References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-9-4115-2009

Impacts of aerosol-cloud interactions on past and future changes in tropospheric composition

Unger

¹ ² Menon

³ Koch

D. M.

¹ Shindell

D. T.

NASA Goddard Institute for Space Studies, New York, NY, USA

Columbia University, New York, NY, USA

Lawrence Berkeley National Laboratory, Berkeley, CA, USA

22 06 2009

9 12 4115 4129

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/9/4115/2009/acp-9-4115-2009.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/9/4115/2009/acp-9-4115-2009.pdf

The development of effective emissions control policies that are beneficial to both climate and air quality requires a detailed understanding of all the feedbacks in the atmospheric composition and climate system. We perform sensitivity studies with a global atmospheric composition-climate model to assess the impact of aerosols on tropospheric chemistry through their modification on clouds, aerosol-cloud interactions (ACI). The model includes coupling between both tropospheric gas-phase and aerosol chemistry and aerosols and liquid-phase clouds. We investigate past impacts from preindustrial (PI) to present day (PD) and future impacts from PD to 2050 (for the moderate IPCC A1B scenario) that embrace a wide spectrum of precursor emission changes and consequential ACI. The aerosol indirect effect (AIE) is estimated to be −2.0 Wm−2 for PD-PI and −0.6 Wm−2 for 2050-PD, at the high end of current estimates. Inclusion of ACI substantially impacts changes in global mean methane lifetime across both time periods, enhancing the past and future increases by 10% and 30%, respectively. In regions where pollution emissions increase, inclusion of ACI leads to 20% enhancements in in-cloud sulfate production and ~10% enhancements in sulfate wet deposition that is displaced away from the immediate source regions. The enhanced in-cloud sulfate formation leads to larger increases in surface sulfate across polluted regions (~10–30%). Nitric acid wet deposition is dampened by 15–20% across the industrialized regions due to ACI allowing additional re-release of reactive nitrogen that contributes to 1–2 ppbv increases in surface ozone in outflow regions. Our model findings indicate that ACI must be considered in studies of methane trends and projections of future changes to particulate matter air quality.

References 1

Albrecht, B.: Aerosols, cloud microphysics, and fractional cloudiness, Science, 245, 1227, 1989.

Bauer, S. E., Koch, D., Unger, N., Metzger, S. M., Shindell, D. T., and Streets, D. G.: Nitrate aerosols today and in 2030: Importance relative to other aerosol species and tropospheric ozone, Atmos. Chem. Phys., 7, 5043–5059, 2007.

Bell, N., Koch, D., and Shindell, D. T.: Impacts of chemistry-aerosol coupling on tropospheric ozone and sulfate simulations in a general circulation model, J. Geophys. Res., 110, D14305, doi:10.1029/2004JD005538, 2005.

Bian, H. and Prather, M. J.: Fast-J2: Accurate simulation of stratospheric photoylsys in global chemical models, J. Atmos. Chem., 41, 281–296, 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., 109, D14203, doi:10.1029/2003JD003697, 2004.

Chen, W.-T., Liao, H., and Seinfeld, J. H.: Future climate impacts of direct radiative forcing of anthropogenic aerosols, tropospheric ozone, and long-lived greenhouse gases, J. Geophys. Res., 112, D14209, doi:10.1029/2006JD008051, 2007.

Dentener, F. J. and Crutzen, P. J.: Reaction of N2O$_5$ on tropospheric aerosols: impact on the global distributions of NOx, O3 and OH, J. Geophys. Res., 98, 7149–7163, 1993.

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, AMS Meteor. Monograph, edited by: Emanuel, K. A., and Raymond, D. A., 24(46), 181–184, Am. Meteor. Soc., 1993.

Fiore, A. M., Horowitz, L. W., Dlugokencky, E. J., and West, J. J.: Impact of meteorology and emissions on methane trends, 1990-2004, Geophys. Res. Lett., 33, L12809, doi:10.1029/2006GL026199, 2006.

Fiore, A. M., Dentener, F. J., Wild, O., Cuvelier, C., Schultz, M. G., Hess, P., Textor, C., Schulz, M., et al.: Multi-model estimates of intercontinental source-receptor relationships for ozone pollution, J. Geophys. Res., 114, D04301, doi:10.1029/2008JD010816, 2009.

Forster, P., Ramaswamy, V., Artaxo, P., et al.: Changes in atmospheric constituents and in radiative forcing, in Climate Change 2007: The Physical Science Basis Cambridge Univ. Press, New York, USA, 131–215,, 2007.

Hansen, J., Sato, Mki., Ruedy, R., et al.: Efficacy of climate forcings, J. Geophys. Res., 110, D18104, doi:10.1029/2005JD005776, 2005.

Koch, D., Menon, S., Del Genio, A., Ruedy, R., Aleinov, I., and Schmidt, G. A.: Dangerous human-made interference with climate: A GISS modelE study, Atmos. Chem. Phys., 7, 2287–2312, 2007.

Jones, A., Haywood, J. M., and Boucher, O.: Aerosol forcing, climate response and climate sensitivity in the Hadley Centre climate model, J. Geophys. Res., 112, D20211, doi:10.1029/2007JD008688, 2007.

Kloster, S., Dentener, F., Feichter, J., Raes, F., Lohmann, U., Roeckner, E., and Fischer-Bruns, I.: A GCM study of future climate response to aerosol pollution reductions, Clim. Dynam., doi:10.1007/s00382-009-0573-0, in press, 2009.

Koch, D., Jacob, D., Tegen, I., Rind, D., and Chin, M.: Tropospheric sulfur simulation and sulfate direct radiative forcing in the Goddard Institute for Space Studies general circulation model, J. Geophys. Res., 104, 23799–23822, doi:10.1029/1999JD900248, 1999.

Koch, D., Schmidt, G. A., and Field, C. V.: Sulfur, sea salt, and radionuclide aerosols in GISS ModelE, J. Geophys. Res., 111, D06206, doi:10.1029/2004JD005550, 2006.

Koch, D., Bond, T. C., Streets, D. Unger, N., and van der Werf, G.: Global impacts of aerosols from particular source regions and sectors, J. Geophys. Res., 112, D02205, doi:10.1029/2005JD007024, 2007.

Koch, D., Menon, S., Del Genio, A., Ruedy, R., Aleinov, I., and Schmidt, G. A.: Distinguishing aerosol impacts on climate over the past century, J. Climate, 2009, in press.

Lohmann, U. and Feichter, J.: Global indirect aerosol effects: A review, Atmos. Chem. Phys., 5, 715–737, 2005.

Liao, H. and Seinfeld, J. H.: Global impacts of gas-phase chemistry-aerosol interactions on direct radiative forcing by anthropogenic aerosols and ozone, J. Geophys. Res., 110, D18208, doi:10.1029/2005JD005907, 2005.

Liu, H., Crawford, J. H., Pierce, R. B., Norris, P., Platnick, S. E., Chen, G., Logan, J. A., Yantosca, R. M., Evans, M. J., Kittaka, C., Feng, Y., and Tie, X.: Radiative effect of clouds on tropospheric chemistry in a global three-dimensional chemical transport model, J. Geophys. Res., 111, D20303, doi:10.1029/2005JD006403, 2006.

Martin, R. V., Jacob, D. J., Yantosca, R. M., Chin, M., and Ginoux, P., Global and regional decreases in tropospheric oxidants from photochemical effects of aerosols, J. Geophys. Res., 108, 4097, doi:10.1029/2002JD002622, 2003.

Menon, S., Del Genio, A. D., Koch, D., and Tselioudis, G.: GCM simulations of the aerosol indirect effect: Sensitivity to cloud parameterization and aerosol burden, J. Atmos. Sci., 59, 692–713, doi:10.1175/1520–0469, 2002.

Menon, S. and Rotstayn, L.: The radiative influence of aerosol effects on liquid-phase cumulus and stratus clouds based on sensitivity studies with two climate models, Climate Dynamics, 27, 345–356, 2006.

Menon, S. and Del Genio, A. D.: Evaluating the impacts of carbonaceous aerosols on clouds and climate, In: Human-Induced Climate Change: An Interdisciplinary Assessment, edited by: Schlesinger, M. E., Kheshgi, H., Smith, J. B., de la Chesnaye, F. C., Reilly, J. M., Wilson, T., and Kolstad, C., Cambridge University Press, pp. 34-48, 2007.

Menon, S., Unger, N., Koch, D., Francis, J., Garrett, T., Sednev, I., Shindell, D., and Streets, D.: Aerosol climate effects and air quality impacts from 1980 to 2030, Environ. Res. Lett., 3, 024004, doi:10.1088/1748-9326/3/2/024004, 2008a.

Menon, S., Del Genio, A. D., Kaufman, Y., Bennartz, R., Koch, D., Loeb, N., and Orlikowski, D.: Analyzing signatures of aerosol-cloud interactions from satellite retrievals and the GISS GCM to constrain the aerosol indirect effect, J. Geophys. Res., 113, D14S22, doi:10.1029/2007JD009442, 2008b.

Olivier, J. G. J. and Berdowski, J. J. M.: Global emissions sources and sinks, in The Climate System, edited by: Berdowski, J., Guicherit, R., and Heij, B. J., 33–78, A. A. Balkema, Brookfield, VT, USA, 2001.

Rayner, N. A., Parker, D. E., Horton, E. B., Folland, C. K., Alexander, L. V., Rowell, D. P., Kent, E. C., and Kaplan, A.: Global analyses of sea surface temperature, sea ice, and night marine air temperature since the late nineteenth century, J. Geophys. Res., 108(D14), 4407, doi:10.1029/2002JD002670, 2003.

Rotstayn, L. D. and Liu, Y.: A smaller global estimate of the second indirect aerosol effect, Geophys. Res. Lett., 32, L05708, doi:10.1029/2004GL021922, 2005.

Schmidt, G. A., Ruedy, R., Hansen, J. E., et al.: Present day atmospheric simulations using GISS ModelE: Comparison to in-situ, satellite and reanalysis data, J. Clim., 19, 153–192, 2006.

Shindell, D. T., Faluvegi, G., and Bell, N.: Preindustrial-to-present-day radiative forcing by tropospheric ozone from improved simulations with the GISS chemistry-climate GCM, Atmos. Chem. Phys., 3, 1675–1702, 2003.

Shindell, D. T., Faluvegi, G., and Emmons, L. K.: Inferring carbon monoxide pollution changes from space-based observations, J. Geophys. Res., 110, D23303, doi:10.1029/2005JD006132, 2005.

Shindell, D. T., Faluvegi, G., Unger, N., Aguilar, E., Schmidt, G. A., Koch, D. M., Bauer, S. E., and Miller, R. L.: Simulations of preindustrial, present-day, and 2100 conditions in the NASA GISS composition and climate model G-PUCCINI, Atmos. Chem. Phys., 6, 4427–4459, 2006.

Shindell, D. T., Faluvegi, G., Bauer, S. E., Koch, D., Unger, N., Menon, S., Miller, R. L., Schmidt, G. A., and Streets, D. G.: Climate response to projected changes in short-lived species under the A1B scenario from 2000–2050 in the GISS climate model, J. Geophys. Res., 112, D20103, doi:10.1029/2007JD008753, 2007.

Stevenson, D. S., Dentener, F. J., Schultz, M. G., et al.: Multimodel ensemble simulations of present-day and near-future tropospheric ozone, J. Geophys. Res., 111, D08301, doi:10.1029/2005JD006338, 2006.

Tie, X., Emmons, L., Horowitz, L., Brasseur, G., Ridley, B., Atlas, E., Stroud, C., Hess, P., Klonecki, A., Madronich, S., Talbot, R., and Dibb, J.: Effect of sulfate aerosol on tropospheric NOx and ozone budgets: Model simulations and TOPSE evidence, J. Geophys. Res., 108(D4), 8364, doi:10.1029/2001JD001508, 2003.

Twomey, S. A.: Aerosols, clouds and radiation, Atmos. Environ., 25A, 2435–2442, 1991.

Unger, N., Shindell, D. T., Koch, D. M., and Streets, D. G.: Cross influences of ozone and sulfate precursor emissions changes on air quality and climate, Proc. Natl. Acad. Sci., 103, 4377–4380, doi:10.1073pnas.0508769103, 2006a.

Unger, N., Shindell, D. T., Koch, D. M., Amann, M., Cofala, J., and Streets, D. G.: Influences of man-made emissions and climate changes on tropospheric ozone, methane and sulfate at 2030 from a broad range of possible futures, J. Geophys. Res., 111, D12313, doi:10.1029/2005JD006518, 2006b.

Wu, S., Mickley, L. J., Leibensperger, E. M., Jacob, D. J., Rind, D., and Streets, D. G.: Effects of 2000-2050 global change on ozone air quality in the United States, J. Geophys. Res., 113, D06302, doi:10.1029/2007JD008917, 2008.