Sulfur dioxide (SO₂) from MIPAS in the upper troposphere and lower stratosphere 2002-2012

Vertically resolved distributions of sulfur dioxide (SO2) with global coverage in the height region from the upper troposphere to ~ 20 km altitude have been derived from observations by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat for the period July 2002 to April 2012. Retrieved volume mixing ratio profiles representing single measurements are characterized by typical errors in the range of 70-100 pptv and by a vertical resolution ranging from 3-5 km. Comparison with ACE-FTS observations revealed a slightly varying bias with altitude of -20 to 50 pptv for the MIPAS dataset in case of volcanically enhanced concentrations. For background concentrations the comparison showed a systematic difference between the two major MIPAS observation periods. After debiasing, the difference could be reduced to biases within -10 to 20 pptv in the altitude range of 10-20 km with respect to ACE-FTS. Further comparisons of the debiased MIPAS dataset with in-situ measurements from various aircraft campaigns showed no obvious inconsistencies within a range of around ±50 pptv. The SO2 emissions of more than thirty volcanic eruptions could be identified in the upper troposphere and lower stratosphere (UTLS). ... mehrEmitted SO2 masses and lifetimes within different altitude ranges in the UTLS have been derived for a large part of these eruptions. Masses are in most cases within estimations derived from other instruments. From three of the major eruptions within the MIPAS measurement period - Kasatochi in August 2008, Sarychev in June 2009 and Nabro in June 2011 - derived lifetimes of SO2 for the altitude ranges 10-14, 14-18, and 18-22 km are 13.3±2.1, 23.6±1.2, and 32.3±5.5 d, respectively. By omitting periods with obvious volcanic influence we have derived background mixing ratio distributions of SO2. At 10 km altitude these indicate an annual cycle at northern mid- and high latitudes with maximum values in summer and an amplitude of about 30 pptv. At higher altitudes of about 16-18 km enhanced mixing ratios of SO2 can be found in the region of the Asian and the North-American monsoon in summer - a possible connection to an aerosol layer discovered by Vernier et al. (2011b) in that region.