

128/228
8/10/93

9/18/90
9/19/95

1/26/93
Source:  QST.
p/castnet/wa24/ampt-2v
-------
 Table 2-23.   Network Precision Values for Wet Deposition Data as Estimated from Collocated Sampling
              Results, Presented as Absolute RPDs, Averaged Over All Years, All Sites
                     Parameter
                                                                  RPD
                        Ca2+

                        H+

                        Mg2+

                        Na+
                        NO;
                        Rain
 3.48

 5.50

 7.21

 7.82

14.07

 5.66

 2.96

 0.30
Note:  RPD = relative percent difference.

Source:  QST.
p/castnet/wa24/anrpt-2v
-------
Table 2-24. Summary Statistics for Collocated Wet Deposition Data for 1994
Parameter
Ca2*
H+
Mg2+
Na2+
NHJ
NO]
Rain
sol
MeanX*
16.72
41.17
3.82
3.66
31.42
30.91
1.49
61.08
MeanY*
20.85
38.54
4.60
4.16
31.72
33.61
1.60
63.82
N
44
41
44
44
44
44
51
44
RPD
-21.95
6.53
-18.74
-12.73
-0.95
-8.36
-6.75
-4.39
Median AD
1.35
3.30
0.54
0.55
2.44
1.21
0.10
2.08
Median APD
17,98
9.32
14.72
19.15
9.92
6.01
12.50
5.80
Note:      median AD  = median absolute difference.
          median APD  = median absolute percent difference.
        mean X and Y  = mean value for primary and collocated sensors, respectively,
                 RPD  = relative percent difference.

*Values in /ig/m3, except rain which is millimeters.

Source:  QST.
 p/castnct/wa24/anrpt-2v
-------








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-------
Table 3-4. Results of Linear Regression Analysis on Annual and Seasonal SO2 Concentrations
Average Upper
Statistics Northeast
Annual
r-squared
P
slope
significant?
Summer fJun-Aug">
r-squared
P
slope
significant?
Winter (Dec-Febl
r-squared
P
slope
significant?

0.92
0.0001
-0.37
Yes

0.58
0.02
-0.18
Yes

0.96
0.0001
-0.71
Yes
Northeast

0.65
0.008
-0.63
Yes

0.52
0.03
-0.47
Yes

0.45
0.05
-0.94
Yes.
Upper
Midwest

0.83
0.004
-0.48
Yes

0.89
0.002
-0.29
Yes

0.66
0.03
-0.33
Yes
Midwest

0.75
0.006
-1.01
Yes

0,66
0.010
-1.13
Yes

0.44
0.07
-0.69
No
South
Central

0,69
0.04
-0.87
Yes

0,65
0.008
-0.58
Yes

0.49
0.03
-1.78
Yes
Southern
Periphery

0,60
0.006
-0.21
Yes

0.40
0.12
-0.12
No

0.18
0.34
-0.14
No
West

0.29
0.21
+0.02
No

ND
NO
ND
ND

ND
ND
ND
ND
East

0.83
0.0007
-0.73
Yes

ND
ND
ND
ND

ND
ND
ND
ND
Note: ND = not determined.



Source: QST.
    p/castnet/w«24/anrpt-3v,wpd
-------
 Table 3-5. Results of Linear Regression Analysis on Annual and Seasonal SO^ Concentrations
Average Upper
Statistics Northeast
Annual
r-squared
P
slope
significant?
Summer (Jun-Aug)
r-squared
P
slope
significant?
Winter (Dec-Feb)
r-squared
P
slope
significant?

0.94
0.0001
-0.18
Yes

0.68
0.006
-0.31
Yes

0.95
0.0001
-0.14
Yes
Northeast

0.66
0.008
-0.15
Yes

0.41
0.06
-0.22
No

0.57
0.02
-0.10
Yes
Upper
Midwest

0.94
0.0003
-0.27
Yes

0.73
0.01
-0.41
Yes

0.14
0.40
-0.05
No
Midwest

0.69
0.01
-0.23
Yes

0.48
0.055
-0.45
No

0.02
0.74
+0.02
No
South
Central

0.74
0.003
-0.26
Yes

0.65
0.009
-0.38
Yes

0.37
0.08
-0.19
No
Southern
Periphery

0.60
0.04
-0.16
Yes

0.64
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-0.36
Yes

0.005
0.88
-0.01
No
West

0.64
0.03
+0.03
Yes

ND
ND
ND
ND

ND
ND
ND
ND
East

0.89
0.001
-0.21
Yes

ND
ND
ND
ND

ND
ND
ND
ND
Note: ND = not determined.




Source: QST.
    p/castnet/wa24/anrpt-3v.wpd
-------
  Table 3-6.  Summary of SURE SC# Data
Annual 1978 SURE
  Concentrations
   SURE
    Site
Annual 1994 CASTNet
    Concentrations
  Corresponding
    CASTNet
       Site
      9.01

     11.71

     10.14

      9.03

      8.88
2 (Scranton, PA)

4 (Duncan Falls, OH)

5 (Rockport, IN)

7 (Fort Wayne, IN)

9 (Lewisburg, VA)
         5.3

         6.4

         6.4

         5.1

         5.8
144 (Washington's Crossing, NJ)

114 (Deer Creek State Park, OH)

140 (Vincennes, IN)

133 (Salamonie Reservoir, IN)

120 (Horton Station, VA)
  Sources:  Shreffler and Barnes, 1996; QST.
      p/castnet/wa24/ampt-3v.wpd
-------
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 Table 3-11. Annual Average Dry Depositions for NHJ*
Region
                                                    NHJasN
1987   1988   1989   1990   1991    1992   1993   1994   1995
Northeast

Upper Northeast

Midwest

Upper Midwest

South Central

Southern Periphery

All Eastern Sites

All Western Sites
              0.552  0.473  0.519  0.444  0.493   0.470  0.457

              0.207  0.208  0.183  0.151  0.120   0.130  0.177

              0.665  0.559  0.565  0.512  0.532   0.593  0.582

              0.425  0.337  ins     0.358  0.301   0.275  0.319

              0.457  0.472  0.408  0.430  0.502   0.463  0.545

              0.265  0.290  0.277  0.293  0.337   0.311  0.338

              0.490  0.454  0.454  0.415  0.449   0.447  0.463

              ins     0.121  0.122  0.128  0.117   0.118  0.105
Note:   —  =  NHJ analysis began in August 1988 and is reported from January 1989.
       ins  =  Insufficient data; a site must have 8 valid samples per season and 3 valid seasons
              per year to be included in summary statistics.

*A11 values in kg/ha (as nitrogen).

Source: QST.
p/castnet/wa24/anrpt-3v.wpd
-------
Table 3-12.   Results of Linear Regression Analysis on Annual and Seasonal SO^ Concentrations in Precipitation
Average Upper
Statistics Northeast Northeast
Summer
r-squared
P
slope
significant?
Winter
r-squared
P
slope
significant?
Annual
r-squared
P
slope
significant?

0.07
0.56
-0.03
No

0.92
0.0006
-0.12
Yes

0.70
0.02
-0.05
Yes

0.01
0.85
-0.04
No

0.95
0.0002
-0.18
Yes

0.44
0.11
-0.09
No
Upper
Midwest

0.47
0.09
-0.15
No

0.009
0.84
-0.02
No

0.46
0.09
-0.14
No
Midwest

0.26
0.24
-0.13
No

0.70
0.02
-0.12
Yes

0.44
0.11
-0.13
No
South
Central

0.08
0.55
-0.08
No

0.53
0.06
-0.08
No

0.47
0.09
-0.09
No
Southern
Periphery

0.16
0.36
-0.09
No

0.0003
0.97
-0.002
No

0.76
0.01
-0.04
Yes
West

0.02
0.76
+0.01
No

0.20
0.31
-0.05
No

0.01
0.85
+0.01
No
East

0.10
0.48
-0.08
No

0.91
o.ooi
-0.11
Yes

0.52
0.07
-0.09
No
Source:  QST.
 p/castnet/wa24/anrpt-3v.wpd
-------
 Table 3-13.  Results of Linear Regression Analysis on Annual and Seasonal NOj Concentrations in Precipitation
Average Upper
Statistics Northeast
Summer
r-squared
P
slope
significant?
Winter
r-squared
P
slope
significant?
Annual
r-squared
P
slope
significant?

0.33
0.17
+0.03
No

0.57
0.05
-0.11
Yes

0.20
0.32
-0.01
No
Northeast

0.04
0.66
+0.03
No

0,62
0.04
-0.07
Yes

0.05
0.62
-0.01
No
Upper
Midwest

0.02
0.74
-0.02
No

0.06
0.60
-0.04
No

0.23
0.28
-0.08
No
Midwest

0.002
0.92
-0.006
No

0.02
0.76
-0.02
No

0.09
0.51
-0.03
No
South
Central

0.01
0.84
-0.01
No

0.57
0.05
-0.04
Yes

0.29
0.21
-0.02
No
Southern
Periphery

0.01
0.85
-0.01
No

0.39
0.13
+0.04
No

0.01
0.83
+0.002
No
West

0.04
0.65
+0.03
No

0.17
0.36
-0.04
No

0.003
0.91
+0.003
No
East

0.002
0.92
+0.005
No

0.51
0.07
-0.04
No

0.18
0.34
-0.02
No
Source:  QST.
p/castnet/wa24/ampt-3v.wpd
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Table 3-34.  Results of Linear Regression Analysis for Wet Deposition of SOJ- as S and NOj as N Using Annual
            Averages of Combined CDN/NADP Data
Average Upper
Statistics Northeast Northeast
Sulfur
r-squared
P
slope
significant?
Nitrogen
r-squared
P
slope
significant?

0.77 0.571
0.01 0.05
-0.321 -0.552
Yes Yes

0.487 0.429
0.08 0.11
-0.089 -0.133
No No
Upper
Midwest

0.283
0.22
-0.277
No

0.263
0.24
-0.081
No
Midwest

0.644
0.03
-0.456
Yes

0.167
0.36
-0.063
No
South Southern
Central Periphery

0.73 0.454
0.01 0.10
-0.367 -0.173
Yes No

0.350 0.036
0.16 0.68
-0.054 -0.019
No No
West

0.417
0.12
-.035
No

0.513
0.07
-0.08
No
East

0.726
0.01
-0.418
Yes '

0.506
0.07
-0.026
No
Source:  QST.
p/casmct/wa24/anrpt-3v.wpd
-------
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All Western Site:

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-------
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-------
Table 3-37. Annual Averages of Ozone Concentrations (ppb) by Region/Site
Region
Northeast











Upper Northeast



Midwest












Upper Midwest


South Central







Site
103/104
106
107
110
112
113
116
117
119
128
144
147
105
109
132
135
114
115
122
123
130
133
136
138
140
146
157
181
572
124
134
149
101
102
108
111
118
120
121
125
1987
30
30
ins
27
ins
ins
ins
ins
ins
ins
ins
ins
34
ins
ins
ins
ins
ins
22
ins
ins
ins
ins
ins
20
22
ins
ins
ins
—
—
ins
30
36
ins
ins
ins
46
ins
ins
1988
30
34
35
40
ins
37
ins
34
29
39
ins
ins
36
ins
ins
ins
21
28
37
ins
36
24
ins
ins
32
29
25
ins
ins
27
26
33
27
36
34
ins
50
48
29
ins
1989
29
29
30
38
37
32
26
28
24
36
29
ins
38
32
ins
32
31
32
33
34
33
35
ins
ins
30
26
33
ins
ins
35
35
37
ins
ins
33
27
45
44
22
ins
1990
27
33
30
37
35
31
25
29
25
36
29
ins
37
30
ins
30
33
31
32
33
31
33
ins
ins
30
24
32
ins
ins
34
32
32
ins
ins
34
31
46
45
22
30
1991
29
33
30
39
38
34
27
31
26
38
31
ins
37
31
ins
32
32
31
33
34
31
33
ins
ins
30
24
31
ins
ins
34
33
34
ins
ins
33
29
46
44
22
36
1992
25
30
27
35
33
29
24
27
23
32
26
ins
34
30
ins
31
29
28
29
31
26
30
ins
ins
27
22
30
ins
ins
30
32
31
ins
ins
31
27
39
40
19
36
1993
31
33
30
40
34
31
26
29
25
35
29
ins
37
27
29
30
31
27
30
32
28
25
30
ins
27
19
29
ins
ins
30
32
31
ins
ins
34
28
45
45
21
38
1994
ins
33
30
39
34
32
24
30
25
37
28
35
ins
30
31
33
30
30
32
32
30
33
39
35
30
ins
31
ins
39
33
34
32
ins
his
33
30
45
42
his
35
1995
his
32
30
40
37
35
29
32
27
36
34
36
his
29
31
34
34
31
32
34
34
37
43
38
30
his
34
2
40
34
35
36
his
his
34
33
46
45
his
38
    p/castnet/wa24/anrpt-3v.wpd
-------
Table 3-37.  Continued, Page 2 of 2
Region
South Central
(continued)







Southern
Periphery

West








All Eastern Sites
All Western Sites
Site
126
127
129/131
137
139
142
152
153
571
150
151
156
161
162
163
164
165
167
168
169
174


1987
ins
ins
30
ins
ins
ins
ins
ins
ins
ins
ins
ins
45
45
37
43
46
41
22
48
47
30.6
..
1988
ins
27
41
33
ins
ins
ins
34
ins
23
ins
ins
ins
ins
ins
ins
ins
ins
ins
ins
ins
34.3
—
1989
45
34
36
28
ins
ins
36
34
ins
28
37
31
43
43
32
43
46
40
24
47
47
33.7
41.1
1990
48
38
38
30
ins
ins
40
41
ins
27
39
32
44
45
39
43
43
41
25
46
47
33.0
41.5
1991
45
36
36
26
ins
ins
34
35
ins
25
36
30
45
46
38
43
47
42
24
48
46
32.9
42.0
1992
43
31
35
27
ins
ins
32
33
ins
24
34
31
43
45
38
42
46
40
21
47
46
31.5
40.9
1993
44
34
36
29
ins
ins
35
35
ins
26
34
31
45
48
38
45
45
41
21
48
45
31.5
41.3
1994
42
33
38
28
ins
35
32
33
39
24
36
29
47
ins
ins
ins
48
43
23
52
49
32.8
43.7
1995
46
37
42
29
54
33
39
39
41
28
41
32
46
ins
ins
ins
46
38
21
48
46
33.0
48.0
Note:         ins = Insufficient data; sites must be 75-percent complete per quarter/year to be included in this
                     table.

Source: QST.
     p/castnet/wa24/anrpt-3v.wpd
-------
Table 3-38. Annual Maxima of Ozone Concentrations (ppb) by Region/Site
Region
Northeast












Upper
Northeast



Midwest












Upper Midwest


South Central





Site
103/104
106
107
110
112
113
116
117
119
128
144
147
175
105
ins
132
135
145
114
115
122
123
130
133
136
138
140
146
157
181
572
124
134
149
101
102
108
111
118
120
1987
162
120
ins
79
ins
ins
ins
ins
ins
ins
ins
ins
ins
117
ins
ins
ins
ins
ins
UTS
85
ins
ins
ins
ins
ins
81
107
ins
ins
ins
ins
ins
ins
118
117
ins
ins
ins
127
1988
212
143
156
126
ins
144
ins
156
134
155
ins
ins
ins
129
109
ins
ins
ins
57
115
164
ins
121
73
ins
ins
119
146
99
ins
ins
126
71
134
137
132
125
ins
160
145
1989
125
104
107
101
102
117
131
110
109
112
159
ins
ins
93
91
ins
103
ins
157
109
109
110
104
109
ins
ins
112
126
133
ins
ins
113
85
107
121
ins
105
95
95
98
1990
150
120
123
93
101
105
137
109
116
124
148
ins
ins
115
86
ins
88
ins
115
111
116
103
106
110
ins
ins
110
97
148
ins
ins
105
74
98
ins
ins
107
117
103
97
1991
149
117
99
109
112
116
156
118
111
122
143
ins
ins
122
98
ins
99
ins
107
101
113
120
145
107
ins
ins
112
132
117
ins
ins
111
79
106
ins
ins
108
108
114
108
1992
144
104
89
102
106
110
118
96
91
105
139
ins
ins
115
100
ins
93
ins
98
126
100
104
98
103
ins
ins
103
131
106
ins
ins
98
95
96
ins
ins
123
96
99
92
1993
129
122
122
109
102
121
134
109
123
125
126
137
ins
72
81
91
77
ins
111
128
124
103
91
78
76
ins
99
73
120
ins
ins
125
84
93
ins
ins
116
118
102
97
1994
ins
104
103
98
88
118
141
111
105
113
134
151
92
ins
85
93
84
91
113
99
106
103
105
109
131
99
103
ins
118
ins
102
108
80
99
ins
ins
106
107
101
99
1995
ins
112
100
96
97
110
166
116
98
119
146
ins
105
ins
78
101
80
103
116
107
116
110
119
118
119
102
108
ins
129
2
136
104
89
113
ins
ins
101
115
107
99
   p/castnet/wa24/anrpt-3v.wpd
-------
Table 3-38. Continued, Page 2 of 2
Region
South Central
(continued)









Southern
Periphery

West








Site
121
125
126
127
129/131
137
139
142
152
153
571
150
151
156
161
162
163
164
165
167
168
169
174
1987
ins
ins
ins
ins
84
ins
ins
ins
his
ins
ins
his
his
ins
his
his
his
his
his
his
his
his
his
1988
128
his
ins
62
143
145
his
his
ins
119
his
67
his
ins
his
his
his
his
his
his
his
his
his
1989
98
his
103
90
102
94
his
his
97
118
his
102
149
84
84
75
66
80
79
89
67
88
80
1990
85
85
110
109
108
85
his
his
117
144
his
94
100
93
88
74
80
78
74
138
66
78
92
1991
96
118
95
98
109
86
his
his
99
123
his
87
110
90
86
88
73
91
76
83
62
81
81
1992
100
102
97
99
97
93
his
his
101
117
his
88
90
88
73
78
73
79
72
76
77
74
81
1993
87
107
98
118
108
85
his
his
114
109
his
92
90
81
88
89
67
84
71
79
58
74
77
1994
his
108
106
101
110
89
his
94
95
119
104
94
98
92
88
ins
ins
his
78
78
61
86
84
1995
ins
118
96
91
108
93
117
97
128
136
107
95
103
86
80
ins
ins
ins
83
69
54
74
64
Note:         his = Insufficient data; sites must be 75-percent complete per quarter/year to be included in this
                     table.

Source: QST.
     p/castnet/wa24/ampt-3v.wpd
-------
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-------
 Table 3-42.  1995 Ozone Concentrations and Measures
Site
135 (Ashland, ME)
134 (Perkinstown, WI)
1 18 (Big Meadows, VA)
120 (Horton Station, VA)
126 (Cranberry, NC)
107 (Parsons, WV)
106 (PSU, PA)
108 (Prince Edward, VA)
114 (Deer Creek, OH)
130 (Bondville, IL)
116(BeltsviUe, MD)
144 (Washington's Crossing,
Land Use Annual
Remote
Remote
Mountainous
Mountainous
Mountainous
Complex Terrain
Rolling
Rolling
Rolling
Rolling
Suburban
NJ) Suburban
34
35
46
45
46
30
32
34
34
34
29
34
SUM06
3.2
17.3
32.2
28.1
27.0
26.3
31.9
18.7*
37.3
37.4
36.5
41.1
4th Highest Highest
Daily Maximum Hourly
W126 Value Based on Value
Rolling 8-Hour (All Year)
Averages (All Year)
3.6
13.7
22.1
19.3
18.8
19.7
24.4
14.2*
27.8
29.2
30.5
34.3
65
75
90
81
79
82
95
83
87
94
104
109
80
89
107
99
96
100
112
101
116
119
166
146
*Lower than previous years.




Source: QST.
    p/castnet/wa24/anrpt-3v.wpd
-------
Table 3-43. 1992 Ozone Concentrations and Measures
Site
135 (Ashland, ME)
134 (Perkinstown, WI)
118 (Big Meadows, VA)
120 (Horton Station, VA)
126 (Cranberry, NC)
107 (Parsons, WV)
106 (PSU, PA)
108 (Prince Edward, VA) '
114 (Deer Creek, OH)
130 (Bondville, IL)
116(Beltsville, MD)
144 (Washington's Crossing,
Land Use Annual
Remote
Remote
Mountainous
Mountainous
Mountainous
Complex Terrain
Rolling
Rolling
Rolling
Rolling
Suburban
NJ) Suburban
31
32
39
40
43
27
30
31
29
26
24
26
SUM06
6.5
15.2
22.9
21.6
29.2
15.2
23.8
22.0
23.8
21.2
30.7
28.6
4th Highest Highest
Daily Maximum Hourly
W126 Value Based on Value
Rolling 8-Hour (All Year)
Averages (All Year)
6.6
10.8
16.9
15.0
19.1
11.0
18.1
15.7
18.0
16.7
24.2
24.1
79
74
81
76
78
70
90
79
83
79
92
102
93
95
99
92
97
89
104
123
98
98
118
139
Source:  QST.
     p/castnet/wa24/anrpt-3v.wpd
-------
 Table 3-44. Sampling History:  Mountain Acid Deposition Program
Sampling
Efforts
Samples 1994
Samples 1995
Samples 1996
Sampling - 1997
Dry Deposition
Whitetop Mt.
Site 302
165
573
211
Began May 16
Weekly Filter Pack
Whiteface Mt.
Site 300
284
768
644
Began June 15
Continuous Gas
Clingman's Dome
Site 303
17
147
123
Began May 23
Weekly Filter Pack
Catskills Mt.

30

Began June 15
_.
  Precipitation Analyses

  Liquid Water Content
  Continuous
  Meteorological

  Ozone
    Collected

5-minute average,
 hourly average

5-minute average,
 hourly average

5-minute average,
 hourly average
                                                 Monitoring (ASRC)
5-minute average,
 hourly average

5-minute average,
 hourly average

5-minute average,
 hourly average
5-minute average,
 hourly average

5-minute average,
 hourly average

 Data from NPS
Wind Direction
  Windspeed
Source: QST.
    p/castnet/wa24/anrpt-3v.wpd
-------
Table 3-45. CASTNet Visibility Sites, October 1993 Through November 1995
Site
No.
510
513
518f
528
530
570
571
572*
573
Discontinued Site
557
Site Name
Connecticut Hill, NY
M.K. Goddard, PA
Shenandoah National Park, VA
Arendtsville, PA
Bondville, IL
Sikes, LA
Cadiz, KY
Quaker City, OH
Livonia, IN

Alhambra, IL
Latitude
<°N)
42.40
41.43
38.52
39.92
40.05
32.07
36.78
39.94
38.58

38.87
Longitude
(°W)
76.65
80.15
78.44
77.31
88.37
92^46
87.85
81.34
86.26

89.62
Operational
Date
09/20/93
09/17/93
10/18/93
09/16/93
09/24/93
06/10/93
09/16/93
07/24/93
12/31/88

03/30/94
*Collocated site.
tCollocated with IMPROVE aerosol sampler.

Source: QST.
      p/castnet/wa24/ampt-3v.wpd
-------
 Table 3-46. Results of Collocated Aerosol Sampling for 1994
Filter Parameter
Nylon Nitrate (/*g/m3)
Sulfate (/*g/m3)
Quartz Elemental-C (/*g/m3)
Organic-C 0*g/m3)
Teflo Fine Mass (jug/m3)
Absorbance (lO'Vm)
Al (ng/m3)
As (ng/m3)
Br (ng/m3)
Ca (ng/m3)
Cr (ng/m3)
Cu (ng/m3)
Fe (ng/m3)
H (ng/m3)
K (ng/m3)
Mg (ng/m3)
Mn (ng/m3)
Na (ng/m3)
Ni (ng/m3)
Pb (ng/m3)
Rb (ng/m3)
S (ng/m3)
Se (ng/m3)
Si (ng/m3)
Sr (ng/m3)
Ti (ng/m3)
V (ng/m3)
Zn (ng/m3)
Zr (ng/m3)
Number
of
Pairs
44
44
39
39
42
42
23
19
42
42
14
39
42
42
42
1
26
25
22
42
7
42
42
42
14
28
10
42
2

MeanX
1.05
6.28
0.76
1.90
12.10
558.21
60.71
0.74
3.07
17.69
2.31
2.22
30.68
555.94
43.19
33.76
6.62
148.31
0.75
5.63
0.27
1578.98
2.20
111.49
0.24
11.77
3.08
13.42
0.45
Average Value
MeanY
1.05
6.61
0.68
1.76
13.81
581.02
67.77
0.72
3.12
19.38
2.80
2.29
33.39
536.47
43.26
26.75
7.82
175.18
0.74
5.63
0.19
1697.39
2.26
118.74
0.21
13.63
4.54
13.69
0.45
Over the Quarter
Median AD
0.02
0.12
0.13
0.31
0.52
31.35
16.18
0.13
0.19
3.09
0.38
0.20
1.77
46.70
3.49
7.01
1.19
33.18
0.08
0.47
0.05
91.10
0.11
7.85
0.04
2.37
1.33
0.68
0.22

Median APD
2.21
2.61
24.00
19.35
5.52
5.88
24.57
20.99
6.35
18.85
18.41
13.04
7.66
12.28
8.87
23.17
21.00
28.35
12.57
7.84
22.22
4.30
6.86
14.88
20.04
27.59
49.75
6.19
54.35
Note:      median AD = median absolute difference.
         median APD = median absolute percent difference.
        mean X and Y = mean value for primary and collocated sensors, respectively.

Source: QST.
     p/castnet/wa24/anrpt-3v.wpd
-------
Table 3-47.  Mobile Dry Deposition System Measurements
       Measurement
       Methods
    Fluxes:
       Ozone
       Sulfur dioxide
       Carbon dioxide
       Nitric Acid
Eddy Correlation
Eddy Correlation
Eddy Correlation
Gradient
    Energy budgets:
        Heat flux
        Latent heat flux
        Soil heat flux
        Soil storage
        Net radiation

    Wind speed/direction (10 m)
    Temperature/relative humidity (3 m)
    Solar radiation
    Wetness/precipitation
    Leaf area index
    Vegetation description
    Sonic anemometer-winds
    Delta temperature
    Mean ozone
    Mean sulfur dioxide
    Pressure
    Wind speed/direction (3 m)
Eddy Correlation
Eddy Correlation
Heat flux plates
Temperature probes
Net radiometer
Eddy Correlation
Gradient fluxes
Deposition velocities
Deposition velocities
 Source: QST.
 p/castnet/wa24/anrpt-3v.wpd
-------
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-------
Table 4-2.  Percent Completeness Rates for Concentration Data by Site for 1987 through 1995 (page 1 of 2)
1987
101 73
102 83
103/104 90
105 83
106 81
107
108 15
109
110 21
111
112
113
114
115
116
117 4
118 —
119 15
120 58
121
122 35
123
124
125
126
127
128
129/131 40
130
132
133 —
134
135
136
137 15
1988
98
83
98
100
100
94
50
2
87
—
—
90
27
37
13
98
33
96
100
88
94
—
33
—
—
15
50
79
71
—
44
27
2
—
79
1989
92
—
100
92
94
98
96
90
98
58
94
92
94
87
96
100
92
98
100
100
100
87
98
—
88
98
98
98
100
—
96
98
94
—
98
1990
—
—
100
100
100
98
100
96
100
98
88
98
100
100
100
100
94
98
100
100
100
100
100
27
100
100
100
96
98
—
94
98
100
—
100
1991
—
—
100
96
100
96
90
98
100
100
100
100
100
96
100
100
100
100
100
100
100
100
100
100
100
100
100
98
92
—
98
98
100
—
98
1992
—
—
100
98
98
96
96
96
100
98
100
100
96
100
96
96
94
100
96
100
100
100
100
94
100
100
100
98
98
12
98
100
96
—
100
1993
—
—
69
23
94
100
100
96
100
94
94
94
94
100
90
100
92
98
100
92
100
81
98
100
100
98
94
96
98
87
96
98
98
37
96
1994
—
—
—
—
94
98
94
85
88
90
94
94
96
94
96
92
92
92
87
—
96
90
94
100
100
94
100
87
94
94
96
98
98
98
•92
1995
—
—
—
—
96
98
73
92
90
71
71
73
69
56
71
73
90
88
85
—
98
69
71
90
73
73
98
73
73
85
88
98
67
73
96
p/castne1/wa23/anrpt_4v.wpd
-------
   Table 4-2.  Percent Completeness Rates for Concentration Data by Site for 1987 through 1995 (page 2 of 2)
                1987
1988
1989
                                             1990
                              1991
                              1992
                                                                          1993
                                                           1994
                                                           1995
138
139
140
142
144
145
146
147
149
150
151
152
153
156
157
161
162
163
164
165
167
168
169
174
175
181
571
572
—
—
40 98 98
—
2 96
—
46 98 98
—
21 96
23 85
2 96
2 87
44 73
— ... Sfi
_ . .•_ QQ
46 96
63
67
	 58
58
~. O8
~~ ™ yo
65
2 92
63
44
—
—
—
—
— •
—
100
—
98
—
96
—
100
100
96
100
100
92
100
100
98
100
98
98
100
100
96
100
—
—
—
—
—
—
100
—
98
—
100
—
100
100
96
100
100
98
100
100
96
100
98
90
98
96
100
100
—
—
—
—
—
—
100
—
98
—
96
—
100
100
67
98
100
100
98
100
100
96
96
100
98
100
92
98
—
—
—
—
...
—
100
—
94
—
23
—
100
100
98
100
98
96
100
98
71
73
67
96
100
98
100
100
—
—
23
23
96
—
94
94
94
60
—
92
96
98
83
96
81
96
96
98
—
—
—
98
96
98
92
92
58
2
94
94
65
23
92
92
90
71
...
90
90
73
71
73
88
98
88
98
...
...
—
79
87
96
88
90
92
98
90
90
Source: QST.
p/castnet/wa23/anrpt_4v.wpd
-------
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   Table 4-5. Percent Completeness* Rates for Ozone Daily Maxima Data (page 1 of 2)
Region State Days+ Site
NE CT 214 147
MD 214 116
NJ 214 144
NY 214 103/104
110
175 ,
PA 214 106
112
113
117
128
WV 214 107
119
UNE NY 214 105
ME 214 132
135
NH 214 109
VT 214 145
MW IL 214 130
138
146
157
IN 183 133
140
KY 214 136
MI 183 115
OH 214 114
122
123
UMW MI 183 124
149
WI 185 134
1987 1988



86.9 98.1
7.9 93.0

70.6 86.9

95.3
97.7
56.5
97.7
94.4
86.9 98.6




82.7

53.3 98.6
30.4

96.7

38.8
2.3
11.2 92.5

23.5
38.8
8.1
1989

98.6
97.7
97.7
99.5

98.6
97.2
98.6
91.1
97.7
96.7
95.8
87.4

98.6
94.4

99.5

99.1
99.1
97.8
99.5

94.5
90.2
99.1
94.4
97.3
99.5
95.7
1990

86.9
97.7
94.4
99.1

97.7
90.7
85.5
97.7
97.7
98.6
98.1
97.7

98.6
96.7

96.7

98.6
96.3
98.9
98.9

98.4
99.1
99.1
83.6
97.8
98.9
98.4
1991

89.3
99.5
97.7
99.5

94.4
98.1
96.7
98.6
97.7
99.1
96.3
99.5

96.7
98.1

92.5

92.5
98.6
98.9
96.2

94.5
97.2
98.6
95.3
99.5
100.0
97.3
1992

93.9
99.5
97.2
100.0

98.1
98.6
9Z7
99.1
95.3
98.1
97.2
97.2

97.7
95.3

93.5

97.7
97.7
99.5
96.2

91.3
95.8
99.1
97.7
95.1
96.7
97.8
1993

97.2
98.6
72.9
93.5

96.7
81.3
97.7
99.1
90.7
96.3
97.7

93.9
90.7
99.5

93.5


93.5
98.4
98.9
29.9
69.9
99.1
98.1
98.1
97.8
97.3
96.8
1994
93.9
99.1
95.8

85.0
4.2
99.1
97.2
96.3
97.7
97.2
98.1
96.3

98.1
99.5
97.2
30.8
97.7
90.2

97.2
96.7
98.4
99.1
93.4
98.6
96.7
88.3
100.0
99.5
95.7
1995
83.6
82.7
84.6

82.7
19.2
95.8
80.4
83.2
82.7
96.3 ,
99.1
83.2

77.1
80.8
98.6
39.7
83.6
75.7

83.2
97.8
94.0
84.1
91.8
81.8
98.1
84.1
97.3
96.2
95.1
p/castnet/wa24/anrpt_4v.wpd
-------
Table 4-5. Percent Completeness* Rates for Ozone Daily Maxima Data (page 2 of 2)
Region State
SC MD
KY


AL
GA
NC




TN


VA


SP AR
FL
MS
WST AZ

CO
ID
MT
NV
UT
WY

Days+
214
214


27
276
214




214


214


276
365
276
365

214
214
122
365
153
214

Site
139
121
129/131
571
152
153
101
125
126
137
142
102
111
127
108
118
120
150
156
151
167
174
161
163
168
164
162
165
169
1987 1988 1989

97.2 99.1
14.5 78.5 93.0

89.9
51.8 70.3
79.0 97.7 94.4

86.9
78.5 80.8

85.5 93.9
50.9
0.0 99.1
57.5 95.8
36.4 96.3
55.1 97.2 95.8
22.1 98.9
86.6
89.5
49.9
44.7
39.3
23.8
97.5
47.9
56.9
93.9
55.1
1990

96.7
85.0

98.9
93.8

9.8
92.1
98.6


90.2
97.7
87.9
87.4
99.5
98.9
84.9
97.1
94.8
99.5
94.4
96.7
99.2
79.2
98.7
98.1
97.2
1991

98.6
91.1

88.8
97.8

98.1
98.1
97.2


97.2
95.3
89.7
90.7
97.7
98.2
87.4
90.6
88.8
96.7
99.1
95.3
99.2
83.6
90.8
82.7
76.6
1992

95.8
99.5

93.5
98.6

99.1
97.2
98.6


96.3
99.1
91.6
85.5
97.7
96.4
96.7
97.5
91.8
92.6
93.5
92.5
96.7
75.3
93.5
96.3
89.3
1993

94.4
96.7

95.7
94.2

97.2
98.6
98.1


98.6
89.7
94.4
91.1
98.1
93.5
87.9
97.1
89.9
87.4
96.3
81.3
99.2
44.9
95.4
97.7
98.1
1994


97.2
93.9
91.7
97.8

95.8
98.6
98.6
86.0

99.5
98.6
94.9
87.4
93.9
98.2
92.6
95.3
97.3
90.7
97.7

98.4


98.1
99.1
1995
25.2

78.5
82.2
76.4
73.9

79.4
83.6
96.3
84.6

80.8
84.1
83.2
93.0
73.4
73.9
89.9
75.4
24.1
15.9
97.7




58.4
94.9
 * Percent Completeness is calculated as: number of valid daily maxima/total ozone season days for a state.
 + Number of days in state's designated ozone season.

 Source: QST.
 p/castnetAva24/ampt_4v.wpd
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               CDN SITE CONFIGURATION
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            Figure 2-5.    Typical CDN site configuration
-------
            Clean Filler
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Figure 2-6.    Flowchart of laboratory operations for filter pack analyses
-------
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Figure 2-7.     Flowchart of laboratory operations for wet deposition analyses
-------
FIELD GROUP PREPARATION
     SAMPLE LOGIN
  SCHEDULE ANALYSES
    INPUT RESULTS
         QC
-DEFINE PARAMETERS FOR ANALYSIS
-ASSIGN TEMPORARY STATION CODES
-DEFINE SAMPLE FRACTIONS
-PRODUCE LABELS AND LOGSHEETS
-PREPARE/SHIP SAMPLE MEDIA

-ACTIVATE SAMPLES
-SET PERMANENT STATION CODES
-STORE COLLECTION TIME AND DATE
-STORE FIELD DATA
-LIST OF SAMPLES AVAILABLE FOR EACH
  PARAMETER SORTED BY DUE DATE
-RESERVE ANALYSIS
-INPUT CALIBRATION, QC,
  AND SAMPLE DATA
-CALCULATE CALIBRATION CURVE, SPIKE,
 REPLICATE. AND REFERENCE SAMPLE
 QC
  CALCULATE RESULTS
    INTERSAMPLE QC
       REPORTS
-CALCULATE AND STORE FINAL SAMPLE
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-CHECK FOR DATA INCONSISTENCIES
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 QC. AND STATISTICAL
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         Figure 2-8.   Flowchart of the CLASS™ program
-------
                                CDN MONITORING SITES
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           (Filter Packs, Precipitation Samples,
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                                                    CONTINUOUS DATA
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                      1
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                      1
                                         VIA      VIA
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                                      Download   Copy
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                                FINAL ATMOSPHERIC CONCENTRATION ARE
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                    Figure 2-9.   Flow of data through CDN
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