Abstract. Water-soluble organic carbon (WSOC) in the cryosphere has an important impact on the biogeochemistry cycling and snow–ice surface energy balance through changes in the surface albedo. This work reports on the chemical characterization of WSOC in 28 representative snowpack samples collected across a regional area of northern Xinjiang, northwestern China. We employed multimodal analytical chemistry techniques to investigate both bulk and molecular-level composition of WSOC and its optical properties, informing the follow-up radiative forcing (RF) modeling estimates. Based on the geographic differences and proximity of emission sources, the snowpack collection sites were grouped as urban/industrial (U), rural/remote (R), and soil-influenced (S) sites, for which average WSOC total mass loadings were measured as 1968 ± 953 ng g−1 (U), 885 ± 328 ng g−1 (R), and 2082 ± 1438 ng g−1 (S), respectively. The S sites showed the higher mass absorption coefficients at 365 nm (MAC365) of 0.94 ± 0.31 m2 g−1 compared to those of U and R sites (0.39 ± 0.11 m2 g−1 and 0.38 ± 0.12 m2 g−1, respectively). Bulk composition of WSOC in the snowpack samples and its basic source apportionment was inferred from the excitation–emission matrices and the parallel factor analysis featuring relative contributions of one protein-like (PRLIS) and two humic-like (HULIS-1 and HULIS-2) components with ratios specific to each of the S, U, and R sites. Additionally, a sample from site 120 showed unique pollutant concentrations and spectroscopic features remarkably different from all other U, R, and S samples. Molecular-level characterization of WSOC using high-resolution mass spectrometry (HRMS) provided further insights into chemical differences among four types of samples (U, R, S, and 120). Specifically, many reduced-sulfur-containing species with high degrees of unsaturation and aromaticity were uniquely identified in U samples, suggesting an anthropogenic source. Aliphatic/protein-like species showed the highest contribution in R samples, indicating their biogenic origin. The WSOC components from S samples showed high oxygenation and saturation levels. A few unique CHON and CHONS compounds with high unsaturation degree and molecular weight were detected in the 120 sample, which might be anthraquinone derivatives from plant debris. Modeling of the WSOC-induced RF values showed warming effects of 0.04 to 0.59 W m−2 among different groups of sites, which contribute up to 16 % of that caused by black carbon (BC), demonstrating the important influences of WSOC on the snow energy budget.

This study reports molecular-level characterization of brown carbon (BrC) attributed to water-soluble organic carbon in six snowpack samples collected from northern Xinjiang, China. The molecular composition and light-absorbing properties of BrC chromophores were unraveled by application of high-performance liquid chromatography (HPLC) coupled to a photodiode array (PDA) detector and high-resolution mass spectrometry. The chromophores were classified into five major types, that is, (1) phenolic/lignin-derived compounds, (2) flavonoids, (3) nitroaromatics, (4) oxygenated aromatics, and (5) other chromophores. Identified chromophores account for ∼23–64% of the total light absorption measured by the PDA detector in the wavelength range of 300–370 nm. In the representative samples from urban and remote areas, oxygenated aromatics and nitroaromatics dominate the absorption in the wavelengths below and above 320 nm, respectively. The highly polluted urban sample shows the most complex HPLC-PDA chromatogram, and more other chromophores contribute to the bulk absorption. Phenolic/lignin-derived compounds are the most light-absorbing species in the soil-influenced sample. Chromophores in two remote samples exhibit ultraviolet–visible features distinct from other samples, which are attributed to flavonoids. Identification of individual chromophores and quantitative analysis of their optical properties are helpful for elucidating the roles of BrC in snow radiative balance and photochemistry.

Light-absorbing particles (LAPs) deposited on snow can decrease snow albedo and affect climate through snow-albedo radiative forcing. In this study, we use MODIS observations combined with a snow-albedo model (SNICAR -Snow, Ice, and Aerosol Radiative) and a radiative transfer model (SBDART -Santa Barbara DISORT Atmospheric Radiative Transfer) to retrieve the instantaneous spectrally integrated radiative forcing at the surface by LAPs in snow (RF LAPs MODIS ) under clear-sky conditions at the time of MODIS Aqua overpass across northeastern China (NEC) in January-February from 2003 to 2017. RF LAPs MODIS presents distinct spatial variability, with the minimum (22.3 W m −2 ) in western NEC and the maximum (64.6 W m −2 ) near industrial areas in central NEC. The regional mean RF LAPs MODIS is ∼ 45.1 ± 6.8 W m −2 in NEC. The positive (negative) uncertainties of retrieved RF LAPs MODIS due to atmospheric correction range from 14 % to 57 % (−14 % to −47 %), and the uncertainty value basically decreases with the increased RF LAPs MODIS . We attribute the variations of radiative forcing based on remote sensing and find that the spatial variance of RF LAPs MODIS in NEC is 74.6 % due to LAPs and 21.2 % and 4.2 % due to snow grain size and solar zenith angle. Furthermore, based on multiple linear regression, the BC dry and wet deposition and snowfall could explain 84 % of the spatial variance of LAP contents, which confirms the reasonability of the spatial patterns of retrieved RF LAPs MODIS in NEC. We validate RF LAPs MODIS using in situ radiative forcing estimates. We find that the biases in RF LAPs MODIS are negatively correlated with LAP concentrations and range from ∼ 5 % to ∼ 350 % in NEC.

Light-absorbing particles in snow can significantly reduce the snow albedo. Quantification of the influence of black carbon (BC), one of the most important light-absorbing particles, on snow albedo is essential for understanding the budgets of solar radiation on snow-covered areas. We measured BC concentration in snow at 28 sites and snow albedo at 18 sites in a vast region across northwestern China in January 2018. The BC concentration was in a wide range of 40-1,850 ng g −1 . The presence of the BC reduced the snow albedo by 0.01-0.20 at the visible wavelength band (400-750 nm). The reduction differed from sites to sites with large values close to industrial areas that are characterized by high pollutants emission. Albedos simulated with a Snow, Ice, and Aerosol Radiation model based on the measured BC agreed well with the measured albedos, with the deviation within ±0.03 and the average underestimation of <0.002. It worth noting that the retrieved optical effective snow grain radius was the key factor in snow albedo calculation. The BC-induced radiative forcing was estimated to be 0.2-6.9 W m −2 , indicating strong acceleration of snowmelt due to BC in northwestern China. All obtained data are extremely valuable for climate model validation associated with the albedo of BC-contaminated snow cover.Plain Language Summary Snow cover on the Earth system is one of the most reflective surfaces and plays a crucial role in the budget of solar radiation energy in the atmosphere. Studies with controlled experiments and model simulations have shown the reductive effect of BC pollution on snow albedo, but the reduction has rarely been assessed with in situ observations. For the first time, we measured both snow albedo and BC concentration in snow in a vast area across northwestern China. Results show a good correlation between the two variables, which is consistent with previous studies, that is, the more BC, the larger reduction. We found that the retrieved optical effective snow grain radius was the key factor to enhance the albedo simulation. We also estimated the radiative forcing of BC in snow and got a nonignorant absorptive effect, which indicates a possible accelerated snowmelt. All the data are extremely valuable for climate model validation associated with the reflection by BC-contaminated snow cover.

Abstract. Mineral dust is a major light-absorbing aerosol, which can significantly reduce snow albedo and accelerate snow/glacier melting via wet and dry deposition on snow. In this study, three scenarios of internal mixing of dust in ice grains were analyzed theoretically by combining asymptotic radiative transfer theory and (core–shell) Mie theory to evaluate the effects on absorption coefficient and albedo of the semi-infinite snowpack consisting of spherical snow grains. In general, snow albedo was substantially reduced at wavelengths of <1.0 µm by internal dust–snow mixing, with stronger reductions at higher dust concentrations and larger snow grain sizes. Moreover, calculations showed that a nonuniform distribution of dust in snow grains can lead to significant differences in the values of the absorption coefficient and albedo of dust-contaminated snowpack at visible wavelengths relative to a uniform dust distribution in snow grains. Finally, using comprehensive in situ measurements across the Northern Hemisphere, we found that broadband snow albedo was further reduced by 5.2 % and 9.1 % due to the effects of internal dust–snow mixing on the Tibetan Plateau and North American mountains. This was higher than the reduction in snow albedo caused by black carbon in snow over most North American and Arctic regions. Our results suggest that significant dust–snow internal mixing is important for the melting and retreat of Tibetan glaciers and North American mountain snowpack.