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The magnitude of solar radiative effects (cooling or warming) of black carbon (BC) particles embedded in the Arctic atmosphere and surface snow layer was explored on the basis of case studies. For this purpose, combined atmospheric and snow radiative transfer simulations were performed for cloudless and cloudy conditions on the basis of BC mass concentrations measured in pristine early summer and more polluted early spring conditions. The area of interest is the remote sea-ice-covered Arctic Ocean in the vicinity of Spitsbergen, northern Greenland, and northern Alaska typically not affected by local pollution. To account for the radiative interactions between the black-carbon-containing snow surface layer and the atmosphere, an atmospheric and snow radiative transfer model were coupled iteratively. For pristine summer conditions (no atmospheric BC, minimum solar zenith angles of 55 ∘) and a representative BC particle mass concentration of 5 ng g -1 in the surface snow layer, a positive daily mean solar radiative forcing of + 0.2 W m -2 was calculated for the surface radiative budget. A higher load of atmospheric BC representing early springtime conditions results in a slightly negative mean radiative forcing at the surface of about - 0.05 W m -2 , even when the low BC mass concentration measured in the pristine early summer conditions was embedded in the surface snow layer. The total net surface radiative forcing combining the effects of BC embedded in the atmosphere and in the snow layer strongly depends on the snow optical properties (snow specific surface area and snow density). For the conditions over the Arctic Ocean analyzed in the simulations, it was found that the atmospheric heating rate by water vapor or clouds is 1 to 2 orders of magnitude larger than that by atmospheric BC. Similarly, the daily mean total heating rate (6 K d -1) within a snowpack due to absorption by the ice was more than 1 order of magnitude larger than that of atmospheric BC (0.2 K d -1). Also, it was shown that the cooling by atmospheric BC of the near-surface air and the warming effect by BC embedded in snow are reduced in the presence of clouds. [ABSTRACT FROM AUTHOR]

Atmospheric aging promotes internal mixing of black carbon (BC), leading to an enhancement of light absorption and radiative forcing. The relationship between BC mixing state and consequent absorption enhancement was never estimated for BC found in the Arctic region. In the present work, we aim to quantify the absorption enhancement and its impact on radiative forcing as a function of microphysical properties and mixing state of BC observed in situ at the Zeppelin Arctic station (78° N) in the spring of 2012 during the CLIMSLIP (Climate impacts of short-lived pollutants in the polar region) project. Single-particle soot photometer (SP2) measurements showed a mean mass concentration of refractory black carbon (rBC) of 39 ngm-3, while the rBC mass size distribution was of lognormal shape, peaking at an rBC mass-equivalent diameter (DrBC) of around 240 nm. On average, the number fraction of particles containing a BC core with DrBC>80 nm was less than 5% in the size range (overall optical particle diameter) from 150 to 500 nm. The BC cores were internally mixed with other particulate matter. The median coating thickness of BC cores with 220 nm < DrBC < 260 nm was 52 nm, resulting in a core--shell diameter ratio of 1.4, assuming a coated sphere morphology. Combining the aerosol absorption coefficient observed with an Aethalometer and the rBC mass concentration from the SP2, a mass absorption cross section (MAC) of 9.8m² g-1 was inferred at a wavelength of 550 nm. Consistent with direct observation, a similar MAC value (8.4m² g-1 at 550 nm) was obtained indirectly by using Mie theory and assuming a coated-sphere morphology with the BC mixing state constrained from the SP2 measurements. According to these calculations, the lensing effect is estimated to cause a 54% enhancement of the MAC compared to that of bare BC particles with equal BC core size distribution. Finally, the ARTDECO radiative transfer model was used to estimate the sensitivity of the radiative balance to changes in light absorption by BC as a result of a varying degree of internal mixing at constant total BC mass. The clear-sky noontime aerosol radiative forcing over a surface with an assumed wavelength-dependent albedo of 0.76-0.89 decreased, when ignoring the absorption enhancement, by -0.12 W in m-2 compared to the base case scenario, which was constrained with mean observed aerosol properties for the Zeppelin site in Arctic spring. The exact magnitude of this forcing difference scales with environmental conditions such as the aerosol optical depth, solar zenith angle and surface albedo. Nevertheless, our investigation suggests that the absorption enhancement due to internal mixing of BC, which is a systematic effect, should be considered for quantifying the aerosol radiative forcing in the Arctic region. [ABSTRACT FROM AUTHOR]

The size and shape of snow grains directly impacts the reflection by a snowpack. In this article, different approaches to retrieve the optical-equivalent snow grain size ( r opt ) or, alternatively, the specific surface area (SSA) using satellite, airborne, and ground-based observations are compared and used to evaluate ICON-ART (ICOsahedral Nonhydrostatic—Aerosols and Reactive Trace gases) simulations. The retrieval methods are based on optical measurements and rely on the r opt -dependent absorption of solar radiation in snow. The measurement data were taken during a three-week campaign that was conducted in the North of Greenland in March/April 2018, such that the retrieval methods and radiation measurements are affected by enhanced uncertainties under these low-Sun conditions. An adjusted airborne retrieval method is applied which uses the albedo at 1700 nm wavelength and combines an atmospheric and snow radiative transfer model to account for the direct-to-global fraction of the solar radiation incident on the snow. From this approach, we achieved a significantly improved uncertainty (<25%) and a reduced effect of atmospheric masking compared to the previous method. Ground-based in situ measurements indicated an increase of r opt of 15 µm within a five-day period after a snowfall event which is small compared to previous observations under similar temperature regimes. ICON-ART captured the observed change of r opt during snowfall events, but systematically overestimated the subsequent snow grain growth by about 100%. Adjusting the growth rate factor to 0.012 µm 2 s − 1 minimized the difference between model and observations. Satellite-based and airborne retrieval methods showed higher r opt over sea ice (<300 µm) than over land surfaces (<100 µm) which was reduced by data filtering of surface roughness features. Moderate-Resolution Imaging Spectroradiometer (MODIS) retrievals revealed a large spread within a series of subsequent individual overpasses, indicating their limitations in observing the snow grain size evolution in early spring conditions with low Sun. [ABSTRACT FROM AUTHOR]