Megan M. Bela

Aerosol transport and wet scavenging in deep convective clouds: A case study and model evaluation using a multiple passive tracer analysis approach

Wet scavenging of aerosols by continental deep convective clouds is studied for a supercell storm complex observed over Oklahoma during the Deep Convective Clouds and Chemistry campaign. A new passive-tracer-based transport analysis framework is developed to characterize convective transport using vertical profiles of several passive trace gases. For this case, the analysis estimates that observed passive gas mixing ratios in the upper troposphere convective outflow consist of 47% low level (<3 km) inflow air, 32% entrained midtroposphere air, and 21% upper troposphere air. The new analysis framework is used to estimate aerosol wet scavenging efficiencies. Observations yield high overall scavenging efficiencies of 81% for submicron aerosol mass. Organic, sulfate, and ammonium aerosols have similar wet scavenging efficiencies (80%–84%). The apparent scavenging efficiency for nitrate aerosol is much lower (57%), but the scavenging efficiency for nitrate aerosol plus nitric acid combined (84%) is close to the other species. Scavenging efficiencies for aerosol number are high for larger particles (84% for 0.15–2.5 µm diameter) but are lower for smaller particles (64% for 0.03–0.15 µm). The storm is simulated using the chemistry version of the Weather Research and Forecasting model. Compared to the observation-based analysis, the standard model strongly underestimates aerosol scavenging efficiencies by 32% and 41% in absolute differences for submicron mass and number. Adding a new treatment of secondary activation significantly improves simulated aerosol scavenging, producing wet scavenging efficiencies that are only 7% and 8% lower than observed efficiencies. This finding emphasizes the importance of secondary activation for aerosol wet removal in deep convective storms.

Wet scavenging of soluble gases in DC3 deep convective storms using WRF-Chem simulations and aircraft observations

We examine wet scavenging of soluble trace gases in storms observed during the Deep Convective Clouds and Chemistry (DC3) field campaign. We conduct high-resolution simulations with the Weather Research and Forecasting model with Chemistry (WRF-Chem) of a severe storm in Oklahoma. The model represents well the storm location, size, and structure as compared with Next Generation Weather Radar reflectivity, and simulated CO transport is consistent with aircraft observations. Scavenging efficiencies (SEs) between inflow and outflow of soluble species are calculated from aircraft measurements and model simulations. Using a simple wet scavenging scheme, we simulate the SE of each soluble species within the error bars of the observations. The simulated SEs of all species except nitric acid (HNO_3) are highly sensitive to the values specified for the fractions retained in ice when cloud water freezes. To reproduce the observations, we must assume zero ice retention for formaldehyde (CH_2O) and hydrogen peroxide (H_2O_2) and complete retention for methyl hydrogen peroxide (CH_3OOH) and sulfur dioxide (SO_2), likely to compensate for the lack of aqueous chemistry in the model. We then compare scavenging efficiencies among storms that formed in Alabama and northeast Colorado and the Oklahoma storm. Significant differences in SEs are seen among storms and species. More scavenging of HNO_3 and less removal of CH_3OOH are seen in storms with higher maximum flash rates, an indication of more graupel mass. Graupel is associated with mixed-phase scavenging and lightning production of nitrogen oxides (NO_x), processes that may explain the observed differences in HNO_3 and CH_3OOH scavenging.

Convective transport and scavenging of peroxides by thunderstorms observed over the central U.S. during DC3

One of the objectives of the Deep Convective Clouds and Chemistry (DC3) field experiment was to determine the scavenging of soluble trace gases by thunderstorms. We present an analysis of scavenging of hydrogen peroxide (H_2O_2) and methyl hydrogen peroxide (CH_3OOH) from six DC3 cases that occurred in Oklahoma and northeast Colorado. Estimates of H_2O_2 scavenging efficiencies are comparable to previous studies ranging from 79 to 97% with relative uncertainties of 5–25%. CH_3OOH scavenging efficiencies ranged from 12 to 84% with relative uncertainties of 18–558%. The wide range of CH_3OOH scavenging efficiencies is surprising, as previous studies suggested that CH_3OOH scavenging efficiencies would be <10%. Cloud chemistry model simulations of one DC3 storm produced CH_3OOH scavenging efficiencies of 26–61% depending on the ice retention factor of CH_3OOH during cloud drop freezing, suggesting ice physics impacts CH_3OOH scavenging. The highest CH_3OOH scavenging efficiencies occurred in two severe thunderstorms, but there is no obvious correlation between the CH_3OOH scavenging efficiency and the storm thermodynamic environment. We found a moderate correlation between the estimated entrainment rates and CH_3OOH scavenging efficiencies. Changes in gas-phase chemistry due to lightning production of nitric oxide and aqueous-phase chemistry have little effect on CH_3OOH scavenging efficiencies. To determine why CH_3OOH can be substantially removed from storms, future studies should examine effects of entrainment rate, retention of CH_3OOH in frozen cloud particles during drop freezing, and lightning-NO_x production.

Convective transport of formaldehyde to the upper troposphere and lower stratosphere and associated scavenging in thunderstorms over the central United States during the 2012 DC3 study

We have developed semi-independent methods for determining CH2O scavenging efficiencies (SEs) during strong midlatitude convection over the western, south-central Great Plains, and southeastern regions of the United States during the 2012 Deep Convective Clouds and Chemistry (DC3) Study. The Weather Research and Forecasting model coupled with chemistry (WRF-Chem) was employed to simulate one DC3 case to provide an independent approach of estimating SEs and the opportunity to study CH2O retention in ice when liquid drops freeze. Measurements of CH2O in storm inflow and outflow were acquired on board the NASA DC-8 and the NSF/National Center for Atmospheric Research Gulfstream V (GV) aircraft employing cross-calibrated infrared absorption spectrometers. This study also relied heavily on the nonreactive tracers i-/n-butane and i-/n-pentane measured on both aircraft in determining lateral entrainment rates during convection as well as their ratios to ensure that inflow and outflow air masses did not have different origins. Of the five storm cases studied, the various tracer measurements showed that the inflow and outflow from four storms were coherently related. The combined average of the various approaches from these storms yield remarkably consistent CH2O scavenging efficiency percentages of: 54% ± 3% for 29 May; 54% ± 6% for 6 June; 58% ± 13% for 11 June; and 41 ± 4% for 22 June. The WRF-Chem SE result of 53% for 29 May was achieved only when assuming complete CH2O degassing from ice. Further analysis indicated that proper selection of corresponding inflow and outflow time segments is more important than the particular mixing model employed.

Evaluation of deep convective transport in storms from different convective regimes during the DC3 field campaign using WRF‐Chem with lightning data assimilation

Deep convective transport of surface moisture and pollution from the planetary boundary layer to the upper troposphere and lower stratosphere affects the radiation budget and climate. This study analyzes the deep convective transport in three different convective regimes from the 2012 Deep Convective Clouds and Chemistry (DC3) field campaign: May 21st Alabama airmass thunderstorms, May 29th Oklahoma supercell severe storm, and June 11th mesoscale convective system (MCS). Lightning data assimilation within the Weather Research and Forecasting (WRF) model coupled with chemistry (WRF-Chem) is utilized to improve the simulations of storm location, vertical structure and chemical fields. Analysis of vertical flux divergence shows that deep convective transport in the May 29th supercell case is the strongest per unit area while transport of boundary layer insoluble trace gases is relatively weak in the MCS and airmass cases. The weak deep convective transport in the strong MCS is unexpected and is caused by the injection into low levels of mid-level clean air by a strong rear inflow jet. In each system, the magnitude of tracer vertical transport is more closely related to the vertical distribution of mass flux density than the vertical distribution of trace gas mixing ratio. Finally, the net vertical transport is strongest in high composite reflectivity regions and dominated by upward transport.

Effects of scavenging, entrainment, and aqueous chemistry on peroxides and formaldehyde in deep convective outflow over the central and Southeast U.S.: DEEP CONVECTIVE SCAVENGING, ENTRAINMENT, AND CHEMISTRY

Deep convective transport of gaseous precursors to ozone (O3) 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 (CH2O) 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 CH2O, methyl hydroperoxide (CH3OOH), and hydrogen peroxide (H2O2) are quantified. Liquid phase microphysical scavenging was the dominant process reducing CH2O and H2O2 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 CH3OOH mixing ratios in the storm cores were primarily due to entrainment of low-background CH3OOH. In the air mass storm, lower CH3OOH and H2O2 scavenging efficiencies (SEs) than in the MCS were partly due to entrainment of higher background CH3OOH and H2O2. Overestimated rain and hail production in WRF-Chem reduces the confidence in ice retention fraction values determined for the peroxides and CH2O.