Summertime influence of Asian pollution in the free troposphere over North America

[1] We analyze aircraft observations obtained during INTEX-A ( 1 July to 14 August 2004) to examine the summertime influence of Asian pollution in the free troposphere over North America. By applying correlation analysis and principal component analysis (PCA) to the observations between 6 and 12 km, we find dominant influences from recent convection and lightning (13% of observations), Asia (7%), the lower stratosphere ( 7%), and boreal forest fires (2%), with the remaining 71% assigned to background. Asian air masses are marked by high levels of CO, O-3, HCN, PAN, C2H2, C6H6, methanol, and SO42-. The partitioning of NOy species in the Asian plumes is dominated by PAN ( similar to 600 pptv), with varying NOx/HNO3 ratios in individual plumes, consistent with individual transit times of 3 - 9 days. Export of Asian pollution occurred in warm conveyor belts of midlatitude cyclones, deep convection, and in typhoons. Compared to Asian outflow measurements during spring, INTEX-A observations display lower levels of anthropogenic pollutants (CO, C3H8, C2H6, C6H6) due to shorter summer lifetimes; higher levels of biogenic tracers ( methanol and acetone) because of a more active biosphere; and higher levels of PAN, NOx, HNO3, and O-3 reflecting active photochemistry, possibly enhanced by efficient NOy export and lightning. The high Delta O-3/Delta CO ratio (0.76 mol/mol) in Asian plumes during INTEX-A is due to strong photochemical production and, in some cases, mixing with stratospheric air along isentropic surfaces. The GEOS-Chem global model captures the timing and location of the Asian plumes. However, it significantly underestimates the magnitude of observed enhancements in CO, O-3, PAN and NOx.