United States
                  Environmental Protection
                  Agency
Atmospheric Research and Exposure
Assessment Laboratory
Research Triangle Park, NC 27711
                  Research and Development
EPA/600/S3-90/058  Sept. 1990
&EPA         Project  Summary
                   An Assessment of Atmospheric
                   Exposure and  Deposition to
                   High  Elevation  Forests in  the
                   Eastern United  States
                  Volker A Mohnen
                   The spruce-fir forests in the higher
                  elevations of  the  Appalachian
                  Mountains from North  Carolina  to
                  Maine are showing visible symptoms
                  of injury and increased mortality.
                  Concern has  been  raised  that
                  exposure  to  and  deposition  of
                  atmospheric pollutants might play a
                  role  in this decline.  The  Mountain
                  Cloud  Chemistry  Project  (MGCP)
                  sponsored by the U.S. Environmental
                  Protection Agency (EPA) and the
                  National   Acid  Precipitation
                  Assessment Program (NAPAP) has
                  studied the exposure and deposition
                  of atmospheric constituents to these
                  forests.
                   Atmospheric pollution  is deposited
                  to the forest in a number of forms,
                  cloud water interception  represents a
                  major deposition pattern  and may
                  exceed deposition by precipitation
                  and  gases. The full report  provides
                  estimates of cloud, precipitation and
                  dry  deposition  to  the spruce-fir
                  forests at the MCCP sites.
                   This  Project  Summary  was
                  developed by EPA's Atmospheric
                  Research and  Exposure  Assessment
                  Laboratory, Research  Triangle Park,
                  NC,  to announce key findings of the
                  research  project that  is fully
                  documented in a  separate report of
                  the same title (see Project Report
                  ordering information at back).

                  Introduction
                   This report is the third in a series of
                  annual summaries of research on the
                  exposure and deposition of  airborne
chemicals to forest canopies and  the
forest floor in eastern North America. The
report is based  on observations and
model  estimates of  atmospheric
deposition at the  high elevation sites in
the eastern United States The report is
produced  by  the  scientists in  the
Mountain Cloud Chemistry Program, a
multi-year study of  atmospheric
chemistry and physics sponsored by the
EPA.
  The  MCCP  has three   primary
objectives:  (1) determine  the  elevational
gradients in wet  and dry deposition of
pollutants and climate variables;  (2)
determine  the relative significance  of
various  deposition mechanisms to  the
fluxes of chemical species   into and
through  forest  canopies;  (3)  determine
the frequency distributions of  chemical,
physical and climatic exposure.
  This report provides estimations  of
forest exposure to chemicals  in air and
cloud water and deposition to  the forests
from precipitation, wind blown clouds and
by dry  deposition  mechanisms.
Measurement methodology used provide
data for these estimations, data sets and
models used for deposition estimates are
discussed  in detail. Comparisons  of
deposition are  made between southern
and  northern MCCP sites.  Elevation
gradients in exposure and deposition are
also discussed.
  Two models are used to estimate cloud
water and chemical deposition flux. One
model was  developed by Lovett and
modified by Mueller. This  model  is
designed for use with  spruce-fir forest
canopies.  The other  model  was

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developed by  Krovetz for  use  with  the
deciduous canopy  at the  Shenandoah
MGCP site. The model used to estimate
dry deposition is the inferential or  "big
leaf"  model.  Since  this model  was
originally developed for  flat terrain  and
the  model   has  not  been  fully
characterized  for mountainous  regions,
deposition estimates reported here reflect
these uncertainties.

Technical Approach
  Resource and logistical considerations
dictate that measurements of  inputs to
high elevation forests in eastern North
America  can  be performed  at only a
limited number of  sites  where proper
access  and  facilities  are  available.  In
order to  meet the  needs of the project,
five  high elevation  sites  have  been
selected  from 45°N to  35°N  to be
representative of  the  geographic  and
meteorological variability  in this  large
region.  This coverage  has been
augmented by the addition of a low  level
site (Howland, ME) to allow evaluation of
the impact of elevational gradient forest
types  and  enhance  geographical
coverage. The research/monitoring  sites
associated with MGCP are  Howland
Forest,  ME, Mt.  Moosilauke,  NH,
Whiteface Mtn.,  NY, Shenandoah,  VA,
Whitetop, VA, and Mt. Mitchell, NC.
  Site specific measurements  of cloud
and  rain  water, of  gaseous  sulfur and
nitrogen  compounds, and of ozone  and
hydrogen peroxide  are sampled hourly or
are  directly  converted  into hourly
concentration values.  In  the  case  of
filterpack  measurements,  samples  are
integrated over a  week's time. These
concentration  values then  represent the
primary  exposure  parameters.  The
concentration of  pollutants  and  the
associated meteorological conditions are
needed  to   provide  estimates  of
deposition by precipitation,clouds,  and
gases.

Results

Deposition of Pollutant Ions in
Precipitation
  Wet  deposition  of  pollutants  was
estimated for the  1987/88  growing
season at the MGCP sites using standard
National    Acid      Deposition
Program/National  Trends   Network
(NADP/NTN)  measurements of rainfall
amounts and  chemistry.  The NADP  sites
selected to  represent MGCP  sites  are
Greenville, ME 09, Whiteface, NY 98,
Hubbard Brook, NH 02, Big Meadows, VA
29, Whitetop, VA  28 and  Clingmans
Peak, NC 45.  The  growing season  is
longest at the Shenandoah and Howland
sites, extending from early April at both
locations  to mid-November and  early
October,  respectively.  Mt.  Mitchell  and
Whitetop Mountain have the next longest
growing   seasons,  followed  by  Mt.
Moosilauke and  Whiteface  with  the
shortest (June to early October).
  The wet deposition data are shown  in
Table 1  for S042-  N03  and NH/ions in
precipitation  (not  cloud).  The  data
indicate that the most  westerly  sites  in
the north, Whiteface, NY and Moosilauke,
NH,  received greater wet deposition  via
precipitation  than  did  the  more
northeasterly  location  in Maine.  The
southern  sites  showed slightly  higher
sulfate and nitrate wet deposition than the
northern sites.

Concentration and Deposition
of Pollutants in Cloud Water
  The  1986-88 results  for the  five high
elevation MGCP sites are summarized in
Table 2 as overall chemical composition
of cloud water  samples  from precipitating
and  non-precipitating  clouds. The
concentrations in non-precipitating clouds
are  significantly   higher  than   in
precipitating clouds. The differences  in
cloud water ion  concentration  between
the sites  is a result of sample  location
with  regard  to cloud base and synoptic
weather  type.  The  southern  sites
frequently are cloudy  under the stable,
warm sector synoptic  type,  while  the
northern  sites experience cloudiness
associated more frequently with frontal
passage.  Hence,  any  north-south
differences in cloud  water concentrations
are likely related to cloud climatology
including cloud  base height.  The
importance of  sample location in relation
to height  above cloud  base  can  be
demonstrated  for  Whiteface-1 (1483 m)
and   Whiteface-2  (1245  m).  For
simultaneously obtained  cloud water
samples, Table 3 shows the differences
in the  mean ion concentration  observed
for the two vertically separated sites.The
substantial  vertical  gradient in cloud
water concentration  is  mainly explained
by increased  dilution  of precursor
substances as liquid water increase with
height above cloud base.
   In  estimating cloud  deposition to  the
forest canopy, MGCP uses  an improved
version  of the  1984 Lovett  Cloud
Deposition  Model   (COM).   Cloud
impaction events at  each MGCP site are
classified according to meteorological
conditions that prevail during each hour
of the event A detailed analysis  of cloud
chemistry  and meteorological variables
(wind speed and liquid water content) has
demonstrated  the usefulness  of  this
technique for  uniquely characterizing
conditions during  events. In addition  to
synoptic  classification,  specific  air
trajectory  directions computed within a
given event type can further characterize
event  conditions. This  technique is  able
to explain  a major  portion of the variance
in the chemistry and meteorological  data
base,  thereby  allowing  more complete
growing  season  estimates  of  cloud
deposition.  Deposition estimates  for
MGCP sites can now be made for periods
when  data are incomplete as long  as
cloud  frequency and event  type can  be
determined. Event types are (1) pre-warm
front, (2)  NW sector of cyclone, (3) post-
cold front, (4) warm sector of cyclone,  (5)
stationary front,  (6)  marine  flow off
Atlantic,  (7)  cutoff   low in  upper
atmosphere, and  (9)  cap  cloud. Cloud
deposition estimates  for each site  are
made by  computing,  for each  subclass,
the mean  water deposition  flux using the
improved CDM and subclass wind speed
and liquid water content. Best estimates
of canopy structure  are then used  to
calculate  the  gross  (pre-evaporaiion)
cloud  water  flux to  specific  forest
canopies at each site.
  Most of the site-differences in cloud
deposition can be  explained on the basis
of differences  in canopy structure. Cloud
deposition is  found  to be  highly site
specific. Despite an almost  2:1 advantage
in cloud  frequency, Whiteface Mountain
mean  deposition estimates for  the
growing season are generally  lower than
those for  Moosilauke  because of lower
canopy surface  area  at  the specific
Whiteface site. Differences  in cloud water
deposition between  the northern  and
southern  sites are significant and likely
caused   by  differences  in  such
parameters  as   canopy  structure,
elevation above cloud base and synoptic
meteorology. It is  also interesting to note
the annual changes  in  cloud water
deposition  as a  result  of  changing
meteorological conditions  from  year to
year.

Dry Deposition of Gases and
Particles
  The Atmospheric Turbulence Diffusion
Laboratory program (DRY  DEPOSITION)
used  in  the  MGCP,   calculates  the
deposition velocities  of sulfur  dioxide,
ozone,  nitric  acid vapor,  and sulfate
particles  from meteorological and  site
specific   biological  information.  Site
information  includes:  major and minor

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                   Table 1.  Concurrent Growing Season Wet Deposition Via Precipitation
                                                  kg ion/ha/mo
Location
Greenville,
ME(Howland)
Whiteface, NY

Hubbard Brook, NY
(Moosilauke)
Whitetop, VA

Clingmans Peak
(Mt. Mitchell, NC)
Big Meadows, VA
(Shenandoah)
NH4 +
0.11

0.33
1.11
0.28
0.11
0.31
0.14
0.46
0.12
0.48
0.92
so42-
1.28

2.27
1.18
2.84
2.16
3.20
2.84
5.15
2.69
2.32
2.90
Table 2. Average Ion Concentrations in 1986-1988 Cloud

H +
Whiteface-1 171
Whiteface-2 225
Moosilauke 263
Shenandoah 171
Whitetop 1 74
Mt. Mitchell 398

so42-
205
352
257
176
321
489

A/03-
73
92
732
94
144
174
N03"
0.65

0.95
0.93
1.46
1.10
1.32
1.17
2.26
1.19
1.43
1.34
Water (jieg/L)

NH4 +
97
157
107
93
152
184
Year Elevation
1987 322 m

1987 622 m
1988
1987 250 m
1988
1987 1689m
1988
1987 1987m
1988
1987 1074 m
1988

Elevation Cloud
(m) Frequency*
1483 37%
1245
1000 19%
1015 11%
1689 30%
1950 29%
             *% of hours in cloud.

Table 3.  Mean Ion Concentrations for  108
         Simultaneously  Collected Cloud
         Water Samples 1987/88 (fj.equiv/L)

             H +   SO42-  NO3-   W/V
Whiteface-1
Whiteface-2
122
218
79
151
48
85
74
142
plant  species  type, leaf  area  index  for
plant  species, and  site location.  All
available meteorological  data  including
canopy  wetness  and  rainfall  are also
used.
  The growing season dry deposition flux
is  presented  in Table 5 for  1987/88,
derived  by  multiplying weekly deposition
velocities (model  calculation)  by the
appropriate weekly  averaged  concen-
trations at each site.
  As is the case with cloud deposition,
the northern sites receive generally less
dry deposition  than  the  southern sites
due  to mainly  differences  in  canopy
structure. This is particularly  obvious for
the Shenandoah  site  which is  the  only
non-coniferous site within  MCCP.
  With the  exception  of ozone, all other
pollutants  showed very  low  ambient
concentrations. Therefore,  only doses for
ozone  are  calculated  in  MCCP  and
presented in Table  6. In  addition to the
MCCP  sites,   other nearby  ozone
monitoring  stations  have  been  included
for the  characterization  of  forest
exposure.  In   order  to  provide   a
biologically  relevant  value, the  sum  of
season dose (ppm/hr) is  calculated by
summing up all  ozone values above 70
ppb  occurring during daylight  hours  (7
am - 6 pm) of the growing season. The
exposure data (dose) in Table 6 suggests
a significant north-south gradient and an
elevational  gradient within a region. The
data also show  a pronounced year  to
year change  in ozone  dose for most of
the stations  with the  1988  exposure
higher by about a factor of two. Howland,
the most northeasterly site received the
lowest ozone  dose,  while  the  most
southern  sites, Mt. Mitchell and Whitetop,
experienced highest exposure.

Summary
  The average monthly  sulfur and acidic
nitrogen  deposition fluxes determined to
date (October 1989)  for the MCCP  sites
and for the 1987-88 growing seasons are
summarized in Table 7.  From these data
it is possible to estimate the importance
of cloud  deposition to the overall  flux of
pollutants  received   by  the forest

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                      Table 4. Calculated Growing Season Cloud Deposition Flux (kg ion/ha)

Moosilauke


Whiteface-2'


Whitetop A


Whitetop B~


Mt. Mitchell



1986
1987
1988
1986
1987
1988
1986
1987
1988
1986
1987
1988
1986
1987
1988
Cloud Water
Flux (cm)
12.9
10.1
3.5
11.6
10.5
6.0
53.1
39.4
34.3
77.3
61.2
54.3
33.5
27.5
21.8
so42-
21
15
6
11
10
6
83
64
56
135
108
95
52
51
76
A/03-
76
11
5
3
4
2
41
32
29
65
53
48
25
25
18
NH4 +
3.4
2.4
1.0
1.9
1.7
1.2
14.0
10.8
9.5
22.1
17.7
15.6
6.9
6.9
5.0
                      "There is no forest on top  of Whiteface Summit (WF-1).  Therefore, deposition has been
                      calculated on a canopy structure slightly above (WF-2).
                      ~  Higher canopy density than Whitetop A.
                         Table 5. Monthly Mean Growing Season Dry Deposition (kg species/ha/mo)

Howland

Moosilauke

Whiteface

Shenandoah

Whitetop
Mt. Mitchell


1987
1988
1987
1988
1987
1988
1987
1988
1988
1987
1988
S02
0.22
0.28


0.30
0.51
3.06

0.75
0.39
1.48
SO/- HNO3 O3
0.11 0.29 5.48
0.15 0.37 5.39
5.96
0.31 1.61 6.57
0.36 6.46
0.28 6.09
0.80 14.06
14.83
11.95
1.64 7.7
12.7
canopy .Although it must be kept in mind
that  cloud  interception  is  highly
dependent  upon  canopy structure  and
location  above cloud  base,  it can  be
nevertheless  concluded,  that  cloud
deposition can deliver to the canopy the
same and up to four times the amount  of
pollutants as  precipitation  does (see
Table 8).At the cloud  free Howland  site,
dry deposition  appears to account for
less  than  one  third  of  the  total  acidic
substances deposited.  The Shenandoah
site  has a  very low  cloud impaction
frequency  due to  its relatively  low
elevation and dry deposition  appears  to
be  of  greater relative  importance
(deciduous  trees).  The estimates  for
Whiteface    suggest   that    dry
sulfurdeposition accounts for less than  a
quarter of the total sulfur deposition flux.
  Based  on these research results, it can
be  concluded that  any assessment  of
forest damage  at  high  elevations must
take  all  delivery  mechanisms  into
account,  in particular, cloud deposition.

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Table 6   Ozone Exposure - Total Season April 15 - October 15
                 (Daylight Hours 7 AM - 6 PM)
                                 Sum of Season Dose (ppm'hr)
                                          > 0.07 ppm
Site Name/State
How/and Forest, ME
Moosilauke, NH
Whiteface Mountain-1, NY
Whiteface Mountain-3, NY
Whiteface Mountain-4, NY
Huntington, NY
Hampshire Co., MA
Beaver Co., PA
Shenandoah-i , VA
Shenandoah-2, VA
Shenandoah-3, VA
Big Meadow, VA
Dickey Ridge, VA
Sawmill Run, VA
Whitetop, TN
Giles Co., TN
Marion, VA
Mt. Mitchell -1, NC
Ml Mitchell-2, NC
1986
ND.
N D
2 29
ND
N D.
509
9 14
N D.
N.D
ND.
ND.
5 56
3 21
11.39
ND.
1638
411
8.34
ND
1987
0.82
7.81
9.68
9.41
3.47
5.74
9.26
13.06
9.49
9.01
6.07
28.50
31.07
26.80
38.54
16.73
9.27
5.14
6.68
1988
4.16
12.51
20.85
16.5
N.D
11.36
34.93
31.70
23.27
39.44
20.88
31.89
40.25
30.16
37.68
28.91
26.92
45.17
19.49
Elevation
(m)
250
1000
1483
1026
604
500
312
1300
1015
716
524
1071
631
453
1689
244
710
1950
1750
     Table 7. Estimated 1987-88 Deposition Budgets at MCCP Sites Growing Season Mean
             Sulfur and Nitrogen Deposition (kg S or N/ha-mo)
                             Wet                 Cloud                Dry

Howland
Moosilauke
White face -2
Shenandoah
Whitetop
Mt. Mitchell
S
0.43
0.84
0.58
0.99
1.01
1.31
N
0.15
0.29
0.21
0.28
0.28
0.39
S N
no clouds
0.69 0.35
0.65 0.17
insufficient data
3.58 1.23
2.65 0.87
S
0.17

0.31
1.80


N
0.08


0.23


                       Table 8.  Estimated Cloud-to-Wet  Depsition  Flux
                                Ratios for 1987-88 Growing Season
                                            Sulfate
             Nitrate
                        Moosilauke
                        Whiteface -2
                        Whitetop
                        Mt. Mitchell
0.8
1.1
3.5
2.0
1.2
0.8
4.4
2.2

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   Volker A. Mohnen is with the State University of New York at Albany, Albany, NY
         12222.
   Ralph Baumgardner is the EPA Project Officer (see below).
   The complete report, entitled "An Assessment of Atmospheric Exposure and
        Deposition to High Elevation Forests in the Eastern United States," (Order
        No. PB 91-100 1641 AS; Cost:  $31.00 subject to  change) will be available
        only from:
            National Technical Information Service
            5285 Port Royal Road
            Springfield, VA22161
            Telephone: 703-487-4650
   The EPA Project Officer can be contacted at:
            Atmospheric Research and Exposure Assessment Laboratory
            U.S. Environmental Protection Agency
            Research Triangle Park, NC 27711
United States                   Center for Environmental Research
Environmental Protection         Information
Agency                         Cincinnati OH 45268
Official Business
Penalty for Private Use $300

EPA/600/S3-90/058

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