Accurate prediction of total lightning flash rate in thunderstorms is important to improve estimates of nitrogen oxides (NOx) produced by lightning (LNOx) from the storm scale to the global scale. In this study, flash rate parameterization schemes from the literature are evaluated against observed total flash rates for a sample of 11 Colorado thunderstorms, including nine storms from the Deep Convective Clouds and Chemistry (DC3) experiment in May‐June 2012. Observed flash rates were determined using an automated algorithm that clusters very high frequency radiation sources emitted by electrical breakdown in clouds and detected by the northern Colorado lightning mapping array. Existing schemes were found to inadequately predict flash rates and were updated based on observed relationships between flash rate and simple storm parameters, yielding significant improvement. The most successful updated scheme predicts flash rate based on the radar‐derived mixed‐phase 35 dBZ echo volume. Parameterizations based on metrics for updraft intensity were also updated but were found to be less reliable predictors of flash rate for this sample of storms. The 35 dBZ volume scheme was tested on a data set containing radar reflectivity volume information for thousands of isolated convective cells in different regions of the U.S. This scheme predicted flash rates to within 5.8% of observed flash rates on average. These results encourage the application of this scheme to larger radar data sets and its possible implementation into cloud‐resolving models.

As part of the Deep Convective Cloud and Chemistry (DC3) experiment, the National Science Foundation/National Center for Atmospheric Research (NCAR) Gulfstream-V (GV) and NASA DC-8 research aircraft probed the chemical composition of the inflow and outflow of two convective storms (north storm, NS, south storm, SS) originating in the Colorado region on 22 June 2012, a time when the High Park wildfire was active in the area. A wide range of trace species were measured on board both aircraft including biomass burning (BB) tracers hydrogen cyanide (HCN) and acetonitrile (ACN). Acrolein, a much shorter lived tracer for BB, was also quantified on the GV. The data demonstrated that the NS had ingested fresh smoke from the High Park fire and as a consequence had a higher VOC OH reactivity than the SS. The SS lofted aged fire tracers along with other boundary layer ozone precursors and was more impacted by lightning NO x (LNO x ) than the NS. The NCAR master mechanism box model was initialized with measurements made in the outflow of the two storms. The NS and SS were predicted to produce 11 and 14 ppbv of O 3 , respectively, downwind of the storm over 2 days. Sensitivity tests revealed that the ozone production potential of the SS was highly dependent on LNO x . Normalized excess mixing ratios, ΔX/ΔCO, for HCN and ACN were determined in both the fire plume and the storm outflow and found to be 7.0 ± 0.5 and 2.3 ± 0.5 pptv ppbv À1, respectively, and 1.4 ± 0.3 pptv ppbv À1 for acrolein in the outflow only.

Abstract. This study examines the occurrence and morphology of frozen-drop aggregates in thunderstorm anvils from the United States Midwest and describes the environmental conditions where they are found. In situ airborne data collected in anvils using several particle imaging and sizing probes and bulk total water instrumentation during the 2012 Deep Convective Clouds and Chemistry experiment are examined for the presence of frozen-drop aggregates. Chains of frozen drops have been only rarely reported before and are hypothesized to aggregate due to electrical forces in the clouds. They were identified in nine of the anvil cases examined to date, suggesting that they are common features in these Midwestern anvils. High concentrations of individual frozen droplets occurred on the tops and edges of one particular set of anvils, while regions closer to the center and bottom of these anvils exhibited fewer frozen drops and more frozen-drop aggregates. Bulk ice water content measurements across these anvils could only be explained by contributions from both small particles (frozen droplets) and large particles (large aggregates of frozen droplets). Dual Doppler radar analysis confirmed the presence of deep and strong (> 15 m s −1 ) updrafts in the parent cloud of one of the anvils. These features contrast with previous anvil measurements in tropical/maritime anvils that evidently do not exhibit the same frequency of frozen-drop aggregates.

Abstract. Quantifying the impacts of aerosols on climate requires a detailed knowledge of both the anthropogenic and the natural contributions to the aerosol population. Recent work has suggested a previously unrecognized natural source of ultrafine particles resulting from breaking waves at the surface of large freshwater lakes. This work is the first modeling study to investigate the potential for this newly discovered source to affect the aerosol number concentrations on regional scales. Using the WRF-Chem modeling framework, the impacts of wind-driven aerosol production from the surface of the Great Lakes were studied for a July 2004 test case. Simulations were performed for a base case with no lake surface emissions, a case with lake surface emissions included, and a default case wherein large freshwater lakes emit marine particles as if they were oceans. Results indicate that the lake surface emissions can enhance the surfacelevel aerosol number concentration by ∼20 % over the remote northern Great Lakes and by ∼5 % over other parts of the Great Lakes. These results were highly sensitive to the new particle formation (i.e., nucleation) parameterization within WRF-Chem; when the new particle formation process was deactivated, surface-layer enhancements from the lake emissions increased to as much as 200 %. The results reported here have significant uncertainties associated with the lake emission parameterization and the way ultrafine particles are modeled within WRF-Chem. Nevertheless, the magnitudes of the impacts found in this study suggest that further study to quantify the emissions of ultrafine particles from the surface of the Great Lakes is merited.

Quantifying the impacts of aerosols on climate requires a detailed knowledge of both the anthropogenic and the natural contributions to the aerosol population. Recent work has suggested a previously unrecognized natural source of ultrafine particles resulting from breaking waves at the surface of large freshwater lakes. This work is the first modeling study to investigate the potential for this newly discovered source to affect the aerosol number concentrations on regional scales. Using the WRF-Chem modeling framework, the impacts of wind-driven aerosol production from the surface of the Great Lakes were studied for a July 2004 test case. Simulations were performed for a base case with no lake surface emissions, a case with lake surface emissions included, and a default case wherein large freshwater lakes emit marine particles as if they were oceans. Results indicate that the lake surface emissions can enhance the surface level aerosol number concentration by ∼20 % over the remote northern Great Lakes and by ∼5 % over other parts of the Great Lakes. These results were highly sensitive the nucleation parameterization within WRF-Chem; when the nucleation process was deactivated, surface-layer enhancements from the lake emissions increased to as much as 200 %. The results reported here have significant uncertainties associated with the lake emission parameterization and the way ultrafine particles are modeled within WRF-Chem. Nevertheless, the magnitude of the impacts found in this study suggest that further study of this phenomena is merited