Chen, Y. and Cheng, Y. and Ma, N. and Wei, C. and Ran, L. and Wolke, R. and Größ, J. and Wang, Q. and Pozzer, A. and Van Der Gon, H.A.C.D. and Spindler, G. and Lelieveld, J. and Tegen, I. and Su, H. and Wiedensohler, A. (2020) Natural sea-salt emissions moderate the climate forcing of anthropogenic nitrate. Atmospheric Chemistry and Physics, 20 (2). pp. 771-786. ISSN 1680-7316
chen_SSA_NitrateAOD_manuscript_yc86_RL07_JG01_NM01_yfc68_cw01_GS02_IT01_AW_JL04_QQ_hs07_AP_ACPD_R01R02_Fig.docx - Accepted Version
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Abstract
Natural sea-salt aerosols, when interacting with anthropogenic emissions, can enhance the formation of particulate nitrate. This enhancement has been suggested to increase the direct radiative forcing of nitrate, called the “mass-enhancement effect”. Through a size-resolved dynamic mass transfer modeling approach, we show that interactions with sea salt shift the nitrate from sub- to super-micron-sized particles (“redistribution effect”), and hence this lowers its efficiency for light extinction and reduces its lifetime. The redistribution effect overwhelms the mass-enhancement effect and significantly moderates nitrate cooling; e.g., the nitrate-associated aerosol optical depth can be reduced by 10 %–20 % over European polluted regions during a typical sea-salt event, in contrast to an increase by ∼10 % when only accounting for the mass-enhancement effect. Global model simulations indicate significant redistribution over coastal and offshore regions worldwide. Our study suggests a strong buffering by natural sea-salt aerosols that reduces the climate forcing of anthropogenic nitrate, which had been expected to dominate the aerosol cooling by the end of the century. Comprehensive considerations of this redistribution effect foster better understandings of climate change and nitrogen deposition.