Effects of Scavenging, Entrainment, and Aqueous Chemistry on Peroxides and Formaldehyde in Deep Convective Outflow Over the Central and Southeast United States

摘要

Deep convective transport of gaseous precursors to ozone (O_3) and aerosols to the upper troposphere is affected by liquid phase and mixed-phase scavenging, entrainment of free tropospheric air and aqueous chemistry. The contributions of these processes are examined using aircraft measurements obtained in storm inflow and outflow during the 2012 Deep Convective Clouds and Chemistry (DC3) experiment combined with high-resolution (dx ≤ 3 km) WRF-Chem simulations of a severe storm, an air mass storm, and a mesoscale convective system (MCS). The simulation results for the MCS suggest that formaldehyde (CH_2O) is not retained in ice when cloud water freezes, in agreement with previous studies of the severe storm. By analyzing WRF-Chem trajectories, the effects of scavenging, entrainment, and aqueous chemistry on outflow mixing ratios of CH_2O, methyl hydroperoxide (CH_3OOH), and hydrogen peroxide (H_2O_2) are quantified. Liquid phase microphysical scavenging was the dominant process reducing CH_2O and H_2O_2 outflow mixing ratios in all three storms. Aqueous chemistry did not significantly affect outflow mixing ratios of all three species. In the severe storm and MCS, the higher than expected reductions in CH_3OOH mixing ratios in the storm cores were primarily due to entrainment of low-background CH_3OOH. In the air mass storm, lower CH_3OOH and H_2O_2 scavenging efficiencies (SEs) than in the MCS were partly due to entrainment of higher background CH_3OOH and H_2O_2. Overestimated rain and hail production in WRF-Chem reduces the confidence in ice retention fraction values determined for the peroxides and CH_2O.