GEOPHYSICAL RESEARCH LETTERS, VOL. 29, NO. 10, 1398, 10.
1029/2002GL014947, 2002
Importance of shapes and compositions of wind-blown dust particles
for remote sensing at solar wavelengths
Olga V. Kalashnikova and Irina N. Sokolik
Program in Atmospheric and Oceanic Sciences, University of Colorado, Boulder, CO, USA
Received 19 February 2002; revised 4 April 2002; accepted 11 April 2002; published 23 May 2002.
[1] The quality of satellite aerosol retrievals depends critically
upon the modeling accuracy of the aerosol optical properties.
The optical properties of mineral aerosols depend on particle
morphology, mineralogy, and state of mixing. Here we investigate
how the realistic morphology and composition of dust particles
affect the optical properties of dust mixtures by utilizing
microscopy data that recently become available of dust samples
collected in the atmosphere. The data were used to reconstruct the
representative composition-shape-size (CSS) distributions and then
the discrete dipole approximation technique was applied to
calculate the optical properties. We demonstrate that the presence
of sharp-edge, angular-type particles results in various differences
in the scattering phase function, asymmetry parameter, optical
depth and single scattering albedo compared to those of the
volume-equivalent spheres or ellipses. These differences are
sufficiently large as to affect the retrievals of aerosol optical
properties from satellite and ground-based remote sensing
observations at the solar wavelengths. INDEX TERMS: 0305
Atmospheric Composition and Structure: Aerosols and particles
(0345, 4801); 0360 Atmospheric Composition and Structure:
Transmission and scattering of radiation; 6969 Radio Science:
Remote sensing
1. Introduction
[2] The retrieval of the aerosol properties on a global scale is
one of the key objectives of several recently launched spacecraft
instruments such as MISR (a multiangle imaging spectral radio-
meter) and MODIS (a moderate resolution imaging spectroradi-
ometer) [Diner et al., 1999]. To fully benefit from the wealth of
data provided by new sensors, the improvement of dust optical
models used in retrieval algorithms is needed.
[3] Current aerosol algorithms prescribe the optical character-
istics for the each aerosol component. It is often assumed that dust
particles have spherical shapes and their composition does not
depend on particle size. However, laboratory and field measure-
ments demonstrate that the scattering phase functions of dust
particles can significantly differ from those predicted for equivalent
spheres [West et al., 1997; Volten et al., 2001]. The only dust
retrieval that account for particle nonsphericity is the MISR
algorithm that uses ellipsoid models derived from T-matrix calcu-
lations [Kahn et al., 1997]. Ellipsoidal models offer a considerable
improvement over use of Mie theory, though there is a need to test
the applicability of these models. Various data demonstrate that
mineral dust particles are not only nonspherical but also in majority
are angular and sharp-edge [Parungo et al., 1997; Buseck and
Posfai, 1999; Gao and Anderson, 2001].
[4] Several previous studies analyzed the optical properties of
nonspherical dust particle [Mishchenko et al., 1997; Yang et al.,
2000]. These studies mainly focused on the comparison of optical
Copyright 2002 by the American Geophysical Union.
0094-8276/02/2002GL014947
38 - 1
properties of particles having a distinct model shape and those of
volume- or surface-equivalent spheres, without being concerned
about how well these model shapes represent actual atmospheric
dust particles. Only one or two values of the refractive indices
were used in previous calculations, overlooking that various
mineral species show distinct refractive indices as a function of
the wavelength [Sokolik and Toon, 1999]. In order to account for
realistic dust particle shapes and compositions, we perform the
modeling of dust optical properties utilizing the new microscopy
data. The goal is to estimate the extent to which the realistic
particle morphology and composition affect the dust optical
properties and hence the retrievals of aerosols from satellite and
ground-based observations.
2. Approach
[5] Our approach considers mineral dust as a mixture of
particles characterized by a given composition-shape-size (CSS)
distribution reconstructed from the microscopy (SEM/TEM) data
of dust samples collected in the atmosphere. The detailed descrip-
tion of the approach is given in [Kalashnikova and Sokolik, 2002].
An ensemble of dust particles can be thought of as an external
mixture of particle classes where each class is defined by a
particular combination of shape and composition. Because the
size-averaged optical properties of the external mixture can be
calculated as a weighted sum of optical properties of individual
components, one can compute size-averaged optical characteristics
of individual classes and then use these results to calculate optical
properties of the dust mixtures of various CSS distributions.
Following this strategy, we computed the optical properties of a
number of dust classes formed with selected regular and recon-
structed irregular shapes identified in the SEM images. To calculate
the orientationally-averaged optical properties of nonspherical
shapes, we used the discrete-dipole approximation (DDA) techni-
que [Draine and Flatau, 1994]. The particle volume-equivalent
diameter was chosen to be in the range 0.1 – 2 mm based on
reported microscopy data, though the geometrical diameter of a
nonspherical particle can be much larger, depending on the particle
thickness. We assumed that dust classes have the same log-normal
size distribution with the medium radius r0 = 0.5 mm and geometric
standard deviation s = 2 [Sokolik and Toon, 1999].
[6] Recently, statistically representative data of dust morpho-
logical properties, that were obtained from analysis of several
thousands of dust particles collected in the atmosphere, become
available. The data were reported in terms of the particle aspect
ratio (AR = a/b, where a is the particle length and b is the particle
width), circularity (CIR = (4p*Area)/Perimeter2) and particle
thickness (or third dimension), h. Using these data, we recon-
structed the following CSS distributions:
CSS1—20% spheres + 50% sharp-edge + 30% smooth
shapes; AR = 1.5, h = b (background dust, [Parungo et al., 1997]).
CSS2—5% spheres + 70% sharp-edge + 25% smooth
shapes; AR = 1.5, h = b (dust storm, [Parungo et al., 1997]).
CSS3—A shape mixture with circularity linearly increasing
with size; AR = 1.5, h = b (long-transported dust, [Huebert et al.,
2000]).
38 - 2 KALASHNIKOVA AND SOKOLIK: OPTICAL PROPERTIES OF NONSPHERICAL MINERALS

Figure 1. Scattering phase functions of the individual particle Figure 2. Scattering phase functions of CSS distributions at l =
shapes at 0.55 mm for (a) Saharan dust analog, and (b) Asian dust 0.55 mm for (a) Saharan dust analog, and (b) Asian dust analog.
analog.

CSS4—A shape mixture of thin particles with circularity approximation the radiance observed by a satellite sensor at a
linearly increasing with size; AR = 1.4, h/b = 0.3 (based on the scattering angle  and a particular wavelength can be expressed as
statistical distribution reported by Okada et al. [2001]). I
P() w0t. Thus, optical depth (or single scattering albedo) can
[7] To calculate the effective spectral refractive indices of dust be inverted from satellite observations if scattering phase function
particles, we followed the approach of Sokolik and Toon [1999] and w0 (or P() and t) are provided from modeling or independent
considering the aggregates of quartz (or clay) and hematite, and measurements.
using the Bruggeman effective medium approximation. The
amount of iron oxides (such as hematite, magnetite, etc.), which
are a strongest absorber of light at solar wavelengths relative to 3. Results
other minerals, may vary on average between 1% and 10% [9] Our calculations show that the optical properties of irregular
[Sokolik and Toon, 1999]. This range defines two cases of weak shapes differ from those of spheres and smooth shapes. Figure 1
and strong absorption considered in our study: 90% clay + 10% illustrates the scattering phase functions of several individual
hematite (Saharan dust analog), and 99% clay + 1% hematite shapes calculated at l = 0.55 mm for Saharan and Asian dust
(Asian dust analog). analogs. These particle shapes were identified in the SEM/TEM
[8] The computed single scattering albedo, w0, and scattering images. As shown in Figure 1, the scattering phase functions of the
phase function, P(), were used to estimate uncertainties in the sharp-edge shapes are lower at the backscattering angles than those
retrievals of aerosol optical depth, t, and the single scattering of equal-volume spheres or smooth ellipsoidal shapes. Thus, a dust
albedo under the single scattering approximation. Under this mixture with the large amount of angular-type particles would differ
not only from spheres but also from ellipses. Figure 1 also shows
the Henyey-Greenstein phase function with the asymmetry param-
Table 1. Single Scattering Albedo w0, Assymmetry Parameter g eter, g, calculated for the volume-equivalent spheres (see Table 1).
and Normalized Extinction Coefficient kext (in units 103cm3/km) The Henyey-Greenstein phase function, which is often used in
aerosol modeling, results in much lower backscattering and lower
Asian dust analog Saharan dust analog forward scattering. Increasing g would cause even lower back-
Shape w0 kext g w0 kext g scattering, but larger forward scattering relative to the phase
Sphere 0.969 1.95 0.70 0.766 1.89 0.74 function of individual shapes considered.
CSS1 0.974 2.22 0.72 0.788 2.16 0.75 [10] Figure 2 demonstrates the differences in phase functions of
CSS2 0.975 2.30 0.73 0.796 2.26 0.76 realistic dust mixtures and those of the equal-volume spheres for
CSS3 0.978 2.55 0.73 0.803 2.43 0.76 Saharan and Asian dust analogs at l = 0.55 mm. This wavelength is
CSS4 0.977 2.64 0.80 0.806 2.45 0.81 often used in remote sensing (e.g., MISR). The phase functions of
 KALASHNIKOVA AND SOKOLIK: OPTICAL PROPERTIES OF NONSPHERICAL MINERALS 38 - 3

racy of such retrievals in the presence of dust, we calculated the

ratio of scattered intensities of considered CSS mixtures and the
intensities of volume-equivalent spheres weighted by the singe
scattering albedo as [P()w0]CSS/[P()w0]sph. The ratios calculated
for the Saharan dust analog at l = 0.55 mm are shown in Figure 4a.
Here we assumed that dust composition is known (i.e., the optical
properties of CSS mixtures and the mixture of spheres were
calculated for the same refractive index). For considered dust
mixtures, the value of the optical depth would be overestimated
(up to about 1.3 times) from ground based measurements (such as
sun aureole measurements) and underestimated (
2 times) by lidars
or by satellites (at scattering angles higher than about 130), if the
spherical particle assumption were used in the retrievals. This raises
a problem in validating satellite retrievals against surface observa-
tions, especially against lidars and sun aureole data.
[14] It has been suggested that collocated satellite and ground-
based observations can be used to retrieve the single scattering
Figure 3. The differences in optical depth between CSS albedo from satellite observations by utilizing the aerosol optical
distributions and volume-equivalent spheres at l = 0.55 mm for depth provided by sunphotometers (or lidars) [Kaufman et al.,
the Saharan dust analog. 2001]. If the ‘‘true’’ optical depth is known from sunphotometer
measurements (i.e., from measurements of direct solar radiation),
then the errors in w0 retrievals would depend on the ratio of the
scattering phase functions P()CSS/P()sph. Because the above
CSS 1, 2, and 3 distributions, calculated under the assumption that ratio is similar to one shown in Figure 4(a), one can expect that w0
the particle thickness is equal to its width [Buseck and Posfai, would be underestimated from satellite observations at the back-
1999], are somewhat similar for both types of absorption. The scattering angles  > 150 but w0 can be under or overestimated
phase function of the CSS4 distribution, calculated using the between 130 – 150. If one uses the optical depth retrieved from
statistical thickness and circularity distribution reported by Okada the lidars, the satellite retrievals overestimate w0 for  < 150.
et al. [2001], has the lowest backscattering. The statistical distri-
bution of the particle thickness used for the CSS4 distribution is the
only one that we are aware of, and the measurement technique
might be limited by an inability to determine a particle thickness of
the very thin particles. Nevertheless, the common features of all
CSS distributions of dust samples considered here are that their
scattering phase functions are larger than those of volume-equiv-
alent spheres or ellipses at the forward scattering angles ( < 10)
and are smaller at the backscattering angles ( > 150 for CSS
1, 2, and 3, and  > 130 for CSS4). Although the low backscattering
by nonspherical particles have been already reported by previous
studies [Yang et al., 2000], our study shows that the magnitude of
nonspherical-spherical differences strongly depends on the degree
of particle irregularity, as well as on dust particle composition.
[11] Along with the differences in the scattering phase func-
tions, the nonspherical-spherical differences in the extinction
coefficient (and optical depth), single scattering albedo and asym-
metry parameter are also important. Table 1 shows w0, g, and kext
(normalized to 1 particle per cm3, units 103cm3/km) for the
considered CSS distributions and for equal-volume spheres. In
general, w0, g, and kext of CSS distributions are larger than those of
spheres.
[12] The nonspherical-spherical differences in w0 increase with
increasing absorption. In the case of Saharan dust, these differences
could change the dust radiative effect from the heating (if equal-
volume spheres are used) to the cooling (if w0 are calculated for
CSS distributions), depending on the surface albedo and sun angle.
In turn, larger values of the extinction coefficient result in the
larger optical depth of a dust layer of realistic dust mixtures
compared to the dust mixture of spherical particles for the same
dust loading. To illustrate, Figure 3 shows the nonspherical-
spherical differences in the optical depth (1km dust layer) at
0.55 mm calculated for the Saharan dust analog. For the particle
number concentration of 1000 cm3 (representative of dust-storm
conditions), CSS3 and CSS4 differ
30% from the equal-volume
spheres (
t = 0.56, tsph = 1.89). In addition, the differences in the
extinction coefficient can hamper the interpretation of visibility
degradation. Visibility observations are often used to evaluate the
aerosol concentration and vertical distribution.
[13] The single scattering approximation is often employed in Figure 4. Ratios of scattered intensities for the Saharan dust
satellite retrievals of aerosol optical depth. To estimate the accu- analog at l = 0.55 mm: (a) ½PðÞw0 CSS ; (b) ½PðÞCSSt lidar .
½PðÞw0 sph ½PðÞtsph
38 - 4 KALASHNIKOVA AND SOKOLIK: OPTICAL PROPERTIES OF NONSPHERICAL MINERALS
Figure 4b demonstrates this effect. Here we assumed that the
optical depth retrieved from the sunphotometer is about twice of
that retrieved from the lidar [Yoon et al., 2001]. In summary, we
conclude that it is critical to account for dust nonsphericity effects
in satellite retrieval algorithms, as well as in the validation
procedures utilizing the ground-based observations.
4. Summary
[15] Our calculations demonstrate that the scattering phase
function of nonspherical particle shapes identified in the SEM/
TEM images show distinct differences from those of spheres and
ellipses. Thin particles with angular, sharp-edge shapes are often a
dominant type. These types of particles result in the scattering
phase functions that have lower values at the backscattering angles
but higher values at forward scattering angles relative to spheres
and ellipses. In addition, these types of particles result in larger
values of the single scattering albedo, asymmetry parameter, and
extinction coefficient (and hence in aerosol optical depth). The
nonspherical-spherical differences in the single scattering albedo
increase with increasing absorption. The scattered intensities of the
irregular shapes studied here could be as much as 1.5 times larger
at forward scattering angles and as
2 times smaller at back-
scattering angles than those of volume-equivalent spheres. This
translates into an underestimation of the optical depth retrieved
from satellite and lidar observations and an overestimation of the
optical depth retrieved from forward scattered intensities measured
from the ground, if the spherical particle assumption were used in
the retrievals.
[16] Acknowledgments. This work was supported by ONR grant
N00014-98-1-0121 and NSF grant ATM-0002746.
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O. V. Kalashnikova and I. N. Sokolik, Program in Atmospheric and
Oceanic Sciences, University of Colorado, Boulder, CO 80309-0392, USA.
(kalashni@colorado.edu; sokolik@lasp.colorado.edu)