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Models assume that mixed‐phase clouds consist of uniformly mixed ice crystals and liquid cloud droplets when observations have shown that they consist of clusters, or "pockets," of ice crystals and liquid cloud droplets. We characterize the spatial distribution of cloud phase over the Arctic and the Southern Ocean using active satellite observations and determine the relative importance of collocated meteorological parameters and aerosols from reanalysis to predict how uniformly mixed mixed‐phase clouds are for the first time. We performed a multi‐linear regression fit to the data set to predict the spatial distribution of the ice and liquid pockets. Contrary to what models suggest, mixed‐phase clouds are rarely perfectly homogeneous. Our results suggest that high temperatures are associated with homogeneously mixed ice and liquid pockets. We also find that a high mixing ratio of black carbon is associated with heterogeneously mixed ice and liquid pockets. Plain Language Summary: The representation of clouds in numerical models remains one of the largest uncertainties in predicting our future climate. Clouds can consist solely of liquid droplets, ice crystals, or the coexistence of both hydrometeor types. The latter cloud type is referred to as mixed phase. Climate models assume that liquid droplets and ice crystals are uniformly mixed in space in mixed‐phase clouds, but observations show that mixed‐phase clouds are organized in separate pockets of clustered liquid droplets and ice crystals. This difference in representation has a large impact on the lifetime of clouds and on their role in climate change. Using satellite observations over the Arctic and the Southern Ocean, we quantify the spatial distribution of ice and liquid in clouds. We used a statistical method to determine the relationship between meteorology and aerosols and the spatial distribution of ice and liquid. Our results suggest that high temperatures are associated with homogeneously mixed mixed‐phase clouds and high concentrations of soot are associated with heterogeneously mixed mixed‐phase clouds. Furthermore, pockets of liquid within ice clouds are larger than pockets of ice within liquid clouds. These results will improve the representation of mixed‐phase clouds in large‐scale models. Key Points: Space‐based observations and reanalysis are considered to determine the factors that control how mixed mixed‐phase clouds areLiquid dominated clouds contain small and isolated ice pockets whereas ice dominated clouds contain large and isolated liquid pocketsTemperature and black carbon play an important role in controlling the cloud phase spatial distribution and increasing phase heterogeneity [ABSTRACT FROM AUTHOR]

Atmospheric transport of aerosols such as black carbon (BC) affects the absorption/scattering of solar radiation, precipitation, and snow/ice cover, especially in areas of low human activity such as the Arctic. The resolution dependency of simulated BC transport from Siberia to the Arctic, related to the well-developed low-pressure systems in September, was evaluated using the Nonhydrostatic Icosahedral Atmospheric Model-Spectral Radiation Transport Model for Aerosol Species (NICAM-SPRINTARS) with fine (~ 56 km) and coarse (~ 220 km) horizontal resolutions. These low-pressure systems have a large horizontal scale (~ 2000 km) with the well-developed central pressure located on the transport pathway from East Asia to the Arctic through Siberia. In recent years, the events analysis of the most developed low-pressure system indicated that the high-BC area in the Bering Sea observed by the Japanese research vessel Mirai on September 26 - 27, 2016, moved to the Arctic with a filamental structure from the low's center to the behind of the cold front and ahead of the warm front in relation to its ascending motion on September 27 - 28, 2016. The composite analysis for the developed low-pressure events in September from 2015 to 2018 indicated that the high-BC area was located eastward of the low's center in relation to the ascending motion over the low's center and northward/eastward area. Since the area of the maximum ascending motion has a small horizontal scale, this was not well simulated by the 220-km experiment. The study identified that the BC transport to the Arctic in September is enhanced by the well-developed low-pressure systems. The results of the transport model indicate that the material transport processes to the Arctic by the well-developed low-pressure systems are enhanced in the fine horizontal resolution (~ 56 km) models relative to the coarse horizontal resolution (~ 220 km) models. [ABSTRACT FROM AUTHOR]

Wet processes, including aqueous-phase chemistry, wet scavenging, and wet surface uptake during dry deposition, are important for global modeling of aerosols and aerosol precursors. In this study, we improve the treatments of these wet processes in the Goddard Earth Observing System with chemistry (GEOS-Chem) v12.6.0, including pH calculations for cloud, rain, and wet surfaces, the fraction of cloud available for aqueous-phase chemistry, rainout efficiencies for various types of clouds, empirical washout by rain and snow, and wet surface uptake during dry deposition. We compare simulated surface mass concentrations of aerosols and aerosol precursors with surface monitoring networks over the United States, European, Asian, and Arctic regions, and show that model results with updated wet processes agree better with measurements for most species. With the implementation of these updates, normalized mean biases (NMBs) of surface nitric acid, nitrate, and ammonium are reduced from 78 %, 126 %, and 45 % to 0.9 %, 15 %, and 4.1 % over the US sites, from 107 %, 127 %, and 90 % to -0.7 %, 4.2 %, and 16 % over European sites, and from 121 %, 269 %, and 167 % to -21 %, 37 %, and 86 % over Asian remote region sites. Comparison with surface measured SO2 , sulfate, and black carbon at four Arctic sites indicated that those species simulated with the updated wet processes match well with observations except for a large underestimate of black carbon at one of the sites. We also compare our model simulation with aircraft measurement of nitric acid and aerosols during the Atmospheric Tomography Mission (ATom)-1 and ATom-2 periods and found a significant improvement of modeling skill of nitric acid, sulfate, and ammonium in the Northern Hemisphere during wintertime. The NMBs of these species are reduced from 163 %, 78 %, and 217 % to -13 %, -1 %, and 10 %, respectively. The investigation of impacts of updated wet process treatments on surface mass concentrations indicated that the updated wet processes have strong impacts on the global means of nitric acid, sulfate, nitrate, and ammonium and relative small impacts on the global means of sulfur dioxide, dust, sea salt, black carbon, and organic carbon. [ABSTRACT FROM AUTHOR]

Snow samples obtained at 36 sites in Alaska, Canada, Greenland, Russia, and the Arctic Ocean in early 2007 were analyzed for light-absorbing aerosol concentration together with a suite of associated chemical species. The light absorption data, interpreted as black carbon concentrations, and other chemical data were input into the EPA PMF 1:1 receptor model to explore the sources for black carbon in the snow. The analysis found four factors or sources: two distinct biomass burning sources, a pollution source, and a marine source. The first three of these were responsible for essentially all of the black carbon, with the two biomass sources (encompassing both open and closed combustion) together accounting for >90% of the black carbon. [ABSTRACT FROM AUTHOR]