JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 107, NO. D3, 4026, 10.

1029/2001JD000483, 2002

A parameterization of aerosol activation

3. Sectional representation
Hayder Abdul-Razzak
Mechanical Engineering Department, Texas A&M University-Kingsville, Kingsville, Texas, USA

Steven J. Ghan
Pacific Northwest National Laboratory, Richland, Washington, USA
Received 3 February 2001; revised 16 July 2001; accepted 20 July 2001; published 8 February 2002.
[1] A parameterization of the activation of a lognormal size distribution of aerosols to form cloud
droplets is extended to a sectional representation of the aerosol size distribution. For each section,
number concentration and chemical composition are uniform functions of particle radius. The
parameterization is applied by calculating an effective critical supersaturation of all sections from
which the maximum supersaturation of the air parcel is calculated using the previously derived
parameterization. The Köhler theory is used to relate the aerosol size distribution and composition
to the number activated for each section as a function of maximum supersaturation. For most cases,
parametric results are within 10% of those obtained by detailed numerical computations for both
idealized and measured aerosol size distributions. The parameterization thus provides an accurate
method of treating the activation process for models that use a sectional representation of the
aerosol size distribution. INDEX TERMS: 0305 Atmospheric Composition and Structure:
Aerosols and particles (0345, 4801); 0320 Atmospheric Composition and Structure: Cloud physics
and chemistry; 0345 Atmospheric Composition and Structure: Pollution –urban and regional
(0305); 0322 Atmospheric Composition and Structure: Constituent sources and sinks; KEYWORDS:
aerosol, activation, cloud, parameterization, sectional

1. Introduction physics of the problem. It is therefore not enough to apply all

we know about the physics to a climate model; the knowledge
[2] Aerosol activation is the process by which aerosol particles
must be condensed enough to permit multidecade global climate
grow by water condensation to form cloud droplets. It is called
simulations.
activation because it involves a threshold wet particle size, above
[5] The effects of aerosols on clouds can be separated into two
which particles will continue to grow spontaneously unless the
processes, namely, the effects of the aerosol particles on cloud
supersaturation with respect to water decreases fast enough to
droplet number, and the effects of droplet number on cloud liquid
deactivate the particles [Nenes et al., 2001].
water content and cloud albedo. This paper is concerned only with
[3] The aerosol activation process is important for several
the first effect. In particular, we focus on the activation of aerosols
reasons. First, it determines the formation of cloud droplets and
to form cloud droplets (droplet number concentration is also
hence affects droplet number concentration, droplet effective
influenced by the coalescence process and by evaporation, which
radius, cloud albedo, and (via its influence on the coalescence of
require separate treatments).
droplets to form precipitation) cloud liquid water content and cloud
[6] Our knowledge about the aerosol activation process is
lifetime; accurate parameterizations of the process are therefore
summarized in text [Pruppacher and Klett, 1997; Seinfeld and
needed for estimates of the so-called indirect forcing by anthro-
Pandis, 1998] and in numerical models having detailed treatments
pogenic aerosols through their role as cloud condensation nuclei.
of aerosol activation [Jensen and Charlson, 1984; Flossmann et
Second, by separating particles into those activated and those not
al., 1985; Ahr et al., 1989; Liu and Wang, 1996; Abdul-Razzak et
activated, the aerosol activation process determines which particles
al., 1998]. However, the treatment in these numerical models is too
can increase their solute mass through aqueous chemistry in cloud
computationally demanding to be applied to global climate models.
droplets and also which particles are removed from the atmosphere
Condensed parameterizations of the aerosol activation process are
through precipitation of the cloud droplets; accurate parameter-
therefore required.
izations of the process are therefore needed for models of cloud
[7] All previous parameterizations have relied upon simplified
processing of aerosols and nucleation scavenging of aerosols.
representations of the aerosol size distribution. The earliest param-
[4] Representing the effects of activation on aerosol particles,
eterizations [Squires, 1958; Twomey, 1959; Squires and Twomey,
cloud droplet number concentration, cloud liquid water content,
1960] implicitly assumed the aerosol size distribution follows a
and cloud albedo is one of the most challenging problems facing
power law [Jiusto and Lala, 1981; Herbert, 1986]. More recent
the atmospheric sciences community today. The problem is diffi-
parameterizations have assumed a single mode [Ghan et al., 1993;
cult enough for a single cloud or cloud system, but is especially
Abdul-Razzak et al., 1998] or multiple mode [Ghan et al., 1995;
difficult because of the need to treat it for the whole Earth so that
Abdul-Razzak and Ghan, 2000] lognormal size distribution.
the potential global climate impacts can be estimated. Any treat-
[8] Although parameterizations based on such simplified aero-
ment of these effects in a model of the global climate system must
sol size distributions accurately predict droplet nucleation when
be computationally affordable, yet must address the essential
the aerosol size distribution can be accurately approximated by
the simplified representation, they cannot be expected to perform
Copyright 2002 by the American Geophysical Union. well when the aerosol size distribution is very different from the
0148-0227/02/2001JD000483 idealized form. In addition, although existing parameterizations

AAC 1- 1
AAC 1-2 ABDUL-RAZZAK AND GHAN: SECTIONAL AEROSOL ACTIVATION

can predict the impact of nucleation on the total number and mass
concentrations of aerosols, they cannot predict changes in details
of the size distribution because the size distribution is constrained
by the simplified representation. In particular, unless many
narrow lognormal modes are used, the parameterizations fail to
predict the sharp transition between particles large enough and
those too small to be activated (Figure 1), and the influence of
the transition on subsequent aerosol activation. Resolving the
transition is important within clouds, which contain both acti-
vated and interstitial particles.
[9] Fortunately, the aerosol dynamics modeling community has
developed a much more general representation of the aerosol size
distribution that has the potential to resolve such sharp transi-
tions. The so-called sectional representation of the aerosol pre-
dicts aerosol number concentration for each of an arbitrary
number (typically 10 – 100) of size sections. Treatments of many
aerosol processes (nucleation, coagulation, condensation, impac-
tion scavenging, gravitational settling, and dry deposition) have
been developed for sectional models [Zhang et al., 1999, and Figure 1. The number fraction of aerosol particles activated for
references therein]. However, no parameterization of aerosol each section from a numerical simulation with 100 bins (diamond)
activation has yet been developed for a sectional model of the and from the sectional parameterization for 10 bins (square). The
aerosol size distribution. This limits the application of sectional updraft velocity is 1 m s1, the aerosol size distribution is lognormal
models to cloud-free conditions (which obviously precludes their with a number concentration of 1000 cm3, a geometric mean radius
application to estimates of effects of aerosols on clouds or vice of 0.05 mm and a standard deviation of 2, the temperature is 15 C,
versa), or requires a computationally intensive explicit treatment and the pressure is 90,000 Pa.
of the activation process [Russell and Seinfeld, 1998] (which
precludes their application to multiyear global simulations). What
is clearly needed is an aerosol activation parameterization that is
applicable to a sectional representation of the aerosol size is the critical supersaturation of a particle with a dry radius equal to
distribution. the geometric mean dry radius am of the size distribution, and
[10] In this paper we extend our previously developed aerosol
activation parameterization for a lognormal representation of the  1=2
aerosol size distribution [Abdul-Razzak et al., 1998] (hereafter 2A aV
z ð5Þ
denoted part 1) to a sectional representation. Given the updraft 3 G
velocity and the size, number concentration, and composition of
each size section, the parameterization predicts the maximum ðaV =GÞ3=2
supersaturation of the rising air parcel and the number and mass h ; ð6Þ
activated for each size section. 2prw gN
[11] In the following section, the procedure by which we can
apply the parameterization of part 1 to sectional representation is where A accounts for surface tension effects in the Köhler
described. The evaluation of this procedure is presented in equilibrium equation (see part 1), B is the hygroscopicity, V is
section 3. Concluding remarks and summary of results are the updraft velocity, G accounts for diffusion of heat and
outlined in section 4. moisture to the particle, rw is the density of water, N is the total
aerosol number concentration, and g and a are coefficients in
the supersaturation balance equation. The hygroscopicity,
2. Parameterization defined
[12] The parameterization of the single mode version (part 1)
relates the maximum supersaturation Smax of the rising air parcel to vfMw ra
four dimensionless parameters as follows: B ð7Þ
Ma rw

Sm
Smax ¼ 
3=2
3=4 1=2 ; ð1Þ depends on particle composition through its dependence on the
V Sm2 number of ions n, the osmotic coefficient f, the aerosol
f ðs Þ h þ g ðsÞ hþ3z
molecular weight Ma, and the aerosol material density ra. Note
that f (s) has been modified by Abdul-Razzak and Ghan [2000].
where [13] For a sectional representation of the size distribution one
might consider simply applying the Abdul-Razzak and Ghan
  [2000] multimodal parameterization to a sectional representation.
f ðsÞ  0:5 exp 2:5 ln2 s ð2Þ
In the multimodal parameterization each mode is assumed to be a
lognormal distribution. To adapt it to a sectional representation,
g ðsÞ  1 þ 0:25 lns ð3Þ one would have to choose an appropriate geometric standard
deviation for each mode. However, such a treatment is inconsistent
are functions of the standard deviation s of the lognormal size with a sectional representation, which typically assumes the
distribution of the aerosol particles, number distribution is uniform rather than gaussian in log radius
within each section, with no overlap of sections. We have found
 3=2 that a more accurate parameterization for the activation of a
2 A
Sm  pffiffiffi ð4Þ sectional distribution of aerosols is to set the standard deviation
B 3am in equation (1) to a value of one and replace the critical super-
 ABDUL-RAZZAK AND GHAN: SECTIONAL AEROSOL ACTIVATION AAC 1-3

X
I
M¼ Mi mi ; ð11Þ
i¼1

where the number and mass fraction activated for each section, ni
and mi, are given by

ni ¼ mi ¼ 0 if Smax < Sil ð12Þ

logðSmax =Sil Þ
ni ¼ if Sil  Smax  Siu ð13Þ
logðSiu =Sil Þ

a3i max  a3il

Figure 2. The number fraction of aerosol particles activated mi ¼ if Sil  Smax  Siu ð14Þ
a3iu  a3il
as a function of geometric mean radius for an updraft velocity of
0.5 m s1, a number concentration of 1000 cm3, and a standard
ni ¼ mi ¼ 1 if Siu < Smax : ð15Þ
deviation of 2 at a temperature of 15 C and a pressure of 90,000 Pa.
The solid line represents single mode parameterization described in
part 1; S10 (triangle) and S30 (square) are sectional results for 10 Analogous functions ni and mi could also be derived if the volume
and 30 sections, respectively; N100 (cross) is numerical result with rather than number distribution is assumed to be uniform within
100 bins. each section. Note that aimax need not be the same for every section
if the hygroscopicity is different for each section. The number and
mass activated for such a treatment are continuous functions of
saturation Sm by an effective critical supersaturation that is calcu- Smax and hence updraft velocity.
lated from
P
I 3. Evaluation
2 Ni
i¼1 [16] To evaluate the activation parameterization for a sectional
Se 3 ¼ . 2= ; ð8Þ
P
I representation of aerosol particles, the aerosol activation is
Ni Si 3 simulated for a variety of aerosol size distributions and a wide
i¼1
range of updraft velocities using the numerical model described
where I is the number of sections, Si is the critical supersaturation in part 1. The simulated number fraction activated (defined as the
at the middle of section i, and Ni is the number of particles in each fraction of particles with radius larger than their critical radius for
section. We cannot offer a rigorous physical basis for (8), but note activation at the time of maximum supersaturation) is compared
that (8) provides a crude estimate of Sm2/3 via (4); other equally with the estimates obtained from the parameterization outlined in
plausible formulations for Se2/3 were tested but did not perform as section 2. All simulations are initialized with a temperature 288
well as (8). Note that because according to (4) the critical super- K, a pressure of 90,000 Pa, and a supersaturation of zero, with
saturation depends on the hygroscopicity and hence the particle particles initially assumed to be in equilibrium with a relative
composition, each section in (8) can have a different composition. humidity of 100%. The gas kinetic parameters are the same as
[14] Using the effective critical supersaturation and assuming those used in part 1, namely, 2.16 105 cm for thermal jump
s = 1, the maximum supersaturation of the air parcel can be length, 1.096 105 cm for vapor jump length, 1.0 for
calculated as follows: condensation coefficient, and 0.96 for thermal accommodation
coefficient.
Se [17] Two different types of aerosol size distributions are
Smax ¼ 
  : ð9Þ
3=2
2 3=4 1=2 considered. In the first the aerosols are composed of ammonium
V Se
0:5 h þ hþ3z sulfate with a lognormal size distribution. The geometric mean
radius am ranges from 0.001 to 0.1 mm, standard deviation s
Note that assuming s = 1 implies the sections are delta functions. ranges from 1.12 to 3.0, number concentration N ranges from
This is consistent with the treatment of activation in numerical
models, which consider the growth of only the central size in each
section. However, for a coarse representation of the aerosol size
distribution (with, for example, 10 sections) it is necessary to treat
the size distribution within each section as uniform so that the
number activated is a continuous function of updraft velocity. This
treatment is described next.
[15] Once the maximum supersaturation of the air parcel is
determined, the activation of each section is determined by
comparing Smax with Sil and Siu (the lower and upper critical
supersaturation bounds of the section) and by comparing the dry
particle radius aimax corresponding to Smax with the radii ail and aiu
corresponding to Sil and Siu. The dry particle radii are related to
supersaturation by equation (4). By integrating the uniform dis-
tribution of number within each section, the concentrations of the
total number and mass activated are then
X
I
N¼ Ni ni ð10Þ Figure 3. As in Figure 2, but as a function of number con-
i¼1 centration for a geometric mean radius of 0.05 mm.
AAC 1-4 ABDUL-RAZZAK AND GHAN: SECTIONAL AEROSOL ACTIVATION
Figure 4. As in Figure 2, but as a function of updraft velocity for
a geometric mean radius of 0.05 mm.
10 to 10,000 cm3, and updraft velocity V ranges from 0.02 to 10 m
s1. The baseline conditions are am = 0.05 mm, s = 2, N = 1000
cm3, and V = 0.5 m s1. For each numerical simulation the aerosol
population is discretized into 100 sections with radius increasing by
a constant factor. For each sectional parameterization estimate the
aerosol population is discretized into 10 or 30 sections with radius
increasing by a constant factor.
[18] Figure 1 illustrates the performance of the parameterization
for a particular updraft velocity and aerosol size distribution. It
shows that the sectional parameterization accurately distinguishes
between size bins with particles too small to be activated and those
with particles large enough to be activated. By treating fractional
activation for each section, the parameterization also accurately
treats the transition between particles too small to be activated and
those large enough to be activated.
[19] Figures 2, 3, 4, and 5 show the number fraction activated
as a function of geometric mean radius, aerosol number, updraft
velocity, and standard deviation, respectively, as simulated using
100 sections, as parameterized using 10 and 30 sections, and as
parameterized according to the lognormal parameterization
described in part 1. The number fraction activated according to
the sectional parameterization is in close agreement (within 10%)
with the numerical simulation for the full range of conditions.
The close agreement for the fraction activated means that the
parameterization of the maximum supersaturation is in close
agreement with the numerical simulation. For a size distribution
with uniform composition, the close agreement for the fraction
activated also means that the transition between activated and
unactivated sections is treated accurately, to within the resolution
Figure 5. As in Figure 2, but as a function of standard deviation
for a geometric mean radius of 0.05 mm.
Figure 6. Distribution of aerosol number concentration with size
for a free troposphere aerosol [Raes et al., 1997], for a marine
aerosol [O’Dowd et al., 1997], for a polluted marine aerosol
[Collins et al., 2000], and for an urban aerosol [Hughes et al.,
1998].
of the size distribution by the sections. The figures also show that
the number of sections has the same effect on the accuracy of
numerical and parametric results, and that the sectional and
numerical results agree as well as the lognormal and numerical
results.
[20] The second type of aerosol size distribution is measured in
the field. Figures 6 and 7 show the size distributions of number
and hygroscopicity, respectively, of four different measured aero-
sols. The first is a free tropospheric aerosol (FT-II) measured by
Raes et al. [1997]. The distribution is dominated by a single mode
that is approximated quite well by a lognormal distribution with a
number concentration of 480 cm3, a number mode radius of 0.03
mm, and a geometric standard deviation of 2.1. For simplicity, the
chemical composition of the free tropospheric aerosol is assumed
to be pure ammonium bisulfate. The sectional resolution is taken
to be the same as that of the measurements, namely, 50 bins
ranging in radius from 0.003 to 0.25 mm. The fraction activated is
plotted as a function of updraft velocity in Figure 8. The param-
eterization estimates the fraction activated to within 5% at all
updraft velocities.
[21] The second measured aerosol size distribution is a marine
aerosol [O’Dowd et al., 1997, Figure 1] typical of the northeast
Figure 7. Distribution of aerosol hygroscopicity with size for the
same aerosols as shown in Figure 6.
 ABDUL-RAZZAK AND GHAN: SECTIONAL AEROSOL ACTIVATION
Figure 8. The sectional parameterization and numerical simula-
tion of the fraction of aerosol particles activated as functions of
updraft velocity for the free troposphere aerosol.
Atlantic for average wind speeds (8 m s1) and a relative humidity
of around 80%. The measurements provide the number concen-
trations for 61 bins ranging in radius from 0.005 to 25 mm. The size
distribution is characterized by the presence of multiple modes
(ultrafine, nucleation, accumulation, and sea salt). The chemical
composition of the aerosol as a function of size is taken from
Katoshevski et al. [1999]. The hygroscopicity ranges from that of
ammonium sulfate (0.7) for ultrafine particles to that of sodium
chloride (1.3) for coarse particles. The total number concentration
is 903 cm3. Figure 9 shows the simulated and parameterized
fraction activated as functions of updraft velocity. Both the
numerical simulations and the sectional parameterization predict
low activation fractions for this aerosol because most of the aerosol
number is at radii less than 0.01 mm while most of the aerosol
surface area is at radii greater than 1 mm. The numerical and
parameterized estimates of activation agree to within 10% for
updrafts stronger than 0.5 m s1, but the parameterized activation
is twice as large as the numerical simulation for updrafts weaker
than 0.1 m s1.
[22] The third measured size distribution is a polluted marine
aerosol corresponding to conditions where aged continental aerosol
from Europe is mixed with marine aerosol, producing a bimodal
distribution with a pronounced accumulation mode [Collins et al.,
2000]. The total number concentration is 1457 cm3, and the
geometric mean radius is 0.068 mm. The chemical composition is
assumed to be ammonium sulfate. The measurements cover 100
Figure 9. The sectional parameterization and numerical simula-
tion of the fraction of aerosol particles activated as functions of
updraft velocity for the marine aerosol.
AAC 1-5
Figure 10. The sectional parameterization and numerical simula-
tion of the fraction of aerosol particles activated as functions of
updraft velocity for the polluted marine aerosol.
bins with radii from 0.002 to 1 mm. Figure 10 compares the
simulated and parameterized fraction activated as functions of
updraft velocity. The numerical model’s results are similar to those
for the lognormal size distribution illustrated in Figure 4. The
parameterization agrees with the numerical simulation to within
5% for updrafts stronger than 0.5 m s1, but underestimates the
fraction activated by as much as a factor of 3 for updrafts weaker
than 0.1 m s1.
[23] The fourth measured aerosol is an urban aerosol [Hughes
et al., 1998]. It is dominated by fine and ultrafine particles, with
a low soluble fraction producing a hygroscopicity ranging from
0.05 for ultrafine particles to 0.1 for coarse particles and 0.25 for
accumulation mode particles. The total number concentration is
3707 cm3, but judging from the shape of the measured size
distribution the measurements probably fail to sample many
particles with radius smaller than 0.035 micron; however, the
unsampled particles are too small to be activated for all but the
strongest updrafts, so we do not expect the limited size range of
the measurements to significantly influence the estimate of the
number or mass of activated particles. Figure 11 compares the
simulated and parameterized fraction activated as functions of
updraft velocity. The parameterized number agrees with the
numerical simulation to within 10% for all updraft velocities.
Although the hygroscopicity decreases abruptly from 0.2 to 0.1
for particles with radius between 0.48 mm and 0.54 mm, the
fraction activated is a monotonic function of particle size for all
Figure 11. The sectional parameterization and numerical simula-
tion of the fraction of aerosol particles activated as functions of
updraft velocity for the urban aerosol.
AAC 1-6 ABDUL-RAZZAK AND GHAN: SECTIONAL AEROSOL ACTIVATION
updraft velocities because for all updraft velocities all particles in
that size range are activated.
4. Conclusions
[24] In this study we have extended the aerosol activation
parameterization of part 1 to the case of a sectional representation
of aerosol particles. The number activated according to the sec-
tional parameterization agrees with numerical simulations to within
10% for idealized lognormal size distributions under a wide variety
of conditions. Agreement for measured size distributions with size-
dependent composition is almost as good, except when the updraft
velocity is weaker than 0.1 m s1. This success has been achieved
by simply calculating an effective critical supersaturation that is
compatible with our physical understanding of the relationship
between the fraction activated and four dimensionless parameters.
This affirms that the relationship accurately represents the aerosol
activation process.
[25] The aerosol activation parameterization described in this
paper should be suitable for any sectional representation of the
aerosol size distribution. Because it is expressed in terms of the
critical supersaturation of each bin, it can be applied to an arbitrary
aerosol composition in each section. Thus the parameterization can
be applied to multiple size distributions with different composi-
tions (e.g., an external mixture of sea salt, sulfate, organic carbon,
and dust particles). For sections that are composed of an internal
mixture of different materials, Abdul-Razzak and Ghan [2000]
describe how the mean hygroscopicity and critical supersaturation
of the section can be calculated. By combining the treatment for an
external mixture of aerosol components described here with the
treatment for an internal mixture, the activation of virtually any
distribution (externally and internally mixed) of aerosol composi-
tion with size can be predicted by the parameterization.
[26] Acknowledgments. Richard Easter’s comments led to improve-
ments in the manuscript. This study was primarily supported by the NASA
Earth Science Enterprise under contract NAS5-98072 and grants NAG5-
8797 and NAG5-9531. Support was also provided by the U.S. Department
of Energy Atmospheric Radiation Measurement Program, which is part of
the DOE Biological and Environmental Research Program. The Pacific
Northwest National Laboratory is operated for the DOE by Battelle
Memorial Institute under contract DE-AC06-76RLO 1830.
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H. Abdul-Razzak, Mechanical Engineering Department, Texas A&M
University-Kingsville, Kingsville, TX 78363, USA.
S. J. Ghan, Pacific Northwest National Laboratory, Richland, WA 99352,
USA. (steve.ghan@pnl.gov)