Partitioning of HNO3, H2O2 and SO2 to cloud ice: Simulations with CMAQ

In the upper troposphere, gas phase species can partition to cloud ice, undergo chemical reaction and contribute to particle mass aloft, affecting chemical cycling in the atmosphere. This manuscript describes the first implementation of gas-to-cloud ice partitioning of three inorganic gases, HNO3, SO2 and H2O2, along with subsequent SO2 oxidation in the Community Multiscale Air Quality (CMAQ) chemical transport model. Four simulations are performed with CMAQv4.7.1 that include lightning production of NO for August 12th–25th of 2005 to investigate the impacts of ice chemistry on CMAQ-predicted gas phase mixing ratios and particle mass concentrations of associated species. Considerable episodic decreases, greater than 25%, in gas phase HNO3 are noted at pressures of 200–600 mb, with the largest changes at 300–400 mb. Effects are also induced on other gases in the nitrogen budget. NOx and HONO mixing ratios decrease up to 20%, but changes are generally less than 10%. Nitrate aerosol mass concentrations increase up to 0.15 μg m−3 for the highest model layers (100 mb). We find that phase changes in nitrogen species induced by ice partitioning are sensitive to CMAQ predictions of the aerosol phase accumulation mode ammonium to sulfate ratios [ NH 4 + ] : [ SO 4 2 − ] . Predicted O3 concentrations do not change (<1%). No changes in H2O2, SO2, or sulfate aerosol concentrations are observed.