JUNE 2005: Impact of new laboratory studies of N2O5 hydrolysis on global model budgets of tropospheric NOx and OHWe investigate the impact of new laboratory studies of N2O5 hydrolysis in aerosols on global model simulations of tropospheric chemistry. The new studies investigate the reactive uptake of N2O5 on a variety of tropospheric appropriate aerosol types (neutralized sulfate and organics) and under tropospheric appropriate temperatures and water vapor levels. We use data from these new studies together with recommendations from the literature to parameterize the reaction probability (γN2O5) in the GEOS-CHEM global model as a function of local aerosol composition, temperature, and relative humidity. We find a much lower global mean γN2O5 (0.02) than commonly assumed in models (0.1). Relative to a model simulation assuming a uniform γN2O5 = 0.1, we find increases in mass-averaged tropospheric NOx, O3, and OH concentrations of 7%, 4%, and 8% respectively. The increases in NOx and O3 concentrations bring the GEOS-CHEM simulation in better agreement with climatological observations of ozone from Logan [1998] and NOx from Emmons et al. [2000]. A full description is given in Evans and Jacob, 2005.
Figure: Calculated zonal mean concentration ratios of OH, O3 and NOx for GEOS-CHEM model simulations with γN2O5 values calculated from the new laboratory studies versus a uniform value of 0.1. Results are seasonal averages for winter (DJF) and summer (JJA). Values greater than 1 indicate higher concentrations with the γN2O5 values calculated from new laboratory studies than with a uniform γN2O5 of 0.1. The lower values of γN2O5 found from the new laboratory studies results in higher NOx concentrations. This then increases O3 and OH concentrations due to higher formation rates of O3 and recycling rates of HO2 to OH. The impacts are largest in the relatively warm and dry downwards branches of the Hadley circulation. |