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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 (HNO3) 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 (CH2O) and hydrogen peroxide (H2O2) and complete retention for methyl hydrogen peroxide (CH3OOH) and sulfur dioxide (SO2), 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 HNO3 and less removal of CH3OOH 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 (NOx), processes that may explain the observed differences in HNO3 and CH3OOH scavenging. more...

A cloud‐resolved storm and chemistry simulation of a severe convective system in Oklahoma constrained by anvil aircraft observations of NOx was used to estimate the mean production of NOx per flash in this storm. An upward ice flux scheme was used to parameterize flash rates in the model. Model lightning was also constrained by observed lightning flash types and the altitude distribution of flash channel segments. The best estimate of mean NOx production by lightning in this storm was 80–110 mol per flash, which is smaller than many other literature estimates. This result is likely due to the storm having been a high flash rate event in which flash extents were relatively small. Over the evolution of this storm a moderate negative correlation was found between the total flash rate and flash extent and energy per flash. A longer‐term simulation at 36‐km horizontal resolution with parameterized convection was used to simulate the downwind transport and chemistry of the anvil outflow from the same storm. Convective transport of low‐ozone air from the boundary layer decreased ozone in the anvil outflow by up to 20–40 ppbv compared with the initial conditions, which contained stratospheric influence. Photochemical ozone production in the lightning‐NOx enhanced convective plume proceeded at a rate of 10–11 ppbv per day in the 9–11 km outflow layer over the 24‐hr period of downwind transport to the Southern Appalachians. Photochemical production plays a large role in the restoration of upper tropospheric ozone following deep convection. Plain Language Summary: Nitrogen oxides are important precursors for tropospheric ozone, an important greenhouse gas. The global amount of nitrogen oxides produced by lightning remains highly uncertain, primarily because of uncertainty in the amount produced per flash. In this paper we use an approach that involves cloud‐resolved modeling with chemistry, constrained by observed flash rates and aircraft measurements of nitrogen oxides, to make an estimate of the mean production per flash for an observed severe storm over Oklahoma. We estimate that the mean production rate was 80–110 mol per flash for this high flash rate storm, which is at the lower end of the range reported in the literature. We use a regional model to follow the outflow of the Oklahoma storm downwind to estimate the amount of ozone produced in the upper tropospheric outflow plume by the lightning‐generated nitrogen oxides. Our estimate is in the range found in previous studies, and we note that the ozone production by photochemistry is an important process in restoring upper tropospheric ozone following storms that lofted low values of ozone from the layer of air near the surface. Key Points: Mean lightning NOx production was 80–110 mol flash−1 for a high flash rate storm, based on a model constrained by flash and NOx observationsNet O3 production in the upper outflow of a high flash rate storm was at a rate of 10–11 ppbv day−1 during 24 hr of downwind transportProduction of O3 due to lightning NOx contributed to the recovery of upper tropospheric O3 following reductions due to convective transport [ABSTRACT FROM AUTHOR] more...

A Lagrangian particle dispersion model (LPDM) is used to study fumigation of pollutants in and above the entrainment zone into a growing convective boundary layer. Probability density functions of particle location with height and time are calculated from particle trajectories driven by the sum of the resolved-scale velocity from a large-eddy simulation (LES) model and the stochastic subgrid-scale (SGS) velocity. The crosswind-integrated concentration (CWIC) fields show good agreement with water tank experimental data. A comparison of the LPDM output with an Eulerian diffusion model output based on the same LES flow shows qualitative agreement with each other except that a greater overshoot maximum of the ground-level concentration occurs in the Eulerian model. The dimensionless CWICs near the surface for sources located above the entrainment zone collapse to a nearly universal curve provided that the profiles are time shifted, where the shift depends on the source heights. The dimensionless CWICs for sources located within the entrainment zone show a different behavior. Thus, fumigation from sources above the entrainment zone and within the entrainment zone should be treated separately. An examination of the application of Taylor's translation hypothesis to the fumigation process showed the importance of using the mean boundary layer wind speed as a function of time rather than the initial mean boundary layer wind speed, because the mean boundary layer wind speed decreases as the simulation proceeds. The LPDM using LES is capable of accurately simulating fumigation of particles into the convective boundary layer. This technique provides more computationally efficient simulations than Eulerian models. more...

Previous studies have shown that a surface cold front often coincides with a heavy band of precipitation commonly designated as a narrow cold-frontal rainband. The maximum rainfall rate within this band can exceed 100-200 mm [h.sup.-1]. This study uses a nonhydrostatic two-dimensional cloud model with ice microphysics to investigate the precipitation processes within this type of rainband. Despite the relatively simple initialization and two-dimensionality, many aspects of these storms were well simulated. In these simulations, the intense but shallow updrafts produced large amounts of cloud water that were transformed primarily into rain and graupel within the zone of heavy precipitation and, to a lesser extent, into snow. The graupel and snow produced a zone of trailing stratiform precipitation. While the heavy rainfall could be represented in a warm rain model of the storm, an ice phase was needed in order to replicate the stratiform precipitation. Feedbacks of microphysical processes upon the dynamics of the flow were investigated. Sublimation and melting of frozen hydrometeors produced a pronounced cooling within the cold air mass, which slowly increased the depth and intensity of the cold air mass. This diabatic cooling within the cold air could potentially play a role in maintaining or even intensifying the circulations that lead to these rainbands. Previous studies of these types of fronts have instead concentrated on the role of melting in maintaining these structures through producing a stable layer across the cold air interface that could inhibit mixing. more...

A two-dimensional numerical cloud model is developed to examine the microphysics, chemistry and stratiform region of a narrow cold-frontal rainband to specify the effects of meteorological and chemical parameters on the winter storm chemical deposition. Peak sulfate and peak nitrate deposition occur behind the primary and main updraft regions, respectively. The sulfate and nitrate deposition depend on the graupel in the storm, with sulfate deposition inversely related to peak vertical velocities. more...

Ozone is a greenhouse gas and air pollutant that is harmful to human health and plants. During the summer in the southeastern U.S., many regional and global models are biased high for surface ozone compared to observations. Past studies have suggested different solutions including the need for updates to model representation of clouds, chemistry, ozone deposition, and emissions of nitrogen oxides (NOx) or biogenic hydrocarbons. Here due to the high biogenic emissions in the southeastern U.S., more comprehensive and updated isoprene and terpene chemistry is added into CESMTM/CAM-chem (Community Earth System Model/Community Atmosphere Model with chemistry) to evaluate the impact of chemistry on simulated ozone. Comparisons of the model results with data collected during the Studies of Emissions Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field campaign and U.S. EPA CASTNET monitoring stations confirm the updated chemistry improves simulated surface ozone, ozone precursors, and NOx reservoir compounds. The isoprene and terpene chemistry updates reduce the bias in the daily maximum 8-hr average (MDA8) surface ozone by up to 7 ppb. In the past, terpene oxidation in particular has been ignored or heavily reduced in chemical schemes used in many regional and global models, and this study demonstrates comprehensive isoprene and terpene chemistry is needed to reduce surface ozone model biases. Sensitivity tests were performed in order to evaluate the impact of lingering uncertainties in isoprene and terpene oxidation on ozone. Results suggest that even though isoprene emissions are higher than terpene emissions in the southeastern U.S., remaining uncertainties in isoprene and terpene oxidation have similar impacts on ozone due to lower uncertainties in isoprene oxidation. Additionally, this study identifies the need for further constraints on aerosol uptake of organic nitrates derived from isoprene and terpenes in order to reduce uncertainty in simulated ozone. [ABSTRACT FROM AUTHOR] more...

Acidity, defined as pH, is a central component of aqueous chemistry. In the atmosphere, the acidity of condensed phases (aerosol particles, cloud water, and fog droplets) governs the phase partitioning of semi-volatile gases such as HNO3, NH3, and HCl, as well as chemical reaction rates. It has implications for the atmospheric lifetime of pollutants, deposition, and human health. Despite its fundamental role in atmospheric processes, only recently has this field seen a growth in the number of studies on particle acidity. Even with this growth, many fine particle pH estimates must be based on thermodynamic model calculations since no operational techniques exist for direct measurements. Current information indicates acidic fine particles are ubiquitous, but observationally-constrained pH estimates are limited in spatial and temporal coverage. Clouds and fogs are also generally acidic, but to a lesser degree than particles, and have a range of pH that is quite sensitive to anthropogenic emissions of sulfur and nitrogen oxides, as well as ambient ammonia. Historical measurements indicate that cloud and fog droplet pH has changed in recent decades in response to controls on anthropogenic emissions, while the limited trend data for aerosol particles indicates acidity may be relatively constant due to the semi-volatile nature of the key acids and bases and buffering in particles. This paper reviews and synthesizes the current state of knowledge on the acidity of atmospheric condensed phases, specifically particles and cloud droplets. It includes recommendations for estimating acidity and pH, standard nomenclature, a synthesis of current pH estimates based on observations, and new model calculations on the local and global scale. [ABSTRACT FROM AUTHOR] more...