Asian Tropopause Aerosol Layer (ATAL): composition, origin, and radiative forcing estimates

Satellite observations from SAGE II and CALIPSO indicate that summertime aerosol extinction has more than doubled in the Asian Tropopause Aerosol Layer (ATAL) since the late 1990s. Here we show remote and in-situ observations, together with results from a chemical transport model (CTM), to explore the likely composition, origin, and radiative forcing of the ATAL. We show in-situ balloon measurements of aerosol backscatter, which support the high levels observed by CALIPSO since 2006. We also show in situ measurements from aircraft, which indicate a predominant carbonaceous contribution to the ATAL (Carbon/Sulfur ratios of ~2-10), which is supported by the CTM results. We show that the peak in ATAL aerosol lags by ~1 month the peak in CO from MLS, associated with deep convection over Asia during the summer monsoon. This suggests that secondary formation and growth of aerosols in the upper troposphere on monthly timescales make a significant contribution to ATAL. Back trajectory calculations initialized from CALIPSO observations provide evidence that deep convection over India is a significant source for ATAL through the vertical transport of pollution to the upper troposphere.