Uniiad States Atmospheric Sciences
gnvirortmenisl Protection Research Laboratory
Agency Research Triangle Paris NC 27711
Research end Development May, 1988
pmSl___ ____ _____
IMPROVED RNWElERIZWnONS FOR SURFACE,
RESISTANCE TO GASEOUS DRY DEPOSITION
IN REGIONAL-SCALE, NU'ERICPL ilGDELS
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IMPROVED PARAMETERIZATION FOR SURFACE RESISTANCE TO GASEOUS DRY DEPOSITION
IN REGIONAL-SCALE, NUMERICAL MODELS
by
M. L. Wesely
Center for Environmental Research
Biological, Environmental, and Medical Research Division
Argonne National Laboratory, Argonne, IL 60439
Interagency Agreement DW89932394-01
to the U.S. Department of Energy
Project Officer
James M. Godowitch
Meteorology and Assessment Division
Atmospheric Sciences Research Laboratory
Research Triangle Park, North Carolina 27711
ATMOSPHERIC SCIENCES RESEARCH LABORATORY
OFFICE OF RESEARCH AND DEVELOPMENT
U.S. ENVIRONMENTAL PROTECTION AGENCY
RESEARCH TRIANGLE PARK, NORTH CAROLINA 27711
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NOTICE
The information in this document has been funded
partly by the United States Environmental Protection
Agency under Interagency Agreement DW89932394-01 to
the U.S. Department of Energy. It has been subject
to the Agency's peer and administrative review, and it
has been approved for publication as an EPA document.
11
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ABSTRACT
Methods for computing the bulk surface resistances to uptake of gases
have been developed for use in numerical models of atmospheric transport and
deposition over regional scales. The surface resistances, which must be
evaluated to compute dry deposition velocities, are broken down into three
major groups that represent distinct pathways of mass transfer: to the upper
portions of vegetative canopies, to the lower portions of canopies or
structures, and to the ground (or water surface). The procedures for summing
the pathway resistances to obtain the overall bulk surface resistances are
designed for use in a module of computer coding on dry deposition. The module
formulations are tailored for use with five seasonal categories and a landuse
map of the United States and southern Canada that contains 11 landuse types.
The equations for each resistance pathway are based primarily on the
experimental information available on resistances to S02 and 03 uptake. With
knowledge of effective Henry's Law constants and chemical reactivity of
various substances relative to the corresponding values for S02 and
03, the surface resistances for other substance can be estimated. These
substances include N02* NO, HN03, methyl hydroperoxide (to represent organic
peroxides), HCOQH (to represent organic acids), NH3, PAN, and HN02- The
results generally conform to expectations, with uptake through the stomata of
leaves controlling the surface resistance of lush vegetation if the value of
the effective Henry's Law constant is near that for S0.2 or if the substance
is considered at least slightly reactive. Hydrogen peroxide is the only
substance of those considered that is strong in both of these removal
properties. Otherwise, either solubility or reactivity tends to dominate. For
extremely soluble substances (with very large effective Henry's Law constant)
such as HN03, all exposed surfaces are computed to have very small
resistances. It is necessary, however, to consider the gas-phase physical
resistances because they can strongly limit transport inside canopies. Other
factors considered include surface temperature, stomataI response to
environmental parameters, the wetting of surfaces by dew and rain, and
covering of surfaces by snow. Surface emissions of gases, the possibility of
"compensation" points in biota, and variations of uptake characteristics by
individual plant species within landuse types are not taken explicitly into
account.
i i i
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CONTENTS
Abstract i i i
Tab I es v i
Figures vi i
Acknow I edgements v i i i
Section
1. Introduction 1
2. Framework of Surface Resistance Formulations for SQ.2 and 03... 3
3. Extension to Other Substances 10
4. Effects of Dew and Ra i n 15
5. Examp I es and D i scuss i on 18
6. Conclusions 22
References 25
Appendix I. Computed surface resistances 29
Appendix II. Code for the Argonne dry deposition module 41
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TABLES
Number
1 Landuse types used to describe surface conditions in
the moduIe
Input resistances (s m~l) to the module for computations
surface res i stances (rc)
Gases considered in the dry deposition module and their
properties relevant to estimating resistances to dry
deposition 11
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FIGURES
Number . Page
1 Schematic diagram of pathway resistances used in the
module, where rc is derived via Equation (2) 5
VI I
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ACKNOWLEDGEMENTS
This research was funded as part of the National Acid Precipitation
Assessment Program by the U.S. Environmental Protection Agency (EPA) through
IAG DW89932394-01 to the U.S. Department of Energy. Much of the information
on the aqueous properties of gases was gathered with the assistance of Dr.
P. V. Doskey of Argonne National Laboratory. Mr. J. M. Godowitch of the EPA
and Dr. B. M. Lesht of Argonne National Laboratory provided advice and
guidance on many aspects of this work.
VIII
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SECTION 1
INTRODUCTION
The removal of gases from the atmosphere by turbulent transfer and uptake
at the surface provides a primary means of cleansing the atmosphere and
delivering chemical doses to surface components. This process of dry
deposition is important in a number of environmental issues, particularly
"acid rain," which deals with transport, chemical transformations, and
deposition over regional or continental scales. Numerical simulations of such
phenomena are often necessary to evaluate the effects of emissions in one area
on deposition in another. The concern here is with dry deposition
parameterizations suitable for use in numerical simulations.
The dry deposition module that has been used with the Regional Acid
Deposition Model (NCAR, 1985, 1986) provides methods to compute the dry
deposition velocities for S02, 03, NOX (defined here as the sum of NO and
N02), sulfate in submicron particles, and HN03 in the United States and
southern Canada (Sheih et al., 1986; Walcek et al.t 1986). The basis for
the parameterizations of the deposition velocities are micrometeorological
formulas and, for S02, 03, and NOX, tables of resistances to uptake. The
main purpose of this report is to put these tables on a more solid scientific
footing, within a framework that enables logical extension to other gaseous
substances. For the Regional Acid Deposition Model, these other substances
include hydrogen peroxide, aldehydes, organic peroxides, peroxyacetic acid,
organic acids, ammonia, and peroxyacetyl nitrate. Improvements in deposition
velocities for particulate substances are not addressed here.
Another improvement needed in dry deposition calculations is a more
explicit means to evaluate changes in surface resistances caused by the
effects of surface wetness associated with dew and rain. Sheih et al. (1986)
suggested that the uptake of 03 is inhibited by dew while the uptake of
S02 may be enhanced for approximately two hours after dewfall if both dew
and good atmospheric mixing are present. For surfaces wetted by rain, Sheih
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et al. implied that the surface resistance to S02 may increase while uptake
of 63 may be unaffected. In this report, further recommendations are
given that will be incorporated into parameterizations for computing surface
resistances for several of the gases of interest.
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SECTION 2
FRAMEWORK OF SURFACE RESISTANCE FORMULATIONS FOR S02 AND 03
The familiar framework used in past dry deposition modules relies on the
simple formulation for gas deposition velocity as follows:
vd = -FC/CZ, (I*)
where Fc is the flux density and Cz is the concentration at height z. The
magnitude of the deposition velocity can be found as
|vdl = (ra * rb + rc)-l, (Ib)
where ra is the aerodynamic resistance (common to all gases) between a
specified height and the surface, r|, is the quasi laminar sublayer resistance
(whose only dependence on the properties of the gas of interest is its
molecular diffusivity in air), and rc is the bulk surface resistance (e.g.,
Wesely and Hicks, 1977; Garland, 1977; Baldocchi et at,., 1987). The absolute
value of vj is taken in Equation (Ib) because it can be negative and all
terms on the right-hand side are constrained to being nonnegative. We assume
that ra and r^ will be evaluated as before but will suggest new methods to
estimate rc for the five seasonal categories and 11 landuse types (Table 1)
employed with the module (Sheih et al., 1979; Sheih et al., 1986; Walcek et
at,., 1986). The tables of rc for S02 and 03 used as primary module inputs in
the past will be replaced with more detailed information.
The approach taken here is to break up the resistance rc into several
components, as is commonly done in resistance models in which series and
parallel resistances are identified for various parts of the canopy (e.g., see
reviews by Unsworth, 1980; Hosker and Lindberg, 1982; Baldocchi et aL.,
1987). These components are illustrated in Fig. 1, beneath the resistances
ra and rj,. Analogously to Ohm's law in electrical circuits, rc can be found as
*rm) + l/r,u + l/(rdc+rc!) * l/(rac+rgs)]-l. (2)
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Table 1. Landuse types used to describe surface conditions in the module. In
the computerized landuse map, the percentage of coverage by each of these
types is given for each increment of 1/4 and 1/6 deg, longitude and
latitude, respectively, from 52 to 134 deg west longitude and from 24 to
55 deg north latitude.
Type Description
Purest-
2 Agricultural land, usually well watered
3 Range land, usually with low soil moisture
4 Deciduous forest
5 Coniferous forest
6 Mixed forest including wetland
7 Water, including both salt and fresh water
8 Barren land, mostly desert
9 Non-forested wetland
10 Mixed agricultural and range land
11 Rocky open areas occupied by low-growing shrubs
This formulation assumes that the concentrations representative of the plant
mesophyll (€,„), plant tissue of leaves in the upper canopy (C|u), substrates
in the lower canopy (Cc|), and substrates at the ground surface (Cg) are in
equilibrium with the concentration (Cz) in air (e.g., by Henry's Law
constant). In this work, all these substrate concentrations will be assumed
to be zero. However, it may be useful to use nonzero values for gases such as
NO, N02, and NH0 that are emitted from the surface, as will be discussed later.
The resistances depicted in Fig. 1 as contributing to rc require some
general explanation. First, they represent bulk properties and are not
usually simply related to a single measurable quantity in the field. Rather,
they correspond to properties or behaviors inferred from measurements of net
vertical fluxes above the bulk surface. For example, rs is the bulk canopy
stomatal resistance and itself consists of series and parallel pathways of
mass transfer due to the diffusion through leaf stomatal apertures that may
exist on one or both sides of the leaves. Further, these leaves are
distributed throughout the canopy and do not have uniform stomatal resistances
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ra . aerodynamic
rb , sublayer
•HW-
Vegetation
Cg "Ground"
Figure 1. Schematic diagram of pathway resistances used in the module, where
rc is derived via Equation (2).
because of varying solar irradiation, temperature, ventilation, etc. The
mesophyll resistance (bulk: rm) and the resistance (bulk: r|u) of the outer
surfaces of leaves in the upper canopy would also vary according to position
in the canopy. Another important point is that the landuse types represent
very broad categories. For example, one type represents all agricultural
crops, regardless of their heights and physiological characteristics. This
lack of detail may result in a poor estimate of surface resistance for any
particular surface cover, at a specific location and time.
The values assumed for baseline resistances are listed in Table 2. They
form the basis for estimating the resistances for all the gases to be
considered here. The values for r; represent the minimum bulk canopy
stomatal resistances for water vapor. It is well known that stomatal
resistance varies with solar radiation and temperature. In the previous dry
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Table 2. Input resistances (s m'1) to the module for
computations of surface resistances (rc). Entries of
9999 indicate that there is no air-surface exchange via
that resistance pathway.
Res 1 stance Landuse type
component 123466789 10 11
Seasonal category 1; midsummer with lush vegetation
r; 9999. 60. 120. 70. 130. 100. 9999. 9999. 80. 100. 150.
PIU 9999. 2000. 2000. 2000. 2000. 2000. 9999. 9999. 2600. 2000. 4000.
r 100. 200. 100. 2000. 2000. 2000. 0. 0. 300. 150. 200.
rasS 400- 1E0' 360' 5SX>. 500. 100. 0. 1000. 0. 220. 400.
rasO 300' 150' 200- 200' 200' 300- 2000' 400' 1000- 180' 200-
rlie 9999. 2000. 2000. 2000. 2000. 2000. 9999. 9999. 2500. 2000. 4000.
re|Q 9999. 1000. 1000. 1000. 1000. 1000. 9999. 9999. 1000. 1000. 1000.
Seasonal category 2; autumn with unharvested cropland
P; 9999. 9999. 9999. 9999. 250. 500. 9999. 9999. 9999. 9999. 9999.
p,u 9999. 9000. 9000. 9000. 4000. 8000. 9999. 9999. 9000. 9000. 9000.
p._ 100. 160. 100. 1500. 2000. 1700. 0. 0. 200. 120. 140.
rasS 400' 200' 360- 500- 600' 100- 0- 1000' 0- 300- 400>
rasO 30°- 150' 200- 200- 200- 300- 2000' 400- 800- 180- 200-
PC 1C 9999. 9000. 9000. 9000. 2000. 4000. 9999. 9999. 9000. 9000. 9000.
PC,O 9999. 400. 400. 400. 1000. 600. 9999. 9999. 400. 400. 400.
Seasonal category 3; late autumn after frost, no snow
r; 9999. 9999. 9999. 9999. 250. 500. 9999. 9999. 9999. 9999. 9999.
p,u 9999. 9999. 9000. 9000. 4000. 8000. 9999. 9999. 9000. 9000. 9000.
r.e 100. 10. 100. 1000. 2000. 1500. 0. 0. 100. 60. 120.
rasS 400- 150- 350- E00- 500- 200- 0- 1000- 0- 200- 400-
rasO 300- 1B0' 200' 200' 200- 300- 2000- 400' 1000' 180- 200'
PC is 9999. 9999. 9000. 9000. 3000. 6000. 9999. 9999. 9000. 9000. 9000.
PCI0 9999. 1000. 400. 400. 1000. 600. 9999. 9999. 800. 600. 600.
Seasonal category 4; winter, snow on ground and subfreezing
r- 9999. 9999. 9999. 9999. 400. 800. 9999. 9999. 9999. 9999. 9999.
PIU 9999. 9999. 9999. 9999. 6000. 9000. 9999. 9999. 9000. 9000. 9000.
rac 100. 10. 10. 1000. 2000. 1600. 0. 0. 60. 10. 50.
rasS 100- 100' 100' 100> 100- 100- 0- 1000- 100- 100- 50-
Pas0 600- 3600' 3500' 3500' 3500- 3500- 2000- 400' 3S00- 3500- 3500-
p"is 9999. 9999. 9999. 9000. 200. 400. 9999. 9999. 9000. 9999. 9000.
PC|O 9999. 1000. 1000. 400. 1600. 600. 9999. 9999. 800. 1000. 800.
Seasonal category 6; tpansitional spring with partially gpeen short annuals
r; 9999. 120. 240. 140. 250. 190. 9999. 9999. 160. 200. 300.
PIU 9999. 4000. 4000. 4000. 2000. 3000. 9999. 9999. 4000. 4000. 8000.
rac 100. 60. 80. 1200. 2000. 1500. 0. 0. 200. 60. 120.
pflsS 600. 160. 360. 600. 600. 200. 0. 1000. 0. 260. 400.
rasO 300- 150' 200' 200' 200' 300- 2000' 400' 1000- 180- 200-
r°|S 9999. 4000. 4000. 4000. 2000. 3000. 9999. 9999. 4000. 4000. 8000.
rc|0 9999. 1000. 600. 600. 1500. 700. 9999. 9999. 600. 800. 800.
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deposition module, solar radiation categories were used to form tables of
resistance, and temperature was not explicitly included (Sheih et at., 1986;
Walcek et aL., 1986). Here we use the following generalized function
to estimate the bulk canopy stomatal resistance:
rs =
[200(G+0.1)-1]2><400[TS(40-TS)]-1>, (3)
where G is the solar irradiation in watts per square meter and Ts is the
surface air temperature in degrees Celsius between 0 and 40 °C. Outside this
range, we set rs to a very large value, to implement the assumption that the
transfer through stomata is stopped. Equation (3) is derived from information
provided by Baldocchi et aL. (1987), who reviewed a number of scientific
studies to formulate similar relationships specific to certain plant species.
While our landuse map does not provide the detailed information necessary to
make species-specific estimates of stomatal resistance, Equation (3) should
provide representative variations caused by solar radiation and temperature.
The combined minimum stomatal and mesophyll resistance for substance x
- *- • :
can be found as
rsmx = rsDH20/Dx * rmx» (4)
where Dx is the molecular diffusivity of gas x in air, D^Q is the molecular
diffusivity for water vapor, and rmx is the mesophyll resistance for the
gas of interest. For 03 and $0*2, the mesophyll resistance is practically
zero, and suggestions wi I I be made later for methods to estimate rmx for
other substances.
The lower canopy resistance rc| is meant to account for uptake pathways
at the leaves, twig, bark, etc., while the ground surface resistance rgs
signifies uptake at the "ground" by soil, leaf litter, snow, water, etc. In
Table 2, separate values for SQ.2 and 63 are indicated by the additional
subscripts "S" and "0," respectively. We expect that all surfaces represented
by rjc and Pgs have a reduced capacity for uptake when cold. For example,
surface resistances for uptake of HN03, S02, and N02 by snow increase markedly
when its temperature decreases below 2 °C (Johansson and Granat, 1986; Valdez,
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1987). Accordingly, we approximate such an effect for all surfaces by adding
the value, in seconds per meter, of lOOOexp [-Ts-4] to r|c and rgs (and r|u)
for all substances. It is unknown whether this procedure is correct for every
substance, and there may be notable exceptions. For example, recent work has
shown that the rate of uptake of ^02 by ice is not reduced when the
temperature drops below freezing (Lee Y.N., Brookhaven National Laboratory,
private communication).
The values of rac are estimated solely by landuse and season, mostly
on the basis of the depth of the structure, which is usually a plant canopy.
The value of rac increases with representative heights and densities of the
"canopies," in accordance with findings concerning ozone deposition velocity
(Wesely, 1983). The resistance r
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land) for ozone, in which rc|Q is allowed to be as small as 1000 s nT1 in order
to allow ozone destruction at the surfaces of dry materials such as bushes
that protrude above the snow.
The gas-phase sublayer resistance r^ is shown as being common to all
lower branches of the pathways in Fig. 1, although it is normally only
applicable to transfer at the upper portions of the overall surface.
Formulation of bulk sublayer resistances in the lower canopy and at the ground
beneath the canopy is quite difficult, because these resistances should depend
on local rates of momentum transfer, for which suitable parameterizations are
not readily available. As a result, the approach represented by Fig. 1 may be
inadequate for situations in which the molecular diffusivity of the substance
of interest is much different from that for SQ.2 and 63, when exchange at
surfaces below the upper canopy comprises a large portion of the net vertical
flux above the canopy.
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SECTION 3
EXTENSION TO OTHER SUBSTANCES
Nitric oxide, nitrogen dioxide, and nitric acid vapor were treated fairly
explicitly by Sheih et aL. (1986), but other compounds such as NH0, ^02,
HCHO, other aldehydes, organic acids, organic peroxides, and peroxyacetic acid
have been treated in a less thorough fashion (Chang et aL., 1987). As a result
of their reactivity or solubiIity, a 11 these substances and others such as PAN
and HN02 may be deposited on the surface of the Earth at a significant rate.
Table 3 lists the properties we will use to estimate the surface resistances
for these gases. As shown in Equation (4), the ratio of their molecular
diffusivities in air to that of water vapor directly affects the stomatal
resistance.
The effective Henry's Law constants in Table 3 are used to estimate
uptake by moist and wet surfaces, including extracellular water in the
substomatal cavities of plant leaves. To represent the ability of the gas to
go into such aqueous solutions, this effective Henry's Law constant
incorporates the effects of acid-base equilibria at a pH of seven. While this
pH may be too high for some fresh water lakes, it is reasonable for ocean
water and some large lakes such the Great Lakes. Also, near-neutral
conditions are typical of plant sap, whose pH presumably is not much different
from that encountered in the substomatal cavities in the leaves of many plants
(Canny, 1984). We assume that the hydration and formation of ions are rapid
(to the extent that they occur), as is the case for S02 (Martin, 1984).
The values listed in Table 3 for the negative log of electron activity
for half redox reactions in neutral aqueous solutions [pe°(W)] and the overall
second-order reaction rates with S(IV) [k(2)] provide a means to estimate a
reactivity factor fg for oxidation of biological substances. Three categories
are used: highly reactive (fQ=l), which implies that the gas is as reactive
as 03; slightly reactive (ffl=0.1); and nonreactive (fg=0). The slightly
10
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Table 3. Gases considered in the dry deposition module and their properties
relevant to estimating resistances to dry deposition.
Gaseous species
Sulfur dioxide
Ozone
Nitrogen dioxide
Nitric oxide
Nitric acid vapor
Hydrogen peroxide
Aceta 1 dehyde
Forma 1 dehyde
Methyl hydroperoxide
Peroxyacetic acid
Formic acid
Ammonia
Peroxyacetyl nitrate
Nitrous acid
Symbo 1
S02
03
N02
NO
HN03
H202
(ALD)f
HCHO
(OP)f
PAA
(ORA)f
NH3
PAN
HN02
0H:
1
1
1
1
1
1
1
1
1
2
1
1
2
1
2o/o,
.9
.6
.6
.3
.9
.4
.6
.3
.6
.0
.6
.0
.6
.6
a H*b»c
(M atm'1)
1X105
0.01
0.01
2X10-3
1X1014
1X105
15
6X103
240
540
4X106
2X104
3.6
1X105
pe°(W)M k(2)e fQ
(M'1 s'1)
-5
28
—
—
7
23
neg.
-3
—
— —
-8
_
—
6
6X108
2X106
<1X10~2
3X1Q3
4X10'4
0
1
0.
0
0
1
0
0
0.
0.
0
0
0.
0.
1
1
1
1
1
-: Not relevant.
—: Information not found.
aComputed as the square root of ratio mx/mn20 of molecular weights.
"Effective values for water with near-neutral pH.
cDrawn primarily from summaries by Schwartz (1984) and Gaffney et aL.
(1987); Lind and Kok, 1986 (methyl hydroperoxide and PAA); Jacob, 1986 (formic
acid).
^Obtained primarily from Stumm and Morgan (1981) and Morel (1983).
ePseudo-first-order rate constants for oxidation of S(IV) in water with
near-neutral pH, derived for 03 (Hoffman, 1986); N02 (Lee and Schwartz,
1983); NO and HN03 (Martin et aL., 1981); H202 (articles reviewed by
Seinfeld, 1986); methyl hydroperoxide and PAA (Lind et aL., 1987); PAN (Lee,
1984; Calvert et aL., 1985); HN02 (Oblath et aL., 1981).
'Class of substances (aldehydes, organic peroxides, and organic acids)
represented by the species shown.
11
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reactive category is intended primarily to set plant leaf mesophylI
resistances to very small values and to allow rapid uptake of gases through
plant leaf stomata. As is evident in Table 3, the value of fn=0.1 is
assigned to substances that have a rather small value of pe°(W) but still
have a significant second-order reaction with S(IV). This procedure is based
on the hypothesis that if a substance can oxidize S(IV), it will be removed
rapidly in the slightly reducing environment of the substomatal materials.
Support for this hypothesis comes from the observations that NO^ seems to
have a very small mesophylI resistance (Wesely et at., 1982; Delaney and
Davis, 1983). The use of reactivity with S(IV) as an indicator, nevertheless,
is only an expedient that takes advantage of the large amount of information
that has become available on this pseudo-first-order reaction rate (see
references listed in Table 3). This is not meant to imply that the S(IV)
components of S02(aq), HS03~, and S03^~ in extracellular water are unaffected
by other reactions [e.g., see Mudd (1975a) for a discussion of the fate of
$02]. The reality may be that the pathways of uptake of substances such
as N0.2 are strongly influenced by enzymatic processes (e.g., Law and Mansfield,
1982). Further, these pathways may be cut off when the gas-phase
concentrations reach a fairly low value corresponding to a compensation point
for the biota (Johansson, 1987).
The mesophylI resistance in Equation (4) is computed for any substance
x on the basis of the key parameters H* and fg:
rmx = (H*/3000 + 100fg)-l. (6)
This relationship assumes that two parallel pathways exist to the
extracellular water inside plant leaf stomata. The pathway based on fg
produces very small values of rmx when fg is 1 or 0.1. The other pathway
is via dissolution in the aqueous solution, and the factor 3000 M atm'l is
derived in part from the consideration that if H* is sufficiently large,
the concentration that can be achieved in the aqueous phase represents a large
sink for the substance. As Equation (6) indicates, values of H* greater
than about ten will result in fairly rapid uptake. The exact value of 3000 is
derived from considerations of C02 uptake by vegetation. For example, it is
well known that uptake rates of 1 mg m~2 s~l are approached with lush
12
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vegetation in optimum ambient conditions (e.g., Monteith, 1973). This rate
corresponds to a (bulk canopy) mesophyll resistance of approximately 600
s m~l. At a pH of seven, H* for CQ.2 is near 4.4, and the value of 3000 as a
rounded-off equivalent to (4.4)(600) is used in Equation (6). Although the
hydration rate of C0.2 is normally slow (Quinn and Otto, 1971), we have assumed
that it is accelerated by enzymatic reactions in the leaf, which would allow
rapid equilibrium to be established.
The resistance of the outer surfaces of leaves in the upper canopy is
computed as
HUX = nu(10-5H* + fo)'1- (?)
This allows for two parallel routes to the substrate, one analogous to 862
pathways and one to 63 pathways. Substances such as HN03 that have a very
high solubility in aqueous solution will be removed rapidly at the surface, as
.is indicated by the first term on the right-hand side. The second term allows
highly reactive substances to behave as 03 and is effective in reducing uptake
for substances classified as slightly reactive (fg=0.1).
For uptake of a gas that has a nonzero value of fg and does not have
an extremely large value of H*, Equation (7) implies that the gas will
diffuse though the outer surfaces of leaves in the same way as do S02 and 63.
No adjustments are made for molecular size and varying diffusivities in air,
just as no differentiation between S0.2 and 03 is made in the values of r|u. We
could, for example, hypothesize that uptake at outer surfaces is limited by
molecular diffusion in air and then modify the terms on the right-hand side
accordingly. This hypothesis would envision the outer surfaces as being
mostly impervious except for tiny air-filled gaps, smaller than stomatal
openings. However, such scaling with diffusivities is questionable even for
00*2, which is one of the few substances other than water vapor that has been
studied with regard to leaf cuticular resistances (e.g., Holmgren et ai.,
1965). In addition, Equation (7) does not account for the possibility that
nonpolar substances might dissolve readily in the waxy covering of the
cuticle. For example, it has been found that vapor-phase PCBs accumulate to a
13
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significant extent in plant leaves (Buckley, 1982), and that the octanol-water
partition coefficient appears to be a key parameter for describing the foliar
uptake of organic compounds (Travis and Hattemer-Frey, 1988).
The resistance of the exposed surfaces in the lower portions of
structures (canopies, buildings) above the ground is computed as the parallel
sum of resistances corresponding to those for S02 and 63:
rclx = [H*/(105rclS) + fn/rc,0]-l. (8)
The two terms on the right-hand side have the same function as the terms on
the right-hand side of Equation (7), but here the individual resistances,
rc|$ and rc|Q, have been incorporated.
Computation of resistance to uptake at the "ground" surface takes an
approach equally simple as that in Equations (7) and (8). For the varied
situations that include bodies of water, bare soil, and litter beneath forest
canopies, the resistance is computed as
rgsx = [H*/(105rgsS) + fo/rgsQ]'1. (9)
For surfaces with a pH significantly less than seven, it would be desirable to
use appropriately adjusted values of H*, even for 50*2 .
14
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SECTION 4
EFFECTS OF DEW AND RAIN
One effect of dew and rain at the surface is the covering of leaf
stomata, which cuts off direct gas exchange when the stomata are open. Field
observations in recent unpublished experiments at Argonne National Laboratory
indicate that about two-thirds of the leaves in a canopy are typically
covered, although the amounts can vary widely. Accordingly, the value of
rs in Equation (4) should be increased by a factor of three. The only other
adjustment we make is in the value of r|u, for the leaves in the upper canopy.
Since we thus assume that altered resistances in other portions of the canopy
are relatively insignificant, care must be taken to make arithmetic adjust-
ments that allow some effects of dew when the "canopy" is not vegetative, such
as in urban areas. For dew, the results of the experiments at Argonne
National Laboratory indicate that the resistance to S02 uptake by vegetation
is probably decreased, but the uptake of 03 is retarded. A reasonable
approximation for the resistance to S02 uptake by a dew-covered surface is
riuS = 100 s m-1, (10)
which results in a very small value of rc. For 03, the dew acts as a barrier
to surface removal:
r|u0 = [1/3000 + l/(3r,u)]-l, (11)
where the second term on the right-hand side takes into account the reduction
of dry areas available for removal. The value of 3000 s m~l in the first term
is only a rough approximation.
Wetting of surfaces by rainfall probably has quite different effects.
Unpublished measurements by Argonne National Laboratory indicate that rainfall
results in an increase of resistance to S02 uptake and may actually decrease
the resistance to 03. This is reasonable because the rainfall may be
sufficiently saturated with S(IV) to prevent further uptake of S02 and
15
-------
allow limited chemical reaction with 03. The extent of such behavior
would depend on the chemical properties of the ambient atmosphere and of the
substrates, as well as those of the rainfall. As a first approximation, we
estimate the resistance to 862 uptake by a surface wetted by rainfall to be
r|uS = [1/5000 + l/(3rrlu)]-l, (12)
which has a structure similar to Equation (11). For 03, rainfall might have
a weaker effect on surface remova I :
riuQ = [1/1000 + l/(3r|u)]-l. (13)
A special exception should be made for SQ.2 uptake in urban areas.
Preliminary results indicate that fairly pervious artificial materials such as
limestone take up SC>2 rather rapidly when wet or when the relative humidity
is high (Youngdahl A.C., Argonne National Laboratory, private communication).
In a attempt to take this factor into account, we recommend that the value of
rluS be adjusted for landuse type 1 when wet conditions prevail, so that
Equations (10) and (12) are then replaced with the following:
rluS = 50 s m~l-
This will probably require modification as better information is obtained.
For substances other than S02 and 83, the following formulation
replaces Equation (7) if either dew or rain wets the surface:
Hux = [l/(3r)u) + 10-7H* + fo/nuO]'1* (14)
where reduction of dry area, solubility in water, and chemical reactivity are
taken into account by the first, second, and third terms, respectively, on the
right-hand side. In this case, r|uQ is taken from Equation (11) for dew
and from Equation (13) for rain.
16
-------
In practical application of Equations (10) through (14), information on
dewfall and rainfall events must be provided from sources external to the dry
deposition module. A direct computation of the surface wetness would be most
desirable, e.g., by estimating the amount of free surface water accumulated
and then evaporated. Alternatively, surface relative humidity might be a
useful index. After dewfall and rainfall events are completed, surface
wetness often disappears as a result of evaporation after approximately two
hours of good atmospheric mixing, the period of time recommended earlier
(Sheih et aL., 1986) and found to be typical for dew during recent
experiments at Argonne Natinal Laboratory. An important subcategory of surface
wetness is that caused by fog or cloud water impaction on surface elements.
Resistances would probably then be altered in the same fashion as they are for
rainfall, since the chemistries may be similar.
17
-------
SECTION 5
EXAMPLES AND DISCUSSION
The tables in Appendix I give examples of surface resistances (rc)
for selected values of solar irradiation and one case each for dew and rain
when G is zero. The surface temperatures assumed were 25, 10, 2, 0, and 10 °C
for seasonal categories 1-5, respectively. The values shown have been
truncated to give no more than two significant digits. For S&2 and 03,
there are some significant differences from the previous version of the dry
deposition module (Sheih et at., 1986), but the present results are more
rigorously derived and probably more realistic. Overall, we anticipate that
the deposition velocities for the two substances as derived with these
procedures will be hardly distinguishable from estimates made from the
previous version of the module. Likewise, little should have changed with
regard to deposition velocities for N02, NO, and HNOs- The latter two are not
represented in Appendix I because the computed values of rc are always
very large (entry of 9999) for NO and zero for HNOs- Neither set of
surfaces resistances is very controversial, except that NO (and some of the
other common nitrogen compounds) may be emitted from the surface rather than
removed from the atmosphere (Galbally 1985; Anderson and Levine, 1987;
Williams et at., 1987) and that notable changes of HN03 fluxes with height
can occur if HN03 is present (Huebert B.J., University of Rhode Island,
private communication) . In practical applications involving regional-scale
atmospheric models, a small value of rc near 10 s m~l should be used rather
than the zeros indicated in Appendix I for HN03 and for some other
substances under certain conditions, in order to avoid unrealistic situations
of extremely high deposition velocities over unusually rough surfaces.
As is desired, the calculated surface resistances for N02 are usually
quite large except for lush vegetation exposed to solar radiation, when leaf
stomata are open. This conforms to a number of experimental investigations
involving atmospheric concentrations of at least a few ppbV of N02 over a
variety of surfaces recognized in each study as not being sources of the gas
18
-------
(e.g., Wesely et al., 1982; Delaney and Davis, 1983; Gravenhorst and Bottger,
1983). Use of the value fQ=0.1 in Equation (6) implies fairly efficient
uptake through stomata. It has been suggested that the measurement methods
used in some of the field work tended to cause underestimates of N02 surface
resistances because of interference by HN03 in sensor response (Huebert,
1983), but subsequent unpublished reevaluations by several investigators have
indicated that overestimates were more likely because the interference may
have increased only the mean concentrations and not the eddy fluctuations
measured. The recommendations of Sheih et aL. (1986), which ignored the
possible HN03 effect, are still plausible: the minimum computed values of rc
for N0.2 should be about 1.75 times the corresponding 03 resistances.
According to the entries for seasonal category 1 for a value of G=800 W
m~2 s~l in Appendix I, the ratios of rc for NQ.2 to rc for 0.3 average to about
1.5 for the landuse types that indicate a surface covered with vegetation.
The resistances for N02 for surfaces other than sunlit vegetation appear
to be quite large (Appendix I). This results from use of relatively small
values of fg and H* in Equations (7), (8), and (9). Sheih et aL. (1986)
suggested that these resistances should be high, near 1000 s m~l, and
recommended that, in general, the sum of NO and N02 should be considered
rather than N02 alone. This was suggested because rapid in-air chemical
reactions can cause a significant change of NO and N02 vertical fluxes
between the surface and the point at which deposition velocities are applied,
but the sum of NO and N02 fluxes should be practically unchanged
(Fitzjarrald and Lenschow, 1983). This summing is clearly a desirable
procedure, especially in nonurban environments away from local anthropogenic
emissions where concentrations of N02 and NO are much smaller than 03
concentrat ions.
The resistances for the other substances in Appendix I are predictions
that in many cases have no supporting field or laboratory observations.
Hydrogen peroxide has the unusual properties of being both moderately soluble
in water, as is S02 near a pH near seven, and as strong an oxidizing agent
as 03. Rapid removal takes place at wet surfaces and moderately rapid
deposition occurs over vegetation. Many surfaces that may seem somewhat
inert, such as in unharvested agricultural areas, remove \\<^2 fairly
19
-------
efficiently. Solubility alone is highlighted in the surface resistances
calculated for formaldehyde (HCHO) , formic acid (HCOOH, or ORA to represent
organic acids), and aceta I dehyde (CHsCHO , or ALD to represent aldehydes
other than HCHO). Formaldehyde is taken up rather rapidly at liquid water
surfaces and by sunlit vegetation, but has much less interaction with soils
and senescent vegetation. The rather large solubility of formic acid allows
it to be taken up rapidly at many different types of surfaces. Variations on
the same theme are seen for NH3 and HNO^. Laboratory and field observations
have shown that NH3 can be taken up quickly through leaf stomata and by
moist surfaces in an agricultural crop (Hutchinson et aL., 1972; Denmead et
a.1. , 1978; Lemon and Van Houtte, 1980; van Hove et aL., 1987). The
resistances to NH3 uptake by green vegetation (seasonal categories 1 and
5) are smaller than the corresponding resistances for 862 because rsmx
calculated with Equation (4) for NH3 is reduced by almost a factor of two
as a result of its smaller molecular diffusivity.
This effort to evaluate surface resistances does not consider the fact
that NH3 is often emitted from soils, particularly when atmospheric
concentrations are lower than a few ppbV (e.g., Dabney and Bouldin, 1985). As
was already discussed, NO and N02 might also be emitted from the surface.
A first approximation to account for these emissions and thus obtain more
realistic estimates of air-surface exchange would involve adjusting rc
values found with Equation (2) for NH3, NO, and N02 by multiplying each rc by
Cc)« where Cc is equal to an assumed compensation point of 2 to 3 ppbV.
The remaining three substances, methyl hydroperoxide (CH302H, or OP to
represent several organic peroxides), peroxy acetic acid [CH3C(0)02H, or PAA] ,
and peroxyacetyl nitrate [CH3(0)02N02, or PAN], have slightly limited
solubility and are moderately reactive as oxidants. PAN is the least soluble
and thus has the largest surface resistance of the three substances for sunlit
green vegetation. Interpretation of data of Mudd (1975b) leads to the
conclusion that PAN (as well as peroxypropionyl nitrate) can be taken up quite
rapidly through leaf stomata; Hill (1971) and Garland and Penkett (1976) found
that deposition velocities for PAN are typically 1/2 to 1/3 of those for 03.
This is at least partially consistent with the entries in Appendix I, from
which we infer that maximum deposition velocities near 0.005 m s~l are
20
-------
possible, for the optimum conditions of a fully sunlit, lush vegetative
canopy. By comparison with the computed surface resistances for acetaldehyde,
it is apparent that the chemical reactivity of PAN is probably the major
factor in affecting its surface resistance, not its solubility in water.
21
-------
SECTION 6
CONCLUSIONS
A scheme has been presented that breaks the surface resistances (rc) for
atmospheric gases into components that represent mass transfer pathways at the
stomatal apertures of leaves, mesophyll of leaves, outer surfaces of leaves in
the upper canopy, exposed surfaces in the lower portions of the canopy or
structure, and "ground" surfaces that include soil, leaf litter, and water.
Gas-phase resistance pathways leading to the latter two locations inside or
beneath canopies are also specified. Because of the relatively large amount
of information available on the dry deposition velocities of S02 and 03, their
resistances are estimated explicitly for the above components. Based on the
solubilities and chemical reactivities relative to those for S02 and 63,
formulas are suggested for the surface resistance components for several other
substances important in acid deposition or related atmospheric chemistry.
These include N02, NO, HNOs, ^2, HCHO, acetaldehyde (to represent
aldehydes other than HCHO), methyl hydroperoxide (to represent organic
peroxides), peroxyacetic acid, HCOOH (to represent organic acids), NH3, PAN,
and HN02- For many of these substances, the resistances computed represent
predictions that have yet to be verified with observations. This scheme can
be used to predict the surface removal of many other substances as well.
The formulations used to compute the surface resistance components and
add them together to obtain values of rc for various substances and types
of surfaces are derived in a form suitable for use in numerical models of
regional-scale atmospheric transport, chemical transformation, and deposition.
This allows updating of the dry deposition module of the Regional Acid
Deposition Model (RADM). Appendix II gives a listing of the Argonne version
of the dry deposition module, which may be adapted for use with RADM or other
models that require the information. It should be noted, however, that the
surface resistances that can be computed are specific to 11 landuse types
(Table 1) and thus might not be directly useful in numerical models that
use different surface characterizations.
22
-------
The scheme for computing surface resistances is rather simplistic because
it categorizes all surfaces by only 11 landuse types and considers five
general seasonal categories. The dry deposition module will probably not
produce very accurate estimates of dry deposition for a short time period at a
particular small area. Rather, the estimates are intended for long-term
averages over at least several weeks and for rather large areas over which the
individual variations of plant species composition and factors such as soil
moisture content are smoothed. For vegetation, uptake resistances by
individual plant species have not been identified, and the influence of
varying leaf areas (green or senescent) has not been tied explicitly to a
measurable quantity such as LAI (leaf area index). The following factors are
considered in a general fashion: vegetation height, aridity or soil moisture
content, surface temperature, and variations of leaf stomatal resistance with
solar radiation and temperature.
Wet surfaces have a variety of surface resistances, which the module
generalizes considerably. For open bodies of water, we have assumed an
aqueous pH near seven, which is undoubtedly too large for many small bodies of
water. For ozone, we have assumed-that the surface resistance suitable for
seawater is relevant (rc=2000 s m~l), which is probably too small for fresh
water. Uptake by vegetation wetted by dewfall is assumed to be enhanced for
S02 and retarded for 03, while the opposite changes are suggested for surfaces
wetted by rainfall. It is likely that surface wetness caused by impaction of
fog or cloud water would alter surface resistances in a manner similar to
rainfall. The effects of dew, rain, fog, and cloud water, however, are not
well understood, and revisions to the approach taken here might be necessary
as further information becomes available.
A number of factors that can strongly influence air-surface exchange
rates are not considered here. Oases that undergo rapid chemical reactions in
the air should be treated cautiously because resulting changes of fluxes with
height might cause unusual variations of deposition velocity with height, e.g.
for 03, NO, or NQ<2 treated separately. Soil alkalinity or acidity can have a
strong influence on the surface resistances of some substances; S02 removal
rates by dry or acidic soils are undoubtedly much slower than by wet or
alkaline soils. For many substances, natural emissions may be much more
23
-------
important than dry deposition in affecting local air chemistry, e.g., for NO
and NH3- In addition, the use of a deposition velocity for NQ2 and NH3 can
be misleading if concentrations near the surface are not considered, because
many surfaces have a compensation point corresponding to an atmospheric
concentration of 2-3 ppbV, below which the surface resistance becomes very
large. This could occur for other substances as well.
24
-------
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28
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Appendix I. Computed surface resistances rc (s
Solar irradiation (W nT^)
Landuse
type
Sulfur d
Seasonal
1
2
3
4
6
6
7
8
9
10
11
S«asona 1
1
2
3
4
6
6
7
8
9
10
11
S«asona 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
S«asona 1
1
2
3
4
E
6
7
8
9
10
11
800
i ox i de
category 1,
490
80
140
120
200
160
0
970
100
120
190
category 2,
490
320
400
1300
380
600
0
970
190
380
480
category 3,
490
160
410
1100
740
940
0
970
100
230
460
category 4,
210
120
120
980
340
430
10
990
160
120
110
category 5,
690
110
220
260
350
310
0
970
120
180
290
500
300
midsummer with lush
490.
90.
140.
130.
210.
170.
0.
970.
100.
120.
200.
autumn with
490.
320.
400.
1300.
400.
620.
0.
970.
190.
380.
480.
late autumn
490.
160.
410.
1100.
770.
950.
0.
970.
100.
230.
460.
winter with
210.
120.
120.
980.
380.
460.
10.
990.
160.
120.
110.
transitional
590.
120.
230.
280.
370.
330.
0.
970.
130.
180.
300.
490.
100.
160.
160.
250.
200.
0.
970.
120.
140.
220.
100
0
0 0
Wetted surface
dew
rain
vegetation
490.
180.
250.
370.
500.
430.
0.
970.
190.
220.
360.
490.
290.
360.
1000.
1000.
940.
0.
970.
260.
300.
600.
40.
70.
80.
90.
90.
90.
0.
970.
70.
70.
80.
40.
300.
370.
1100.
1100.
1000.
0.
970.
260.
310.
490.
unharvested cropland
490.
320.
400.
1300.
460.
680.
0.
970.
190.
380.
480.
490.
320.
410.
1300.
770.
960.
0.
970.
190.
380.
480.
after frost, no
490.
160.
410.
1100.
820.
990.
0.
970.
100.
230.
460.
show on
210.
120.
120.
980.
450.
520.
10.
990.
160.
120.
110.
spr i ng
590.
120.
250.
330.
410.
370.
0.
970.
140.
190.
320.
490.
160.
410.
1100.
1000.
1100.
0.
970.
100.
230.
460.
ground
210.
120.
120.
990.
680.
690.
10.
990.
160.
120.
110.
490.
330.
410.
1400.
1300.
1300.
0.
970.
190.
390.
490.
snow
490.
160.
420.
1100.
1300.
1200.
0.
980.
100.
240.
480.
210.
120.
120.
1000.
1300.
1200.
10.
990.
160.
120.
110.
with partial green
690.
160.
320.
620.
640.
630.
0.
970.
160.
240.
410.
690.
180.
370.
1100.
1000.
1000.
0.
970.
180.
280.
470.
40.
70.
80.
90.
90.
90.
0.
970.
60.
80.
80.
40.
160.
80.
90.
90.
90.
0.
980.
60.
70.
80.
210.
120.
120.
1000.
1300.
1200.
10.
990.
160.
120.
110.
coverage
40.
60.
80.
90.
90.
90.
0.
970.
60.
70.
80.
40.
310.
390.
1200.
1300.
1100.
0.
970.
190.
370.
460.
40.
160.
390.
1000.
1300.
1100.
0.
980.
90.
230.
450.
210.
120.
120.
1000.
1300.
1200.
10.
990.
160.
120.
110.
40.
180.
370.
1000.
1100.
1000.
0.
970.
180.
270.
450.
29
-------
Appendix I continued
Ozone
Season* 1
1
2
3
4
6
6
7
8
9
10
11
Season* 1
1
2
3
4
E
6
7
8
9
10
11
Seasons 1
1
2
3
4
5
6
7
8
9
10
11
Season* 1
1
2
3
4
6
6
7
8
9
10
11
Season* 1
1
2
3
4
6
6
7
8
9
10
11
category 1,
390.
70.
100.
100.
160.
130.
1900.
390.
110.
100.
130.
cateaory 2.
390.
190.
190.
430.
300.
360.
1900.
390.
360.
190.
210.
cateaory 3.
390.
140.
190.
390.
500.
470.
1900.
390.
600.
170.
220.
cateaory 4,
700.
900.
900.
550.
1000.
660.
1900.
410.
730.
820.
730.
cateaory 5,
390.
100.
140.
180.
300.
230.
1900.
390.
190.
130.
170.
midsummer with lush
390.
80.
110.
110.
170.
140.
1900.
390.
120.
100.
140.
autumn with
390.
200.
200.
460.
320.
390.
1900.
390.
390.
200.
220.
late autumn
390.
140.
200.
420.
530.
500.
1900.
390.
510.
180.
230.
winter with
700.
940.
940.
610.
1000.
700.
1900.
410.
770.
860.
770.
transitional
390.
100.
140.
190.
320.
240.
1900.
390.
210.
130.
180.
390.
90.
120.
130.
200.
170.
1900.
390.
140.
120.
160.
veoetati
390.
170.
180.
320.
420.
380.
1900.
390.
310.
190.
240.
ion
390.
290.
260.
950.
960.
970.
1900.
390.
790.
270.
350.
390.
290.
250.
950.
950.
970.
1900.
390.
750.
270.
330.
390.
240.
210.
680.
680.
690.
1900.
390.
500.
230.
270.
unharvested cropland
390.
210.
210.
520.
370.
440.
1900.
390.
420.
210.
230.
390.
240.
240.
700.
630.
690.
1900.
390.
540.
240.
260.
after frost, no
390.
140.
210.
460.
570.
650.
1900.
390.
640.
180.
230.
snow on
700.
1000.
1000.
700.
1100.
780.
1900.
410.
830.
910.
830.
spring
390.
110.
160.
220.
360.
280.
1900.
390.
240.
140.
190.
390.
150.
240.
600.
770.
740.
1900.
390.
630.
190.
260.
ground
700.
1200.
1200.
1000.
1300.
1000.
1900.
410.
1000.
1100.
1000.
390.
280.
280.
1200.
1200.
1300.
1900.
390.
820.
280.
310.
snow
390.
160.
280.
950.
1200.
1200.
1900.
390.
890.
220.
300.
700.
2500.
2500.
3000.
2300.
2400.
1900.
410.
2000.
2000.
2000.
with partial green
390.
150.
200.
430.
670.
600.
1900.
390.
430.
180.
240.
390.
180.
250.
940.
960.
1000.
1900.
390.
850.
220.
290.
390.
260.
260.
940.
1000.
1000.
1900.
390.
670.
260.
290.
390.
160.
260.
760.
1000.
970.
1900.
390.
720.
210.
280.
700.
2600.
2500.
3000.
2300.
2400.
1900.
410.
2000.
2000.
2000.
coverage
390.
180.
240.
810.
960.
910.
1900.
390.
740.
210.
270.
390.
220.
220.
570.
610.
610.
1900.
390.
460.
220.
240.
390.
160.
220.
500.
610.
590.
1900.
390.
490.
180.
230.
700.
2500.
2500.
3000.
2300.
2400.
1900.
410.
2000.
2000.
2000.
390.
160.
210.
620.
580.
560.
1900.
390.
490.
180.
230.
30
-------
Appendix I continued
Nitrogen
Season* 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
e
6
7
8
9
10
11
Seasona 1
1
2
3
4
5
6
7
8
9
10
11
Seasona 1
1
2
3
4
E
6
7
8
9
10
11
dioxide
category 1 .
3000.
100.
190.
120.
210.
170.
9999.
3800.
140.
160.
230.
category 2.
3000.
1100.
1300.
1800.
460.
780.
9999.
3800.
2600.
1200.
1300.
category 3,
3000.
1300.
1300.
1700.
1200.
1600.
9999.
3800.
4200.
1400.
1500.
category 4.
6900.
7600.
7600.
3800.
8100.
4900.
9999.
4000.
6000.
7000.
6000.
category 6.
3000.
220.
390.
270.
460.
360.
9999.
3800.
320.
340.
480.
midsummer wi
3000.
100.
200.
130.
230.
180.
9999.
3800.
160.
170.
260.
autumn with
3000.
1100.
1300.
1800.
600.
830.
9999.
3800.
2600.
1200.
1300.
late autumn
3000.
1300.
1300.
1700.
1200.
1600.
9999.
3800.
4200.
1400.
1600.
winter with
6900.
7600.
7600.
3800.
8200.
6000.
9999.
4000.
6100.
7000.
6100.
transitional
3000.
240.
420.
290.
600.
390.
9999.
3800.
350.
370.
610.
th lush
3000.
130.
260.
160.
280.
220.
9999.
3800.
180.
210.
300.
vegetation
3000.
370.
620.
480.
770.
660.
9999.
3800.
690.
540.
730.
3000.
1400.
1700.
2800.
2800.
3300.
9999.
3800.
6300.
1600.
1800.
3000.
1400.
1600.
2700.
2700.
3100.
9999.
3800.
4800.
1600.
1800.
3000.
1200.
1500.
2300.
2300.
2600.
9999.
3800.
3600.
1400.
1600.
unharvested cropland
3000.
1100.
1300.
1800.
690.
970.
9999.
3800.
2700.
1300.
1400.
3000.
1200.
1400.
1900.
1300.
1700.
9999.
3800.
2900.
1300.
1400.
after frost, no
3000.
1300.
1400.
1700.
1400.
1800.
9999.
3800.
4200.
1400.
1600.
snow on
6900.
7600.
7600.
3900.
8400.
5100.
9999.
4000.
6100.
7100.
6100.
spring
3000.
280.
490.
350.
600.
470.
9999.
3800.
430.
430.
690.
3000.
1300.
1400.
1800.
2100.
2300.
9999.
3800.
4400.
1400.
1500.
ground
6900.
7900.
7900.
4300.
9200.
6600.
9999.
4000.
6400.
7400.
6400.
3000.
1400.
1700.
2600.
3000.
3400.
9999.
3800.
4700.
1600.
1800.
snow
3000.
1400.
1700.
2300.
3000.
3300.
9999.
3800.
6800.
1600.
1800.
6900.
9999.
9999.
9500.
9999.
9999.
9999.
4000,
9900.
9999.
9900.
with partial areen
3000.
640.
940.
850.
1300.
1100.
9999.
3800.
1100.
870.
1100.
3000.
1300.
1700.
2400.
2900.
3100.
9999.
3800.
6300.
1600.
1800.
3000.
1300.
1600.
2400.
2800.
3100.
9999.
3800.
4100.
1600.
1700.
3000.
1400.
1600.
2200.
2800.
3000.
9999.
3800.
4900.
1600.
1700.
6900.
9999.
9999.
ocdm
9DW •
9999.
9999.
9999.
4000,
9900.
9999.
9900.
coverage
3000.
1300.
1600.
2300.
2800.
2900.
9999.
3800.
4700.
1500.
1700.
3000.
1200.
1500.
2100.
2400.
2600.
9999.
3800.
3200.
1400.
1500.
3000.
1400.
1500.
1900.
2400.
2500.
9999.
3800.
3700.
1400.
1500.
6900.
9999.
9999.
9500.
9999.
9999.
9999.
4000.
9900.
9999.
9900.
3000.
1200.
1500.
2000.
2300.
2400.
9999.
3800.
3600.
1400.
1500.
31
-------
Appendix I continued
Hydrogen
Season! 1
1
2
3
4
6
6
7
8
9
10
11
Season* 1
1
2
3
4
6
6
7
8
9
10
11
Seasons 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
5
6
7
8
9
10
11
Seasona 1
1
. 2
3
4
5
6
7
8
9
10
11
perox i da
category 1. midsummer with lush
260.
60.
80.
80.
130.
110.
0.
280.
70.
80.
110.
260.
60.
80.
90.
140.
120.
0.
280.
80.
80.
120.
category 2. autumn with
260.
160.
1S0.
400.
240.
310.
0.
280.
140.
160.
180.
category 3,
260.
80.
160.
360.
400.
410.
0.
280.
90.
120.
180.
category 4.
190.
110.
110.
390.
300.
330.
10.
290.
130.
110.
100.
category 6 .
280.
70.
110.
160.
220.
190.
0.
280.
100.
90.
140.
260.
160.
160.
430.
260.
330.
0.
280.
150.
160.
180.
late autumn
260.
80.
160.
380.
410.
430.
0.
280.
90.
120.
180.
winter with
190.
110.
110.
420.
340.
370.
10.
290.
130.
110.
100.
260.
70.
90.
110.
160.
140.
0.
280.
90.
90.
130.
vegetation
260.
130.
140.
250.
320.
290.
0.
280.
150.
140.
200.
260.
210.
180.
640.
640.
630.
0.
280.
230.
190.
270.
260.
60.
60.
80.
80.
80.
0.
280.
70.
60.
70.
260.
60.
60.
80.
80.
80.
0.
280.
60.
60.
70.
unharvested cropland
260.
170.
170.
480.
290.
380.
0.
280.
150.
170.
190.
260.
190.
180.
640.
500.
590.
0.
280.
160.
190.
210.
after frost, no
260.
80.
170.
420.
450.
480.
0.
280.
90.
120.
•190.
snow on
190.
110.
110.
460.
400.
420.
10.
290.
140.
110.
100.
transitional spring
280.
70.
110.
170.
230.
200.
0.
280.
100.
100.
140.
280.
80.
120.
190.
260.
230.
0.
280.
110.
100.
150.
260.
80.
180.
540.
600.
640.
0.
280.
90.
130.
200.
ground
190.
110.
110.
610.
600.
610.
10.
290.
140.
110.
100.
260.
210.
210.
1000.
940.
1100.
0.
280.
180.
210.
260.
snow
260.
80.
210.
?30.
94C.
1000.
0.
280.
90.
130.
230.
190.
120.
120.
980.
1100.
1000.
10.
290.
160.
120.
110.
with partial green
280.
100.
150.
370.
410.
400.
0.
280.
140.
130.
190.
280.
110.
180.
740.
640.
720.
0.
280.
180.
160.
230.
260.
60.
60.
90.
90.
90.
0.
280.
60.
60.
70.
260.
80.
60.
80.
90.
90.
0.
280.
40.
60.
60.
190.
120.
120.
980.
1100.
1000.
10.
290.
150.
120.
110.
coverage
280.
50.
60.
80.
80.
80.
0.
280.
60.
60.
60.
260.
60.
60.
80.
80.
80.
0.
280.
60.
60.
60.
260.
80.
60.
80.
80.
80.
0.
280.
40.
50.
60.
190.
120.
120.
980.
1100.
1000.
10.
290.
150.
120.
110.
280.
60.
60.
80.
80.
80.
0.
280.
60.
60.
60.
32
-------
Appendix I continued
Acetaldahyde
Seasona 1
1
2
3
4
5
6
7
8
9
10
11
Season* 1
1
2
3
4
E
6
7
8
9
10
11
Season* 1
1
2
3
4
S
6
7
8
9
10
11
Seasonal
1
2
3
4
5
6
7
8
9
10
11
Seasona 1
1
2
3
4
S
6
7
8
9
10
11
category 1, midsummer with lush
9999.
300.
410.
320.
430.
380.
6400.
9999.
320.
380.
470.
category 2,
9999.
9999.
9999.
9999.
760.
1300.
6400.
9999.
6S00.
9999.
9999.
category 3.
9999.
9999.
9999.
9999.
2400.
4600.
9999.
9999.
9999.
9999.
9999.
category 4,
9999.
9999.
9999.
9999.
9999.
9999.
9999.
QQQQ
Wtfjf m
9999.
9999.
9999.
category 6,
9999.
470.
740.
610.
760.
630.
6400.
9999.
520.
660.
880.
9999.
310.
430.
330.
450.
390.
6400.
9999.
340.
390.
490.
autumn with
9999.
9999.
9999.
9999.
810.
1400.
6400.
9999.
6S00.
9999.
9999.
late autumn
9999.
9999.
9999.
9999.
2600.
6000.
9999.
9999.
9999.
9999.
9999.
winter with
9999.
9999.
QQGQ
wyy •
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
transitional
9999.
490.
790.
640.
810.
670.
6400.
9999.
640.
690.
940.
9999.
340.
490.
370.
620.
440.
6400.
9999.
370.
440.
670.
vegetation
9999.
710.
1200.
790.
1300.
1000.
6400.
9999.
780.
1000.
1400.
9999.
9999.
9999.
9999.
9999.
9999.
6400.
9999.
6900.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
6400.
9999.
6800.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
6400.
9999.
6800.
9999.
9999.
unharvested cropland
9999.
9999.
9999.
9999.
970.
1700.
6400.
9999.
6600.
9999.
9999.
9999.
9999.
9999.
9999.
2800.
6400.
6400.
9999*
6500.
AOOO
0*7*nr.
9999.
after frost, no
9999.
9999.
9999.
9999.
3200.
6200.
OQQQ
9999.
9999.
9999.
9999.
9999.
snow on
9999.
9999.
9999.
9999.
9999.
9999*
9999.
9999.
9999.
OQQQ
9999.
9999.
spring
9999.
660.
930.
630.
970.
780.
6400.
9999.
620.
810.
1100.
9999.
9999.
9999.
oooo
W99*
9999.
9999.
9999.
9999.
9999.
9999.
9999.
ground
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999*
9999.
9999.
9999.
9999.
6400.
9999.
6600.
9999.
9999.
snow
9999.
9999.
9999.
9999.
9999.
9999.
9999.
QQQQ
99.7V.
9999.
9999.
9999.
QQQQ
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
with partial green
9999.
1400.
2700.
1600.
2800.
2200.
6400.
9999.
1400.
2300.
3300.
9999.
9999.
9999.
9999.
QOQO
9999.
9999.
6400.
9999.
6800.
9999.
QQQQ
VWtf*
9999.
9999.
9999.
9999.
9999.
9999.
6400.
9999.
6600.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
oooo
WV9«
9999.
9999.
9999.
coverage
9999.
9999.
9999.
OGOO
Wtftf*
9999.
OOOQ
WVtV*
6400.
9999.
6700.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
6400.
9999.
6500.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
oooo
9999.
GOQQ
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
9999.
6400.
9999.
6700.
9999.
9999.
33
-------
Appendix I continued
Forma 1 dehy de
Seasonal category 1. midsummer with lush
1
2
3
4
6
6
7
8
9
10
11
Season* 1
1
2
3
4
6
6
7
8
9
10
11
Season* 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
0300.
80.
170.
100.
180.
140.
10.
9999.
80.
140.
210.
6300.
90.
180.
110.
200.
160.
10.
9999.
90.
160.
230.
6300.
110.
220.
130.
260.
180.
10.
9999.
100.
180.
280.
vegetati
6300.
360.
690.
460.
790.
660.
10.
9999.
200.
660.
870.
on
6300.
2300.
4600.
6600.
6600.
3000.
10.
9999.
310.
3100.
6700.
6300.
990.
1200.
1300.
1300.
1100.
10.
9999.
260.
1100.
1300.
6300.
990.
1200.
1300.
1300.
1100.
10.
9999.
260.
1100.
1300.
category 2. autumn with unharvestod cropland
6300.
3200.
6200.
8100.
430.
710.
10.
9999.
210.
4600.
6900.
category 3,
6400.
2400.
6300.
7800.
1400.
2000.
40.
9999.
140.
3100.
6900.
category 4,
2000.
1900.
1900.
2800.
1800.
2200.
300.
9999.
1900.
1900.
1100.
category 6.
7800.
200.
400.
250.
430.
320.
10.
9999.
120.
330.
600.
6300.
3200.
6200.
8100.
470.
760.
10.
9999.
210.
4600.
6900.
late autumn
6400.
2400.
6300.
7800.
1600.
2100.
40.
9999.
140.
3100.
6900.
winter with
2000.
1900.
1900.
2800.
1800.
2200.
300.
9999.
1900.
1900.
1100.
transitional
7800.
210.
440.
270.
460.
350.
10.
9999.
120.
360.
650.
6300.
3200.
6200.
8100.
670.
890.
10.
9999.
210.
4600.
6900.
6300.
3200.
6200.
8100.
1600.
1800.
10.
9999.
210.
4600.
6900.
after frost, no
6400.
2400.
6300.
7800.
1800.
2300.
40.
9999.
140.
3100.
6900.
snow on
2000.
1900.
1900.
2800.
1900.
2200.
300.
9999.
1900.
1900.
1100.
spring
7800.
260.
630.
330.
670.
420.
10.
9999.
140.
440.
670.
6400.
2400.
6300.
7800.
4000.
3600.
40.
9999.
140.
3100.
6900.
9POURQ
2000.
1900.
1900.
2800.
2000.
2300.
300.
9999.
1900.
1900.
1100.
6300.
3200.
6200.
8100.
7400.
3100.
10.
9999.
210.
4600.
6900.
snow
6400.
2400.
6300.
78P0.
7800.
4600.
40.
9999.
140.
3100.
6900.
2000.
1900.
1900.
2800.
2900.
2800.
300.
9999.
1900.
1900.
1100.
with partial green
7800.
720.
1400.
1000.
1600.
1100.
10.
9999.
180.
1100.
1800.
7800.
2300.
6000.
7600.
6600.
4100.
10.
9999.
210.
3700.
6100.
6300.
1100.
1200.
1300.
1300.
1000.
10.
9999.
190.
1200.
1300.
6400.
2400.
1200.
1300.
1300.
1200.
40.
9999.
130.
1100.
1300.
2000.
1900.
1900.
2800.
2900.
2800.
300.
9999.
1900.
1900.
1100.
coverage
7800.
990.
1200.
1300.
1300.
1200.
10.
9999.
190.
1100.
1300.
6300.
1100.
1200.
1300.
1300.
1000.
10.
9999.
190.
1200.
1300.
6400.
2400.
1200.
1300.
1300.
1200.
40.
9999.
130.
1100.
1300.
2000.
1900.
1900.
2800.
2900.
2800.
300.
9999.
1900.
1900.
1100.
7800.
990.
1200.
1300.
1300.
1200.
10.
9999.
190.
1100.
1300.
34
-------
Appendix I continued
Methyl hydroparoxide
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
5
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
^
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
category 1.
midsummer with lush
2900.
100.
190.
120.
210.
170.
400.
3800
B
110.
160.
230.
category 2.
2900
1100
1300
1800
460
780
400
3800
610
1200
1300
category 3.
2900
1200
1300
1700
1200
1600
970
3800
900
1300
1600
category 4.
6300
6600
6600
3600
6600
4400
6200
4000
6300
6100
4900
category 5.
2900
220
390
270
460
360
400
3800
210
340
f
f
•
.
.
f
.
.
a
•
B
B
.
f
.
m
B
.
w
•
t
f
f
f
•
B
m
m
f
•
f
f
m
m
f
f
f
f
.
480.
2900.
100.
200.
130.
230.
180.
400.
3800.
120.
170.
260.
autumn with
2900.
1100.
1300.
1800.
600.
830.
400.
3800.
610.
1200.
1300.
late autumn
2900.
1200.
1300.
1700.
1200.
1600.
970.
3800.
900.
1300.
1600.
winter with
6300.
6600.
6600.
3600.
6600.
4400.
6200.
4000.
6400.
6100.
6000.
transitional
2900.
240.
410.
290.
600.
390.
400.
3800.
220.
360.
610.
2900.
130.
240.
160.
280.
220.
400.
3800.
160.
210.
300.
vegetation
2900.
370.
620.
480.
770.
660.
400.
3800.
330.
640.
730.
2900.
1400.
1700.
2800.
2800.
3200.
400.
3800.
660.
1600.
1800.
2900.
1300.
1600.
2600.
2500.
2800.
400.
3800.
640.
1600.
1700.
2900.
1200.
1400.
2100.
2100.
2400.
400.
3800.
610.
1300.
1600.
unharvested cropland
2900.
1100.
1300.
1800.
690.
960.
400.
3800.
620.
1200.
1300.
2900
1200
1400
1900
1300
1700
400
3800
620
1300
1400
u
f
f
m
f
f
.
2900
1400
1700
2600
3000
3300
400
3800
f
f
.
s
.
B
,
660.
f
•
after frost, no
2900.
1200.
1300.
1700.
1400.
1700.
970.
3800.
900.
1300.
1600.
snow on
6300.
6600.
6600.
3600.
6800.
4600.
6200.
4000.
6400.
6200.
6000.
spring
2900.
280.
480.
360.
600.
470.
400.
3800.
260.
430.
690.
2900
1300
1400
1800
2100
2300
970
3800
910
1400
1600
ground
6300
6800
6800
4000
7300
4900
6200
4000
6700
6400
6200
^
f
B
f
f
9
f
B
B
•
•
B
f
f
f
m
f
f
f
•
1600
1700
snow
2900
1300
1700
2300
3000
3300
970
3800
960
1600
1800
6300
9600
9600
8000
9600
8400
6200
4000
8200
8600
7300
m
•
f
f
9
f
f
B
f
w
^
•
B
B
a
B
f
B
f
f
f
•
with partial green
2900
640
930
840
1300
1100
400
3800
410
860
1000
,
.
t
.
B
.
t
.
B
.
2900
1300
1700
2400
2900
3100
400
3800
670
1600
1800
m
_
.
_
.
,
.
.
B
.
2900.
1300.
1600.
2300.
2600.
2800.
400.
3800.
660.
1400.
1600.
2900.
1300.
1600.
2100.
2600.
2800.
970.
3800.
910.
1400.
1600.
6300.
9600.
9600.
8000.
9600.
8400.
6200.
4000.
8200.
8600.
7300.
coverage
2900.
1200.
1600.
2100.
2600.
2700.
400.
3800.
660.
1400.
1600.
2900.
1200.
1400.
2000
2200
2300
400
3800
630
1300
1400
2900
1300
1400
1800
2200
2300
970
3800
860
1300
1400
6300
9600
9600
8000
9600
8400
6200
4000
8200
8600
7300
2900
1100
1400
1900
2200
2300
400
3800
630
1300
1600
.
B
.
.
m
f
f
•
f
f
a
.
^
m
f
f
.
•
,
.
^
m
f
f
.
.
B
•
m
m
f
_
.
f
f
_
m
.
35
-------
Appendix I continued
Peroxy acetic acid
Seasonal
1
2
3
4
6
6
7
8
9
10
11
Seasonal
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
category 1. midsummer with lush
2900.
120.
230.
140.
260.
200.
180.
3800.
120.
190.
280.
category 2,
2900.
1100.
1300.
1800.
650.
890.
180.
3800.
340.
1200.
1300.
category 3.
2900.
1200.
1300.
1700.
1300.
1700.
440.
3800.
600.
1300.
1600.
category 4.
4700.
6600.
6600.
3300.
6400.
3900.
2800.
3900.
4700.
6300.
4100.
category 6.
2900.
260.
460.
320.
660.
440.
180.
3800.
190.
400.
650.
2900.
130.
240.
160.
280.
220.
180.
3800.
130.
210.
300.
autumn with
2900.
1100.
1300.
1800.
690.
940.
180.
3800.
340.
1200.
1300.
late autumn
2900.
1200.
1300.
1700.
1400.
1700.
440.
3800.
600.
1300.
1600.
winter with
4700.
6600.
6600.
3300.
6500.
4000.
2800.
3900.
4700.
6300.
4100.
2900.
160.
290.
190.
340.
270.
180.
3800.
160.
260.
360.
vegetation
2900.
430.
700.
670.
890.
760.
180.
3800.
290.
610.
820.
2900.
1300.
1600.
2800.
2800.
3100.
180.
3800.
460.
1600.
1800.
2900.
1200.
1500.
2300.
2300.
2500.
180.
3800.
440.
1400.
1600.
2900.
1100.
1300.
2000.
2000.
2100.
180.
3800.
430.
1200.
1400.
unharvested cropland
2900.
1100.
1300.
1800.
700.
1000.
180.
3800.
340.
1200.
1300.
2900.
1100.
1400.
1900.
1400.
1800.
180.
3800.
360.
1300.
1400.
after frost, no
2900.
1200.
1300.
1700.
1600.
1800.
440.
3800.
600.
1300.
1600.
snow on
4700.
6700.
6700.
3400.
6600.
4000.
2800.
3900.
4800.
6400.
4100.
transitional spring
2900.
280.
480.
350.
600.
470.
180.
3800.
200.
430.
690.
2900.
330.
650.
420.
700.
660.
180.
3800.
220.
490.
670.
2900.
1200.
1400.
1800.
2200.
2300.
440.
3800.
600.
1300.
1600.
ground
4700.
6900.
5900.
3700.
6900.
4300.
2800.
3900.
6000.
6500.
4200.
2900.
1300.
1700.
2600.
3000.
3200.
180.
3800.
360.
1600.
1700.
snow
2900.
1300.
1700.
2300.
3000.
3200.
440.
3800.
610.
1600.
1700.
4700.
7700.
7700.
6800.
7700.
7000.
2800.
3900.
6800.
7100.
6600.
with partial areei
2900.
700.
990.
960.
1400.
1200.
180.
3800.
300.
930.
1100.
2900.
1300.
1700.
2400.
2800.
3000.
180.
3800.
360.
1600.
1800.
2900.
1200.
1500.
2100.
2400.
2600.
180.
3800.
360.
1400.
1600.
2900.
1300.
1600.
1900.
2400.
2500.
440.
3800.
490.
1300.
1600.
4700.
7700.
7700.
6800.
7700.
7000.
2800.
3900.
6800.
7100.
6600.
i coverage
2900.
1200.
1500.
2000.
2400.
2400.
180.
3800.
360.
1300.
1600.
2900.
1100.
1300.
1800.
2100.
2100.
180.
3800.
340.
1200.
1300.
2900.
1300.
1300.
1700.
2100.
2100.
440.
3800.
480.
1200.
1400.
4700.
7700.
7700.
6800.
7700.
7000.
2800.
3900.
6800.
7100.
6600.
2900.
1100.
1300.
1800.
2000.
2100.
180.
3800.
360.
1200.
1400.
36
-------
Append i x I cont i nued
Formic »cid
Season* 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
Season* 1
1
2
3
4
6
6
7
8
9
10
11
Season* 1
1
2
3
4
5
6
7
8
9
10
11
Season* 1
1
2
3
4
6
6
7
8
9
10
11
category 1, midsummer with lush
100.
20.
20.
30.
30.
30.
0.
20.
30.
20.
40.
category 2.
100.
70.
60.
130.
60.
100.
0.
20.
80.
60.
70.
category 3.
100.
10.
60.
130.
70.
110.
0.
20.
60.
40.
70.
category 4,
90.
10.
10.
270.
80.
100.
0.
20.
30.
10.
30.
category 5,
100.
20.
30.
60.
30.
60.
0.
20.
40.
30.
60.
100.
20.
20.
30.
30.
30.
0.
20.
30.
20.
40.
autumn with
100.
70.
60.
140.
60.
110.
0.
20.
80.
70.
70.
late autumn
100.
10.
60.
130.
70.
120.
0.
20.
60.
40.
70.
winter with
90.
10.
10.
300.
90.
110.
0.
20.
40.
10.
30.
transitional
100.
20.
30.
60.
40.
60.
0.
20.
60.
30.
60.
100.
30.
20.
30.
30.
30.
0.
20.
30.
30.
60.
vegetation
100.
30.
30.
40.
40.
40.
0.
20.
40.
30.
60.
100.
40.
30.
40.
40.
40.
0.
20.
60.
30.
60.
100.
0.
0.
0.
0.
0.
0.
20.
0.
0.
0.
100.
0.
0.
0.
0.
0.
0.
20.
0.
0.
0.
unharvested cropland
100.
80.
60.
160.
70.
120.
0.
20.
• 90.
70.
70.
100.
80.
60.
160.
80.
160.
0.
20.
90.
70.
80.
100.
90.
70.
190.
90.
170.
0.
20.
100.
80.
80.
100.
0.
0.
0.
0.
0.
0.
20.
0.
0.
0.
100.
0.
0.
0.
0.
0.
0.
20.
0.
0.
0.
after frost, no snow
100.
10.
60.
140.
70.
130.
0.
20.
60.
40.
70.
snow on
90.
10.
10.
330.
100.
130.
0.
20.
40,
10.
30.
spring
100.
30.
40.
60.
40.
60.
0.
20.
60.
30.
60.
100.
10.
60.
160.
80.
160.
0.
20.
60.
40.
70.
ground
90.
10.
10.
460.
120.
160.
0.
20.
40,
10.
40.
with partial
100.
30.
40.
80.
40.
60.
0.
20.
60.
30.
70.
100.
10.
70.
180.
90.
170.
0.
20.
60.
40.
80.
90.
10.
10.
660.
130.
190.
0.
20.
40,
10.
40.
green
100.
30.
40.
90.
40.
70.
0.
20.
60.
40.
70.
100.
10.
0.
0.
0.
0.
0.
20.
0.
0.
0.
90.
10.
10.
660.
130.
190.
0.
20.
40,
10.
40.
coverage
100.
0.
0.
0.
0.
0.
0.
20.
0.
0.
0.
100.
10.
0.
0.
0.
0.
0.
20.
0.
0.
0.
90.
10.
10.
660.
130.
190.
0.
20.
40.
10.
40.
100.
0.
0.
0.
0.
0.
0.
20.
0.
0.
0.
37
-------
Appendix I continued
Ammonia
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
Seasonal
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
category 1.
2000.
60.
120.
70.
130.
100.
0.
4600.
60.
90.
150.
category 2.
2000.
1000.
1600.
3200.
300.
600.
0.
4600.
200.
1400.
1900.
category 3.
2000.
760.
1600.
2900.
930.
1200.
10.
4600.
110.
1000.
1900.
category 4,
680.
690.
690.
1500.
830.
1000.
90.
4700.
620.
580.
380.
category 5.
2600.
130.
270.
180.
300.
220.
0.
4600.
100.
220.
330.
midsummer with lush
2000.
60.
130.
80.
140.
110.
0.
4600.
70.
100.
160.
autumn with
2000.
1000.
1600.
3200.
330.
630.
0.
4600.
200.
1400.
1900.
late autumn
2000.
760.
1600.
2900.
980.
1200.
10.
4600.
110.
1000.
1900.
winter with
680.
690.
590.
1600.
860.
1000.
90.
4700.
620.
680.
380.
transitional
2600.
140.
290.
190.
320.
240.
0.
4600.
100.
230.
360.
2000.
80.
160.
100.
180.
130.
0.
4600.
80.
130.
200.
vegetation
2000.
220.
420.
310.
620.
390.
0.
4600.
170.
340.
640.
2000.
830.
1400.
2600.
2600.
1800.
0.
4600.
290.
1000.
1800.
2000.
310.
380.
430.
430.
400.
0.
4600.
180.
340.
390.
2000.
310.
380.
430.
430.
400.
0.
4600.
180.
340.
390.
unharvested cropland
2000.
1000.
1600.
3200.
390.
620.
0.
4600.
200.
1400.
1900.
2000.
1000.
1600.
3200.
1000.
1100.
0.
4600.
200.
1400.
1900.
after frost, no
2000.
760.
1600.
2900.
1100.
1300.
10.
4600.
110.
1000.
1900.
snow on
680.
690.
690.
1600.
910.
1100.
90.
4700.
•620.
680.
380.
sprina
2600.
170.
340.
230.
390.
290.
0.
4600.
120.
280.
430.
2000.
760.
1600.
2900.
2000.
1800.
10.
4600.
110.
1000.
1900.
ground
680.
690.
690.
1500.
1100.
1200.
90.
4700.
620.
680.
380.
2000.
1000.
1600.
3300.
3100.
1900.
0.
4600.
200.
1400.
1900.
snow
2000.
760.
1700.
2900.
3200.
2200.
10.
4600.
110.
1000.
1900.
680.
690.
590.
1500.
1900.
1700.
90.
4700.
620.
580.
380.
2000.
340.
380.
430.
430.
400.
0.
4600.
140.
370.
390.
2000.
760.
380.
430.
430.
410.
10.
4600.
90.
330.
390.
680.
590.
690.
1500.
1900.
1700.
90.
4700.
620.
580.
380.
2000.
340.
380.
430.
430.
400.
0.
4600.
140.
370.
390.
2000.
760.
380.
430.
430.
410.
10.
4600.
90.
330.
390.
680.
590.
690.
1500.
1900.
1700.
90.
4700.
620.
680.
380.
with_partial green coverage
2500.
370.
770.
670.
960.
740.
0.
4600.
160.
610.
960.
2600.
760.
1600.
2800.
2600.
1900.
0.
4600.
200.
1100.
1900.
2600.
300.
380.
430.
430.
400.
0.
4600.
140.
350.
400.
2500.
300.
380.
430.
430.
400.
0.
4600.
140.
350.
400.
38
-------
Appendix I continued
Peroxyacetyl nitrate
Seasonal category 1, midsummer with lush
1
2
3
4
E
6
7
8
9
10
11
Seasonal
1
2
3
4
S
6
7
8
9
10
11
Seasona 1
1
2
3
4
6
6
7
8
9
10
11
S«asona 1
1
2
3
4
6
6
7
8
9
10
11
Seasona 1
1
2
3
4
E
6
7
8
9
10
11
3000.
150.
290.
190.
330.
260.
9999.
3900.
220.
240.
3S0.
category 2.
3000.
1100.
1300.
1800.
680.
1000.
9999.
3900.
2400.
1200.
1300.
category 3,
3000.
1300.
1300.
1700.
1500.
1800.
9999.
3900.
4000.
1400.
1500.
category 4.
6000.
7700.
7700.
3800.
8400.
6000.
9999.
4000.
6100.
7100.
6100.
category E.
3000.
330.
540.
400.
680.
540.
9999.
3900.
490.
490.
660.
3000.
160.
310.
200.
350.
280.
9999.
3900.
240.
260.
370.
autumn with
3000.
1100.
1300.
1800.
730.
1100.
9999.
3900.
2400.
1300.
1300.
late autumn
3000.
1300.
1300.
1700.
1600.
1900.
9999.
3900.
4000.
1400.
1E00.
winter with
6000.
7700.
7700.
3900.
8500.
5000.
9999.
4000.
6100.
7100.
6100.
transitional
3000.
350.
570.
430.
730.
580.
9999.
3900.
630.
610.
690.
3000.
200.
370.
2E0.
430.
3E0.
9999.
3900.
290.
310.
440.
vegetati
3000.
610.
820.
700.
1000.
940.
9999.
3900.
850.
720.
950.
on
3000.
1400.
1700.
2800.
2800.
3300.
9999.
3900.
4600.
1600.
1800.
3000.
1400.
1600.
2700.
2700.
3100.
9999.
3900.
4100.
1600.
1800.
3000.
1200.
1500.
2300.
2300.
2600.
9999.
3900.
3200.
1400.
1600.
unharvested cropland
3000.
1100.
1300.
1800.
850.
1200.
9999.
3900.
2500.
1300.
1400.
3000.
1200.
1400.
1900.
1600.
2000.
9999.
3900.
2600.
1300.
1400.
after frost, no
3000.
1300.
1400.
1700.
1700.
2000.
9999.
3900.
4000.
1400.
1500.
•now on
6000.
7800.
7800.
4000.
8700.
6100.
9999.
4000.
6200.
7200.
6200.
spring
3000.
410.
650.
610.
850.
690.
9999.
3900.
640.
690.
780.
3000.
1300.
1400.
1800.
2300.
2400.
9999.
3900.
4100.
1400.
1600.
ground
6000.
8100.
8100.
4400.
9200.
6500.
9999.
4000.
6500.
7600.
6600.
3000.
1400.
1700.
2600.
3000.
3400.
9999.
3900.
4100.
1600.
1800.
•now
3000.
1400.
1700.
2400.
3000.
3300.
9999.
3900.
5400.
1600.
1800.
ttOUJUJt
wwKnOa
9999.
9999.
9700.
9999.
9900.
9999.
4000.
9999.
9999.
9999.
with partial greet
3000.
800.
1000.
1000.
1600.
1400.
9999.
3900.
1500.
1000.
1200.
3000.
1300.
1700.
2400.
2900.
3100.
9999.
3900.
4500.
1600.
1800.
3000.
1300.
1600.
2400.
2800.
3100.
9999.
3900.
3600.
1S00.
1700.
3000.
1400.
1700.
2200.
2800.
3000.
9999.
3900.
4600.
1500.
1700.
6000.
9999.
9999.
9700.
9999*
9900.
9999.
4000.
9999.
9999.
9999.
i coverage
3000.
1300.
1600.
2300.
2800.
2900.
9999.
3900.
4000.
1600.
1700.
3000.
1200.
1600.
2100.
2300.
2600.
9999.
3900.
2900.
1400.
1600.
3000.
1400.
1600.
1900.
2400.
2500.
9999.
3900.
3500.
1400.
1500.
6000.
9999.
9999.
9700.
9999.
9900.
9999.
4000.
9999.
9999.
9999.
i
3000.
1200.
1500.
2000.
2300.
2400.
9999.
3900.
3200.
1400.
1600.
39
-------
Appendix I continued
Nitrous acid
Seasons 1
1
2
3
4
6
6
7
8
9
10
11
Seasons 1
1
2
3
4
5
6
7
8
9
10
11
Seasons 1
1
2
3
4
5
6
7
8
9
10
11
Seasons 1
1
2
3
4
6
6
7
8
9
10
11
Seasons 1
1
2
3
4
6
6
7
8
9
10
11
category 1, midsummer with lush
490.
70.
120.
100.
170.
140.
0.
970.
90.
100.
170.
category 2,
490.
320.
400.
1300.
340.
650.
0.
970.
190.
. 380.
480.
category 3 ,
490.
160.
410.
1100.
710.
910.
0.
970.
100.
230.
460.
category 4,
210.
120.
120.
980.
340.
430.
10.
990.
160.
120.
110.
category 6.
590.
100.
210.
230.
320.
280.
0.
970.
120.
160.
270.
490.
80.
130.
110.
190.
150.
0.
970.
90.
110.
180.
autumn with
490.
320.
400.
1300.
370.
580.
0.
970.
190.
380.
480.
late autumn
490.
160.
410.
1100.
730.
920.
0.
970.
100.
230.
460.
winter with
210.
120.
120.
980.
380.
460.
10.
990.
160.
120.
110.
transitional
690.
110.
220.
250.
330.
290.
0.
970.
120.
170.
280.
490.
90.
160.
140.
220.
180.
0.
970.
100.
130.
200.
vegetati
490.
170.
240.
340.
460.
400.
0.
970.
180.
210.
340.
on
490.
290.
350.
1000.
1000.
940.
0.
970.
260.
300.
500.
490.
70.
80.
90.
90.
90.
0.
970.
70.
70.
80.
490.
70.
80.
90.
90.
90.
0.
970.
70.
70.
80.
unharvested cropland
490.
320.
400.
1300.
420.
640.
0.
970.
190.
380.
480.
490.
320.
410.
1300.
730.
930.
0.
970.
190.
380.
480.
after frost, no
490.
160.
410.
1100.
780.
960.
0.
970.
100.
230.
460.
snow on
210.
120.
120.
980.
450.
.520.
10.
990.
160.
120.
110.
spring
690.
120.
240.
290.
380.
340.
0.
970.
130.
180.
300.
490.
160.
410.
1100.
1000.
1100.
0.
970.
100.
230.
460.
ground
210.
120.
120.
990.
680.
690.
10.
990.
160.
120.
110.
490.
330.
410.
1400.
1300.
1300.
0.
970.
190.
390.
490.
snow
490.
160.
420.
1100.
1300.
1200.
0.
970.
100.
240.
480.
210.
120.
120.
1000.
1300.
1200.
10.
990.
160.
120.
110.
with partial areei
690.
160.
310.
680.
620.
600.
0.
970.
160.
240.
400.
690.
180.
370.
1100.
1000.
1000.
0.
970.
180.
280.
470.
490.
70.
80.
90.
90.
90.
0.
970.
60.
80.
80.
490.
160.
80.
90.
90.
90.
0.
970.
60.
70.
80.
210.
120.
120.
1000.
1300.
1200.
10.
990.
160.
120.
110.
i coverage
590.
60.
80.
90.
90.
90.
0.
970.
60.
70.
80.
490.
70.
80.
90.
90.
90.
0.
970.
60.
80.
80.
490.
160.
80.
90.
90.
90.
0.
970.
50.
70.
80.
210.
120.
120.
1000.
1300.
1200.
10.
990.
160.
120.
110.
590.
60.
80.
90.
90.
90.
0.
970.
60.
70.
80.
40
-------
Appendix II. Code for the Argonne dry deposition module.
C . MODULE.FOR
C*** Argonne National Laboratory version of a dry deposition
C module that can be adapted for use in RAOM.
C*«* This module is an uptdated version, as of 3/1/88,
C and contains elements of the version completed on 6/11/86.
C*«* This revision was made by M. L. Wesely and 8. M. Lesht,
C and is now designed to computed dry deposition velocities
C of a greater number of substance's, and with a more explicit
C derivation of surface resistances.
C*** The main program and the subroutine METERO show below are
C used only as an example for the use of the deposition
C velocity subroutine DEPVEL.
C
C*** The following main program substitutes inputs from an
C atmospheric transport model (e.g., RADM).
C
IMPLICIT INTEGER*2 (I-N)
LOGICAL*! COM(70),DUMMY(70)
COMMON/METVAR/ HV(328,186),UUSTAR(328,186),
1 RADIAT(328,186),TCZ(328,186),TC0(328,186),
2 ZINV(328,186),USTAR(328,186),VD(15,328,186)
C
C*** Open file for values of maximum S04 deposition velocities.
C (VDSMAX), surface roughness lengths (IZO), and surface
C components (RI, RLU, RAC, RGSS, RGSO, RCLS, RCLO).
OPEN(UNIT=5,FILE='MOOINP.DAT',RECORDTYPE='VARIABLE',
1STATUS='OLD',FORM=»FORMATTED')
C
C*** Open direct access file for landuse map.
OPEN(UNIT=10,FILE='3DISK1:[LESHT.LANDUSE]DNEM085.DAT*,
1ACCESS='DIRECT',READONLY,RECL=14,STATUS='OLD')
C
C*** Open file for optional, averaged output for test runs.
OPEN(UNIT=8,FILE='MODAV.DAT',RECORDTYPE='VARIABLE',
1 STATUS='NEW, FORM='FORMATTED')
C
C*** Define season and height of required deposition velocity.
INIT=1
CZ=10.
DO 10 ISESN=1,5
C
C*** Call METERO to obtain meteorological parameters for
C computation of deposition velocity.
CALL METERO(ISESN,IDEW,IRAIN)
CALL DEPVEL(INIT,CZ,ISESN,IDEW,IRAIN)
10 CONTINUE
C
C*** INIT=1 defined intially in data assignment to permit
C initialization of parameters only once and then set
C INIT=0 to bypass initialization in subroutine DEPVEL.
C
INIT=0
STOP
END
41
-------
SUBROUTINE METERO(ISESN,IDEW,IRA1N)
C*** Meteorological module
IMPLICIT INTEGERS (I-N)
DIMENSION SOLAR(5),TEMP(5)
COMMON/METVAR/ HV(328,186), UUSTAR(328,186),
1 RADIAT(328,186),TCZ(328,186),TC0(328,188) ,
2 ZINV(328,186),USTAR(328,186),VD(16,328,186)
C**» TEMP is the surface temperature (C) assumed for preliminary
C output, here specific to season.
DATA TEMP/25.,10.,2.,0.,10./
C*** SOLAR is the insolation (W/m»»2) assumed for preliminary
C output; here we can choose any level.
DATA SOLAR/800.,500.,300.,100.,0./
11=2
C«*» Set IDEW = 1 for dewfalt, IRAIN = l for rain-wetted surface.
IOEW=0
IRAIN=0
C*** Initialize variables for all locations.
LONOB=328
LATOB=186
CU=3.9
DO 10 I=1,LONOB
DO 10 J=1,LATOB
C*** These dummy values are only to provide a test case.
HV(I,J)=150.
USTAR(I,J)=0.30
UUSTAR(I,J)=CU»USTAR(I,J)
RADIAT (I, J) =SOLAR (II)
TCZ (I, J) =TEMP (ISESN)
TC0 (I, J) =TEMP (ISESN)
ZINV(I,J)=1000.
10 CONTINUE
RETURN
END
42
-------
SUBROUTINE DEPVEL(INIT,CZ,ISESN,IDEW,IRAIN)
C*** This subroutine was constructed by M. L. Wesely and
C B. M. Lesht, with earlier imput by C. M. Sheih, at
C Argonne National laboratory.
C*** This subroutine is for computing the dry deposition
C velocities for for (1) S02, (2) 03, (3) N02, (4) NO,
C (B) HN03, (6) H202, (7) ALD actually acetaIdehyde,
C (8) HCHO, (9) OP actually methyl hydroperoxide, (10) PAA,
C (11) ORA actually formic acid, (12) NH3, (13) PAN, (14) HN02,
C and (15) S04.
C*** No estimates are made of surface emissions.
C
C*«* Input parameter* are ISESN, , and ZINV as defined below:
C INIT= 1 (yes) or 0 (no) for initialization of parameters;
C ISESN =1, midsummer with lush vegetation
C 2, autumn with unharvested cropland
C 3, late autumn after frost, no snow
C 4, winter with snow on ground
C 5, transitional spring with partial green coverage;
C HV = virtual heat flux (W/m*«2);
C USTAR = friction velocity (m/s);
C RAOIAT = solar irradiation (W/m**2);
C CZ = height (m) where deposition velocities are needed;
C TCZ = temperature at height CZ;
C TC0 = surface temperature;
C ZINV = inversion height (m).
C*** Some other code names are as follows:
C VDSMAX = maximum permissable surface S04 deposition
C velocity for various landuse types and seasons;
C HSTAR = Henry's Law constant for substances 1 through 14,
C for water pH near 7;
C FO = measure of reactivity for substances 1 through 14,
C relative to 03;
C DIFRAT = ratio of molecular diffusivity for water vapor
C in air to diffusivity for substances 1 through 14;
C VO = deposition velocities (m/s);
C R = bulk surface (non-gaseous) resistances.
C
C*** Resistances and deposition velocities are computed for
C specific landuse types in the landuse map, which was
C derived from surface landuse and land cover inventory
C by S. H. Page of Lockheed Engineering and Management
C Services Inc., Remote Sensing Laboratory, Las Vegas,
C Nevada 89114.
C*** There are eleven landuse types as follows:
C 1, urban land, almost no vegetation;
C 2, agricultural land, usually well watered;
C 3, range land, usually with low soil moisture;
C 4, deciduous forest;
C E, coniferous forest;
C 6, mixed forest including wetland;
C 7, water, sea water assumed but used for fresh water also;
C 8, barren land, mostly desert;
C 9, non-forested wetland;
C 10, mixed agricultrual and range land;
C 11, rocky open areas occupied by low growing schrubs.
C*** The landuse data set is arranged in latitude degree,
C number of 1/12 (at. deg. (which is at the grid center,
C with grid increments of 1/6 deg), longitude degree,
C number of 1/8 long. deg. (with increments of 1/4 deg.),
C and the 11 values of percentage cover of each landuse
C type.
C*** The grid domain is from 52+1/8 to 133+7/8 deg. west longitude
C and from 24+1/12 to 54+11/12 deg. north latitude, for which
C there are NX=328 points and NY=186 points. Grid points start
C from the SE corner and runs from E to W and from S to N.
C
C
43
-------
C*«* Set variables for direct access file for landuse map.
IMPLICIT INTEGER.2 (I-N)
INTEGERS NREC, IROW, ICOL
C
LOGICAL*1 COM(70),DUMMY(70)
DIMENSION IUSE(11),HSTAR(14),FO(14),DIFRAT(14),
1 120(11) ,20(11) ,CXO(328) ,CYO(186) ,VDSMAX(11) ,
2 XRI(ll) ,XRLU(11) ,XRAC(11) ,XRGSS(11) ,XRGSO(11) ,XRCLS(11) ,
3 XRCLO(ll) ,RI(11) ,RLU(11) ,RAC(11) ,RGSS(11) ,RGSO(11) ,RCLS(11) ,
4 RCLO(ll) ,R(15,11) ,DC(14) ,C1X(14) ,ITUSE(11) ,IPUSE(11) ,VX(15)
COMMON/METVAR/ HV(328,186),UUSTAR(328,188) ,
1 RADIAT(328,186),TC2(328,188),TC0(328,186) ,
2 2INV(328,186),USTAR(328,186),VD(15,328,186)
C
C*** Set values for substance chemical and physical properties.
DATA HSTAR/1.0E+5,0.01, .01,.003,1.0E+14,1.0E+06,16.,6000.,240.
1,640.,4.0E+06,20000.,3.6,1.0E»05/
DATA FO/0.,1.,.1,0.,0.,1.,0.,0.,.1,.1,0.,0.,.1,0./
DATA DIFRAT/1.9,1.8,1.6,1.3,1.9,1.4,1.6,1.3,1.6,2.0,1.6,.97,
1 2.6,1.6/
C
C THETA is the terrain slope, assumed to be zero radians for RADM
THETA=0.
C
C
C*** READ IN MODINP.DAT
IF(INIT.NE.l) GOTO 25
PRINT *,' Reading in inputs for S04 max dep. vel., 2o,
1 and resistance components'
LONST=1
LATST=1
LONOB=328
LATOB=186
C*«» Use the following four values to only consider 6X6 deg.
C square centered at 92.5 deg. long, and 42.5 deg. I at.
C LONST=153
C LONOB=173
C LATST=97
C LATOB=127
C*** Set up coordinates (if needed) for the grid network.
C Cl=52.-l./8.
C DO 10 I=1,LONOB
C 10 CXO(I)=Cl+I/4.
C Cl=24.-l./12.
C DO 12 J=1,LATOB
C 12 CYO(J)=Cl+J/6.
C**» Read in maximum permissible S04 deposition velocities.
C*** I is landuse type.
C*** Read a dummy line first.
READ(5,1000) DUMMY
READ(5,1000) DUMMY
1000 FORMAT(70A1)
DO 16 L=1,S
IF(L.NE.ISESN) GOTO 14
READ(5,1100) COM, (VDSMAX(I) ,1=1,11)
1100 FORMAT(70A1/(11F6.3))
GOTO 16
14 READ(5,1100) COM, (Cl, 1=1,11)
16 CONTINUE
C*** Read a dummy line.
READ(5,1000) DUMMY
C*** Read 120 (surface roughness) of proper season.
DO 22 L=l,5
IF(L.NE.ISESN) GOTO 20
READ(5,1200) COM,(120(I),1=1,11)
1200 FORMAT(70A1/11I6)
GOTO 22
20 READ(5,1200) COM,(IC1,I=1,11)
22 CONTINUE
C*** Read a dummy line.
READ(5,1000) DUMMY
44
-------
C*** Read in inital values of surface resistance components.
L=0
23 L=L+1
READ(5,1000) COM
READ(5,1400) (XRI(I),1=1,11)
REAO(5,1400) (XRLU(I),I=1,11)
READ(5,1400) (XRAC(I),I=1,11)
READ(6,1400) (XRGSS(I),I=1,11)
READ(6,1400) (XRGSO(I),I=1,11)
READ(6,1400) (XRCLS(I),I=1,11)
READ(6,1400) (XRCLO(I),I=1,11)
1400 FORMAT(6X,11F6.0)
IF(L.NE.ISESN) GOTO 23
REWIND 6
C*** Convert to appropriate units.
DO 24 1=1,11
ZO(I)=IZO(I)«l.E-4
24 CONTINUE
26 CONTINUE
C
C*** This is the end of parameter initialization and
C the beginning of computing deposition velocities.
C
C
C*** BEGIN ITERATING THROUGH GEOGRAPHICAL DOMAIN.
C*** Flag for subroutine AVERAGE.
IFLAG=1
C*** Step through all grid points.
PRINT *,' Beginning iterations for seasonal
1 category number ',ISESN
DO 70 J=LATST,LATOB
DO 70 I=LONST,LONOB
C*** Initialize variables.
Cl=(273.VTC0(I,J))/273.
C2=Cl»«1.75*1.0E-04
DO 31 K=l,16
VD(K,I,J)=0.
31 DC(K)=0.219*C2/DIFRAT(K)
XNU=0.1Sl«Cl**1.77*1.0E-04
C
C*** Compute bulk surface resistances for gases.
C*** Adjust external surface resistances for temperature.
RT=1000.*EXP(-TC0(I,J)-4.)
DO 40 N=l,ll
RI(N)=XRI(N)
RLU(N)=XRLU(N)+RT
RAC (N) =XRAC (N)
RGSS(N)=XRGSS(N)+RT
RGSO(N)=XRGSO(N)+RT
RCLS(N)=XRCUS(N)+RT
40 RCLO(N)=XRCLO(N)+RT
DO 44 N=l,ll
C**« Set initial max. and rain, values for resistance components.
IF(RI(N).GE.9999.) RI(N)=100000.
IF(RLU(N).GE.9999.) RLU(N)=100000.
IF(RAC(N).GE.9999.) RAC(N)=100000.
IF(RGSS(N).GE.9999.) RGSS(N)=100000.
IF(RGSO(N).GE.9999.) RGSO(N)=100000.
IF(RCLS(N).GE.9999.) RCLS(N)=100000.
IF(RCLO(N).GE.9999.) RCLO(N)=100000.
IF(RAC(N).LT.1.) RAC(N)=1.
IF(RGSS(N).LT.l.) RGSS(N)=1.
GFACTOR=100.
RIX=RI(N)
C*** Adjust stomatal resistances for insolation and temp.
IF(RI(N).GE.9999.) GOTO 42
IF(TC0(I,J).LE.0..0R.TC0(I,J).GE.40.) GOTO 41
GFACTOR=400./TC0(I,J)/(40.-TC0(I,J))
41 RIX=RI(N)»(1.+(200./(RADIAT(I,J)+0.1))*«2.)*GFACTOR
C*»* Adjust stomatal resistances for liquid water coverage.
IF(IDEW.EQ.l.OR.IRAIN.EQ.l) RIX=3.»RIX
45
-------
C*«* Compute aerodynamic resistance to lower elements in lower
C part of canopy or structure.
42 RDC=100.*(1.+1000./(RAOIAT(I,J)+10.))/(1.+1000.»THETA)
C*** Compute resistances for S02.
X=1./(3.*RLU(N))
RLUX=RLU(N)
IF(TC0(I,J).GT.0.5) THEN
C Adjust for effects of dew and rain.
IF(RLUX.LT.9999..AND.IDEW.EQ.l) RLUX=100.
IF(RLUX.LT.9999..AND.IRAIN.EQ.1) RLUX=1./(1./B000.+X)
IF(N.Eq.l.AND.(IDEW+IRAIN).GE.l) RLUX=50.
END IF
R (1 ,N) =1. / (1. / (DIFRAT (1) «RIX) +1./RLUX+1./(RAC (N) +RGSS (N) )
1 +1./(RDC+RCLS(N)))
C*** Compute resistance for 03.
RLUX=RLU(N)
IF(TC0(I,J).GT.0.S) THEN
C Adjust for effects of dew and rain.
IF(RLUX.LT.9999..AND.IDEW.EQ.l) RLUX=1./(1./3000.-OC)
IF(RLUX.LT.9999..AND.IRAIN.EQ.1) RLUX=1./(1./1000.+X)
END IF
R (2,N) =1. / (1. / (DIFRAT (2) *RIX) +1. /RLUX+1. / (RAC (N) +RGSO (N) )
1 +1./(RDC+RCLO(N)))
C**« Compute resistances for (3) N02,(4) NO, (5) HN03, AND (4-12)
C other substances for which solubility, aqueous redox, and
C diffusivity ratio relative to water vapor in air are specified.
DO 43 K=3,14
RIXX=RIX*DIFRAT(K)+1./(HSTAR(K)/3000.+100*FO(K))
RLUXX=RLU(N)/(HSTAR(K)/1.0E+5 + FO(K))
C Adjust for effects of dew or rain
IF((IDEW+IRAIN).GE.1.AND.TC0(I,J).GT.0.6.AND.RLU(N).LT.9999.)
1 RLUXX=1./(1./(3.»RLUXX)+HSTAR(K)/I.0E+07+FO(K)/RLUX)
RGSX=1./(HSTAR(K)/I.0E+0S/RGSS(N)+FO(K)/RGSO(N))
RCLX=1./(HSTAR(K)/1.0E+06/RCLS(N) +FO (K)/RC! .0(N))
R(K,N)=1./(1./RIXX+1./RLUXX+1./(RAC(N)+RGSX)
1 +1./(RDC+RCLX))
43 CONTINUE
44 CONTINUE
C*** Set max. and min. values for bulk surface resistances.
DO 45 K=l,14
DO 45 N=l,ll
IF(R(K,N).GT.9999.)R(K,N)=9999.
45 IF(R(K,N).LE.1.)R(K,N)=10.
C
C*** Read landuse data.
ICOL=I
IROW=J
NREC=(IROW-1)*328+ICOL
DO 46 IL=1,11
46 IUSE(IL)=0.
READ(10'NREC) LAT,LATF,LON,LONF.NPAIR,
1 (ITUSE(IL),IPUSE(IL),IL=1,NPAIR)
DO 47 IL=1,NPAIR
47 IUSE(ITUSE(IL))=IPUSE(IL)
C
C*** Loop through different landuse types.
DO 70 N=l,ll
IF(IUSE(N).EQ.0) GOTO 70
C*** Transfer heat flux to CHV to avoid being erased.
CHV=HV(I,J)
IF(N.NE.7) GOTO 60
C»»« Set values of roughness length and heat flux for water.
ZO(7)=1.4E-02*USTAR(I,J)»USTAR(I,J)/9.8
1 +1.1E-01*XNU/USTAR(I,J)
CHV=20.
50 CONTINUE
46
-------
C**« Compute local USTAR by assuirming U»USTAR (UUSTAR) constant.
C First choice assumes neutral conditions.
CUSTA=SQRT(0.4*UUSTAR(I,J)/(ALOG(CZ/ZO(N))))
ICNT=«
C Start iteration.
60 XX=CUSTA
Cl=-0.00327«CZ*CHV/((273.+TCZ(I,J))*USTAR(I,J)**3.)
IF(C1.LT.0.) GOTO 61
IF(Cl.CE.l.) Cl=0.99
SIM=-5.*C1
GOTO 62
61 ZF(C1.LE.-1.) Cl=-0.99
C2=ALOG(-C1)
SIM=EXP(0.032*0.448»C2-0.132*C2*C2)
62 CONTINUE
IF(N.EQ,.7) ZO(7)=1.4E-02*USTAR(I,J)*USTAR(I,J)/
1 9.8+l.lE-01*XNU/USTAR(I,J)
CUSTA=SQ.RT (0. 4*UUSTAR (I, J) / (ALOG (CZ/ZO (N) ) -SIM) )
ERR=ABS((CUSTA-XX)/XX)
ICNT=ICNT*1
IF(ICNT.GT.5) GOTO 63
IF(ERR.GT.0.01) GOTO 60
63 SIC=SIM
IF(Cl.LT.0.) SIC=EXP(0.598*0.39«C2-0.09*C2*C2)
CKUSTA=0.4*CUSTA
OBKHOV=CZ/C1
C*«* Compute S04 surface deposition velocities.
VDS=0.002*USTAR(I,J)
IF(OBKHOV.LT.0.) VDS=VDS*(1.+(-300./OBKHOV)**0.6667)
C1=ZINV (I, J) /OBKHOV
IF(Cl.LT.-30.) VDS=0.0009*USTAR(I,J)*(-C1)**0.6667
C**« Set YDS to be less than VDSMAX.
CVDS=VDS
IF (CVDS.GT. VDSMAX (N)) CVDS=VDSMAX(N)
IF(ZO(N).LE.0.001) GOTO 65
C1=ALOG(CZ/ZO(N))-SIC
00 64 K=l,14
C*** Compute deposition velocities for each grid point.
64 C1X(K)=C1+CKUSTA*R(K,N)+1.75«(DIFRAT(K))**0.667
GOTO 67
65 CONTINUE
DO 66 K=l,14
66 C1X(K)=ALOG(CZ*CKUSTA/DC(K))+CKUSTA*R(K,N)-SIC
67 DO 68 K=l,14
VX(K)=VD(K,I,J)
88 VD(K,I,J)=CKUSTA*IUSE(N)/C1X(K)
VX(15)=VD(15,I,J)
VD (15,1, J) =
-------
SUBROUTINE AVERAGE (I, J,LL,ISESN,IUSE, USTAR, R.CVDS.VD, IFLAG)
O •••««•*•»*»••*•***•*•»•*•»*«*•••«•**»«*••***•••*•*•*•****
C*** This subroutine i» optional for checking out the module
C for • limited amount of input data. It is not intended for
C use with RAOM or other numerical models. By changing when
C IFLAG is set to 2 in the calling program, averages over
C long assumed time periods may be computed. Then, thAe
C numerical value of 600 used between statements 30 and 40 of
C this subroutine would have to be changed to the actual
C number of samples used in the summations.
C*** Four matrices are produced whenever averages are produced
C (IFLAG=2, which routes program to statement label 30).
C The matrices consist of (1) a compressed landuse file with
C USTAR values for each 6 by 5 deg square, and (2-4) values
C of bulk surface resistances for IS substances.
C
IMPLICIT INTEGER*2 (I-N)
INTEGER*4 IUSEA
DIMENSION IUSE(11) ,USTARA(15,6) ,R(15,11) , IUSEA (11, 15, 6) ,
1 IUSEX(15,6) , YDS (15,15,6) ,VOA(15,1S,6) ,CVDSA(16,6) ,
2 USTAR (328 , 186) , VD (15 , 328 , 186)
C
C*** Check for beginning and ending of run.
IF (IFLAG. EQ.0) GOTO 25
IF(IFLAG.EQ.2) GOTO 30
C
C*** Initialize summation variables.
DO 20 11=1,15
DO 20 JJ=1,6
USTARA(II,JJ)=0.
CVDSA(II,JJ)=0.
IUSEX(II,JJ)=0
DO 15 N=l,ll
IS IUSEA (N, II, JJ)=0.
DO 20 K=l,16
VDS(K,II,JJ)=0.
20 VDA(K,II,JJ)=0.
IFLAG=0
C
C*** Compute sums.
25 IF(I.LT.13.0R.I.GT.312) GOTO 100
IF(J.LT.7) GOTO 100
JJ=(J-7)/30*l
USE=IUSE(UL)
USE=USE/100.
IUSEA(LL,II,JJ)=IUSEA(LL,II,JJ)«.IUSE(LL)
USTARA (II , J J) =USTARA (II , J J) +
1USTAR(I, J) *USTAR(I, J) *USE
CVDSA (II , J J) =CVDSA (II , J J) +CVDS*USE
DO 26 K=l,15
IF(K.NE.15) YDS(K,II,JJ)=VDS(K,II,JJ)+1./R(K,LL)«USE
26 VDA(K,II,JJ)=VDA(K,II,JJ)+VD(K,I,J)
GOTO 100
C
C*** Compute averages.
30 DO 40 11=1,15
DO 40 JJ=1,6
DO 38 LL=1,11
IUSEA (LL , II , J J) =IUSEA (UL , II , J J) /600 .
38 IUSEX (II , J J) =IUSEX (II , J J) +IUSEA (LL , II , J J)
DO 39 K=l,15
C Convert surface deposition velocities to resistances.
IF(VDS(K,II,JJ).NE.0.) VDS(K,II,JJ)=
1 l./VDS(K,II,JJ)*600.
IF(VDS(K,II,JJ).EQ.0.)VDS(K,II,JJ)=9999.
39 VDA(K,II,JJ)=VDA(K,II,JJ)/600.
IF (CVDSA (II, JJ) .NE.0.) VDS(15,II,JJ) =
1 1. /(CVDSA (II, JJ)/600.)
USTARA (II , J J) =SQRT (USTARA (II , J J) /600 . )
40 CONTINUE
48
-------
C*** OUTPUTS
C**« Writ* out averaged friction velocities and landuse data.
WRITE(8,1000)
1000 FORMAT (' FRICTION VELOCITY (m/s) and LANDUSE COVERAGES
1 (percent coverage)')
WRITE(8,1010) ISESN
WRITE(8,1001)
1001 FORMAT(' Long. Lat. USTAR Type: 123456
1 7 8 9 10 ll*/)
00 50 11=1,15
00 60 JJ=1,6
IF(IUSEX(II,JJ).LT.90) GOTO 60
XLONG=52.5+11*5
XLAT=22.5+JJ*S
WRITE(8,1002) XLONG,XLAT,USTARA(II,JJ),
1 (IUSEA(LL,II,JJ),LL=1,11)
50 CONTINUE
1002 FORMAT(2F6.1,F6.2,4X,11I4)
WRITE(8,2000)
2000 FORMAT('l')
C*«* Write out averaged surface res.'s and dep. vel.'s.
C**« First write out values for S02, S04, 03, N03, AN) NO.
WRITE(8,1003)
1003 FORMAT(' SURFACE RESISTANCES (s/m) and DEPOSITION
1 VELOCITIES (cm/s)')
WRITE(8,1010) ISESN
WRITE(8,1004)
1004 FORMAT(» Long. Lat. S02 S04 03
1 N02 NO'/)
00 60 11=1,15
DO 60 JJ=1,6
IF(IUSEX(II,JJ).LT.90) GOTO 60
XLONG=52.5+11*5
XLAT=22.S+JJ*5
WRITE(8,1005) XLONG,XLAT,VDS(1,II,JJ),VDA(1,II,JJ),
1 VDS(15,II, JJ) ,VDA(15,II, JJ) ,VDS(2,II, JJ) ,VDA(2,II, JJ) ,
2 VDS(3,II,JJ),VDA(3,II,JJ),VDS(4,II,JJ),VDA(4,II,JJ)
60 CONTINUE
1005 FORMAT(2F6.1,5(F6.0,F7.3))
WRITE(8,2000)
C*«* Write out values for HN03, H202, ALD, HCHO, and OP.
WRITE(8,1003)
WRITE(8,1010) ISESN
WRITE(8,1006)
1006 FORMAT(> Long. Lat. HN03 H202 ALD
1 HCHO OP'/)
DO 70 11=1,15
DO 70 JJ=1,6
IF(IUSEX(II,JJ).LT.90) GOTO 70
XLONG=52.5+11*5
XLAT=22.5+JJ»5
WRITE(8,100S) XLONG,XLAT,VDS(6,II, JJ) ,VDA(6,II. JJ) ,
1 VDS(6,II, JJ) ,VDA(6,II, JJ) ,VDS(7,II, JJ) ,VDA(7,II, JJ) ,
2 VDS(8,II, JJ) ,VDA(8,II, JJ) ,VDS(9,II, JJ) ,VDA(9,II, JJ)
70 CONTINUE
WRITE(8,2000)
C*«* Write out values for PAA, ORA, HN3, PAN, and HN02.
WRITE(8,1003)
WRITE(8,1010) ISESN
WRITE(8,1007)
1007 FORMAT(' Long. Lat. PAA ORA NH3
1 PAN HN02'/)
DO 80 11=1,15
DO 80 JJ=1,6
IF(IUSEX(II,JJ).LT.90) GOTO 80
XLONG=52.6+11*5
XLAT=22.6+JJ*5
WRITE(8,100S) XLONG,XLAT,VDS(10,II,JJ),VDA(10,II,JJ),
1 VDS(11,II,JJ),VDA(11,II,JJ),VDS(12,II,JJ),VDA(12,II,JJ),
2 VDS(13,II,JJ),VDA(13,II,JJ),VDS(14,II,JJ),VDA(14,II,JJ)
80 CONTINUE
WRITE(8,2000)
1010 FORMAT(' Seasonal category number',I3/)
PRINT «,' End of writing out on MODAV.DAT'
100 CONTINUE
RETURN
END 49
-------
C MOOINP.DAT
C*********** Maximum S04 dep. velocities (m/s;llF6.3), types 1-11
C 1, Midsummer with lush vegetation
0.001 0.01 0.01 0.01 0.01 0.01 0.001 0.01 0.01 0.01 0-01
C 2, Autumn with unharvested cropland
0.001 0.01 0.01 0.001 0.008 0.004 0.001 0.01 0.01 0.01 0.01
C 3, Late autmn after frost, no snow
0.001 0.01 0.01 0.001 0.008 0.004 0.001 0.01 0.01 0.01 0.01
C 4, Winter with snow on ground
0.001 0.01 0.01 0.001 0.008 0.004 0.001 0.01 0.01 0.01 0.01
C 6, Transitional spring with partial green coverage
0.001 0.01 0.01 0.01 0.01 0.01 0.001 0.01 0.01 0.01 0.01
C********** Values of Zo (l.E-4 m; 1116), landuse types 1-11
C 1, Midsummer with lush vegetation
10000 2600 600 10000 10000 10000 1 20 1600 1000 1000
C 2, Autumn with unharvested cropland
40000 ,1000 600 10000 10000 10000 1 20 1000 800 800
C 3, Late autumn after frost, no snow
10000 60 500 10000 10000 10000 1 20 1000 200 600
C 4, Winter with snow on ground
10000 10 10 10000 10000 10000 1 20 10 10 400
C 6, Transitional spring with partial green coverage
10000 300 200 10000 10000 10000 1 20 1000 300 600
C********** Values of surface resistance components (s/m)
C 1, Midsummer with lush vegetation
ri 9999. 60. 120. 70. 130. 100. 9999. 9999. 80. 100. 160.
rlu 9999. 2000. 2000. 2000. 2000. 2000. 9999. 9999. 2600. 2000. 4000.
rac 100. 200. 100. 2000. 2000. 2000. 0. 0. 300. 150. 200.
rgsS 400. 150. 360. 600. 500. 100. 0. 1000. 0. 220. 400.
rgsO 300. 160. 200. 200. 200. 300. 2000. 400. 1000. 180. 200.
rcIS 9999. 2000. 2000. 2000. 2000. 2000. 9999. 9999. 2500. 2000. 4000.
rcIO 9999. 1000. 1000. 1000. 1000. 1000. 9999. 9999. 1000. 1000. 1000.
C 2, Autumn with unharvested cropland
ri 9999. 9999. 9999. 9999. 250. 600. 9999. 9999. 9999. 9999. 9999.
rlu 9999. 9000. 9000. 9000. 4000. 8000. 9999. 9999. 9000. 9000. 9000.
rac 100. 150. 100. 1500. 2000. 1700. 0. 0. 200. 120. 140.
rgsS 400. 200. 350. 500. 600. 100. 0. 1000. 0. 300. 400.
rgsO 300. 150. 200. 200. 200. 300. 2000. 400. 800. 180. 200.
rcIS 9999. 9000. 9000. 9000. 2000. 4000. 9999. 9999. 9000. 9000. 9000.
rcIO 9999. 400. 400. 400. 1000. 600. 9999. 9999. 400. 400. 400.
C 3, Late autumn after frost, no snow
ri 9999. 9999. 9999. 9999. 250. 600. 9999. 9999. 9999. 9999. 9999.
rlu 9999. 9999. 9000. 9000. 4000. 8000. 9999. 9999. 9000. 9000. 9000.
rac 100. 10. 100. 1000. 2000. 1600. 0. 0. 100. 60. 120.
rgsS 400. 150. 350. 500. 500. 200. 0. 1000. 0. 200. 400.
rgsO 300. 150. 200. 200. 200. 300. 2000. 400. 1000. 180. 200.
rcIS 9999. 9999. 9000. 9000. 3000. 6000. 9999. 9999. 9000. 9000. 9000.
rcIO 9999. 1000. 400. 400. 1000. 600. 9999. 9999. 800. 600. 600.
C 4, Winter with snow on ground
ri 9999. 9999. 9999. 9999. 400. 800. 9999. 9999. 9999. 9999. 9999.
rlu 9999. 9999. 9999. 9999. 6000. 9000. 9999. 9999. 9000. 9000. 9000.
rac 100. 10. 10. 1000. 2000. 1600. 0. 0. 50. 10. 60.
rgsS 100. 100. 100. 100. 100. 100. 0. 1000. 100. 100. 50.
rgsO 600. 3500. 3500. 3600. 3600. 3500. 2000. 400. 3500. 3600. 3500.
rcIS 9999. 9999. 9999. 9000. 200. 400. 9999. 9999. 9000. 9999. 9000.
rcIO 9999. 1000. 1000. 400. 1600. 600. 9999. 9999. 800. 1000. 800.
C 5, Transitional spring with partial green coverage
ri 9999. 120. 240. 140. 260. 190. 9999. 9999. 160. 200. 300.
rlu 9999. 4000. 4000. 4000. 2000. 3000. 9999. 9999. 4000. 4000. 8000.
rac 100. 60. 80. 1200. 2000. 1500. 0. 0. 200. 60. 120.
rgsS 500. 160. 350. 500. 500. 200. 0. 1000. 0. 260. 400.
rgsO 300. 150. 200. 200. 200. 300. 2000. 400. 1000. 180. 200.
rcIS 9999. 4000. 4000. 4000. 2000. 3000. 9999. 9999. 4000. 4000. 8000.
rcIO 9999. 1000. 600. 600. 1600. 700. 9999. 9999. 600. 800. 800.
50
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