Investigation of Heterogeneous NAT Nucleation Mechanisms using CALIOP Polar Stratospheric Cloud Observations

In the two plus decades since it became evident that polar stratospheric clouds (PSCs) play a major role in the springtime depletion of polar ozone, the detailed composition and morphology of PSCs has been an area of interest. Although our PSC knowledge base is substantial, there is still considerable uncertainty in specific key areas related to their composition and formation. Probably the least well understood of these is the nucleation process responsible for the formation of nitric acid trihydrate (NAT) particles and the circumstances under which NAT formation and growth leads to stratospheric denitrification. CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) is an excellent instrument for observing PSCs and has already produced an extensive set of PSC observations with unprecedented spatial and temporal resolution covering five winters. These observations are providing new insight into the key remaining questions regarding PSC composition and formation mechanisms. In this paper, we examine the CALIOP PSC observations in combination with a microphysical model in attempt to better understand the underlying physical mechanisms for NAT nucleation. Of particular interest is the early phase of the 2009-2010 Arctic winter when CALIOP frequently observed extended regions of tenuous NAT clouds, clearly before ice was present in the polar vortex. This provides unprecedented large-scale evidence that ice particles are not the only nuclei on which NAT may form. Microphysical model calculations along backward trajectories from these CALIOP NAT cloud observations are used to investigate possible ice-independent, heterogeneous NAT nucleation mechanisms. These analyses will then be expanded to other winters to assess the overall significance of an ice-independent nucleation mechanism for NAT PSCs.