ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH GΓΆttingen, Germany 10.5194/acp-10-2129-2010 Evaluation of aerosol distributions in the GISS-TOMAS global aerosol microphysics model with remote sensing observations Lee Y. H. 1 Adams P. J. 1 2 Department of Civil and Environmental Engineering, Carnegie Mellon University, Pittsburgh, PA, USA Department of Engineering and Public Policy, Carnegie Mellon University, Pittsburgh, PA, USA 01 03 2010 10 5 2129 2144 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. This article is available from http://www.atmos-chem-phys.net/10/2129/2010/acp-10-2129-2010.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/2129/2010/acp-10-2129-2010.pdf

The Aerosol Optical Depth (AOD) and Angstrom Coefficient (AC) predictions in the GISS-TOMAS model of global aerosol microphysics are evaluated against remote sensing data from MODIS, MISR, and AERONET. The model AOD agrees well (within a factor of two) over polluted continental (or high sulfate), dusty, and moderate sea-salt regions but less well over the equatorial, high sea-salt, and biomass burning regions. Underprediction of sea-salt in the equatorial region is likely due to GCM meteorology (low wind speeds and high precipitation). For the Southern Ocean, overprediction of AOD is very likely due to high sea-salt emissions and perhaps aerosol water uptake in the model. However, uncertainties in cloud screening at high latitudes make it difficult to evaluate the model AOD there with the satellite-based AOD. AOD in biomass burning regions is underpredicted, a tendency found in other global models but more severely here. Using measurements from the LBA-SMOCC 2002 campaign, the surface-level OC concentration in the model are found to be underpredicted severely during the dry season while much less severely for EC concentration, suggesting the low AOD in the model is due to underpredictions in OM mass. The potential for errors in emissions and wet deposition to contribute to this bias is discussed.

 References Abdou, W. A., Diner, D. J., Martonchik, J. V., Bruegge, C. J., Kahn, R. A., Gaitley, B. J., Crean, K. A., Remer, L. A., and Holben, B.: Comparison of coincident Multiangle Imaging Spectroradiometer and Moderate Resolution Imaging Spectroradiometer aerosol optical depths over land and ocean scenes containing Aerosol Robotic Network sites, J. Geophys. Res.-Atmos., 110(D10), D10S07, doi:10.1029/2004JD004693, 2005. Adams, P. J. and Seinfeld, J. H.: Predicting global aerosol size distributions in general circulation models, J. Geophys. Res.-Atmos., 107, 4370, doi:10.1029/2001JD001010, 2002. Bond, T. C., Streets, D. G., Yarber, K. F., Nelson, S. M., Woo, J. H. and Klimont, Z.: A technology-based global inventory of black and organic carbon emissions from combustion, J. Geophys. Res.-Atmos., 109, D14203, doi:10.1029/2003JD003697, 2004. Bond, T. C. and Bergstrom, R. W.: Light absorption by carbonaceous particles: An investigative review, Aerosol Science and Technology, 40(1), 27–67, 2006. Brennan, J. I., Kaufman, Y. J., Koren, I., and Li, R. R.: Aerosol-cloud interaction-misclassification of MODIS clouds in heavy aerosol, Ieee Transactions on Geoscience and Remote Sensing, 43(4), 911–915, 2005. Clarke, A. D., Owens, S. R., and Zhou, J. C.: An ultrafine sea-salt flux from breaking waves: Implications for cloud condensation nuclei in the remote marine atmosphere, J. Geophys. Res.-Atmos., 111, D06202, doi:10.1029/2005JD006565, 2006. Decesari, S., Fuzzi, S., Facchini, M. C., Mircea, M., Emblico, L., Cavalli, F., Maenhaut, W., Chi, X., Schkolnik, G., Falkovich, A., Rudich, Y., Claeys, M., Pashynska, V., Vas, G., Kourtchev, I., Vermeylen, R., Hoffer, A., Andreae, M. O., Tagliavini, E., Moretti, F., and Artaxo, P.: Characterization of the organic composition of aerosols from Rondτnia, Brazil, during the LBA-SMOCC 2002 experiment and its representation through model compounds, Atmos. Chem. Phys., 6, 375–402, 2006. Del Genio, A. D. and Yao, M. S.: Efficient cumulus parameterization for long-term climate studies: The GISS scheme, in The Representation of Cumulus Convection in Numerical Models, American Meteorological Society, Boston, Mass., 1993. Del Genio, A. D., Yao, M. S., Kovari, W., and Lo, K. K. W.: A prognostic cloud water parameterization for global climate models, J. Climate, 9(2), 270–304, 1996. Di Girolamo, L. and Wilson, M. J.: A first look at band-differenced angular signatures for cloud detection from MISR, Ieee Transactions on Geoscience and Remote Sensing, 41(7), 1730–1734, 2003. Dick, W. D., Saxena, P., and McMurry, P. H.: Estimation of water uptake by organic compounds in submicron aerosols measured during the Southeastern Aerosol and Visibility Study, J. Geophys. Res.-Atmos., 105(D1), 1471–1479, 2000. Diner, D. J., Beckert, J. C., Reilly, T. H., Bruegge, C. J., Conel, J. E., Kahn, R. A., Martonchik, J. V., Ackerman, T. P., Davies, R., Gerstl, S. A. W., Gordon, H. R., Muller, J. P., Myneni, R. B., Sellers, P. J., Pinty, B. and Verstraete, M. M.: Multi-angle Imaging SpectroRadiometer (MISR) – Instrument description and experiment overview, Ieee Transactions on Geoscience and Remote Sensing, 36(4), 1072–1087, 1998. 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 Aerosol Robotic Network (AERONET) Sun and sky radiance measurements, J. Geophys. Res.-Atmos., 105(D8), 9791–9806, 2000. Forster, P., Ramaswamy, V., Artaxo, P., Berntsen, T., Betts, R., Fahey, D. W., Haywood, J., Lean, J., Lowe, D. C., Myhre, G., Nganga, J., Prinn, R., Raga, G., Schulz, M., and Dorland, R. V.: Changes in Atmospheric Constituents and in Radiative Forcing, Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 2007. Gates, W. L., Boyle, J. S., Covey, C., Dease, C. G., Doutriaux, C. M., Drach, R. S., Fiorino, M., Gleckler, P. J., Hnilo, J. J., Marlais, S. M., Phillips, T. J., Potter, G. L., Santer, B. D., Sperber, K. R., Taylor, K. E., and Williams, D. N.: An overview of the results of the Atmospheric Model Intercomparison Project (AMIP I), B. Am. Meteorol. Soc., 80(1), 29–55, 1999. Guelle, W., Schulz, M., Balkanski, Y., and Dentener, F.: Influence of the source formulation on modeling the atmospheric global distribution of sea salt aerosol, J. Geophys. Res.-Atmos., 106(D21), 27509–27524, 2001. Hale, G. M. and Querry, M. R.: Optical-Constants of Water in 200-Nm to 200-Mum Wavelength Region, Appl. Optics, 12(3), 555–563, 1973. Hansen, J., Russell, G., Rind, D., Stone, P., Lacis, A., Lebedeff, S., Ruedy, R., and Travis, L.: Efficient 3-Dimensional Global-Models for Climate Studies – Model-I and Model-Ii, Mon. Weather Rev., 111(4), 609–662, 1983. Hansen, J., Sato, M., Ruedy, R., Nazarenko, L., Lacis, A., Schmidt, G. A., Russell, G., Aleinov, I., Bauer, M., Bauer, S., Bell, N., Cairns, B., Canuto, V., Chandler, M., Cheng, Y., Del Genio, A., Faluvegi, G., Fleming, E., Friend, A., Hall, T., Jackman, C., Kelley, M., Kiang, N., Koch, D., Lean, J., Lerner, J., Lo, K., Menon, S., Miller, R., Minnis, P., Novakov, T., Oinas, V., Perlwitz, J., Rind, D., Romanou, A., Shindell, D., Stone, P., Sun, S., Tausnev, N., Thresher, D., Wielicki, B., Wong, T., Yao, M., and Zhang, S.: Efficacy of climate forcings, J. Geophys. Res.-Atmos., 110(D18), D18104, doi:10.1029/2005JD005776, 2005. Hartke, G. J. and Rind, D.: Improved surface and boundary layer models for the Goddard Institute for Space Studies general circulation model, J. Geophys. Res.-Atmos., 102(D14), 16407–16422, 1997. Hess, M., Koepke, P., and Schult, I.: Optical properties of aerosols and clouds: The software package OPAC, B. Am. Meteorol. Soc., 79(5), 831–844, 1998. Holben, B. N., Eck, T. F., Slutsker, I., Tanre, D., Buis, J. P., Setzer, A., Vermote, E., Reagan, J. A., Kaufman, Y. J., Nakajima, T., Lavenu, F., Jankowiak, I., and Smirnov, A.: AERONET -A federated instrument network and data archive for aerosol characterization, Remote Sens. Environ., 66(1), 1–16, 1998. Holben, B. N., Tanre, D., Smirnov, A., Eck, T. F., Slutsker, I., Abuhassan, N., Newcomb, W. W., Schafer, J. S., Chatenet, B., Lavenu, F., Kaufman, Y. J., Castle, J. V., Setzer, A., Markham, B., Clark, D., Frouin, R., Halthore, R., Karneli, A., O'Neill, N. T., Pietras, C., Pinker, R. T., Voss, K., and Zibordi, G.: An emerging ground-based aerosol climatology: Aerosol optical depth from AERONET, J. Geophys. Res.-Atmos., 106(D11), 12067–12097, 2001. IPCC: Intergovernmental Panel on Climate Change 2001: The Scientific Basis – Technical Summary, 2001. Jin, Y. F., Gao, F., Schaaf, C. B., Li, X. W., Strahler, A. H., Bruegge, C. J., and Martonchik, J. V.: Improving MODIS surface BRDF/Albedo retrieval with MISR multiangle observations, IEEE Trans. Geosci. Remote Sensing, 40(7), 1593–1604, 2002. Kahn, R. A., Ogren, J. A., Ackerman, T. P., Bosenberg, J., Charlson, R. J., Diner, D. J., Holben, B. N., Menzies, R. T., Miller, M. A., and Seinfeld, J. H.: Aerosol data sources and their roles within PARAGON, B. Am. Meteorol. Soc., 85(10), 1511–1522, 2004. Kahn, R. A., Gaitley, B. J., Martonchik, J. V., Diner, D. J., Crean, K. A., and Holben, B.: Multiangle Imaging Spectroradiometer (MISR) global aerosol optical depth validation based on 2 years of coincident Aerosol Robotic Network (AERONET) observations, J. Geophys. Res.-Atmos., 110(D10), D10S04, doi:10.1029/2004JD004706, 2005. Kerminen, V. M., Anttila, T., Lehtinen, K. E. J., and Kulmala, M.: Parameterization for atmospheric new-particle formation: Application to a system involving sulfuric acid and condensable water-soluble organic vapors, Aerosol Sci. Technol., 38(10), 1001–1008, 2004. Kinne, S., Lohmann, U., Feichter, J., Schulz, M., Timmreck, C., Ghan, S., Easter, R., Chin, M., Ginoux, P., Takemura, T., Tegen, I., Koch, D., Herzog, M., Penner, J., Pitari, G., Holben, B., Eck, T., Smirnov, A., Dubovik, O., Slutsker, I., Tanre, D., Torres, O., Mishchenko, M., Geogdzhayev, I., Chu, D. A., and Kaufman, Y.: Monthly averages of aerosol properties: A global comparison among models, satellite data, and AERONET ground data, J. Geophys. Res.-Atmos., 108(D20), 4634, doi:10.1029/2001JD001253, 2003. Kinne, S., Schulz, M., Textor, C., Guibert, S., Balkanski, Y., Bauer, S. E., Berntsen, T., Berglen, T. F., Boucher, O., Chin, M., Collins, W., Dentener, F., Diehl, T., Easter, R., Feichter, J., Fillmore, D., Ghan, S., Ginoux, P., Gong, S., Grini, A., Hendricks, J., Herzog, M., Horowitz, L., Isaksen, I., Iversen, T., Kirkevåg, A., Kloster, S., Koch, D., Kristjansson, J. E., Krol, M., Lauer, A., Lamarque, J. F., Lesins, G., Liu, X., Lohmann, U., Montanaro, V., Myhre, G., Penner, J., Pitari, G., Reddy, S., Seland, O., Stier, P., Takemura, T., and Tie, X.: An AeroCom initial assessment – optical properties in aerosol component modules of global models, Atmos. Chem. Phys., 6, 1815–1834, 2006. Koren, I., Remer, L. A., Kaufman, Y. J., Rudich, Y., and Martins, J. V.: On the twilight zone between clouds and aerosols, Geophys. Res. Lett., 34(8), L08805, doi:10.1029/2007GL029253, 2007. Lee, Y. H., Chen, K., and Adams, P. J.: Development of a global model of mineral dust aerosol microphysics, Atmos. Chem. Phys., 9, 2441–2458, 2009. Li, R. R., Remer, L., Kaufman, Y. J., Mattoo, S., Gao, B. C., and Vermote, E.: Snow and ice mask for the MODIS aerosol products, IEEE Geosci. Remote Sens. Lett., 2(3), 306–310, 2005. Liousse, C., Penner, J. E., Chuang, C., Walton, J. J., Eddleman, H., and Cachier, H.: A global three-dimensional model study of carbonaceous aerosols, J. Geophys. Res.-Atmos., 101(D14), 19411–19432, 1996. Liu, L., Lacis, A. A., Carlson, B. E., Mishchenko, M. I., and Cairns, B.: Assessing Goddard Institute for Space Studies ModelE aerosol climatology using satellite and ground-based measurements: A comparison study, J. Geophys. Res.-Atmos., 111(D20), D20212, doi:10.1029/2006JD007334, 2006. Liu, Y., Sarnat, J. A., Coull, B. A., Koutrakis, P., and Jacob, D. J.: Validation of multiangle imaging spectroradiometer (MISR) aerosol optical thickness measurements using aerosol robotic network (AERONET) observations over the contiguous United States, J. Geophys. Res.-Atmos., 109(D6), D06205, doi:10.1029/2003JD003981, 2004. Martensson, E. M., Nilsson, E. D., de Leeuw, G., Cohen, L. H., and Hansson, H. C.: Laboratory simulations and parameterization of the primary marine aerosol production, J. Geophys. Res.-Atmos., 108(D9), 4297, doi:10.1029/2002JD002263, 2003. Miller, R. L., Cakmur, R. V., Perlwitz, J., Geogdzhayev, I. V., Ginoux, P., Koch, D., Kohfeld, K. E., Prigent, C., Ruedy, R., Schmidt, G. A., and Tegen, I.: Mineral dust aerosols in the NASA goddard institute for Space Sciences ModelE atmospheric general circulation model, J. Geophys. Res.-Atmos., 111, D06208, doi:10.1029/2005JD005796, 2006. Myhre, G., Stordal, F., Johnsrud, M., Diner, D. J., Geogdzhayev, I. V., Haywood, J. M., Holben, B. N., Holzer-Popp, T., Ignatov, A., Kahn, R. A., Kaufman, Y. J., Loeb, N., Martonchik, J. V., Mishchenko, M. I., Nalli, N. R., Remer, L. A., Schroedter-Homscheidt, M., TanrΓ©, D., Torres, O., and Wang, M.: Intercomparison of satellite retrieved aerosol optical depth over ocean during the period September 1997 to December 2000, Atmos. Chem. Phys., 5, 1697–1719, 2005. Nenes, A., Pandis, S. N., and Pilinis, C.: ISORROPIA: A new thermodynamic equilibrium model for multiphase multicomponent inorganic aerosols, Aquatic Geochemistry, 4(1), 123–152, 1998. Odowd, C. D., Smith, M. H., Consterdine, I. E., and Lowe, J. A.: Marine aerosol, sea-salt, and the marine sulphur cycle: A short review, Atmos. Environ., 31(1), 73–80, 1997. Penner, J. E., Eddleman, H., and Novakov, T.: Towards the Development of a Global Inventory for Black Carbon Emissions, Atmos. Environ., 27(8), 1277–1295, 1993. Pierce, J. R. and Adams, P. J.: Global evaluation of CCN formation by direct emission of sea salt and growth of ultrafine sea salt, J. Geophys. Res.-Atmos., 111, D06203, doi:10.1029/2005JD006186, 2006. Pierce, J. R., Chen, K., and Adams, P. J.: Contribution of primary carbonaceous aerosol to cloud condensation nuclei: processes and uncertainties evaluated with a global aerosol microphysics model, Atmos. Chem. Phys., 7, 5447–5466, 2007. Pierce, J. R. and Adams, P. J.: Uncertainty in global CCN concentrations from uncertain aerosol nucleation and primary emission rates, Atmos. Chem. Phys., 9, 1339–1356, 2009a. Pierce, J. R. and Adams, P. J.: A Computationally Efficient Aerosol Nucleation/Condensation Method: Pseudo-Steady-State Sulfuric Acid, Aerosol Sci. Technol., 43(3), 216–226, 2009b. Pierce, J. R., Theodoritsi, G., Adams, P. J., and Pandis, S. N.: Parameterization of the effect of sub-grid scale aerosol dynamics on aerosol number emission rates, J. Aerosol Sci., 40(5), 385–393, 2009. Prather, M. J.: Numerical Advection by Conservation of 2nd-Order Moments, J. Geophys. Res.-Atmos., 91(D6), 6671–6681, 1986. Redemann, J., Zhang, Q., Russell, P. B., Livingston, J. M., and Remer, L. A.: Case studies of aerosol remote sensing in the vicinity of clouds, J. Geophys. Res.-Atmos., 114, D06209, doi:10.1029/2008JD010774, 2009. Remer, L. A., Kleidman, R. G., Levy, R. C., Kaufman, Y. J., Tanre, D., Mattoo, S., Martins, J. V., Ichoku, C., Koren, I., Yu, H. B., and Holben, B. N.: Global aerosol climatology from the MODIS satellite sensors, J. Geophys. Res.-Atmos., 113(D14), D14S07, doi:10.1029/2007JD009661, 2008. Rosenzweig, C. and Abramopoulos, F.: Land-surface model development for the GISS GCM, J. Climate, 10(8), 2040–2054, 1997. Savoie, D. L. and Prospero, J. M.: Aerosol Concentration Statistics for Northern Tropical Atlantic, J. Geophys. Res.-Oceans and Atmospheres, 82(37), 5954–5964, 1977. Schmidt, G. A., Ruedy, R., Hansen, J. E., Aleinov, I., Bell, N., Bauer, M., Bauer, S., Cairns, B., Canuto, V., Cheng, Y., Del Genio, A., Faluvegi, G., Friend, A. D., Hall, T. M., Hu, Y. Y., Kelley, M., Kiang, N. Y., Koch, D., Lacis, A. A., Lerner, J., Lo, K. K., Miller, R. L., Nazarenko, L., Oinas, V., Perlwitz, J., Rind, D., Romanou, A., Russell, G. L., Sato, M., Shindell, D. T., Stone, P. H., Sun, S., Tausnev, N., Thresher, D., and Yao, M. S.: Present-day atmospheric simulations using GISS ModelE: Comparison to in situ, satellite, and reanalysis data, J. Climate, 19(2), 153–192, 2006. Schulz, M., Textor, C., Kinne, S., Balkanski, Y., Bauer, S., Berntsen, T., Berglen, T., Boucher, O., Dentener, F., Guibert, S., Isaksen, I. S. A., Iversen, T., Koch, D., Kirkevεg, A., Liu, X., Montanaro, V., Myhre, G., Penner, J. E., Pitari, G., Reddy, S., Seland, Ø., Stier, P., and Takemura, T.: Radiative forcing by aerosols as derived from the AeroCom present-day and pre-industrial simulations, Atmos. Chem. Phys., 6, 5225–5246, 2006. Shettle, E. P. and Fenn, R. W.: Models of the aerosols of the loweratmosphere and the effects of humidity variations on their optical properties, Air Force Geoph. Lab., Massachusetts,1979. Stier, P., Feichter, J., Kinne, S., Kloster, S., Vignati, E., Wilson, J., Ganzeveld, L., Tegen, I., Werner, M., Balkanski, Y., Schulz, M., Boucher, O., Minikin, A., and Petzold, A.: The aerosol-climate model ECHAM5-HAM, Atmos. Chem. Phys., 5, 1125–1156, 2005. Tang, I. N.: Chemical and size effects of hygroscopic aerosols on light scattering coefficients, J. Geophys. Res.-Atmos., 101(D14), 19245–19250, 1996. Tegen, I. and Fung, I.: Modeling of Mineral Dust in the Atmosphere - Sources, Transport, and Optical-Thickness, J. Geophys. Res.-Atmos., 99(D11), 22897–22914, 1994. Torres, O., Bhartia, P. K., Herman, J. R., Sinyuk, A., Ginoux, P. and Holben, B.: A long-term record of aerosol optical depth from TOMS observations and comparison to AERONET measurements, J Atmos Sci., 59(3), 398–413, 2002. Twohy, C. H., Coakley, J. A., and Tahnk, W. R.: Effect of changes in relative humidity on aerosol scattering near clouds, J. Geophys. Res.-Atmos., 114, D05205, doi:10.1029/2008JD010991, 2009. van der Werf, G. R., Randerson, J. T., Collatz, G. J., Giglio, L., Kasibhatla, P. S., Arellano, A. F., Olsen, S. C., and Kasischke, E. S.: Continental-scale partitioning of fire emissions during the 1997 to 2001 El Nino/La Nina period, Science, 303(5654), 73–76, 2004. van der Werf, G. R., Randerson, J. T., Giglio, L., Collatz, G. J., Kasibhatla, P. S., and Arellano Jr., A. F.: Interannual variability in global biomass burning emissions from 1997 to 2004, Atmos. Chem. Phys., 6, 3423–3441, 2006.