Abstract

We present effective radius, volume, surface-area, and number concentrations as well as mean complex refractive index of tropospheric particle size distributions based on lidar measurements at six wavelengths. The parameters are derived by means of an inversion algorithm that has been specifically designed for the inversion of available optical data sets. The data were taken on 20 June and on 20 July 1997 during the Aerosol Characterization Experiment ACE 2 (North Atlantic/Portugal) and on 9 August 1998 during the Lindenberg Aerosol Characterization Experiment LACE 98 (Lindenberg/Germany). Measurements on 20 June 1997 were taken in a clean-marine boundary layer, and a large value of 0.64 µm for the effective radius, a low value of 1.45 for the real part, and a negligible imaginary part of the complex refractive index were found. The single-scatter albedo was 0.98 at 532 nm. It was derived from the particle parameters with Mie-scattering calculations. In contrast, the particles were less than 0.2 µm in effective radius in a continental-polluted aerosol layer on 20 July 1997. The real part of the complex refractive index was ∼1.6; the imaginary part showed values near 0.03i. The single-scatter albedo was 0.84. On 9 August 1998 an elevated particle layer located from 3000 to 6000 m was observed, which had originated from an area of biomass burning in northwestern Canada. Here the effective radius was ∼0.24 µm, the real part of the complex refractive index was above 1.6, the imaginary part was ∼0.04i, and the single-scatter albedo was 0.81. Excellent agreement has been found with results based on sunphotometer and in situ measurements that were performed during the field campaigns.

© 2000 Optical Society of America

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2000

A. Ansmann, D. Althausen, U. Wandinger, K. Franke, D. Müller, F. Wagner, J. Heintzenberg, “Vertical profiling of the Indian aerosol plume with six-wavelength lidar during INDOEX: a first case study,” Geophys. Res. Lett. 27, 963–966 (2000).
[CrossRef]

1999

1998

J.-L. Jaffrezo, C. I. Davidson, H. D. Kuhns, M. H. Bergin, R. Hillamo, W. Maenhaut, J. W. Kahl, J. M. Harris, “Biomass burning signatures in the atmosphere of central Greenland,” J. Geophys. Res. 103, 31,067–31,078 (1998).
[CrossRef]

1996

B. E. Anderson, W. B. Grant, G. L. Gregory, E. V. Browell, J. E. Collins, G. W. Sachse, D. B. Bagwell, C. H. Hudgins, D. R. Blake, N. J. Blake, “Aerosols from biomass burning over the tropical South Atlantic region: distributions and impacts,” J. Geophys. Res. 101, 24,117–24,137 (1996).
[CrossRef]

J. Heintzenberg, H.-F. Graf, R. J. Charlson, P. Warneck, “Climate forcing and the physico-chemical life cycle of the atmospheric aerosol—Why do we need an integrated interdisciplinary global research programme?” Contrib. Atmos. Phys. 69, 261–271 (1996).

P. K. Quinn, T. L. Anderson, T. S. Bates, R. Dlugi, J. Heintzenberg, W. von Hoyningen-Huene, M. Kulmala, P. B. Russell, E. Swietlicki, “Closure in tropospheric aerosol-climate research: a review and future needs for addressing aerosol direct shortwave radiative forcing,” Contr. Atmos. Phys. 69, 547–577 (1996).

P. Posse, W. von Hoyningen-Huene, “New method for retrieval of particle size distribution from combined data of spectral extinction and aureole scattering,” J. Aerosol Sci. 27, S567–S568 (1996).
[CrossRef]

1995

U. Leiterer, A. Naebert, T. Naebert, G. Alekseeva, “A new star photometer developed for spectral aerosol optical thickness measurements in Lindenberg,” Contrib. Atmos. Phys. 68, 133–141 (1995).

C. Liu, “Humidity effect on the aerosol particle spectra in the atmospheric boundary layer,” J. Aerosol Sci. 26, 489–495 (1995).
[CrossRef]

1994

R. G. Pinnick, G. Fernandez, E. Martinez-Andazola, B. D. Hinds, A. D. A. Hansen, K. Fuller, “Aerosol in the arid southwestern United States: measurements of mass loading, volatility, size distribution, absorption characteristics, black carbon content, and vertical structure to 7 km above sea level,” J. Geophys. Res. 98, 2651–2666 (1994).
[CrossRef]

Y. J. Kaufman, A. Gitelson, A. Karnieli, E. Ganor, R. S. Fraser, T. Nakajima, S. Mattoo, B. N. Holben, “Size distribution and scattering phase function of aerosol particles retrieved from sky brightness measurements,” J. Geophys. Res. 99, 10,341–10,356 (1994).
[CrossRef]

P. K. Koutsenogii, R. Jaenicke, “Number concentration and size distribution of atmospheric aerosol in Siberia,” J. Aerosol Sci. 25, 377–383 (1994).
[CrossRef]

R. F. Pueschel, J. M. Livingston, G. V. Ferry, T. E. DeFelice, “Aerosol abundances and optical characteristics in the Pacific Basin free troposphere,” Atmos. Environ. 28, 951–960 (1994).
[CrossRef]

B. Stein, M. Del Guasta, J. Kolenda, M. Morandi, P. Rairoux, L. Stefanutti, J. P. Wolf, L. Wöste, “Stratospheric aerosol size distribution from multispectral lidar measurements at Sodankylä during EASOE,” Geophys. Res. Lett. 21, 1311–1314 (1994).
[CrossRef]

W. von Hoyningen-Huene, M. Wendisch, “Variability of aerosol optical parameters by advective processes,” Atmos. Environ. 28, 923–933 (1994).
[CrossRef]

M. Wendisch, W. von Hoyningen-Huene, “Possibility of refractive index determination of atmospheric aerosol particles by ground-based solar extinction and scattering measurements,” Atmos. Environ. 28, 785–792 (1994).
[CrossRef]

I. S. Kristament, J. B. Liley, M. J. Harvey, “Aerosol variability in the vertical in the southwest Pacific,” J. Geophys. Res. 98, 7129–7139 (1994).
[CrossRef]

I. N. Tang, H. R. Munkelwitz, “Water activities, densities, and refractive indices of aqueous sulfates and sodium nitrate droplets of atmospheric importance,” J. Geophys. Res. 99, 18,801–18,808 (1994).
[CrossRef]

1993

D. Gutkowicz-Krusin, “Multiangle lidar performance in the presence of horizontal inhomogeneities in atmospheric extinction and scattering,” Appl. Opt. 32, 3266–3272 (1993).
[CrossRef] [PubMed]

J. D. Lindberg, R. E. Douglass, D. M. Garvey, “Carbon and the optical properties of atmospheric dust,” Appl. Opt. 32, 6077–6086 (1993).
[CrossRef] [PubMed]

D. S. Covert, J. Heintzenberg, “Size distribution and chemical properties of aerosol at Ny Ålesund, Svalbard,” Atmos. Environ. 27 Part A 2989–2997 (1993).

T. R. Karl, P. D. Jones, R. W. Knight, G. Kukla, N. Plummer, V. Razovayev, K. P. Gallo, J. Lindseay, R. J. Charlson, T. C. Peterson, “A new perspective on recent global warming,” Bull. Am. Meteorol. Soc. 74, 1007–1023 (1993).
[CrossRef]

T. Deshler, B. J. Johnson, W. R. Rozier, “Balloonborne measurements of Pinatubo aerosol during 1991 and 1992 at 41 °N: vertical profiles, size distribution, and volatility,” Geophys. Res. Lett. 20, 1435–1438 (1993).
[CrossRef]

J. T. Kiel, B. P. Briegleb, “The relative roles of sulfate aerosols and greenhouse gases,” Science 260, 311–314 (1993).
[CrossRef]

1992

J. E. Penner, R. E. Dickinson, C. A. O’Neill, “Effects of aerosols from biomass burning on the global radiation budget,” Science 256, 1432–1434 (1992).
[CrossRef] [PubMed]

R. J. Charlson, S. E. Schwartz, J. M. Hales, R. D. Cess, J. A. Coakley, J. E. Hansen, D. J. Hofmann, “Climate forcing by anthropogenic aerosols,” Science 255, 423–430 (1992).
[CrossRef] [PubMed]

A. Ansmann, U. Wandinger, M. Riebesell, C. Weitkamp, E. Voss, W. Lahmann, W. Michaelis, “Combined Raman elastic-backscatter lidar for vertical profiling of moisture, aerosol extinction, backscatter, and lidar ratio,” Appl. Phys. B 55, 18–28 (1992).
[CrossRef]

M. Wendisch, W. von Hoyningen-Huene, “Optically equivalent refractive index of atmospheric aerosol particles,” Contr. Atmos. Phys. 65, 293–308 (1992).

J. B. Gillespie, J. D. Lindberg, “Seasonal and geographic variations in imaginary refractive index of atmospheric particulate matter,” Appl. Opt. 31, 2107–2111 (1992).
[CrossRef] [PubMed]

J. B. Gillespie, J. D. Lindberg, “Ultraviolet and visible imaginary refractive index of strongly absorbing atmospheric particulate matter,” Appl. Opt. 31, 2112–2115 (1992).
[CrossRef] [PubMed]

A. Ansmann, M. Riebesell, U. Wandinger, C. Weitkamp, W. Michaelis, “Independent measurement of extinction and backscatter profiles in cirrus clouds by using a combined Raman elastic-backscatter lidar,” Appl. Opt. 29, 3266–3272 (1992).

1990

A. Ansmann, M. Riebesell, C. Weitkamp, “Measurements of atmospheric aerosol extinction profiles with a Raman lidar,” Opt. Lett. 15, 746–748 (1990).
[CrossRef] [PubMed]

T. Hayasaka, T. Nakajima, M. Tanaka, “The coarse particle aerosols in the free troposphere around Japan,” J. Geophys. Res. 95, 14,039–14,047 (1990).
[CrossRef]

M. Tanaka, T. Hayasaka, T. Nakajima, “Airborne measurements of optical properties of tropospheric aerosols over an urban area,” J. Meteorol. Soc. Jpn. 68, 335–345 (1990).

1989

1985

1984

F. G. Fernald, “Analysis of atmospheric lidar observations: some comments,” Appl. Opt. 23, 652–653 (1984).
[CrossRef] [PubMed]

E. M. Patterson, C. K. McMahon, “Absorption characteristics of forest fire particulate matter,” Atmos. Environ. 18, 2541–2551 (1984).
[CrossRef]

1983

1982

1981

1980

J. K. Agarwal, C. J. Sem, “Continuous flow, single-particle-counting condensation nucleus counter,” J. Aerosol. Sci. 11, 343–357 (1980).
[CrossRef]

1979

G. H. Golub, M. Heath, G. Wahba, “Generalized cross-validation as a method for choosing a good ridge parameter,” Technometrics 21, 215–223 (1979).
[CrossRef]

P. Craven, G. Wahba, “Smoothing noisy data with spline functions: estimating the correct degree of smoothing by the method of generalized cross-validation,” Numer. Math. 31, 377–403 (1979).
[CrossRef]

1977

1975

E. O. Knutson, K. T. Whitby, “Aerosol classification by electric mobility: apparatus, theory, and applications,” J. Aerosol. Sci. 6, 443–451 (1975).
[CrossRef]

1972

1969

S. H. Melfi, J. D. Lawrence, M. P. McCormick, “Observation of Raman scattering by water vapor in the atmosphere,” Appl. Phys. Lett. 15, 295–297 (1969).
[CrossRef]

J. A. Cooney, J. Orr, C. Tomasetti, “Measurements separating the gaseous and aerosol components of laser atmospheric backscatter,” Nature 224, 1098–1099 (1969).
[CrossRef]

Agarwal, J. K.

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A. Ansmann, D. Althausen, U. Wandinger, K. Franke, D. Müller, F. Wagner, J. Heintzenberg, “Vertical profiling of the Indian aerosol plume with six-wavelength lidar during INDOEX: a first case study,” Geophys. Res. Lett. 27, 963–966 (2000).
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D. Müller, F. Wagner, D. Althausen, U. Wandinger, A. Ansmann, “Physical properties and radiative impact of Indian aerosol plume derived from 6-wavelength lidar observations on 25 March 1999 of Indian Ocean Experiment,” Geophys. Res. Lett. (to be published).

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T. R. Karl, P. D. Jones, R. W. Knight, G. Kukla, N. Plummer, V. Razovayev, K. P. Gallo, J. Lindseay, R. J. Charlson, T. C. Peterson, “A new perspective on recent global warming,” Bull. Am. Meteorol. Soc. 74, 1007–1023 (1993).
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T. R. Karl, P. D. Jones, R. W. Knight, G. Kukla, N. Plummer, V. Razovayev, K. P. Gallo, J. Lindseay, R. J. Charlson, T. C. Peterson, “A new perspective on recent global warming,” Bull. Am. Meteorol. Soc. 74, 1007–1023 (1993).
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B. Stein, M. Del Guasta, J. Kolenda, M. Morandi, P. Rairoux, L. Stefanutti, J. P. Wolf, L. Wöste, “Stratospheric aerosol size distribution from multispectral lidar measurements at Sodankylä during EASOE,” Geophys. Res. Lett. 21, 1311–1314 (1994).
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T. R. Karl, P. D. Jones, R. W. Knight, G. Kukla, N. Plummer, V. Razovayev, K. P. Gallo, J. Lindseay, R. J. Charlson, T. C. Peterson, “A new perspective on recent global warming,” Bull. Am. Meteorol. Soc. 74, 1007–1023 (1993).
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Rood, M. J.

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J. Kolenda, B. Mielke, P. Rairoux, B. Stein, D. Weidauer, J. P. Wolf, L. Wöste, F. Castagnoli, M. Del Guasta, M. Morandi, V. M. Sacco, L. Stefanutti, V. Venturi, L. Zuccagnoli, “Aerosol size distribution measurements using a multispectral lidar-system,” in Lidar for Remote Sensing, R. J. Becherer, R. M. Hardesty, J. P. Meyzonette, eds., Proc. SPIE1714, 208–219 (1992).
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B. Stein, M. Del Guasta, J. Kolenda, M. Morandi, P. Rairoux, L. Stefanutti, J. P. Wolf, L. Wöste, “Stratospheric aerosol size distribution from multispectral lidar measurements at Sodankylä during EASOE,” Geophys. Res. Lett. 21, 1311–1314 (1994).
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J. Kolenda, B. Mielke, P. Rairoux, B. Stein, D. Weidauer, J. P. Wolf, L. Wöste, F. Castagnoli, M. Del Guasta, M. Morandi, V. M. Sacco, L. Stefanutti, V. Venturi, L. Zuccagnoli, “Aerosol size distribution measurements using a multispectral lidar-system,” in Lidar for Remote Sensing, R. J. Becherer, R. M. Hardesty, J. P. Meyzonette, eds., Proc. SPIE1714, 208–219 (1992).
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B. Stein, M. Del Guasta, J. Kolenda, M. Morandi, P. Rairoux, L. Stefanutti, J. P. Wolf, L. Wöste, “Stratospheric aerosol size distribution from multispectral lidar measurements at Sodankylä during EASOE,” Geophys. Res. Lett. 21, 1311–1314 (1994).
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J. Kolenda, B. Mielke, P. Rairoux, B. Stein, D. Weidauer, J. P. Wolf, L. Wöste, F. Castagnoli, M. Del Guasta, M. Morandi, V. M. Sacco, L. Stefanutti, V. Venturi, L. Zuccagnoli, “Aerosol size distribution measurements using a multispectral lidar-system,” in Lidar for Remote Sensing, R. J. Becherer, R. M. Hardesty, J. P. Meyzonette, eds., Proc. SPIE1714, 208–219 (1992).
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P. K. Quinn, T. L. Anderson, T. S. Bates, R. Dlugi, J. Heintzenberg, W. von Hoyningen-Huene, M. Kulmala, P. B. Russell, E. Swietlicki, “Closure in tropospheric aerosol-climate research: a review and future needs for addressing aerosol direct shortwave radiative forcing,” Contr. Atmos. Phys. 69, 547–577 (1996).

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T. Hayasaka, T. Nakajima, M. Tanaka, “The coarse particle aerosols in the free troposphere around Japan,” J. Geophys. Res. 95, 14,039–14,047 (1990).
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M. Tanaka, T. Hayasaka, T. Nakajima, “Airborne measurements of optical properties of tropospheric aerosols over an urban area,” J. Meteorol. Soc. Jpn. 68, 335–345 (1990).

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I. N. Tang, H. R. Munkelwitz, “Water activities, densities, and refractive indices of aqueous sulfates and sodium nitrate droplets of atmospheric importance,” J. Geophys. Res. 99, 18,801–18,808 (1994).
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Thomalla, E.

Tomasetti, C.

J. A. Cooney, J. Orr, C. Tomasetti, “Measurements separating the gaseous and aerosol components of laser atmospheric backscatter,” Nature 224, 1098–1099 (1969).
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N. C. Hsu, J. R. Herman, J. F. Gleason, O. Torres, C. J. Seftor, “Satellite detection of smoke aerosols over a snow/ice surface by TOMS,” Geophys. Res. Lett. 26, 1165–1168 (1999).
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J. Kolenda, B. Mielke, P. Rairoux, B. Stein, D. Weidauer, J. P. Wolf, L. Wöste, F. Castagnoli, M. Del Guasta, M. Morandi, V. M. Sacco, L. Stefanutti, V. Venturi, L. Zuccagnoli, “Aerosol size distribution measurements using a multispectral lidar-system,” in Lidar for Remote Sensing, R. J. Becherer, R. M. Hardesty, J. P. Meyzonette, eds., Proc. SPIE1714, 208–219 (1992).
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P. K. Quinn, T. L. Anderson, T. S. Bates, R. Dlugi, J. Heintzenberg, W. von Hoyningen-Huene, M. Kulmala, P. B. Russell, E. Swietlicki, “Closure in tropospheric aerosol-climate research: a review and future needs for addressing aerosol direct shortwave radiative forcing,” Contr. Atmos. Phys. 69, 547–577 (1996).

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Wagner, F.

A. Ansmann, D. Althausen, U. Wandinger, K. Franke, D. Müller, F. Wagner, J. Heintzenberg, “Vertical profiling of the Indian aerosol plume with six-wavelength lidar during INDOEX: a first case study,” Geophys. Res. Lett. 27, 963–966 (2000).
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A. Ansmann, D. Althausen, U. Wandinger, K. Franke, D. Müller, F. Wagner, J. Heintzenberg, “Vertical profiling of the Indian aerosol plume with six-wavelength lidar during INDOEX: a first case study,” Geophys. Res. Lett. 27, 963–966 (2000).
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Manufactured by Particle Measuring Systems, Inc., Boulder, Colo.

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Figures (7)

Fig. 1
Fig. 1

(a) Mean profiles of the backscatter coefficients on 20 June for the time period from 2:40 to 4:40 UTC. For the retrieval the Klett method was used. The error bars denote sums of statistical and systematic error. The range resolution is 30 m. (b) Mean profile of the backscatter coefficient at 532 nm obtained by applying the Raman-lidar technique and of the relative humidity based on Raman measurements and respective temperature data from radiosonde. In the case of the backscatter coefficient the error bars denote the statistical error. The range resolution is 30 m. With respect to the relative humidity profile, the error is the sum of statistical uncertainty and calibration error. The smoothing length was set to 180 m. (c) Spectral optical thickness on 20 June 1997 from scanning lidar measurements for the time period from 2:40 to 4:40 UTC, from sunphotometer measurements from 6:00 to 7:00 UTC, and from starphotometer measurements from 23:11 to 1:10 UTC at the lidar field site. The error bars are the sums of systematic and statistical uncertainty.

Fig. 2
Fig. 2

(a) Mean profiles of the backscatter coefficients on 20 July for the time period from 3:53 to 4:53 UTC. The Klett method was used for the retrieval. The range resolution of the unsmoothed profiles is 50 m. (b) Mean profile of the backscatter coefficient at 532 nm obtained by applying the Raman-lidar method and of the relative humidity based on Raman measurements and respective temperature data from radiosonde. Because of signal noise, no values for the relative humidity are available above 3000 m. The range resolution of the unsmoothed backscatter coefficient is 50 m. With respect to the relative humidity profiles, the smoothing length was ∼600 m. (c) Spectral optical thickness on 20 July 1997 from sunphotometer measurements at the lidar field site and at a height of 900 m atop Mt. Foia, 50 km to the northeast of the field site. The data were taken from 6:00 to 8:00 UTC. Also shown is the optical thickness at 532 nm derived from the extinction profile based on the Raman-lidar method from 2:40 to 4:40 UTC for the altitude range 900–3000 m. For the meaning of the error bars see Fig. 1.

Fig. 3
Fig. 3

(a), (b) Spectral backscatter and extinction coefficients from 20 June that were used in the inversion procedure. The backscatter coefficients on 20 June were taken for a height of 375 m. The value at 355 nm was obtained by extrapolation of the backscatter spectrum with a logarithmic spline. The extinction coefficients were taken from the optical thickness data from the scanning method, divided by the marine boundary layer height of 525 ± 25 m. (c), (d) Spectral backscatter and extinction coefficients from 20 July that were used in the inversion procedure. The backscatter coefficients represent the average of the values for the two altitude ranges from 900 to 2300 m and from 2300 to 3000 m; see Fig. 2(a). The values at 355 and 1064 m were obtained from extrapolation with a logarithmic spline (thin solid and thin dashed curves, respectively). The extinction coefficients (open squares) at 355 and 532 nm are based on the spectral optical thickness data from the sunphotometer atop Mt. Foia; see Fig. 2(c). The extinction coefficients were obtained through linear interpolation of the optical thickness spectrum and with the layer height of 2100 m taken into account. Also shown is the respective extinction coefficient from the Raman-lidar method (open diamond).

Fig. 4
Fig. 4

Solution space for the complex refractive index based on the number of accepted inversion windows in the inversion process for (a) 20 June 1997 and (b) 20 July 1997. The values have been normalized to the total number of solutions and in each case represent the relative probability that the refractive index is the correct solution.

Fig. 5
Fig. 5

Vertical profiles of the backscatter coefficient at 532 nm and of the relative humidity determined with the Raman-lidar method in combination with temperature data from a radiosonde on 9 August 1998. The lidar observations were taken from 20:00 to 22:00 UTC. Because of signal noise, no values for the relative humidity are available above approximately 5000 m. In the case of the backscatter coefficient the error bars denote the statistical error. With respect to the relative humidity profile, the error is the sum of statistical uncertainty and calibration error.

Fig. 6
Fig. 6

(a) Spectral backscatter and (b) extinction coefficients on 9 August 1998 that were used in the inversion procedure. The respective data are based on profiles of the six backscatter coefficients and the extinction coefficients at 355 and 532 nm taken from 20:00 to 22:00 UTC.3 The 2-h mean backscatter and extinction coefficients represent the average values from 3600- to 4300-m height. Also shown are the backscatter and extinction coefficients based on Mie-scatter calculations with the particle size distributions taken in situ and under the assumption of different refractive indices. The error bars represent the variability of the different results.

Fig. 7
Fig. 7

Solution space for the complex refractive index based on the number of accepted inversion windows in the inversion process for the data of 9 August 1998. The values have been normalized to the total number of solutions and in each case represent the relative probability that the complex refractive index is the correct solution.

Tables (2)

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Table 1 Physical Particle Parameters from the Inversion of the ACE 2 lidar and sunphotometer data on 20 June 1997 (Clean-Marine Case) and on 20 July 1997 (Continental-Polluted Case)a

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Table 2 Physical Particle Parameters from Inversion of the LACE-98 Lidar Data and from in situ Measurements of Particle Size Distributions by a Passive Cavity Aerosol Spectrometer Probe Aboard an Aircraft on 9 August 1998a

Equations (1)

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giλ=0 Kir, m, λ, s34r vrdr,  i=α, β,

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