A set of parameterizations is developed for spectral single-scattering properties of clean and black carbon (BC)-contaminated snow based on geometric-optics surface wave (GOS) computations, which explicitly resolves BC–snow internal mixing and various snow grain shapes. GOS calculations show that, compared with nonspherical grains, volume-equivalent snow spheres show up to 20% larger asymmetry factors and hence stronger forward scattering, particularly at wavelengths <1 μm. In contrast, snow grain sizes have a rather small impact on the asymmetry factor at wavelengths <1 μm, whereas size effects are important at longer wavelengths. The snow asymmetry factor is parameterized as a function of effective size, aspect ratio, and shape factor and shows excellent agreement with GOS calculations. According to GOS calculations, the single-scattering coalbedo of pure snow is predominantly affected by grain sizes, rather than grain shapes, with higher values for larger grains. The snow single-scattering coalbedo is parameterized in terms of the effective size that combines shape and size effects, with an accuracy of >99%. Based on GOS calculations, BC–snow internal mixing enhances the snow single-scattering coalbedo at wavelengths <1 μm, but it does not alter the snow asymmetry factor. The BC-induced enhancement ratio of snow single-scattering coalbedo, independent of snow grain size and shape, is parameterized as a function of BC concentration with an accuracy of >99%. Overall, in addition to snow grain size, both BC–snow internal mixing and snow grain shape play critical roles in quantifying BC effects on snow optical properties. The present parameterizations can be conveniently applied to snow, land surface, and climate models including snowpack radiative transfer processes.

Abstract. We implement a set of new parameterizations into the widely used Snow, Ice, and Aerosol Radiative (SNICAR) model to account for effects of snow grain shape (spherical vs. nonspherical) and black carbon (BC)–snow mixing state (external vs. internal). We find that nonspherical snow grains lead to higher pure albedo but weaker BC-induced albedo reductions relative to spherical snow grains, while BC–snow internal mixing significantly enhances albedo reductions relative to external mixing. The combination of snow nonsphericity and internal mixing suggests an important interactive effect on BC-induced albedo reduction. Comparisons with observations of clean and BC-contaminated snow albedo show that model simulations accounting for both snow nonsphericity and BC–snow internal mixing perform better than those using the common assumption of spherical snow grains and external mixing. We further apply the updated SNICAR model with comprehensive in situ measurements of BC concentrations in the Tibetan Plateau snowpack to quantify the present-day (2000–2015) BC-induced snow albedo effects from a regional and seasonal perspective. The BC concentrations show distinct and substantial sub-regional and seasonal variations, with higher values in the non-monsoon season and low altitudes. As a result, the BC-induced regional mean snow albedo reductions and surface radiative effects vary by up to an order of magnitude across different sub-regions and seasons, with values of 0.7–30.7 and 1.4–58.4 W m−2 for BC externally mixed with fresh and aged snow spheres, respectively. The BC radiative effects are further complicated by uncertainty in snow grain shape and BC–snow mixing state. BC–snow internal mixing enhances the mean albedo effects over the plateau by 30–60 % relative to external mixing, while nonspherical snow grains decrease the mean albedo effects by up to 31 % relative to spherical grains. Based on this study, extensive measurements and improved model characterization of snow grain shape and aerosol–snow mixing state are urgently needed in order to precisely evaluate BC–snow albedo effects.

A stochastic approach has been developed to model the positions of BC (black carbon)/dust internally mixed with two snow grain types: hexagonal plate/column (convex) and Koch snowflake (concave). Subsequently, light absorption and scattering analysis can be followed by means of an improved geometric-optics approach coupled with Monte Carlo photon tracing to determine BC/dust single-scattering properties. For a given shape (plate, Koch snowflake, spheroid, or sphere), the action of internal mixing absorbs substantially more light than external mixing. The snow grain shape effect on absorption is relatively small, but its effect on asymmetry factor is substantial. Due to a greater probability of intercepting photons, multiple inclusions of BC/dust exhibit a larger absorption than an equal-volume single inclusion. The spectral absorption (0.2-5 μm) for snow grains internally mixed with BC/dust is confined to wavelengths shorter than about 1.4 μm, beyond which ice absorption predominates. Based on the single-scattering properties determined from stochastic and light absorption parameterizations and using the adding/doubling method for spectral radiative transfer, we find that internal mixing reduces snow albedo substantially more than external mixing and that the snow grain shape plays a critical role in snow albedo calculations through its forward scattering strength. Also, multiple inclusion of BC/dust significantly reduces snow albedo as compared to an equal-volume single sphere. For application to land/snow models, we propose a two-layer spectral snow parameterization involving contaminated fresh snow on top of old snow for investigating and understanding the climatic impact of multiple BC/dust internal mixing associated with snow grain metamorphism, particularly over mountain/snow topography.

We estimate the snow albedo forcing and direct radiative forcing (DRF) of black carbon (BC) in the Tibetan Plateau using a global chemical transport model in conjunction with a stochastic snow model and a radiative transfer model. The annual mean BC snow albedo forcing is 2.9 W m À2 averaged over snow-covered plateau regions, which is a factor of 3 larger than the value over global land snowpack. BC-snow internal mixing increases the albedo forcing by 40-60% compared with external mixing, and coated BC increases the forcing by 30-50% compared with uncoated BC aggregates, whereas Koch snowflakes reduce the forcing by 20-40% relative to spherical snow grains. The annual BC DRF at the top of the atmosphere is 2.3 W m À2 with uncertainties of À70-85% in the plateau after scaling the modeled BC absorption optical depth to Aerosol Robotic Network observations. The BC forcings are attributed to emissions from different regions.

Light-absorbing carbonaceous aerosols (LACs), including black carbon and light-absorbing organic carbon (brown carbon, BrC), have an important role in the Earth system via heating the atmosphere, dimming the surface, modifying the dynamics, reducing snow/ice albedo, and exerting positive radiative forcing. The lifecycle of LACs, from emission to atmospheric evolution further to deposition, is key to their overall climate impacts and uncertainties in determining their hygroscopic and optical properties, atmospheric burden, interactions with clouds, and deposition on the snowpack. At present, direct observations constraining some key processes during the lifecycle of LACs (e.g., interactions between LACs and hydrometeors) are rather limited. Large inconsistencies between directly measured LAC properties and those used for model evaluations also exist. Modern models are starting to incorporate detailed aerosol microphysics to evaluate transformation rates of water solubility, chemical composition, optical properties, and phases of LACs, which have shown improved model performance. However, process-level understanding and modeling are still poor particularly for BrC, and yet to be sufficiently assessed due to lack of global-scale direct measurements. Appropriate treatments of size- and composition-resolved processes that influence both LAC microphysics and aerosol–cloud interactions are expected to advance the quantification of aerosol light absorption and climate impacts in the Earth system. This review summarizes recent advances and up-to-date knowledge on key processes during the lifecycle of LACs, highlighting the essential issues where measurements and modeling need improvement.

Abstract. We develop and examine a microphysics-based black carbon (BC) aerosol aging scheme that accounts for condensation, coagulation, and heterogeneous chemical oxidation processes in a global 3-D chemical transport model (GEOS-Chem) by interpreting the BC measurements from the HIAPER Pole-to-Pole Observations (HIPPO, 2009–2011) using the model. We convert aerosol mass in the model to number concentration by assuming lognormal aerosol size distributions and compute the microphysical BC aging rate (excluding chemical oxidation aging) explicitly from the condensation of soluble materials onto hydrophobic BC and the coagulation between hydrophobic BC and preexisting soluble particles. The chemical oxidation aging is tested in the sensitivity simulation. The microphysical aging rate is  ∼  4 times higher in the lower troposphere over source regions than that from a fixed aging scheme with an e-folding time of 1.2 days. The higher aging rate reflects the large emissions of sulfate–nitrate and secondary organic aerosol precursors hence faster BC aging through condensation and coagulation. In contrast, the microphysical aging is more than 5-fold slower than the fixed aging in remote regions, where condensation and coagulation are weak. Globally, BC microphysical aging is dominated by condensation, while coagulation contribution is largest over eastern China, India, and central Africa. The fixed aging scheme results in an overestimate of HIPPO BC throughout the troposphere by a factor of 6 on average. The microphysical scheme reduces this discrepancy by a factor of  ∼  3, particularly in the middle and upper troposphere. It also leads to a 3-fold reduction in model bias in the latitudinal BC column burden averaged along the HIPPO flight tracks, with largest improvements in the tropics. The resulting global annual mean BC lifetime is 4.2 days and BC burden is 0.25 mg m−2, with 7.3 % of the burden at high altitudes (above 5 km). Wet scavenging accounts for 80.3 % of global BC deposition. We find that, in source regions, the microphysical aging rate is insensitive to aerosol size distribution, condensation threshold, and chemical oxidation aging, while it is the opposite in remote regions, where the aging rate is orders of magnitude smaller. As a result, global BC burden and lifetime show little sensitivity (< 5 % change) to these three factors.

Aerosol-cloud interactions (aerosol indirect effects) play an important role in regional meteorological variations, which could further induce feedback on regional air quality. While the impact of aerosol-cloud interactions on meteorology and climate has been extensively studied, their feedback on air quality remains unclear. Using a fully coupled meteorology-chemistry model, we find that increased aerosol loading due to anthropogenic activities in China substantially increases column cloud droplet number concentration and liquid water path (LWP), which further leads to a reduction in the downward shortwave radiation at surface, surface air temperature and planetary boundary layer (PBL) height. The shallower PBL and accelerated cloud chemistry due to larger LWP in turn enhance the concentrations of particulate matter with diameter less than 2.5 μm (PM2.5) by up to 33.2 μg m−3 (25.1%) and 11.0 μg m−3 (12.5%) in January and July, respectively. Such a positive feedback amplifies the changes in PM2.5 concentrations, indicating an additional air quality benefit under effective pollution control policies but a penalty for a region with a deterioration in PM2.5 pollution. Additionally, we show that the cloud processing of aerosols, including wet scavenging and cloud chemistry, could also have substantial effects on PM2.5 concentrations.

We extend a stochastic aerosol-snow albedo model to explicitly simulate dust internally/ externally mixed with snow grains of different shapes and for the first time quantify the combined effects of dust-snow internal mixing and snow nonsphericity on snow optical properties and albedo. Dust-snow internal/external mixing significantly enhances snow single-scattering coalbedo and absorption at wavelengths of <1.0 μm, with stronger enhancements for internal mixing (relative to external mixing) and higher dust concentrations but very weak dependence on snow size and shape variabilities. Compared with pure snow, dust-snow internal mixing reduces snow albedo substantially at wavelengths of <1.0 μm, with stronger reductions for higher dust concentrations, larger snow sizes, and spherical (relative to nonspherical) snow shapes. Compared to internal mixing, dust-snow external mixing generally shows similar spectral patterns of albedo reductions and effects of snow size and shape. However, relative to external mixing, dust-snow internal mixing enhances the magnitude of albedo reductions by 10%-30% (10%-230%) at the visible (near-infrared) band. This relative enhancement is stronger as snow grains become larger or nonspherical, with comparable influences from snow size and shape. Moreover, for dust-snow external and internal mixing, nonspherical snow grains have up to~45% weaker albedo reductions than spherical grains, depending on snow size, dust concentration, and wavelength. The interactive effect of dust-snow mixing state and snow shape highlights the importance of accounting for these two factors concurrently in snow modeling. For application to land/climate models, we develop parameterizations for dust effects on snow optical properties and albedo with high accuracy.Plain Language Summary Mineral dust is one of the most common and abundant aerosols by mass, playing a key role in the Earth/climate system. Dust can significantly reduce snow albedo and accelerate snow/glacier melting after deposition. Previous modeling studies have mainly assumed dust mixed outside spherical snow grains, whereas in reality dust can also be mixed inside nonspherical snow grains. Thus, it is imperative to understand and quantify the effects of dust-snow mixing type (outside vs. inside snow grains) and snow grain shape (spherical vs. nonspherical) on snow albedo. This study uses an advanced snow albedo model to simulate dust mixed with snow grains of different shapes. Results show that dust mixed with snow grains can enhance snow absorption of sunlight and hence reduce snow albedo. Dust reduces snow albedo more when mixed inside snow grains than when mixed outside snow grains, while dust reduces snow albedo less when mixed with nonspherical snow grains than when mixed with spherical snow grains. This intertwined effect from dust-snow mixing type and snow shape highlights the importance of including these two factors simultaneously in snow models. This study further develops parameterizations to account for dust effects on snow albedo for co...