Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 7 11 2007 10.5194/acp-7-2797-2007 http://www.atmos-chem-phys.net/7/2797/2007/ http://www.atmos-chem-phys.net/7/2797/2007/acp-7-2797-2007.html http://www.atmos-chem-phys.net/7/2797/2007/acp-7-2797-2007.pdf 2797 2815 2007-06-06 Retrieval of aerosol complex refractive index from a synergy between lidar, sunphotometer and in situ measurements during LISAIR experiment J.-C. Raut jean-christophe.raut@cea.fr P. Chazette Laboratoire des Sciences du Climat et de l'Environnement, Laboratoire mixte CEA-CNRS-UVSQ, CEA Saclay, 91191 Gif-sur-Yvette, France Particulate pollutant exchanges between the streets and the Planetary Boundary Layer (PBL), and their daily evolution linked to human activity were studied in the framework of the LIdar pour la Surveillance de l'AIR (LISAIR) experiment. This program lasted from 10 to 30 May 2005. A synergetic approach combining dedicated active (lidar) and passive (sunphotometer) remote sensors as well as ground based in situ instrumentation (nephelometer, aethalometer and particle sizers) was used to investigate urban aerosol optical properties within Paris. Aerosol complex refractive indices were assessed to be 1.56–0.034 i at 355 nm and 1.59–0.040 i at 532 nm, thus leading to single-scattering albedo values between 0.80 and 0.88. These retrievals are consistent with soot components in the aerosol arising from traffic exhausts indicating that these pollutants have a radiative impact on climate. We also discussed the influence of relative humidity on aerosol properties. A good agreement was found between vertical extinction profile derived from lidar backscattering signal and retrieved from the coupling between radiosounding and ground in situ measurements. Ackerman, F. and Chung, H.: Radiative effects of airborne dust and regional energy budget at the top of the atmosphere, J. Appl. Meteorol., 31, 223–233, 1992. Ackerman, T. P. and Toon, O. B.: Absorption of visible radiation in atmosphere containing mixtures of absorbing and non absorbing particles, Appl. Opt., 20, 3661–3667, 1981. Anderson, T. L., Masonis, S. J., Covert, D. S., Charlson, R. J., and Rood, M. J.: In situ measurement of the aerosol extinction-to-backscatter lidar ratio at a polluted continental site, J. Geophys. Res., 105(D22), 26 907, doi:10.1029/2000JD900400, 2000. Angström, A.: The parameters of atmospheric turbidity, Tellus, 16, 64–75, 1964. Baumgardner, D. G., Raga, G. B., Kok, G., Ogren, J., Rosas, I., Baez, A., and Novakov, T.: On the evolution of aerosols properties at a mountain site above Mexico City, J. Geophys. Res., 105, 22 243–22 253, 2000. Bergin, M. H., Cass, G. R., Xu, J., Fang, C., Zeng, L. M., Yu, T., Salmon, L. G., Kiang, C. S., Tang, X. Y., Zhang, Y. H., and Chameides, W. L.: Aerosol radiative, physical, and properties in Beijing during June, 1999, J. Geophys. Res., 106, 17 969–17 980, 2001. Berthier, S., Chazette, P., Couvert, P., Pelon, J., Dulac, F., Thieuleux, F., Moulin, C., and Pain, T.: Desert dust aerosol columnar properties over ocean and continental Africa from Lidar in-Space Technology Experiment (LITE) and Meteosat synergy, J. Geophys. Res., 111(D21202), doi:10.1029/2005JD006999, 2006. Bissonnette, L. R.: Sensitivity analysis of lidar inversion algorithms., Appl. Opt., 25, 2122–2125, 1986. Bodhaine, B. A., Ahlquist, N. C., and Schnell, R. C.: Threewavelength nephelometer suitable for aircraft measurements of background aerosol scattering coefficient, Atmos. Environ., 10, 2268–2276, 1991. Bodhaine, B. A.: Aerosol absorption measurements at Barrow, Mauna Loa and the South Pole, J. Geophys. Res., 100, 8967–8975, 1995. Bond, T. C., Charleson, R. J., and Heitzenberg, J.: Quantifying the emission of light-absorbing particles: Measurements tailored to climate studies, Geophys. Res. Lett., 25, 337–340, 1998. Bond, T. C., Anderson, T. L., and Campbell, D.: Calibration and intercomparison of filter-based measurements of visible light absorption by aerosols, Aerosol Sci. Technol., 30, 582–600, 1999. Boucher, O. and Anderson, L.: General circulation model assessment of the sensitivity of direct climate forcing by anthropogenic sulfate aerosols to aerosol size and chemistry, J. Geophys. Res., 100(D12), 26 117–26 134, 1995. Cachier, H., Aulagnier, F., Sarda, R., et al.: Aerosol studies during the ESCOMPTE experiment: An overview, Atmos. Res., 74, 547–563, 2005. Carlson, T. N. and Caverly, R. S.: Radiative characteristics of Saharan dust at solar wavelengths, J. Geophys. Res., 82, 3141–3152, 1977. Carrico, C. M., Kus, P., Rood, M. J., Quinn, P. K., and Bates, T. S.: Mixtures of pollution, dust, sea salt, and volcanic aerosol during ACE-Asia: radiative properties as a function of relative humidity, J. Geophys. Res., 108(D23), 8650, doi:10.1029/2003JD003405, 2003. Cattrall, C., Reagan, J. R., Thome, K., and Dubovik, O.: Variability of aerosol and spectral lidar and backscatter and extinction ratios of key aerosol types derived from selected Aerosol Robotic Network locations, J. Geophys. Res., 110(D10S11), doi:10.1029/2004JD005124, 2005. Charlson, R. J., Schwartz, S. E., Hales, J. M., Cess, R. D., Coakley Jr., J. A., Hansen, J. E., and Hoffman, D. J.: Climate forcing by anthropogenic aerosols, Science, 255, 423–430, 1992. Chazette, P., David, C., Lefrère, J., Godin, S., Pelon, J., and Mégie, G.: Comparative lidar study of the optical, geometrical, and dynamical properties of stratospheric postvolcanic aerosols, following the eruption of El Chichon and Mount Pinatubo, J. Geophys. Res., 100(D11), 23 195–23 207, 1995. Chazette, P. and Liousse, C.: A case study of optical and chemical apportionment for urban aerosols in Thessaloniki, Atmos. Environ., 35, 2497–2506, 2001. Chazette, P., Randriamiarisoa, H., Sanak, J., Flamant, C., and Pelon, J.: Airborne lidar for the surveyof the Paris aerosol production in the frame of ESQUIF program, in: Lidar Remote Sensing in Atmospheric and Earth Sciences, vol. 1. Defence R&D Canada Valcartier, edited by: Bissonnette, L. R., Royet, G., and Vallée, G., Val-Bélair, Canada, pp. 173–175, 2002. Chazette, P.: The monsoon aerosol extinction properties at Goa during INDOEX as measured with lidar, J. Geophys. Res., 108(D6), 4187, doi:10.1029/2002JD002074, 2003. Chazette, P., Couvert, P., Randriamiarisoa, H., Sanak, J., Bonsang, B., Moral, P., Berthier, S., Salanave, S., and Toussaint, F.: Three-dimensional survey of pollution during winter in French Alps valleys, Atmos. Environ., 39, 1035–1047, 2005a. Chazette, P., Randriamiarisoa, H., Sanak, J., Couvert, P., and Flamant, C.: Optical properties of urban aerosol from airborne and ground based in situ measurements performed during the ESQUIF program, J. Geophys. Res., 110, D02206, doi:10.1029/2004JD004810, 2005b. Covert, D. S., Charlson, R. J., and Ahlquist, N. C.: A study of the relationship of chemical composition and humidity to light scattering by aerosols, J. Appl. Meteorol., 11, 968–976, 1972. Cros, B., Durand, P., Cachier, H., et al.: An overview of the ESCOMPTE campaign, Atmos. Res., 69, 3–4, 241–279, 2004. D'Almeida, G. A.: On the variability of desert aerosol radiative characteristics, J. Geophys. Res., 92, 3017–3026, 1987. D'Almeida, G. A., Koepke, P., and Shettle, E. P.: Atmospheric Aerosols – Global Climatology and Radiative Characteristics, in: Atmospheric Aerosols. Global Climatology and Radiative Characteristics, edited by: Deepak, A., Hampton, VA, USA, pp561, 1991. Dubovik, O., Smirnov, A., Holben, B. N., King, M. D., Kaufman, Y. J., Eck, T. F., and Slutsker, I.: Accuracy assessments of aerosol optical properties retrieved from AERONET sun and sky-radiance measurements, J. Geophys. Res., 105, 9791–9806, 2000. Dubovik, O., Holben, B. N., Eck, T. F., Smirnov, A., Kaufman, Y. J., King, M. D., Tanre, D., and Slutsker, I.: Variability of absorption and optical properties of key aerosol types observed in worldwide locations, J. Atmos. Sci., 59, 590–608, 2002. Durieux, E., Fiorani, L., Calpini, B., Flamm, M., Jaquet, L., and Van der Bergh, H.: Tropospheric ozone measurements over the greater Athens area during the MEDCAPHOT-TRACE campaign in Athens, Greece (20 August–20 September), Atmos. Environ., 32, 2141–2150, 1998. Dye, J. E. and Baumgardner, D.: Evaluation of the forward scattering spectrometer probe: I. Electronic and optical studies, J. Atmos. Ocean. Technol., 1, 329–344, 1984. Eleftheriadis, K., Balis, D., Colbeck, I., and Manalis, N.: Atmospheric aerosol and gaseous species in Athens, Greece, Atmos. Environ., 32, 2183–2191, 1998. Ebert, M., Weinbruch, S., Hoffmann, P., and Ortner, H. M.: The chemical composition and complex refractive index of rural and urban influenced aerosols determined by individual particle analysis, Atmos. Environ., 38, 6531–6545, 2004. Faxvog, F. R. and Roessler, D. M.: Carbon aerosol visibility vs particle size distribution, Appl. Opt., 17, 2612–2616, 1978. Ferrare, R. A., Melfi, S. H. , Whiteman, D. N., Poellot, M., and Kaufman, Y. J.: Raman lidar measurements of aerosol extinction and backscattering, 2. Derivations of aerosol real refractive index, single-scattering albedo, and humification factor using a Raman lidar and aircraft size distribution measurements, J. Geophys. Res., 103, 19 673–19 689, 1998. Flamant, C., Pelon, J., Chazette, P., Trouillet, V., Quinn, P. K., Frouin, R., Bruneau, D., Leon, J. F., Bates, T. S., Johnson, J., and Livingston, J.: Airborne lidar measurements of aerosol spatial distribution and optical properties over the Atlantic Ocean during a European pollution outbreak of ACE-2, Tellus B, 52(2), 662–677, 2000. Gasso, S., Hegg, D. A., Covert, D. S., Collins, D., Noone, K. J., Oström, E., Schmid, B., Russel, P. B., Livingston, J. M., Durkee, P. A., and Josson, H.: Influence of humidity on the aerosol scattering coefficient and its effect on the upwelling radiance during ACE-2, Tellus, 52B, 546–567, 2000. Hänel, G.: The properties of atmospheric aerosol particles as functions of the Relative humidity at thermodynamic equilibrium with the surrounding moist air, Adv. Geophys., 19, 73–188, 1976. Hamonou, E., Chazette, P., Balis, D., Dulac, F., Schneider, X., Galani, E., Ancellet, G., and Papayannis, A.: Characterization of the vertical structure of Saharan dust export to the Mediterranean basin, J. Geophys. Res., 104, 22 257–22 270, 1999. Hansen, A. D. A. and Novakov, T.: Real time measurements of aerosol black carbon during the carbonaceous species methods comparison study, Aerosol Sci. Technol., 12, 194–199, 1990. Higurashi, A. and Nakajima, T.: Detection of aerosol types over the East China Sea near Japan from four-channel satellite data, Geophys. Res. Lett., 29(17), 1836, doi:10.1029/2002GL015357, 2002. Hitzenberger, R. and Puxbaum, H.: Comparisons of the measured and calculated specific absorptiton coefficient for Vienna urban aerosols samples, Aerosol Sci. Technol., 18, 323–345, 1993. Holben, B. N., Eck, T. F., Slutsker, I., et al.: AERONET – A federated instrument network and data archive for aerosol characterisation, Rem. Sens. Environ., 66, 1–16, 1998. Hughes, H. G., Ferguson, J. A., and Stephens, D. H.: Sensitivity of a lidar inversion algorithm to parameters relating atmospheric backscatter and extinction, Appl. Opt., 24(11), 1609–1613, 1985. Ignatov, A. M., Stowe, L. L., Sakerin, S. M., and Korotaev, G. K.: Validation of the NOAA/NESDIS satellite aerosol product over the North Atlantic in 1989, J. Geophys. Res., 100, 5123–5132, 1995. Intergovernmental Panel on Climate Control (IPCC): Climate Change 2001, the Third Assessment Report of the IPCC, Cambridge Univ. Press, New York, 2001. Kambezidis, H. D., Peppes, A. A., and Melas, D.: An environmental experiment over Athens urban area under sea breeze conditions, Atmos. Res., 36, 139–156, 1995. Kaufman, Y. J., D. Tanré,Dubovik, O., Karnieli, A., and Remer, L. A.: Absorption of sunlight by dust as inferred from satellite and groundbased measurements, Geophys. Res. Lett., 28, 1479–1482, 2001. Kent, G. S., Yue, G. K., Farrukh, U. O., and Deepak, A.: Modelling atmospheric aerosol backscatter at CO2 laser wavelengths. 1: Aerosol properties, modelling techniques, and associated problems, Appl. Opt., 22, 1655–1665, 1983. Keskinen, J., Pietarinen, K., and Lehtimäki, M.: Electrical Low Pressure Impactor, J. Aerosol. Sci., 23(4), 353–360, 1992. Key, J.: Streamer User's Guide, Cooperative Institute for Meteorological Satellite Studies, University of Wisconsin, 96 pp, 2001. Kilsby C. G. and Smith M. H.: Comparison of the physical and optical properties of the atmospheric aerosol from airborne and surface measurements on the east coast of England, Atmos. Environ., 21, 2233–2246, 1987. Kitchen, M. and Squires, E. C.: Aircraft observation of solar radiation in cloud free atmosphere, Boundary-Layer Meteorol., 29, 321–342, 1984. Klett, J. D.: Stable analytical inversion solution for processing lidar returns, Appl. Opt., 20, 211–220, 1981. Klett, J. D.: Lidar inversion with variable backscatter/extinction ratios, Appl. Opt., 24, 1638–1643, 1985. Kotchenruther, R. A., Hobbs, P. V., and Hegg, D. A.: Humidification factors for atmospheric aerosol off the mid-Atlantic coast of United States, J. Geophys. Res., 104(D2), 2239–2252, 1999. Kovalev, V. A.: Lidar measurement of the vertical aerosol extinction profiles with range-dependent backscatter-to-extinction ratios, Appl. Opt., 32, 6053–6065, 1993. Landulfo, E., Papayannis, A., Artaxo, P., Castanho, A. D. A., De Freitas, A. Z., Souza, R. F., Vieira Junior, N. D., Jorge, M. P. M. P., Sanchez-Ccoyllo, O. R., and Moreira, D. S.: Synergetic measurements of aerosol over Sao Paulo, Brazil, using LIDAR, sunphotometer and satellite data during the dry season, Atmos. Chem. Phys., 3, 1523–1539, 2003. Lenoble, J.: Atmospheric Radiative Transfer, edited by: Deepak, A., Hampton VA, U.S.A., pp532, 1993. Léon, J. F., Chazette, P., Pelon, J., Dulac, F., and Ramdriamarisoa, H., Aerosol direct radiative impact over the INDOEX area based on passive and active remote sensing, J. Geophys. Res., 107(D19), 8006, doi:10.1029/2000JD000116, 2002. Liousse, C., Cachier, H., and Jennings, S. G.: Optical and thermal measurements of black carbon aerosol content in different environments: Variation of the specific attenuation cross-section, sigma, Atmos. Environ., 27A, 1203–1211, 1993. Lurmann, F. W., Wexler, A. S., Pandis, S. N., Musarra, S., Kumar, N., and Seinfeld, J. H.: Modeling urban and regional aerosols: II. Application to California's South coast air basin, Atmos. Environ., 31, 2695–2715, 1997. Mallet, M., Roger, J. C., Despiau, S., Dubovik, O., and Putaud, J. P.: Microphysical and optical properties of aerosol particles in urban zone during ESCOMPTE, Atmos. Res., 69, 73–97, 2003. Malm, W. C., Day, D. E., Kreidenweis, S. M., Collett, J. L., and Lee, T.: Humidity-dependent optical properties of fine particles during the big bend regional aerosol and visibility observational study, J. Geophys. Res., 108(D9), 4279, doi:10.1029/2002JD002998, 2003. Marley, N. A., Gaffney, J. S., Baird, J. C., Blazer, C. A., Drayton, P. J., and Frederick, J. E.: An Empirical Method for the Determination of the Complex Refractive Index of Size-Fractionated Atmospheric Aerosols for Radiative Transfer Calculations, Aerosol Sci. Technol., 34, 535–549, 2001. Measures, R. M.: Laser Remote Sensing, Wiley-Interscience, New York, pp217, 1984. Menut, L., Flamant, C., Pelon, J., and Flamant, P. H.: Urban boundary layer height determination from lidar measurements over the Paris area, Appl. Opt., 38(6), 945–954, 1999. Menut, L., Vautard, R., Flamant, C., et al.: Measurements and modeling of atmospheric pollution over the Paris area: An overview of the ESQUIF project, Ann. Geophys., 18(11), 1467–1481, 2000. Moores W. H.: Direct measurements of radiative and turbulent flux convergence in the lowest 1000 m of the convective boundary layer, Boundary Layer Meteorol., 22 283–22 294, 1982. Moulin, C., Dulac, F., Lambert, C. E. , Chazette, P., Jankowiak, I., Chatenet, B., and Lavenu, F.: Long-term daily monitoring of Saharan dust load over ocean using Meteosat ISCCP-B2 data 2. Accuracy of the method and validation using sun photometer measurements, J. Geophys. Res., 102, 16 959–16 969, 1997. Müller, D., Wandinger, U., and Ansmann, A.: Microphysical particle parameters from extinction and backscatter lidar data by inversion with regularization: Theory, Appl. Opt., 38, 2346–2357, 1999. Müller, D., Ansmann, A., Wagner, F., Franke, K., and Althausen, D.: European pollution outbreaks during ACE 2: Microphysical particle properties and single-scattering albedo inferred from multiwavelength lidar observations, J. Geophys. Res., 107(D15), 4248, doi:10.1029/2001JD001110, 2002. Ouimette, J. R. and Flagan, R. C.: The extinction coefficient of multicomponent aerosols, Atmos. Environ., 16, 2405–2419, 1982. Patterson, E. M., Gillete, D. A., and Stockton, B. H.: Complex index of refraction between 300 and 700 nm for Saharan aerosol, J. Geophys. Res., 82, 3153–3160, 1977. Penner, J. E., Charlson, R. J., Hales, J. M., Laulainen, N. S., Leifer, R., Novakov, T., Ogren, J., Radke, L. F., Schwartz, S. E., and Travis, L.: Quantifying and minimizing uncertainty of climate forcing by anthropogenic aerosols, Bull. Am. Meteorol. Soc., 75, 375–400, 1994. Quinn, P. K. and Coffman, D. J.: Local closure during the First Aerosol Characterization Experiment (ACE1): aerosol mass concentration and scattering and backscattering coefficients, J. Geophys. Res., 103, 15 575–15 596, 1998. Randriamiarisoa H., Chazette, P., and Mégie, G.: The columnar retrieved single scattering albedo from NO2 photolysis rate, Tellus B, 56, 118–127, 2004. Randriamiarisoa, H., Chazette, P., Couvert, P., Sanak, J., and Mégie, G.: Relative humidity impact on aerosol parameters in a Paris suburban area, Atmos. Chem. Phys., 6, 1389–1407, 2006. Ross, J. L., Hobbs, P. V., and Holben, B.: Radiative characteristics of regional hazes dominated by smoke from biomass burning in Brazil: Closure tests and direct radiative forcing, J. Geophys. Res., 103(D24), 31 925–31 941, 1998. Sasano, Y., Browell, E. V., and Ismail, S.: Error caused by using a constant extinction/backscattering ratio in the lidar solution, Appl. Opt., 24, 3929–3932, 1985. Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics, John Wiley & Sons, New York, 408–440, 1998. Sicard, M., Chazette, P., Pelon, J., Won, J. G., and Yoon, S. C.: Variational method for the retrieval of the optical thickness and the backscatter coefficient from multiangle lidar profiles, Appl. Opt., 41, 493–502, 2002. Sinyuk, A., Torres, O., and Dubovik, O.: Combined use of satellite and surface observations to infer the imaginary part of refractive index of Saharan dust, Geophys. Res. Lett., 30(2), 1081, doi:10.1029/2002GL016189, 2003. Sokolik, I. N., Andronova, A., and Johnson, T. C.: Complex refractive index of atmospheric dust aerosols, Atmos. Environ., 27, 2495–2502, 1993. Sokolik, I. N. and Toon, O. B.: Incorporation of mineralogical composition into models of the radiative properties of mineral aerosol from UV to IR wavelengths, J. Geophys. Res. (D), 104(D8), 9423–9444, 1999. Sokolik, I. N., Winker, D. M., Bergametti, G., Gillette, D. A., Carmichael, G., Kaufman, Y. J., Gomes, L., Schuetz, L., and Penner, J. E.: Introduction to special section: Outstanding problems in quantifying the radiative impacts of mineral dust, J. Geophys. Res. (D), 106(D16), 18 015–18 027, 2001. Stelson, A.: Urban aerosol refractive index prediction by partial molar refraction approach, Environ. Sci. Technol., 24(11), 1676–1679, 1990. Takamura, T., Sasano, Y., and Hayasaka, T.: Tropospheric aerosol optical properties derived from lidar, sunphotometer and optical particle counter measurements, Appl. Opt., 33, 7132–7140, 1994. Tang, I. N., Wong, W. T., and Munkelwitz, H. R.: The relative importance of atmospheric sulfates and nitrates in visibility reduction, Atmos. Environ., 12, 2463–2471, 1981. Tang, I. N. and Munkelwitz, H. R.: Composition and temperature dependence of the deliquescence properties of hygroscopic aerosols, Atmos. Environ., 27A, 467–473, 1993. Todd, M. C., Martins, V., Washington, R., Lizcano, G., M'Bainayel, S., and Engelstaedter, S.: Optical properties of mineral dust from the Bodélé depression, Northern Chad during BoDEx 2005, J. Geophys. Res.,(D), in press, 2007. Tomasi, C., Vitale, V., and Caroli, E.: Sahara dust program – II. Determination of the vertical particulate mass loading by using extinction models based on Junge-type size distributions, J. Aerosol Sci., 14, 529–539, 1983. Volz, F. E.: Infrared Optical Constants of Ammonium Sulfate, Sahara Dust, Volcanic Pumice, and Fly ash, Appl. Opt., 12, 564–568, 1973. Wang, J., Christopher, S. A., Brechtel, F., Kim, J., Schmid, B., Redemann, J., Russell, P. B., Quinn, P., and Holben, B. N.: Geostationary Satellite Retrievals of Aerosol Optical Thickness during ACE-Asia, J. Geophys. Res., 108(23), 8657, doi:10.1029/2003JD003580, 2003. White, W. H. and Roberts, P. T.: On the nature and origins of visibility-reducing aerosols in the Los Angeles air basin, Atmos. Environ., 11, 803–812, 1977.