Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 9 3 2009 10.5194/acpd-9-13475-2009 http://www.atmos-chem-phys-discuss.net/9/13475/2009/ http://www.atmos-chem-phys-discuss.net/9/13475/2009/acpd-9-13475-2009.html http://www.atmos-chem-phys-discuss.net/9/13475/2009/acpd-9-13475-2009.pdf 13475 13521 2009-06-18 Assessment of vertically-resolved PM₁₀ from mobile lidar observations J.-C. Raut jean-christophe.raut@lmd.polytechnique.fr P. Chazette Laboratoire de Météorologie Dynamique, Ecole Polytechnique, 91128 Palaiseau, France Laboratoire des Sciences du Climat et de l'Environnement, Laboratoire mixte CEA-CNRS-UVSQ, CEA Saclay, 91191 Gif-sur-Yvette, France We investigate in this study the role of the Paris Peripherique (the ring around Paris agglomeration) in local particulate pollution and the horizontal gradient of pollution between Paris centre and its remote suburbs. For this purpose, we combine in situ surface measurements with active remote sensing observations obtained from a great number of research programs in Paris area since 1999. Two approaches, devoted to the conversion of vertical profiles of lidar-derived extinction coefficients into PM₁₀, have been set up. A very good agreement is found between the theoretical and empirical methods with a discrepancy of 3%. Hence, specific extinction cross-sections at 355 nm are provided with a reasonable uncertainty for urban (4.5 m²/g), periurban (5.9 m²/g), rural (7.1 m²/g), biomass burning (2.6 m²/g) and dust (1.1 m²/g) aerosols. The high spatial and temporal resolutions of the mobile lidar (respectively 1.5 m and 1 min) enable to follow the spatiotemporal variability of various layers carrying aerosols in the troposphere. Appropriate specific extinction cross-sections are applied in each layer detected in the vertical heterogeneities from the lidar profiles. The standard deviation between lidar-derived PM₁₀ at 200 m above ground and surface network stations measurements was ~14 μg m^−3. This difference is particularly ascribed to a decorrelation of mass concentrations in the first meters of the boundary layer, as highlighted through multiangular lidar observations. Lidar signals can be used to follow mass concentrations at the surface and provide useful information on PM₁₀ peak forecasting that affect air quality. Adam, M., Pahlow, M., Kovalev, V. A., Ondov, J. M., Parlange, M. B., and Nair, N.: Aerosol optical characterization by nephelometer and lidar: The Baltimore Supersite experiment during the Canadian forest fire smoke intrusion, J. Geophys. Res., 109, D16S02, doi:10.1029/2003JD004047, 2004. Alfaro, S. C., Gomes, L., Rajot, J. L., Lafon, S., Gaudichet, A., Chatenet, B., Maille, M., Cautenet, G., Lasserre, F., Cachier, H., and Zhang, X. Y.: Chemical and optical characterization of aerosols measured in spring 2002 at the ACE-Asia supersite, Zhenbeitai, China, J. Geophys. Res., 108(D23), 8641, doi:10.1029/2002JD003214, 2003. Andreae, T. W., Andreae, M. O., Ichoku, C., Maenhaut, W., Cafmeyer, J., Karnieli, A., and Orlovsky, L.: Light scattering by dust and anthropogenic aerosol at a remote site in the Negev desert, Israel, J. Geophys. Res., 107(D2), 4008, doi:10.1029/2001jd900252, 2002. Badger, C. L., George, I., Griffiths, P. T., Braban, C. F., Cox, R. A., and Abbatt, J. P. D.: Phase transitions and hygroscopic growth of aerosol particles containing humic acid and mixtures of humic acid and ammonium sulphate, Atmos. Chem. Phys., 6, 755–768, 2006. 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, 17969–17980, 2001. 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. Cachier, H., Brémond, M. P., and Patrick, B. M.: Determination of atmospheric soot carbon with a simple thermal method, Tellus, 41B, 379–390, 1989. Carrico, C. M., Bergin, M. H., Xu, J., Baumann, K., and Maring, H.: Urban aerosol radiative properties: Measurements during the 1999 Atlanta Supersite Experiment, J. Geophys. Res., 108(D7), 8422, doi:10.1029/2001JD001222, 2003. 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., Pelon J., Moulin C., Dulac F., Carrasco I., Guelle W., Bousquet P., and Flamant P. H.: Airborne lidar and Meteosat synergy to characterize a Saharan dust plume over the Azores during SOFIA/ASTEX, Atmos. Environ., 35, 4297–4304, 2001. 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. Chazette, P., Sanak., J., and Dulac, F.: New Approach for Aerosol Profiling with a Lidar Onboard an Ultralight Aircraft: Application to the African Monsoon Multidisciplinary Analysis, Environ. Sci. Technol., 41, 8335–8341, 2007. Chu, D. A., Kaufman, Y. J., Zibordi, G., Chern, J. D., Mao, J., Li, C., and Holben, B. N.: Global monitoring of air pollution over land from the Earth observing System-Terra Moderate Resolution Imaging Spectroradiometer (MODIS), J. Geophys. Res., 108(D21), 4661, doi:10.1029/2002JD003179, 2003. Clarke, A. D., Porter, J. N., Valero, F. P. J., and Pilewskie, P.: Vertical profiles, aerosol microphysics, and optical closure during the Atlantic Stratocumulus Transition Experiment: Measured and modeled column optical properties, J. Geophys. Res., 101, 4443–4453, 1996. Dockery, D. and Pope, A.: Epidemiology of acute health effects: summary of time-series, in: Particles in Our Air: Concentration and Health Effects, edited by: Wilson, R. and Spengler, J. D., Harvard University Press, Cambridge, MA, USA, 123–147, 1996. Donaldson, K., Li, X. Y., and MacNee, W.: Ultrafine (nanometer) particle mediated lung injury, J. Aerosol Sci., 29, 553–560, 1998. Dupont, E., Pelon, J., and Flamant, C.: Study of the moist Convective Boundary Layer structure by backscattering lidar, Bound.-Lay. Meteorol., 69, 1–25, 1994. Dzubay, T. G., Stevens, R. K., Lewis, C. W., Hern, D. H., Courtney, W. J., Tesch, J. W., and Mason, M. A.: Visibility and aerosol composition in Houston, Texas, Environ. Sci. Technol., 16, 514–525, 1982. Elias, T., Haeffelin, M., Drobinski, P., Gomes, L., Rangognio, J., Bergot, T., Chazette, P., Raut, J.-C., and Coulomb, M.: Particulate contribution to extinction of visible radiation: pollution, haze, and fog, Atmos. Res., 92(4), 443–454, doi:10.1016/j.atmosres.2009.01.006, 2009. Flamant, C., Pelon, J., Flamant, P. H., and Durand, P.: Lidar determination of the entrainment zone thickness at the top of the unstable marine atmospheric boundary-layer, Bound.-Lay. Meteorol., 83, 247–284, 1997. Gysel, M., Weingartner, E., and Baltensperger, U.: Hygroscopicity of aerosol particles at low temperatures, 2. Theoretical and experimental hygroscopic properties of laboratory generated aerosols, Environ. Sci. Technol., 36, 63–68, 2002. Gysel, M., Weingartner, E., Nyeki, S., Paulsen, D., Baltensperger, U., Galambos, I., and Kiss, G.: Hygroscopic properties of water-soluble matter and humic-like organics in atmospheric fine aerosol, Atmos. Chem. Phys., 4, 35–50, 2004. Haeffelin, M., Bergot, T., Elias, T., Tardif, R., Carrer, D., Chazette, P., Colomb, M., Drobinski, P., Dupont, E., Dupont, J.-C., Gomes, L., Musson-Genon, L., Pietras, C., Plana-Fattori, A., Protat, A., Rangognio, J., Raut, J.-C., Rémy, S., Richard, D., Sciare, J., and Zhang, X.: PARISFOG, shedding new light on fog physical processes, B. Am. Meteorol. Soc., in review, 2009. 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. Hegg, D. A., Hobbs, P. V., Ferek, R. J., and Waggoner, A. P.: Measurements of some aerosol properties relevant to radiative forcing on the east coast of the United States, J. Appl. Meteorol., 34, 2306–2315, 1995. Hegg, D. A., Livingston, J., Hobbs, P. V., Novakov, T., and Russell, P.: Chemical apportionment of aerosol column optical depth off the mid-Atlantic coast of the United States, J. Geophys. Res., 102, 25293–25303, 1997. Hodzic, A., Vautard, R., Chazette, P., Menut, L., and Bessagnet, B.: Aerosol chemical and optical properties over the Paris area within ESQUIF project, Atmos. Chem. Phys., 6, 3257–3280, 2006. Hoff, R. M., Guise-Bagley, L., Staebler, R. M., Wiebe, H. A., Brook, J., Georgi, B., and Düsterdiek, T.: Lidar, nephelometer, and in situ aerosol experiments in southern Ontario, J. Geophys. Res., 101(D14), 19199–19209, 1996. Holben, B. N., Eck, T. F., Slutsker, I., et al.: AERONET – A federated instrument network and data archive for aerosol characterisation, Remote Sens. Environ., 66, 1–16, 1998. Ichoku, C., Andreae, M. O., Andreae, T. W., Meixner, F. X., Schebeske, G., Formenti, P., Maenhaut, W., Cafmeyer, J., Karnieli, A., and Orlovsky, L.: Interrelationships between aerosol characteristics and light scattering in an eastern Mediterranean arid environment, J. Geophys. Res., 104, 24371–24393, 1999. 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. Keskinen, J., Pietarinen, K., and Lehtimäki, M.: Electrical Low Pressure Impactor, J. Aerosol Sci., 23(4), 353–360, 1992. Klett, J. D.: Stable analytical inversion solution for processing lidar returns, Appl. Optics, 20, 211–220, 1981. Koloutsou-Vakakis, S., Carrico, C. M., Kus, P., Rood, M. J., Li, Z., Shrestha, R., Ogren, J. A., Chow, J. C., and Watson, J. G.: Aerosol properties at a midlatitude Northern Hemisphere continental site, J. Geophys. Res. 106(D3), 3019–3032, 2001. 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., Sánchez-Ccoyllo, O. R., and Moreira, D. S.: Synergetic measurements of aerosols over São Paulo, Brazil using LIDAR, sunphotometer and satellite data during the dry season, Atmos. Chem. Phys., 3, 1523–1539, 2003. Lavigne, C., Roblin, A., Chervet, P., and Chazette, P.: Experimental and theoretical studies of the aureole about a point source that is due to atmospheric scattering in the middle ultraviolet, Appl. Optics, 44, p 1250, 2005. Li, X., Maring, H., Savoie, D., Voss, K., and Prospero, J. M.: Dominance of mineral dust in aerosol light-scattering in the North Atlantic trade winds, Nature, 380, 416–419, 1996. Liu, Y., Park, R. J., Jacob, D. J., Li, Q., Kilaru, V., and Sarnat, J. A.: Mapping annual mean ground-level PM$_2.5$ concentrations using multiangle imaging spectroradiometer aerosol optical thickness over the contiguous united states, J. Geophys. Res., 109, D22206, doi:10.1029/2004jd005025, 2004. 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. McMurry, P. H., Wang, X., Park, K., and Ehara, K.: The relationship between mass and mobility for atmospheric particles: A new technique for measuring particle density, Aerosol Sci. Tech., 36, 227–238, 2002. Menut, L., Vautard, R., Flamant, C., Abonnel, C., Beekmann, M., Chazette, P., Flamant, P. H., Gombert, D., Guédalia, D., Kley, D., Lefebvre, M. P., Lossec, B., Martin, D., Mégie, G., Perros, P., Sicard, M., and Toupance, G.: Measurements and modelling of atmospheric pollution over the Paris area: an overview of the ESQUIF Project, Ann. Geophys., 18, 1467–1481, 2000. Mestayer, P. and Coll, I.: The Urban Boundary Layer Field experiment over Marseille UBL/CLU-Escompte: Experimental set-up and first results, Bound.-Lay. Meteorol., 114, 315–365, 2005. Nenes, A., Pandis, S. N., and Pilinis, C.: ISORROPIA: A new thermodynamic equilibrium model for multiphase multicomponent inorganic aerosols, Aquat. Geochem., 4, 123–152, 1998. Parkhurst, W. J., Tanner, R. L., Weatherford, F. P., Valente, R. J., and Meagher, J. F.: Historic PM$_2.5$/PM$_10$ concentrations in the southeastern United States - Potential implications of the revised particulate matter standard, J. Air Waste Manage., 49, 1060–1067, 1999. Pelletier, B., Santer, R., and Vidot, J.: Retrieving of particulate matter from optical measurements: A semiparametric approach, J. Geophys. Res., 112, D06208, doi:10.1029/2005JD006737, 2007. 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, B. Am. Meteorol. Soc., 75, 375–400, 1994. Pereira, S., Wagner, F., and Silva, A. M.: Scattering properties and mass concentration of local and long-range transported aerosols over the South Western Iberia Peninsula, Atmos. Environ., 42, 7623–7631, 2008. 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. Raut, J.-C. and Chazette, P.: Retrieval of aerosol complex refractive index from a synergy between lidar, sunphotometer and in situ measurements during LISAIR experiment, Atmos. Chem. Phys., 7, 2797–2815, 2007. Raut, J.-C. and Chazette, P.: Vertical profiles of urban aerosol complex refractive index in the frame of ESQUIF airborne measurements, Atmos. Chem. Phys., 8, 901–919, 2008a. Raut, J.-C. and Chazette, P.: Radiative budget in the presence of multi-layered aerosol structures in the framework of AMMA SOP-0, Atmos. Chem. Phys., 8, 6839–6864, 2008b. Raut, J.-C., Chazette, P., and Fortain, A.: New approach using lidar measurements to characterize spatiotemporal aerosol mass distribution in an underground railway station in Paris, Atmos. Environ., 43(3), 575–583, 2009. Reid, J. S., Eck, T. F., Christopher, S. A., Koppmann, R., Dubovik, O., Eleuterio, D. P., Holben, B. N., Reid, E. A., and Zhang, J.: A review of biomass burning emissions part III: intensive optical properties of biomass burning particles, Atmos. Chem. Phys., 5, 827–849, 2005. Roy, D. P., Jin, Y., Lewis, P. E., and Justice, C. O.: Prototyping a global algorithm for systematic fire affected area mapping using MODIS time series data, Remote Sens. Environ., 97, 137–162, 2005. Shinozuka, Y., Clarke, A. D., Howell, S. G., Kapustin, V. N., McNaughton, C. S., Zhou, J., and Anderson, B. E.: Aircraft profiles of aerosol microphysics and optical properties over North America: Aerosol optical depth and its association with PM$_2.5$ and water uptake, J. Geophys. Res., 112, D12S20, doi:10.1029/2006JD007918, 2007. 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. Optics, 41, 493–502, 2002. Tang, I. N. and Munkelwitz, H. R.: Composition and temperature dependence of the deliquescence properties of hygroscopic aerosols, Atmos. Environ., 27A, 467–473, 1993. Tang, I. N. and Munkelwitz, H. R.: Water activities, densities, and refractive indices of aqueous sulfates and sodium nitrate droplets of atmospheric importance, J. Geophys. Res., 99, 18801–18808, 1994. Tang, I. N.: Chemical and size effects of hygroscopic aerosols on light scattering coefficient, J. Geophys. Res., 101, 19245–19250, 1996. Tombette, M., Chazette, P., Sportisse, B., and Roustan, Y.: Simulation of aerosol optical properties over Europe with a 3-D size-resolved aerosol model: comparisons with AERONET data, Atmos. Chem. Phys., 8, 7115–7132, 2008. Trentmann, J., Andreae, M. O., Graf, H.-F., Hobbs, P. V., Ottmar, R. D., and Trautmann, T.: Simulation of a biomass-burning plume: Comparison of model results with observations, J. Geophys. Res., 107(D2), 4013, doi:10.1029/2001jd000410, 2002. van Donkelaar, A., Martin, R. V., and Park, R. J.: Estimating ground-level PM$_2.5$ using aerosol optical depth determined from satellite remote sensing, J. Geophys. Res., 111, D21201, doi:10.1029/2005JD006996, 2006. Vautard, R., Menut, L., Beekmann, M., Chazette, P., Flamant, P. H., Gombert, D., Guédalia, D., Kley, D., Lefebvre, M.-P., Martin, D., Mégie, G., Perros, P., and Toupance, G.: A synthesis of the Air Pollution Over the Paris Region (ESQUIF) field campaign, J. Geophys. Res., 108(D17), 8558, doi:10.1029/2003JD003380, 2003. Vrekoussis, M., Liakakou, E., Koçak, M., Kubilay, N., Oikonomou, K., Sciare, J., and Mihalopoulos, N.: Seasonal variability of optical properties of aerosols in the Eastern Mediterranean M., Atmos. Environ., 39, 7083–7094, 2005. Waggoner, A. P., Weiss, A. P., Ahlquist, N. C., Covert, D. S., and Charlson, R. J.: Optical characteristics of atmospheric aerosols, Atmos. Environ., 15, 1891–1909, 1981. Wang, J. and Christopher, S. A.: Intercomparison between satellite-derived aerosol optical thickness and PM$_2.5$ mass: implications for air quality studies, Geophys. Res. Lett., 30(21), 2095, doi:10.1029/2003GL018174, 2003. White, W. H., Macias, E. S., Nininger, R. C., and Schorran, D.: Size-resolved measurements of light scattering by ambient particles in the Southwestern USA, Atmos. Environ., 28, 909–921, 1994.