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.

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.

We perform a comprehensive intercomparison of the geometric-optics surface-wave (GOS) approach, the superposition T-matrix method, and laboratory measurements for optical properties of fresh and coated/aged black carbon (BC) particles with complex structures. GOS and T-matrix calculations capture the measured optical (i.e., extinction, absorption, and scattering) cross sections of fresh BC aggregates, with 5-20% differences depending on particle size. We find that the T-matrix results tend to be lower than the measurements, due to uncertainty in theoretical approximations of realistic BC structures, particle property measurements, and numerical computations in the method. On the contrary, the GOS results are higher than the measurements (hence the T-matrix results) for BC radii < 100 nm, because of computational uncertainty for small particles, while the discrepancy substantially reduces to 10% for radii > 100 nm. We find good agreement (differences < 5%) between the two methods in asymmetry factors for various BC sizes and aggregating structures. For aged BC particles coated with sulfuric acid, GOS and T-matrix results closely match laboratory measurements of optical cross sections. Sensitivity calculations show that differences between the two methods in optical cross sections vary with coating structures for radii < 100 nm, while differences decrease to ~10% for radii > 100 nm. We find small deviations (≤ 10%) in asymmetry factors computed from the two methods for most BC coating structures and sizes, but several complex structures have 10-30% differences. This

The climatic and health effects of aerosols are strongly dependent on the intra-annual variations in their loading and properties. While the seasonal variations of regional aerosol optical depth (AOD) have been extensively studied, understanding the temporal variations in aerosol vertical distribution and particle types is also important for an accurate estimate of aerosol climatic effects. In this paper, we combine the observations from four satellite-borne sensors and several ground-based networks to investigate the seasonal variations of aerosol column loading, vertical distribution, and particle types over three populous regions: the Eastern United States (EUS), Western Europe (WEU), and Eastern and Central China (ECC). In all three regions, column AOD, as well as AOD at heights above 800 m, peaks in summer/spring, probably due to accelerated formation of secondary aerosols and hygroscopic growth. In contrast, AOD below 800 m peaks in winter over WEU and ECC regions because more aerosols are confined to lower heights due to the weaker vertical mixing. In the EUS region, AOD below 800 m shows two maximums, one in summer and the other in winter. The temporal trends in low-level AOD are consistent with those in surface fine particle (PM 2.5 ) concentrations. AOD due to fine particles (< 0.7 µm diameter) is much larger in spring/summer than in winter over all three regions. However, the coarse mode AOD (> 1.4 µm diameter), generally shows small variability, except that a peak occurs in spring in the ECC region due to the prevalence of airborne dust during this season. When aerosols are classified accord-ing to sources, the dominant type is associated with anthropogenic air pollution, which has a similar seasonal pattern as total AOD. Dust and sea-spray aerosols in the WEU region peak in summer and winter, respectively, but do not show an obvious seasonal pattern in the EUS region. Smoke aerosols, as well as absorbing aerosols, present an obvious unimodal distribution with a maximum occurring in summer over the EUS and WEU regions, whereas they follow a bimodal distribution with peaks in August and March (due to crop residue burning) over the ECC region.