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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]

Black carbon (BC), the most efficient atmospheric aerosol for absorbing light in the visible spectrum, exerts a warming effect on a region undergoing unprecedented climatic changes. Here, BC is studied indirectly using filter-based methods to ascertain aerosol light absorption parameters. We investigated long-term changes using a harmonised 21-year data set of light absorption measurements, in conjunction with air mass source analysis. The measurements were performed at Zeppelin Observatory (ZEP), Svalbard, from 2002 to 2022. We report a statistically significant (s.s.) decreasing long-term trend for the light absorption coefficient, measured at the site for the entirety of the data set. However, the last 7 years, 2016–2022, showed a slightly increasing s.s. trend for the haze season. In addition, we observed an increasing trend in the single scattering albedo from 2002 to 2022. Five distinct source regions were identified; the trends involving air masses from the five regions showed decreasing absorption coefficients, except for the air masses influenced by emissions from Eurasia. We show that the changes in the occurrences of each transport pathway cannot explain the reductions in the absorption coefficient observed at the Zeppelin station; an increase in contributions of air masses from more marine regions, with lower absorption coefficients, is compensated by the influence from high-emission regions. Along with aerosol optical properties, we also show an increasing trend in accumulated surface precipitation experienced by air masses en route to the Zeppelin Observatory. We argue that rainfall, as a sink of aerosol, plays a role in the long-term trends in the absorption coefficient, explaining approximately a quarter of the overall trend. A decreasing trend in the scavenging ratio further suggests an increase in the aerosol removal processes. We note that there is an increasing potential influence from active forest fires, particularly in the last few summers (i.e. 2015–2022). Active fires have been shown to have a significant impact on the mean seasonal absorption coefficient especially during northern hemispheric summer. However, no noticeable alteration in annual long-term trends can be observed. [ABSTRACT FROM AUTHOR]

Black carbon (BC) absorbs solar radiation, increasing the buoyancy and vertical ascent of absorbing aerosol in the atmosphere. This self‐lofting process has been observed for individual plumes in the troposphere and lower stratosphere but here we show it occurring at broader scales through enhanced large‐scale ascent over BC‐rich regions. This is demonstrated in a pair of simulation using the UKESM1 Earth‐System model where BC aerosols were modeled either with or without the ability to absorb radiation. With absorption included the annual global mean concentration of BC in the upper troposphere and lower stratosphere (8–22 km) rose by up to 50% and the column loading over some remote oceanic regions more than doubled. The increase in aerosol height was particularly notable over the southeast Atlantic where biomass burning aerosol from Africa was elevated up to 1 km higher when their absorption was included. Similar effects were seen over the Arctic where the absorbing haze was transported in at higher levels and surface concentrations were halved. The absorption by BC also increased ascent over southern Asia, which tended to thicken the Asian brown cloud during the dry season but in the wet season enhancing ascent promoted deep convection and had the tendency to deplete the aerosol through wash‐out. We conclude that representing aerosol absorption accurately is important in simulating the vertical distribution, transport and abundance of aerosol in the Earth‐system that will affect their interactions with climate. Plain Language Summary: Black carbon is an important component of atmospheric aerosols as it absorbs solar radiation thereby heating the atmosphere and potentially warming climate. The localized heating can also affect clouds and atmospheric motions making the regional and climate effects more complex and uncertain. The vertical distribution and geographic spread of the aerosol is also key to how it interacts with the climate system. In this paper we highlight the fact that the absorption taking place in BC aerosols can affect its vertical ascent in the atmosphere and therefore how it becomes distributed across the globe. This self‐lofting process was demonstrated in a climate model and was particularly important in aiding the elevation and downwind transport of absorbing smoke layers from regions such as central Africa, as well as increasing the amount of BC reaching the upper troposphere and lower stratosphere. Key Points: Absorption of solar radiation helps to raise the altitude of black carbon aerosol by increasing buoyancy and vertical ascentThis self‐lofting mechanism has been captured in a climate model where radiative heating affects the large‐scale ascent and circulationSelf‐lofting increased the altitude and long‐range transport of black carbon to remote regions and the upper troposphere [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]