ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-12-1239-2012 The role of carbonyl sulphide as a source of stratospheric sulphate aerosol and its impact on climate Brühl C. 1 Lelieveld J. 1 3 Crutzen P. J. 1 Tost H. 2 Atmospheric Chemistry Department, Max-Planck-Institute for Chemistry, Mainz, Germany Institute for Physics of the Atmosphere, Johannes Gutenberg University, Mainz, Germany The Cyprus Institute, Nicosia, Cyprus, and King Saud University, Riyadh, Saudi Arabia 01 02 2012 12 3 1239 1253 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/12/1239/2012/acp-12-1239-2012.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/1239/2012/acp-12-1239-2012.pdf

Globally, carbonyl sulphide (COS) is the most abundant sulphur gas in the atmosphere. Our chemistry-climate model (CCM) of the lower and middle atmosphere with aerosol module realistically simulates the background stratospheric sulphur cycle, as observed by satellites in volcanically quiescent periods. The model results indicate that upward transport of COS from the troposphere largely controls the sulphur budget and the aerosol loading of the background stratosphere. This differs from most previous studies which indicated that short-lived sulphur gases are also important. The model realistically simulates the modulation of the particulate and gaseous sulphur abundance in the stratosphere by the quasi-biennial oscillation (QBO). In the lowermost stratosphere organic carbon aerosol contributes significantly to extinction. Further, using a chemical radiative convective model and recent spectra, we compute that the direct radiative forcing efficiency by 1 kg of COS is 724 times that of 1 kg CO<sub>2</sub>. Considering an anthropogenic fraction of 30% (derived from ice core data), this translates into an overall direct radiative forcing by COS of 0.003 W m<sup>−2</sup>. The direct global warming potentials of COS over time horizons of 20 and 100 yr are GWP(20 yr) = 97 and GWP(100 yr) = 27, respectively (by mass). Furthermore, stratospheric aerosol particles produced by the photolysis of COS (chemical feedback) contribute to a negative direct solar radiative forcing, which in the CCM amounts to −0.007 W m<sup>−2</sup> at the top of the atmosphere for the anthropogenic fraction, more than two times the direct warming forcing of COS. Considering that the lifetime of COS is twice that of stratospheric aerosols the warming and cooling tendencies approximately cancel.

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