Sensitivity of Methane Lifetime and Transport to Sulfate Geoengineering

Monday, 15 December 2014
Giovanni Pitari1, Valentina Aquila2, Simone Tilmes3, Irene Cionni4, Natalia de Luca1, Glauco Di Genova1 and Daniela Iachetti1, (1)University of L'Aquila, L'Aquila, Italy, (2)Johns Hopkins University, Earth and Planetary Science, Baltimore, MD, United States, (3)Univ. of Leeds, Leeds, United Kingdom, (4)ENEA National Agency for New Technologies, Energy and Sustainable Economic Development, Rome, Italy
Sulfate geoengineering, made by sustained injection of SO2 in the tropical lower stratosphere, may impact the abundance of tropospheric methane through several photochemical mechanisms affecting the tropospheric OH abundance and hence the methane lifetime. Changes of the stratospheric Brewer-Dobson circulation also play a role in the upper tropospheric CH4 transport. Three mechanisms lead to lower OH concentrations and a longer CH4 lifetime: (a) solar radiation scattering increases the planetary albedo and cools the surface, with a tropospheric water vapor decrease as a response to this cooling. (b) The tropospheric UV budget is upset by the additional aerosol scattering and stratospheric ozone changes: the net effect is meridionally not uniform, with a net decrease in the tropics, thus producing less tropospheric O(1D). (c) The extra-tropical downwelling motion from the lower stratosphere tends to increase the sulfate aerosol surface area density available for heterogeneous chemical reactions in the mid-upper troposphere, thus reducing the amount of NOx and tropospheric O3 production. On the other hand, the tropical lower stratosphere is warmed by solar and planetary radiation absorption by the aerosols. The heating rates perturbation are strongly latitude dependent, producing a significant change of the pole-to-equator temperature gradient and mean zonal wind distribution, with a net increase of tropical upwelling. A stronger meridional component of the Brewer-Dobson circulation increases the extra-tropical stratosphere to troposphere transport of CH4 poorer air, resulting in less CH4 transported in the UTLS. The net effect on tropospheric OH may be positive or negative depending on the net result of different superimposed species perturbations in the UTLS, i.e. CH4 (negative), NOy and O3 (positive). Three climate-chemistry coupled models are used here to explore the above radiative, chemical and dynamical mechanisms affecting the methane lifetime (ULAQ-CCM, GEOSCCM, CCSM-CAM4). First results show that the CH4 lifetime may become significantly longer (by about 10%) with a sustained injection of 2.5 Tg-S/yr started in year 2020, which implies an increase of tropospheric CH4 (200 ppbv) and a positive indirect radiative forcing of sulfate geoengineering due to CH4 changes (+0.1 W/m2 in the 2045).