The Extinction-to-Backscatter Ratio of Tropospheric Aerosol: A Numerical Study
The Extinction-to-Backscatter Ratio of Tropospheric Aerosol: A Numerical Study
The Extinction-to-Backscatter Ratio of Tropospheric Aerosol: A Numerical Study
ABSTRACT
An adequate estimation of the aerosol extinction-to-backscatter ratio S is important for solving the under-
determined single scattering lidar equation and for investigating the climate impact of aerosols. In this study,
the extinction-to-backscatter ratios for the Nd:YAG wavelengths are calculated for continental, maritime, and
desert aerosols; the corresponding aerosol components are varied within the expected natural variabilities of the
particle number mixing ratios.
For continental aerosol, S increases with the relative humidity f from 40 to 80 sr. For maritime aerosol, the
extinction-to-backscatter ratios lie between 15 and 30 sr for 355 and 532 nm and between 25 and 50 sr for 1064
nm. The desert aerosol exhibits a weak dependence of S on f and ranges between 42 and 48 sr for 355 nm and
between 17 and 25 sr for 532 and 1064 nm. For practical applications, the calculated values of S are fitted by
a power series expansion with respect to their dependence on f.
the physical–chemical properties and the size distribu- bining Eqs. (1) and (2), the lognormal distribution can
tion of the aerosol particles along the lidar line are be expressed by
known. However, the fulfillment of these requirements
would make the lidar measurements unnecessary. Thus,
the lidar ratio must be estimated with respect to the
measurement site and to any available a priori infor-
n i(r) 5
Ntot m i
(2p)1/2 lns i r
exp
2 ln 2s i[
2ln 2 (r/r m,i )
OE Q
`
systematic and extensive numerical investigation about M
the lidar ratio of tropospheric aerosols. The physical Ext, i (r, m i , l)pr 2 n i (r) dr
i51
OE Q
0
basis and the input data are presented in sections 2 and S5 , (5)
`
3, respectively. The results for the different aerosol types M
are discussed separately in sections 4 to 6, whereby the Back,i (r, m i , l)pr n i (r) dr
2
i51 0
main emphasis is put on the calculation of the lidar ratio
for varying aerosol components and different relative where the numerator expresses the extinction contri-
humidities. bution a i and the denominator the backscatter contri-
bution b i , that is,
2. Physical basis
In the following considerations, it is assumed that the
EO ` M
i51
a i dr
EO
0
aerosol is an external mixture of internally mixed com- S5 ` M
. (6)
ponents. Each aerosol component (index i) is lognor- b i dr
mally distributed with respect to the particle radius r: 0 i51
n i (r) 5
(2p)
1/2
Ni
lns i r [
exp 2
2 ln 2s i ]
ln 2 (r/r m,i )
(1)
Figure 1 illustrates an example for the calculation of
the lidar ratio. A continental aerosol, which consists of
the three components water soluble, soot, and insoluble,
is chosen (Fig. 1a). The relative humidity, which influ-
where N i is the number density of the component, and
r m,i and s i denote the median radius and the standard ences the microphysical properties of the water soluble
deviation of n i (r), respectively. component, is assumed to be 90%, and the wavelength
The number mixing ratio m i (i.e., the normalized num- of the incident light is 532 nm.
ber particle concentration) is defined as With knowledge of the refractive indices, the extinc-
tion efficiencies and backscatter efficiencies are calcu-
Ni Ni lated. These quantities are weighted with the size dis-
mi 5 5
ON
M . (2)
Ntot tribution of the corresponding aerosol component. To
i51
i obtain the extinction and backscattering for a distinct
particle radius, the contributions of the three aerosol
Here, M is the number of aerosol components and Ntot components are summed. The resulting curves are plot-
is the total number of particles per unit volume. Com- ted in Fig. 1b. From the maxima of the curves note that,
AUGUST 1998 NOTES AND CORRESPONDENCE 1045
TABLE 1. The real parts (h) and imaginary parts (k) of the refractive indices for the aerosol components used in this study. The
subscripts denote the three considered wavelengths in nanometers.
TABLE 2. The parameters of the lognormal distributions for different relative humidities of the aerosol components used in this study. The
unity of rm is in micrometers (Hess et al. 1998).
that the sum of these mixing ratios equals 1. In the continental areas. The high soot content of 0.9 is of the
following, the mixing ratios for water soluble, insoluble, same order of magnitude as the value of 0.823 proposed
and soot particles are denoted m1 , m 2 , and m 3 , respec- by Hess et al. (1998) for the aerosol type ‘‘urban.’’
tively. To respect the influence of the relative humidity f on
The mixing ratio m1 is varied between 0.1 and 1 in the water soluble component and hence on the lidar
steps of 0.1. Accordingly, since m 2 is about four orders ratio, the calculations are performed for relative hu-
less, m 3 has values between 0.9 and 0. To account for midities of 0%, 50%, 70%, 80%, 90%, 95%, 98%, and
the influence of the insoluble component, m 2 is varied 99%, respectively.
between 6 3 1026 and 6 3 1025 in steps of 6 3 1026 . Figure 2 shows the calculated mean lidar ratios Ŝ and
Compared to the composition of the standard aerosol the deviations from Ŝ for relative humidities of 0%,
types proposed by Hess et al. (1998), it is expected that 50%, 90%, and 99%, and for the wavelengths 355, 532,
the choice of these 100 different combinations covers and 1064 nm, respectively. These nine contour plots
the high variability of the aerosol that can occur over enable us to investigate in detail the influence of the
three aerosol components on the values of S.
For all three wavelengths, the variabilities of S have
their maxima at f 5 0%. In particular, a high soot con-
tent can cause large positive deviations of the lidar ratio
from its mean value. This result is due to the large
imaginary part of the refractive index and hence the
extinction of these particles. For 1064 nm, this effect
can be compensated or even exceeded by a high amount
of insoluble particles (see Fig. 2 at the lower left).
The contributions of the three different components
to the lidar ratio can be estimated from the slopes of
the isolines in Fig. 2. When the absolute of the slopes
is near zero, the influence of the mixing ratios of soot
and water soluble particles is small, whereas when the
absolute of the slopes grows to infinity, the insoluble
component has hardly any influence on S. Thus, the
mixing ratio of the insoluble particles has for all relative
humidities a small influence on the lidar ratio for 355
nm. In contrast, the change of the insoluble component
plays the dominant role for the variability of the lidar
ratio at 1064 nm.
The standard deviation s of the lidar ratio is calculated
for each wavelength and relative humidity. The result
is shown in Fig. 3. The error bars of length 2s at a
definite relative humidity must be regarded as the vari-
ability of the lidar ratio driven by the assumption made
on the variability of the distinct values of m1 , m 2 , and
FIG. 2. Deviations of the calculated lidar ratios from the mean m3.
values of Ŝ for 355, 532, and 1064 nm and relative humidities of 0%, Since the water soluble component is the only com-
50%, and 90%. The dotted, dashed, and full lines indicate negative,
zero, and positive deviations from Ŝ, respectively, and the contour
ponent whose properties are affected by the relative hu-
interval is 1 sr. The mixing ratios of the four standard aerosol types midity, all variations of Ŝ and s with respect to their
proposed by Hess et al. (1998) are shown by open symbols. values for f 5 0% are considered as variations of the
AUGUST 1998 NOTES AND CORRESPONDENCE 1047
614% and 618%; for 532 nm, they lie between 68% Ŝ( f ) ø j
j21
, (7)
j51
and 613%; and for 1064 nm, the corresponding values
are 61% and 65%. with a j the polynomial coefficients and J the total num-
ber of the coefficients. The value of J is found by min-
imizing a least squares merit function (Press et al. 1992)
6. Desert aerosol
and varies between 5 and 10 depending on the shape
The desert aerosol originates from desert areas and of the original function. The resulting coefficients are
mainly consists of the water soluble component and the listed in Table 3.
nucleation, accumulation, and coarse particle mode of To compare the polynomial fit with the input data,
minerals. Since the mineral components do not change the fitted curves and the computed values of Ŝ( f ) are
their physical–chemical properties with relative humid- plotted in Figs. 3–5 for continental, maritime, and desert
ity, all changes of the lidar ratio of desert aerosol with aerosol, respectively. In all cases, the curves lie within
the relative humidity result from the water soluble com- the error bars of the computed lidar ratios, indicating
ponent. that the power series expansions are mathematically suf-
The calculation of the lidar ratios is performed in the ficiently accurate.
same manner as described in section 4. For the com- A comparison between these results and the outcomes
putations, the water soluble component varies between of the experimental studies mentioned in section 1 is
0.6 and 0.9 (step width: 0.1), the mineral accumulation rather difficult because of the different wavelengths used
mode ranges from 1 3 1022 to 4 3 1022 (step width: and in most cases the lack of information about the
1 3 1022 ), and the mineral coarse mode lies between variability of the considered aerosols with relative hu-
5 3 1025 and 8 3 1025 (step width: 1 3 1025 ). The midity.
mixing ratio of the mineral nucleation mode is chosen For continental aerosols, Salemink et al. (1984) report
to sum up the total mixing ratio to 1. a stronger dependence of S on f, but their absolute val-
The calculated lidar ratios and their standard devia- ues (25–70 sr) do not disagree with the values deter-
tions are summarized in Fig. 5. The values of Ŝ for 355 mined in this study. The data of Takamura et al. (1994)
nm are about twice the values for 532 and 1064 nm. do not conflict with the results of this study, even if
Similar to the dominance of the accumulation mode of they determined low values of about 20 sr, too. The
sea salt for the lidar ratio of maritime aerosol, the lidar values of Waggoner et al. (1972) seem to be very high,
ratio of desert aerosol is governed by the mineral ac- even when a large soot content is assumed. Low values
AUGUST 1998 NOTES AND CORRESPONDENCE 1049
1022
1023
1025
1027
101
numerical study of McCormick et al. (1968), which ne-
1064 nm
1.706 3
22.101 3
1.263 3
22.411 3
1.480 3
glected the wavelength dependence and the imaginary
0.
0.
0.
0.
0.
part of the refractive index (i.e., absorption) and as-
sumed a Junge size distribution.
By a minimum search technique, Sasano and Browell
(1989) determined the lidar ratio of maritime aerosol
1022
1023
1025
1027
101 from multiple wavelength lidar observations. For 300
532 nm
Desert
1.993 3
24.398 3
2.865 3
25.518 3
3.430 3
nm, they reported values ranging from 5.1 to 19.4 sr,
0.
0.
0.
0.
0.
which are somewhat lower than the values given in this
study for 355 nm. However, from the wavelength de-
pendence of S shown in Fig. 4, it seems that calculated
values for 300 nm would lie close to the values reported
1023
1023
1025
1027
101
355 nm
fits well with the values given in Fig. 5 for dry particles.
1021
1022
1024
1026
1027
1029
101
Eq. (7) provides 51.9, 38.6, and 31.0 sr for 355, 532,
0.
0.
0.
0.
0.
of 50%.
0.
0.
0.
0.
0.
8. Concluding remarks
101
Continental
532 nm
4.531 3
2.628 3
23.085 3
1.334 3
22.356 3
1.412 3
doubtful even if the relative humidity along the mea- as well as for their fruitful comments. The comments
surement path is known. of the two anonymous reviewers significantly improved
First, as is clear from Fig. 2, there exist atmospheric an earlier version of the paper.
conditions and hence mixing ratio combinations whose
resulting lidar ratios differ considerably from an as- REFERENCES
sumed mean value. This is especially true for a high
soot amount and low relative humidities, as in the case Bissonnette, L. R., 1986: Sensitivity analysis of lidar inversion al-
gorithms. Appl. Opt., 25, 2122–2125.
of continental aerosol. This problem can only be elim- Bohren, C. F., and D. R. Huffman, 1983: Absorption and Scattering
inated by using larger wavelengths, where the influence of Light by Small Particles. Wiley and Sons, 530 pp.
of soot is slightly diminished. d’Almeida, G., P. Koepke, and E. P. Shettle, 1991: Atmospheric Aer-
Second, the simultaneous existence of different aero- osols: Global Climatology and Radiative Characteristics. A.
Deepak, 561 pp.
sol types in different heights above the measurement Fitzgerald, J. W., 1984: Effect of relative humidity on the aerosol
site prevents the evaluation of the lidar signal over the backscattering coefficient at 0.694- and 10.6-mm wavelengths.
whole range domain. For example, over the oceans, the Appl. Opt., 23, 411–418.
occurrence of the sea salt components is mainly limited Hänel, G., 1976: The properties of atmospheric aerosol particles as
to the PBL. Above the PBL, the aerosol composition is functions of the relative humidity at thermodynamic equilibrium
with the surrounding moist air. Advances in Geophysics, Vol.
expected to be similar to that of continental aerosol but 19, Academic Press, 73–188.
with a small amount of insoluble particles. In this case, Hess, M., P. Koepke, and I. Schult, 1998: Optical Properties of Aer-
the height of the PBL must be estimated from the lidar osols and Clouds: The software package OPAC. Bull. Amer.
signal or the relative humidity profile. Accordingly, both Meteor. Soc., 79, 831–844.
Hughes, H. G., J. A. Ferguson, and D. H. Stephens, 1985: Sensitivity
parts of the measurement path, that is, the PBL and the of a lidar inversion algorithm to parameters relating atmospheric
free troposphere, are evaluated separately. Using the backscatter and extinction. Appl. Opt.,
data of Hess et al. (1998) for a free troposphere with Klett, J. D., 1981: Stable analytical inversion solution for processing
50% relative humidity, the computed lidar ratios are lidar returns. Appl. Opt., 20, 211–220.
56.9, 58.4, and 51.3 sr for the wavelengths of 355, 532, , 1985: Lidar inversion with variable backscatter/extinction ra-
tios. Appl. Opt., 24, 1638–1643.
and 1064 nm, respectively. Kovalev, V. A., 1993: Lidar measurement of the vertical aerosol
A similar problem can occur when mineral aerosol is extinction profiles with range-dependent backscatter-to-extinc-
transported from its source in the deserts to regions tion ratios. Appl. Opt., 32, 6053–6065.
where other aerosol types are present. In that case the McCormick, M. P., J. D. Lawrence, and F. R. Crownfield, 1968: Mie
total and differential backscattering cross sections at laser wave-
mineral particles form an aerosol layer above the aerosol lengths for Junge aerosol models. Appl. Opt., 7, 2424–2425.
layer of the PBL (Hess et al. 1998). By sedimentation, Pratt, R. W., 1985: Review of radiosonde humidity and temperature
the aerosol components of both layers are externally errors. J. Atmos. Oceanic Technol., 2, 404–407.
mixed and thus the microphysical properties of the orig- Press, W. H., S. A. Teukolsky, W. T. Vetterling, and B. P. Flannery,
inal aerosol layer are considerably changed. Under these 1992: Numerical Recipes in FORTRAN. Cambridge University
Press, 963 pp.
conditions, a lidar ratio determination is ambiguous and Rosen, J. M., R. G. Pinnick, and D. M. Garvey, 1997: Measurement
useful results cannot be expected. For the mineral-trans- of the extinction-to-backscatter for near-surface aerosols. J. Geo-
ported component alone, from the data of Hess et al. phys. Res., 102, 6017–6024.
(1998), the calculated lidar ratios are 22.0 (355 nm), Salemink, H., P. Schotanus, and J. B. Bergwerff, 1984: Quantitative
lidar at 532 nm for vertical extinction profiles in the lidar so-
12.5 (532 nm), and 26.6 sr (1064 nm). lution. Appl. Phys., 34B, 187–189.
Another source of error is the inaccuracy of the rel- Sasano, Y., and E. V. Browell, 1989: Light scattering characteristics
ative humidity determined with the hygrometer of the of various aerosol types derived from multiple wavelength lidar
radiosonde. These inaccuracies are mainly caused by observations. Appl. Opt., 28, 1670–1679.
, , and S. Ismail, 1985: Error caused by using a constant
the thermal lag and the solar heating of the instrument extinction/backscattering ratio in the lidar solution. Appl. Opt.,
during the ascent. Both effects provoke an overesti- 24, 3929–3932.
mation of f, and their strength depends on the actual Shettle, E. P., and R. W. Fenn, 1979: Models for the aerosols of the
state of the atmosphere. The mean relative humidity lower atmosphere and the effects of humidity variations on their
errors are 6% between 1013 and 700 hPa and 10% be- optical properties. Air Force Geophysics Laboratory Environ-
mental Research Papers 676, AFGL-TR79-TR79-0214, 94 pp.
tween 700 and 500 hPa (Pratt 1985). Thus, especially [Available from Air Force Geophysics Laboratory, Hanscom
for large relative humidities, the accuracy of the lidar AFB, Massachusetts 01731.]
ratio determination is not only limited by insufficient a Spinhirne, J. D., J. A. Reagan, and B. M. Herman, 1980: Vertical
priori knowledge about the composition of the aerosols distribution of aerosol extinction cross section and inference of
aerosol imaginary index in the troposphere by lidar technique.
but also by the uncertainty of the relative humidity de- J. Appl. Meteor., 19, 426–438.
termination. Takamura, T., Y. Sasano, and T. Hayasaka, 1994: Tropospheric aerosol
optical properties derived from lidar, sun photometer, and optical
particle counter measurements. Appl. Opt., 33, 7132–7140.
Acknowledgments. Peter Koepke and Peter Völger Waggoner, A. P., N. C. Ahlquist, and R. J. Charlson, 1972: Mea-
from the University of Munich are gratefully acknowl- surement of the aerosol total scatter-backscatter ratio. Appl. Opt.,
edged for the delivery of aerosol data and the Mie code, 11, 2886–2889.