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The aim of this study is to assess the probability of black carbon (BC) transfer from high-intensity model forest fires in the taiga zone, determine the fields of concentrations and deposition of BC on the ice–snow surface, and assess the BC contribution to climate change in the Arctic. Model regions with the highest probability of large forest fires (the Komi Republic, Krasnoyarsk krai, and the Republic of Sakha (Yakutia)) are selected based on an analysis of remote monitoring data. The probability of a BC cloud from model fires transferring to the snowy-ice surface of the Arctic is analyzed using the HYSPLIT trajectory model. The probability of a particle emitted from the boreal taiga zone to traverse the sea ice-covered part of the Arctic Ocean is found to be between 1–10%. Effects of BC (the balance of shortwave radiation) on the Arctic climate are estimated on the basis of global climate model of the Institute of Numerical Mathematics Russian Academy of Sciences (INM RAS). According to the results of model experiments, the effect of BC on the balance of shortwave radiation from all model fires in the Northern Hemisphere is 0.11 W m–2 under cloudy conditions and 0.21 W m–2 in a clear sky. The estimated effect on the shortwave radiation balance is a 1.5–2% larger income when compared to the scenario without emission sources. The simulation results showed that the effect of BC emissions from forest fires on the ice-covered Arctic region is negligible. [ABSTRACT FROM AUTHOR]

Black carbon (BC) aerosol particles in the Arctic heat the atmosphere and snow/ice surfaces and may strengthen the snow-albedo feedback that amplifies Arctic warming. Model simulations of BC concentrations in the Arctic depend strongly on the representation of microphysical processes such as aging, activation, and wet removal. Most BC modeling studies have classified BC particles into hydrophobic BC, which cannot form cloud droplets, and hydrophilic BC, which can form cloud droplets, by assuming a globally constant critical supersaturation threshold value (Sthre), without considering its consistency with cloud maximum supersaturation (Smax). Here we show that it is essential to consider the consistency of Sthre with Smax in global model simulations to reduce uncertainties in near-surface ambientBCconcentrations in the Arctic. Previous studies often obtained good agreement between simulated and observed near-surface Arctic BC mass concentrations when a low Sthre (;0.1%) was assumed in their models. However, this Sthre may be too low (activation and wet removal of BCmay be underestimated) for the Arctic, because some recent observations and our model simulations suggest that Smax may actually be higher (;0.3%) there. We also demonstrate that spatially varying Sthre values and their consistency with Smax, which previous studies did not consider, must be represented in models for more accurate estimation of BC budget in the Arctic. Because both Smax and BC-aging speed depend on climatic conditions, our findings are an important step toward better simulations of BC impacts on past, present, and future Arctic climates. [ABSTRACT FROM AUTHOR]

There is ample evidence that Black Carbon (BC) is harmful to the Arctic. BC can darken the otherwise highly reflective surfaces of snow and ice and increase atmospheric and ice surface temperatures. Because of the importance of BC to the Arctic, this work was designed to resolve the most significant source regions of Arctic BC as measured by monitoring stations in the Arctic. Using a bottom‐up approach, it is shown for the first time that there is one particular BC transport pathway from lower latitudes into the Arctic that registers at all but one of the Arctic surface monitoring stations included in this study. Through this pathway, pollutants are transported from the Indo‐Gangetic plane over Central Asia into the high Arctic in as little as 7 days. The measurement sites and BC pathways in this study are shown to be well representative of the Arctic as a whole. Plain Language Summary: Snow and sea ice are two of the most reflective surfaces occurring naturally on planet Earth. Light absorbing aerosols, such as wind blown black carbon, that stick to these pristine surfaces can make them less reflective, thus converting more sunlight into heat. The added heat leads to increased surface temperatures and is detrimental to the Arctic climate. There are few sources of light absorbing aerosols in the Arctic compared to the vast amounts of black carbon aerosols that are emitted closer to the equator. This research highlights an important pathway for light absorbing aerosols to enter the Arctic. Light absorbing aerosols that enter the Arctic through this pathway can then subsequently spread out throughout the Arctic. This pathway is shown to transport light absorbing airborne pollutants from South Asia, over Central Asia, and into the high Arctic in quantities that well exceed the background levels, thus highlighting the importance of this newly found pathway. Key Points: Black Carbon aerosols can travel from South Asia over Central Asia and to the Arctic in 7 daysBlack Carbon transported via this pathway measures well above the station average at almost all Arctic stationsThe identified pathway is significant for Black Carbon concentrations throughout the Arctic [ABSTRACT FROM AUTHOR]

In this study we introduce an in-cloud wet deposition scheme for liquid and ice phase clouds for global aerosol–climate models which use a size-segregated aerosol description. For in-cloud nucleation scavenging, the scheme uses cloud droplet activation and ice nucleation rates obtained from the host model. For in-cloud impaction scavenging, we used a method where the removal rate depends on the wet aerosol size and cloud droplet radii. We used the latest release version of ECHAM-HAMMOZ (ECHAM6.3-HAM2.3-MOZ1.0) with the Sectional Aerosol module for Large Scale Applications version 2.0 (SALSA) microphysics package to test and compare our scheme. The scheme was compared to a scheme that uses fixed scavenging coefficients. The comparison included vertical profiles and mass and number distributions of wet deposition fluxes of different aerosol compounds and for different latitude bands. Using the scheme presented here, mass concentrations for black carbon, organic carbon, sulfate, and the number concentration of particles with diameters larger than 100 nm are higher than using fixed scavenging coefficients, with the largest differences in the vertical profiles in the Arctic. On the other hand, the number concentrations of particles smaller than 100 nm in diameter show a decrease, especially in the Arctic region. These results could indicate that, compared to fixed scavenging coefficients, nucleation scavenging is less efficient, resulting in an increase in the number concentration of particles larger than 100 nm. In addition, changes in rates of impaction scavenging and new particle formation (NPF) can be the main cause of reduction in the number concentrations of particles smaller than 100 nm. Without further adjustments in the host model, our wet deposition scheme produced unrealistically high aerosol concentrations, especially at high altitudes. This also leads to a spuriously long lifetime of black carbon aerosol. To find a better setup for simulating aerosol vertical profiles and transport, sensitivity simulations were conducted where aerosol emission distribution and hygroscopicity were altered. Vertical profiles of aerosol species simulated with the scheme which uses fixed scavenging rates and the abovementioned sensitivity simulations were evaluated against vertical profiles from aircraft observations. The lifetimes of different aerosol compounds were also evaluated against the ensemble mean of models involved in the Aerosol Comparisons between Observations and Models (AEROCOM) project. The best comparison between the observations and the model was achieved with our wet deposition scheme when black carbon was emitted internally mixed with soluble compounds instead of keeping it externally mixed. This also produced atmospheric lifetimes for the other species which were comparable to the AEROCOM model means. [ABSTRACT FROM AUTHOR]

The representation of aerosol activation into cloud droplets in climate models is important for accurate understanding of aerosol radiative impacts on the Arctic climate, but it remains highly uncertain. Here we show that the uncertainty range of subgrid vertical velocity (SVV) and maximum supersaturation (SSmax) in aerosol activation produces fourfold to fivefold differences in the direct radiative effect of black carbon (BC) in the Arctic (0.091–0.40 W m−2) because SVV and SSmax determine the activated fraction and wet removal efficiency of aerosols. Aerosols are particularly sensitive to SVV in remote regions but not near their sources because many aerosols near sources are not yet influenced by wet removal processes. Our results demonstrate that SVV treatment is a major source of uncertainty in Arctic aerosol simulations and may be key for reducing the large discrepancies among global models in estimates of BC and its radiative effects in the Arctic. Plain Language Summary: Black carbon aerosol, emitted mainly in midlatitude regions by combustion of fossil fuel and biomass, is transported to the Arctic and deposited on snow and ice surfaces, where it contributes to Arctic heating. However, estimates of its importance in Arctic warming have large uncertainties. Because global climate models usually use a coarse horizontal grid spacing, they rely on many assumptions to represent the small‐scale atmospheric processes within clouds. This study uses a global climate model to investigate the importance of one of these assumptions, the treatment of "subgrid vertical velocity," to aerosol simulations. We show that varying the subgrid vertical velocity within its uncertainty range changes the calculated heating effect of black carbon in the Arctic by as much as five times. Our results underscore the importance of treating subgrid vertical velocity treatment accurately in estimating how much black carbon from midlatitudes is warming the Arctic. Key Points: The importance of subgrid vertical velocity in activation to aerosol burden and radiative effects was investigated by using a global modelThe current uncertainty in subgrid vertical velocity produces fivefold differences in the radiative effect of black carbon in the ArcticThe subgrid treatment of updraft is important in estimating the long‐range transport of black carbon and its impacts on Arctic climate [ABSTRACT FROM AUTHOR]

In this study we introduce an in-cloud wet deposition scheme for liquid and ice phase clouds for global aerosol-climate models which use a size-segregated aerosol description. For in-cloud nucleation scavenging, the scheme uses cloud droplet activation and ice nucleation rates obtained from the host model. For in-cloud impaction scavenging, we used a method where the removal rate depends on the aerosol size and cloud droplet radii. The scheme was compared to a scheme that uses fixed scavenging coefficients. The comparison included vertical profiles and mass and number distributions of wet deposition fluxes of different aerosol compounds and for different latitude bands. Using the scheme presented here, mass concentrations for black carbon, organic carbon, sulfate, and the number concentration of particles with diameters larger than 100nm are higher than using fixed scavenging coefficients, with the largest differences in the vertical profiles in the Arctic. On the other hand, the number concentrations of small particles show a decrease, especially in the Arctic region. These results indicate that, compared to using fixed scavenging coefficients, nucleation scavenging is less efficient and impaction scavenging is increased in the scheme introduced here. Without further adjustments in the host model, our wet deposition scheme produced unrealistically high aerosol concentrations, especially at high altitudes. This also leads to a spuriously long lifetime of black carbon aerosol. To find a better setup for simulating aerosol vertical profiles and transport, sensitivity simulations were conducted where aerosol emission distribution and hygroscopicity were altered. The simulated vertical profiles of aerosol in these sensitivity studies were evaluated against aircraft observations. The lifetimes of different aerosol compounds were also evaluated against the ensemble mean of models involved in the Aerosol Comparisons between Observations and Models (AEROCOM) project. The best comparison between the observations and the model was achieved with the new wet deposition scheme when black carbon was emitted internally mixed with soluble compounds instead of keeping it externally mixed. This also produced atmospheric lifetimes for the other species which were comparable to the AEROCOM model means. [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]

Two months (Oct.–Nov. 2015) of online elemental carbon (EC) and organic carbon (OC) measurements were performed by two field OC/EC Sunset Laboratory analysers working in parallel with an 8-h time resolution at a subarctic remote station in Finland. During such a time resolution, thermal OC and EC concentrations were usually close to or below the recent limits of detection for the analyser. Thus, this work highlights the possible issues to consider during the online measurements of OC/EC analysers working at the threshold of their analytical possibilities. A detailed analysis of the data showed that even though the OC concentrations were always above the detection limit of the analyser, up to 70% of the given concentration was due to the dynamic blank (gaseous phase). The majority of the OC aerosol was present in the less volatile fractions that evolved during steps at 300–450 °C and 450–650 °C. The main bias at low EC concentrations originated from the automatically determined split point between OC and EC. The results from the RTCalc526 software often led to an early determination of the OC-EC split point, resulting in an overestimation of the EC concentrations. However, the comparison of the results was performed after processing the OC/EC raw data in the different RTCalc software versions 526 and 703. The results showed that the EC values from the newer version of the RTCalc703 software were more consistent with the equivalent black carbon (eBC) results from optical instruments (aethalometer and MAAP) measured in parallel in comparison with results from the older RTCalc526 software. Equivalent BC data from the laser attenuation measurement of the Sunset Lab. analyser also provided better agreement with the newer version of the RTCalc software (RTCalc703). Image 1 • A major part of the organic carbon (OC) was present in the less volatile fractions. • Up to 70% of the OC concentration was caused by a contribution of the dynamic blank (gaseous phase). • The elemental carbon (EC) results were overestimated in the earlier RTCalc526 evaluation software. • The updated RTCalc703 software provides reasonable results for very low EC concentrations. • The EC results are comparable to the parallel measurements of the equivalent black carbon. [ABSTRACT FROM AUTHOR]