Seasonal variability of aerosol vertical profiles over east US and west Europe: GEOS-Chem/APM simulation and comparison with CALIPSO observations

摘要

In this study, we employed 5 years (2007-2011) of the CALIPSO level-3 monthly aerosol extinction product to compare with the GEOS-Chem/APM simulations for the same time period over two major industrial regions (east US and west Europe). The objective is to understand which aerosol types or species significantly determine the vertical profiles by comparing the seasonal variability between the simulations and observations. Our study shows that the model successfully produces the magnitude of aerosol extinction, profile shape, and their seasonal variability observed by CALIPSO over both east US (EUS) and west Europe (WEU). The extinctions below 1 km make up 44-79% to the total, from either the model simulations or satellite retrievals, with larger percentages in winter seasons (62-79%) and smaller percentages in summer seasons (44-57%) associated with the strength of vertical transport. The shape of the vertical profiles has, therefore, a distinct seasonal variability, with a more like quasi-exponential shape in DJF (December, January, and February) and SON (September, October, and November) than in MAM (March, April, and May) and JJA (June, July, and August), which have been discerned from both measurements and simulations. Analysis of modeled aerosol species indicates that secondary particles (SP), containing sulfate, ammonia, nitrate, and secondary organic aerosols (SOAs), predominantly determine the total aerosol vertical profiles while black carbon (BC), primary organic carbon (OC), and sea salt (SS), only account for a small fraction and are also limited near the surface. Mineral dust (DS) contributes more to the total extinction over WEU than over EUS, particularly in MAM, a result of being adjacent to the North Africa desert. Secondary inorganic aerosol (SIA, i.e. sulfate, ammonia, and nitrate) contributes most of the total SP mass in DJF and SON while SOA is particularly important in MAM and JJA when the emissions from leafed plants are active. Our study also indicates that, compared to aerosol extinction, the number concentration of particles larger than 10 nm (CN10) exhibits a different seasonal variation and vertical profile, but Cloud Condensation Nuclei (CCN) concentration at supersaturation of 0.4% (CCN0.4) presents a consistent seasonal variation and similar vertical profile. Therefore, aerosol extinction could be a good indicator for CCN0.4 with regard to seasonal variations of vertical profiles.