The role of halogen species (e. g., Br, Cl) in the troposphere of polar regions has been investigated since the discovery of their importance for boundary layer ozone destruction in the polar spring about 25 years ago. Halogen species take part in an auto-catalytic chemical reaction cycle, which releases Br-2 and BrCl from the sea salt aerosols, fresh sea ice or snowpack, leading to ozone depletion. In this study, three different chemical reaction schemes are investigated: a bromine-only reaction scheme, which then is subsequently extended to include nitrogen-containing compounds and chlorine species and corresponding chemical reactions. The importance of specific reactions and their rate constants is identified by a sensitivity analysis. The heterogeneous reaction rates are parameterized by considering the aerodynamic resistance, a reactive surface ratio, beta, i.e., the ratio of reactive surface area to total ground surface area, and the boundary layer height, L-mix. It is found that for beta = 1, a substantial ozone decrease occurs after five days and ozone depletion lasts for 40 h for L-mix = 200 m. For about beta >= 20, the time required for major ozone depletion ([O-3] < 4 ppb) to occur becomes independent of the height of the boundary layer, and for beta = 100 it approaches two days, 28 h of which are attributable to the induction and 20 h to the depletion time. In polar regions, a small amount of NOx may exist, which stems from nitrate contained in the snow, and may have a strong impact on the ozone depletion. Therefore, the role of nitrogen-containing species on the ozone depletion rate is studied. The results show that the NOx concentrations are influenced by different chemical reactions over different time periods. During ozone depletion, the reaction cycle involving the BrONO2 hydrolysis is dominant. A critical value of 0.0004 of the uptake coefficient of the BrONO2 hydrolysis reaction at the aerosol and saline surfaces is identified, beyond which the existence of NOx species accelerates the ozone depletion event, whereas for lower values, deceleration occurs

This work examines the relationships of entrainment rate to vertical velocity, buoyancy, and turbulent dissipation rate by applying stepwise principal component regression to observational data from shallow cumulus clouds collected during the Routine Atmospheric Radiation Measurement (ARM) Aerial Facility (AAF) Clouds with Low Optical Water Depths (CLOWD) Optical Radiative Observations (RACORO) field campaign over the ARM Southern Great Plains (SGP) site near Lamont, Oklahoma. The cumulus clouds during the RACORO campaign simulated using a large-eddy simulation (LES) model are also examined with the same approach. The analysis shows that a combination of multiple variables can better represent entrainment rate in both the observations and LES than any single-variable fitting. Three commonly used parameterizations are also tested on the individual cloud scale. A new parameterization is thus presented that relates entrainment rate to vertical velocity, buoyancy, and dissipation rate; the effects of treating clouds as ensembles and humid shells surrounding cumulus clouds on the new parameterization are discussed. Physical mechanisms underlying the relationships of entrainment rate to vertical velocity, buoyancy, and dissipation rate are also explored.

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