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.
Abstract. Water-soluble organic carbon (WSOC) in the cryosphere can significantly influence the global carbon cycle and radiation budget. However, WSOC in the snowpack has received little scientific attention to date. This study reports the fluorescence characteristics, absorption properties, and radiative effects of WSOC based on 34 snow samples collected from sites in northeastern China. A significant degree of regional WSOC variability is found, with concentrations ranging from 0.5±0.2 to 5.7±3.7 µg g−1 (average concentration: 3.6±3.2 µg g−1). The three principal fluorescent components of WSOC are identified as (1) the high-oxygenated humic-like substances (HULIS-1) of terrestrial origin, (2) the low-oxygenated humic-like substances (HULIS-2) of mixed origin, and (3) the protein-like substances (PRLIS) derived from autochthonous microbial activity. In southeastern Inner Mongolia (SEIM), a region dominated by desert and exposed soils, the WSOC exhibits the highest humification index (HIX) but the lowest fluorescence (FI) and biological (BIX) indices; the fluorescence signal is mainly attributed to HULIS-1 and thus implicates soil as the primary source. By contrast, the HIX (FI and BIX) value is the lowest (highest), and the percentage of PRLIS is the highest in the remote area of northeastern Inner Mongolia (NEIM), suggesting a primarily biological source. For south and north of northeastern China (SNC and NNC), both of which are characterized by intensive agriculture and industrial activity, the fluorescence signal is dominated by HULIS-2, and the HIX, FI, and BIX values are all moderate, indicating the mixed origins for WSOC (anthropogenic activity, microbial activity, and soil). We also observe that, throughout northeastern China, the light absorption of WSOC is dominated by HULIS-1, followed by HULIS-2 and PRLIS. The contribution of WSOC to albedo reduction (average concentration: 3.6 µg g−1) in the ultraviolet–visible (UV–Vis) band is approximately half that of black carbon (BC average concentration: 0.6 µg g−1). Radiative forcing is 3.8 (0.8) W m−2 in old (fresh) snow, equating to 19 % (17 %) of the radiative forcing of BC. These results indicate that WSOC has a profound impact on snow albedo and the solar radiation balance.
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