References

ACPD

Atmospheric Chemistry and Physics Discussions

ACPD

1680-7375

Copernicus GmbH

Göttingen, Germany

10.5194/acpd-9-27791-2009

Airborne measurements of aerosol optical properties related to early spring transport of mid-latitude sources into the Arctic

Adam de Villiers

¹ Ancellet

¹ Pelon

¹ Quennehen

² Scharwzenboeck

² Gayet

J. F.

² Law

K. S.

UPMC Univ. Paris 06, Université Versailles St-Quentin, CNRS/INSU, LATMOS-IPSL, UMR 8190, France

Laboratoire de Météorologie Physique, Université B. Pascal, CNRS, UMR 6016, France

23 12 2009

9 6 27791 27836

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

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The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/9/27791/2009/acpd-9-27791-2009.pdf

Airborne lidar and in-situ measurements of the aerosol properties were conducted between Svalbard Island and Scandinavia in April 2008. Evidence of aerosol transport from Europe and Asia is given. The analysis of the aerosol optical properties based on a multiwavelength lidar (355, 532, 1064 nm) including depolarization at 355 nm aims at distinguishing the role of the different aerosol sources (Siberian wild fires, Eastern Asia and European anthropogenic emissions). Combining, first aircraft measurements, second FLEXPART simulations with a calculation of the PBL air fraction originating from the three different mid-latitude source regions, and third level-2 CALIPSO data products (i.e. backscatter coefficient, depolarisation and color ratio in aerosol layers) along the transport pathways, appears a valuable approach to identify the role of the different aerosol sources even after a transport time larger than 4 days. Above Asia, CALIPSO data indicate more depolarisation (up to 15%) and largest color ratio (>0.5) for the northeastern Asia emissions (i.e. an expected mixture of Asian pollution and dust), while low depolarisation together with smaller and quasi constant color ratio (≈0.3) are observed for the Siberian biomass burning emissions. A similar difference is visible between two layers observed by the aircraft above Scandinavia. The analysis of the time evolution of the aerosol optical properties revealed by CALIPSO between Asia and Scandinavia shows a gradual decrease of the aerosol backscatter, depolarisation ratio and color ratio which suggests the removal of the largest particles in the accumulation mode. A similar study conducted for a European plume has shown aerosol optical properties intermediate between the two Asian sources with color ratio never exceeding 0.4 and moderate depolarisation ratio being always less than 8%, i.e. less aerosol from the accumulation mode.

References 1

Atlas,~E L., Ridley,~B A., and Cantrell,~C.: The Tropospheric Ozone Production about the Spring Equinox (TOPSE) Experiment: introduction, J. Geophys. Res., 108(D4), 8353, \doi10.1029/2002JD003172, 2003.

Bethan,~S., Vaughan,~G., and Reid,~S.: A~comparison of ozone and thermal tropopause heights and the impact of tropopause definition on quantifying the ozone content of the troposphere, Q. J. Roy. Meteor. Soc., 122, 929–944, 1996.

Browell, E V., Hair, J., Butler, C., Grant, W., DeYoung, R., Fenn, M., Brackett, V., Clayton, M., Brasseur, L., Harper, D., Ridley, B., Klonecki, A., Hess, P., Emmons, L., Tie, X., Atlas, E., Cantrell, C., Wimmers, A., Blake, D., Coffey, M., Hannigan, J., Dibb, J., Talbot, R., Flocke, F., Weinheimer, A., Fried, A., Wert, B., Snow, J., and Lefer, B.: Ozone, aerosol, potential vorticity, and trace gas trends observed at high-latitudes over North America from February to May 2000, J. Geophys. Res., 108(D4), 8369, doi:10.1029/2001JD001 390, 2003.

Bucholtz,~A.: Rayleigh-scattering calculations for the terrestrial atmosphere, Appl. Optics, 34, 2765–2773, \doi10.1364/AO.34.002765, http://ao.osa.org/abstract.cfm?URI=ao-34-15-2765, 1995.

Cairo,~F., Donfrancesco,~G D., Adriani,~A., Pulvirenti,~L., and Fierli,~F.: Comparison of various linear depolarization parameters measured by lidar, Appl. Optics, 38, 4425–4432, http://ao.osa.org/abstract.cfm?URI=ao-38-21-4425, 1999.

Cattrall,~C., Reagan,~J., 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, \doi10.1029/2004JD005124, 2005.

Coheur, P.-F., Clarisse, L., Turquety, S., Hurtmans, D., and Clerbaux, C.: IASI measurements of reactive trace species in biomass burning plumes, Atmos. Chem. Phys., 9, 5655–5667, 2009.

Duce, R A., Unni,~C K., Ray,~B J., Prospero,~J M., and Merrill,~J T.: Long-range atmospheric transport of soil dust from Asia to the Tropical North Pacific: temporal variability, Science, 209, 1522–1524, http://www.jstor.org/stable/1684974, 1980.

Engvall,~A., Krejci,~R., Ström,~J., Minikin,~A., Treffeisen,~R., Stohl,~A., and Herber,~A.: In-situ airborne observations of the microphysical properties of the Arctic tropospheric aerosol during late spring and summer, Tellus~B, 60(3), 392–404, \doi10.1111/j.1600-0889.2008.00348.x, 2008.

Fehsenfeld,~F C., Ancellet,~G., Bates,~T S., Goldstein,~A H., Hardesty,~R M., Honrath,~R., Law,~K S., Lewis,~A C., Leaitch,~R., McKeen,~S., Meagher,~J., Parrish,~D D., Pszenny,~A A P., Russell,~P B., Schlager,~H., Seinfeld,~J., Talbot,~R., and Zbinden,~R.: International Consortium for Atmospheric Research on Transport and Transformation (ICARTT): North America to Europe overview of the 2004 summer field study, J. Geophys. Res., 111, D23S01, \doi10.1029/2006JD007829, 2006.

Fisher, J. A., Jacob, D. J., Purdy, M. T., Kopacz, M., Le Sager, P., Carouge, C., Holmes, C. D., Yantosca, R. M., Batchelor, R. L., Strong, K., Diskin, G. S., Fuelberg, H. E., Holloway, J. S., Hyer, E. J., McMillan, W. W., Warner, J., Streets, D. G., Zhang, Q., Wang, Y., and Wu, S.: Source attribution and interannual variability of Arctic pollution in spring constrained by aircraft (ARCTAS, ARCPAC) and satellite (AIRS) observations of carbon monoxide, Atmos. Chem. Phys. Discuss., 9, 19035–19080, 2009.

Freudenthaler,~V., Esselborn,~M., Wiegner,~M., Heese,~B., Tesche,~M., Ansmann,~A., Müller,~D., Althausen,~D., Wirth,~M., Fix,~A., Ehret,~G., Knippertz,~P., Toledano,~C., Gasteiger,~J., Garhammer,~M., and Seefeldner,~M.: Depolarization ratio profiling at several wavelengths in pure Saharan dust during SAMUM~2006, Tellus, 61B, 165–179, \doi10.1111/j.1600-0889.2008.00396.x, http://dx.doi.org/10.1111/j.1600-0889.2008.00396.x, 2009.

Fuelberg, H. E., Harrigan, D. L., and Sessions, W.: A meteorological overview of the ARCTAS~2008 mission, Atmos. Chem. Phys. Discuss., 9, 18417–18478, 2009.

Garrett,~T. and Zhao,~C.: Increased Arctic cloud longwave emissivity associated with pollution from mid-latitudes, Nature, 440, 787–789, 2006.

Gobbi, G. P., Barnaba, F., Van Dingenen, R., Putaud, J. P., Mircea, M., and Facchini, M. C.: Lidar and in situ observations of continental and Saharan aerosol: closure analysis of particles optical and physical properties, Atmos. Chem. Phys., 3, 2161–2172, 2003.

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, 22257–22270, 1999.

Jacob, D. J., Crawford, J. H., Maring, H., Clarke, A. D., Dibb, J. E., Ferrare, R. A., Hostetler, C. A., Russell, P. B., Singh, H. B., Thompson, A. M., Shaw, G. E., McCauley, E., Pederson, J. R., and Fisher, J. A.: The ARCTAS aircraft mission: design and execution, Atmos. Chem. Phys. Discuss., 9, 17073–17123, 2009.

Law,~K. and Stohl,~A.: Arctic Air Pollution: Origins and Impacts, Science, 315(5818), 1537–1540, doi:10.1126/science.1137 695, 2007.

Liu,~Z., Vaughan,~M., Winker,~D., Kittaka,~C., Getzewich,~B., Kuehn,~R., Omar,~A., Powell,~K., Trepte,~C., and Hostetlerd,~C.: The CALIPSO lidar cloud and aerosol discrimination: version~2 algorithm and initial assessment of performance, J. Atmos. Ocean. Tech., 26, 1198–1213, \doi10.1175/2009JTECHA1229.1, 2009.

Methven,~J., Arnold,~S R., Stohl,~A., Avery,~M., Law,~K., Lewis,~A., Parrish,~D., Reeves,~C., Schlager,~H., Atlas,~E., Blake,~D., and Rappenglück,~B.: Establishing Lagrangian connections between observations within air masses crossing the Atlantic during the ICARTT experiment, J. Geophys. Res., 111, D23S62, \doi10.1029/2006JD007540, 2006.

Omar,~A., Winker,~D., Kittaka,~C., Vaughan,~M., Liu,~Z., Hu,~Y., Trepte,~C., Rogers,~R., Ferrare,~R., Lee,~K., Kuehn,~R., and Hostetler,~C.: The CALIPSO automated aerosol classification and lidar ratio selection algorithm, J. Atmos. Ocean. Tech., 26, 1994–2014, \doi10.1175/2009JTECHA1231.1, 2009.

O'Neill,~N., Eck,~T., Smirnov,~A., Holben,~B., and Thulasiraman,~S.: Spectral discrimination of coarse and fine mode optical depth, J. Geophys. Res., 108, 4559, \doi10.1029/2002JD002975, 2003.

Paris,~J.-D., Arshinov,~M Y., Ciais,~P., Belan,~B D., and Nédélec,~P.: Large-scale aircraft\break observations of ultra-fine and fine particle concentrations in the remote Siberian\break troposphere: new particle formation studies, Atmos. Environ., 43, 1302–1309, doi:10.1016/\break j.atmosenv.2008.11.032, https://acces-distant.upmc.fr:443/http/www.sciencedirect.com/science/article/B6VH3-4V35470-5/2/1fb175cceb8cd16d86d47a1c8ca60cf0, 2009.

Pueschel,~R. and Kinne,~S.: Physical and radiative properties of Arctic atmospheric aerosols, Sci. Total Environ., 160–161, 811–824, \doi10.1016/0048-9697(95)04414-V, 1995.

Quinn, P. K., Bates, T. S., Baum, E., Doubleday, N., Fiore, A. M., Flanner, M., Fridlind, A., Garrett, T. J., Koch, D., Menon, S., Shindell, D., Stohl, A., and Warren, S. G.: Short-lived pollutants in the Arctic: their climate impact and possible mitigation strategies, Atmos. Chem. Phys., 8, 1723–1735, 2008.

Rahn,~K A.: Relative importances of North America and Eurasia as sources of arctic aerosol, Atmos. Environ., 15, 1447–1455, \doi10.1016/0004-6981(81)90351-6, 1981.

Scheuer,~E., Talbot,~R W., Dibb,~J E., Seid,~G K., DeBell,~L., and Lefer,~B.: Seasonal distributions of fine aerosol sulfate in the North American Arctic basin during TOPSE, J. Geophys. Res., 108(D4), 8370, \doi10.1029/2001JD001364, 2003.

Seibert, P. and Frank, A.: Source-receptor matrix calculation with a Lagrangian particle dispersion model in backward mode, Atmos. Chem. Phys., 4, 51–63, 2004.

Sellegri, K., Hanke, M., Umann, B., Arnold, F., and Kulmala, M.: Measurements of organic gases during aerosol formation events in the boreal forest atmosphere during QUEST, Atmos. Chem. Phys., 5, 373–384, 2005.

Shindell, D. T., Chin, M., Dentener, F., Doherty, R. M., Faluvegi, G., Fiore, A. M., Hess, P., Koch, D. M., MacKenzie, I. A., Sanderson, M. G., Schultz, M. G., Schulz, M., Stevenson, D. S., Teich, H., Textor, C., Wild, O., Bergmann, D. J., Bey, I., Bian, H., Cuvelier, C., Duncan, B. N., Folberth, G., Horowitz, L. W., Jonson, J., Kaminski, J. W., Marmer, E., Park, R., Pringle, K. J., Schroeder, S., Szopa, S., Takemura, T., Zeng, G., Keating, T. J., and Zuber, A.: A multi-model assessment of pollution transport to the Arctic, Atmos. Chem. Phys., 8, 5353–5372, 2008.

Stohl,~A., Hittenberger,~M., and Wotawa,~G.: Validation of the Lagrangian particle dispersion model FLEXPART against large scale tracer experiment data, Atmos. Environ., 32, 4245–4264, 1998.

Stohl,~A., Eckhardt,~S., Forster,~C., James,~P., Spichtinger,~N., and Seibert,~P.: A~replacement for simple back trajectory calculations in the interpretation of atmospheric trace substance measurements, Atmos. Environ., 36, 4635–4648, 2002.

Stohl,~A., Cooper,~O R., Damoah,~R., Fehsenfeld,~F C., Forster,~C., Hsie,~E Y., Hübler,~G., Parrish,~D D., and Trainer,~M.: Forecasting for a~Lagrangian aircraft campaign, Atmos. Environ., 4, 2405–2433, 2004.

Stohl, A., Berg, T., Burkhart, J. F., Fjæraa, A. M., Forster, C., Herber, A., Hov, Ø., Lunder, C., McMillan, W. W., Oltmans, S., Shiobara, M., Simpson, D., Solberg, S., Stebel, K., Ström, J., Tørseth, K., Treffeisen, R., Virkkunen, K., and Yttri, K. E.: Arctic smoke - record high air pollution levels in the European Arctic due to agricultural fires in Eastern Europe in spring 2006, Atmos. Chem. Phys., 7, 511–534, 2007.

Stohl, A., Forster, C., Huntrieser, H., Mannstein, H., McMillan, W. W., Petzold, A., Schlager, H., and Weinzierl, B.: Aircraft measurements over Europe of an air pollution plume from Southeast Asia - aerosol and chemical characterization, Atmos. Chem. Phys., 7, 913–937, 2007.

Streets,~D. and Waldhoff,~S.: Present and future emissions of air pollutants in China: \chemSO_2, NO<sub>x</sub>, and CO, Atmos. Environ., 34, 363–374, \doi10.1016/S1352-2310(99)00167-3, http://www.sciencedirect.com/science/article/B6VH3-3Y162CG-3/2/dfaeb3ef6e2170f1b0e299716e58ee1f, 2000.

Sugimoto,~N. and Lee,~C H.: Characteristics of dust aerosols inferred from lidar depolarization measurements at two wavelengths, Appl. Optics., 45, 7468–7474, http://ao.osa.org/abstract.cfm?URI=ao-45-28-7468, 2006.

Warneke,~C., Bahreini,~R., Brioude,~J., Brock,~C., de~Gouw,~J., Fahey,~D., Froyd,~K., Holloway,~J., Middlebrook,~A., Miller,~L., Montzka,~S., Murphy,~D., Peischl,~J., Ryerson,~T., Schwarz,~J., Spackman,~J., and Veres,~P.: Biomass burning in Siberia and Kazakhstan as an important source for haze over the Alaskan Arctic in April~2008, Geophys. Res. Lett., 36, L02813, \doi10.1029/2008GL036194, 2009.

Weber,~R., Orsini,~D., Wang,~B., Scheuer,~E., Talbot,~R., Dibb,~J., Seid,~G., DeBell,~L., Mauldin,~R., Kosciuch,~E., Cantrell,~C., and Eisele,~F.: Investigations into free tropospheric new particle formation in the central Canadian arctic during the winter/spring transition as part of TOPSE, J. Geophys. Res., 108(D4), 8357, \doi10.1029/2002JD002239, 2003.