Estimating Top-of-Atmosphere (TOA) flux and radiance is essential for understanding Earth's radiation budget and climate dynamics. This study utilized polar nephelometer measurements of aerosol scattering coefficients at 17 angles (9-170 degrees), enabling the experimental determination of aerosol phase functions and the calculation of Legendre moments. These moments were then used to estimate TOA flux and radiance. Conducted at a tropical coastal site in India, the study observed significant seasonal and diurnal variations in angular scattering patterns, with the highest scattering during winter and the lowest during the monsoon. Notably, a prominent secondary scattering mode, with varying magnitude across different seasons, was observed in the 20-30 degrees angular range, highlighting the influence of different air masses and aerosol sources. Chemical analysis of size-segregated aerosols revealed that fine-mode aerosols were dominated by anthropogenic species, such as sulfate, nitrate, and ammonium, throughout all seasons. In contrast, coarse-mode aerosols showed a clear presence of sea-salt aerosols during the monsoon and mineral dust during the pre-monsoon periods. The presence of very large coarse-mode non-spherical aerosols caused increased oscillations in the phase function beyond 60 degrees during the pre-monsoon and monsoon seasons. This also led to a weak association between the phase function derived from angular scattering measurements and those predicted by the Henyey-Greenstein approximation. As a result, TOA fluxes and radiances derived using the Henyey-Greenstein approximation (with the asymmetry parameter as input in the radiative transfer model) showed a significant difference- up to 24% in seasons with substantial coarse-mode aerosol presence- compared to those derived using the Legendre moments of the phase function. Therefore, TOA flux and radiance estimates using Legendre moments are generally more accurate in the presence of complex aerosol scattering characteristics, particularly for non-spherical or coarse-mode aerosols, while the Henyey-Greenstein phase function may yield less accurate results due to its simplified representation of scattering behavior.

Indian monsoon circulation is the primary driver of the long-range transboundary mercury (Hg) pollution from South Asia to the Himalayas and Tibet Plateau region, yet the northward extent of this transport remains unknown. In this study, a strong delta Hg-202 signature overlapping was found between Lake Gokyo and Indian anthropogenic sources, which is an indicative of the Hg source regions from South Asia. Most of the sediment samples were characterized with relatively large positive Delta Hg-199 values (mean = 0.07 parts per thousand-0.44 parts per thousand) and small positive Delta Hg-200 values (mean = 0.03 parts per thousand-0.08 parts per thousand). Notably, the Delta Hg-199 values in the lake sediments progressively increased from southwest to northeast. Moreover, the Delta Hg-199 values peaked at Lake Tanglha (mean = 0.44 parts per thousand +/- 0.04 parts per thousand) before decreased at Lake Qinghai that is under the influence of the westerlies. Our results suggest that transboundary atmospheric transport could transport Hg from South Asia northwards to at least the Tanglha Mountains in the northern Himalaya-Tibet.

Rainfall can alter the hydrothermal state of permafrost, subsequently affecting organic carbon decomposition and CO2 transport. However, the mechanisms by which rainfall influences organic carbon decomposition and carbon dioxide transport processes in permafrost remain unclear. In this study, a coupled permafrost water-heatvapor-carbon model, based on the surface energy-water balance theory, is employed to explore the effects of increased precipitation on permafrost moisture, temperature, organic carbon decomposition, and carbon dioxide transport through numerical simulations. The results are as follows: (1) with increased rainfall, surface latent heat flux rises while surface sensible heat flux declines, leading to a reduction in surface heat flux. The annual mean surface heat fluxes for the three precipitation conditions of no change in precipitation (zP = 0 mm), 50 mm increase in precipitation (zP = 50 mm) and 100 mm increase in precipitation (zP = 100 mm) are -0.1 W/m2, -0.2 W/m2 and -0.4 W/m2 respectively; and (2) as rainfall increases, soil moisture content increases significantly, but the impact of rainfall on soil moisture content diminishes with increasing soil depth; and (3) increased rainfall results in a decrease in soil carbon fluxes, soil organic matter decomposition rates, and CO2 concentrations. Compared to the case of constant precipitation, the surface carbon fluxes decreased by 0.04 mu mol center dot m-2s-1 and 0.08 mu mol center dot m-2s-1 under zP = 50 mm and zP = 100 mm, respectively. Additionally, the decomposition rate of soil organic matter at 10 cm depth decreased by 3.2 E-8 mol center dot m-2s-1 and 6.3 E-8 mol center dot m-2s-1, respectively, while the soil carbon concentration decreased by 3 mu mol/mol and 5 mu mol/mol, respectively.

Aerosols affect Earth's climate both directly and indirectly, which is the largest uncertainty in the assessment of radiative forcings affecting anthropogenic climate change. The standard Aerosol Robotic Network (AERONET) aerosol products have been widely used for more than 30 years. Currently, there is strong community interest in the possibility of determining aerosol composition directly from remote sensing observations. This work presents the results of applying such a recently developed approach by Li et al. to extended datasets of the directional sky radiances and spectral aerosol optical depth (AOD) measured by AERONET for the retrievals of aerosol components. First, the validation of aerosol optical properties retrieved by this component approach with AERONET standard products shows good agreement. Then, spatiotemporal variations of the obtained aerosol component concentration are characterized globally, especially the absorbing aerosol species (black carbon, brown carbon, and iron oxides) and scattering aerosol species (organic carbon, quartz, and inorganic salts). Finally, we compared the black carbon (BC) and dust column concentration retrievals to the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2), products in several regions of interest (Amazon zone, Desert, and Taklamakan Desert) for new insights on the quantitative assessment of MERRA-2 aerosol composition products (R = 0.60-0.85 for BC; R = 0.75-0.90 for dust). The new value-added and long-term aerosol composition product globally is available online (https://doi.org/10.6084/ m9.figshare.25415239.v1), which provides important measurements for the improvement and optimization of aerosol modeling to enhance estimation of the aerosol radiative forcing. SIGNIFICANCE STATEMENT: In the assessment of climate change, the uncertainty associated with aerosol radiative forcing is the largest one. The purpose of this study is to provide a new value-added and long-term aerosol composition (including absorbing and scattering aerosol species) inversion dataset derived from Aerosol Robotic Network (AERONET) measurements for characterizing their spatiotemporal variations at global scale. We find some new insights on the quantitative assessment of black carbon and dust column concentration products in the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2). Our results and aerosol composition inversion dataset will provide robust support for the overall improvement and optimization of aerosol modeling to better understand the aerosol radiative forcing.

High uncertainty in optical properties of black carbon (BC) involving heterogeneous chemistry has recently attracted increasing attention in the field of atmospheric climatology. To fill the gap in BC optical knowledge so as to estimate more accurate climate effects and serve the response to global warming, it is beneficial to conduct site-level studies on BC light absorption enhancement (E-abs) characteristics. Real-time surface gas and particulate pollutant observations during the summer and winter over Wuhan were utilized for the analysis of E-abs simulated by minimum R squared (MRS), considering two distinct atmospheric conditions (2015 and 2017). In general, differences in aerosol emissions led to E-abs differential behaviors. The summer average of E-abs (1.92 +/- 0.55) in 2015 was higher than the winter average (1.27 +/- 0.42), while the average (1.11 +/- 0.20) in 2017 summer was lower than that (1.67 +/- 0.69) in winter. E-abs and R-BC (representing the mass ratio of non-refractory constituents to elemental carbon) constraints suggest that E-abs increased with the increase in R-BC under the ambient condition enriched by secondary inorganic aerosol (SIA), with a maximum growth rate of 70.6% in 2015 summer. However, E-abs demonstrated a negative trend against R-BC in 2017 winter due to the more complicated mixing state. The result arose from the opposite impact of hygroscopic SIA and absorbing OC/irregular distributed coatings on amplifying the light absorbency of BC. Furthermore, sensitivity analysis revealed a robust positive correlation (R > 0.9) between aerosol chemical compositions (including sulfate, nitrate, ammonium and secondary organic carbon), which could be significantly perturbed by only a small fraction of absorbing materials or restructuring BC through gaps filling. The above findings not only deepen the understanding of BC, but also provide useful information for the scientific decision-making in government to mitigate particulate pollution and obtain more precise BC radiative forcing.

While the direct impact of climate change on reference evapotranspiration (ET0) has been extensively studied, there is limited research on the indirect impact resulting from the interaction between climatic variables. This gap hinders a comprehensive understanding of climate change effects on ET0. Additionally, there is scarce exploration into the quantitative effect of freeze-thaw cycles on ET0 variation. In this study, we employed path analysis and dependent variable variance decomposition methods to discern the direct and interactive effects of climatic variables on ET0 in the Tibetan Plateau from 1960 to 2022. Annual ET0 exhibited variation across basins, with the coefficient of variability during the thawed period smaller than that during the non-thawed period. On an annual scale, the largest contribution to ET0 variation came from water vapor pressure deficit (VPD) at 47.7%. This contribution was amplified by its coupled interaction with temperature (T) at 47.1%, although the contribution was partially offset by the interactive effects of VPD with downward shortwave radiation and wind speed at -2.4% and - 27.6%, respectively. During different freezing-thawing periods, VPD primarily controlled ET0 variation, with its interaction with other climatic variables enhancing its impact. Furthermore, soil moisture, influenced by freeze-thaw cycles, exhibited a strong correlation with T and VPD, indicating the significant effect of freeze-thaw cycles on ET0 variation. The weak correlation between ET0 and NDVI suggested that vegetation growth had a limited regulatory effect on ET0. These findings provide valuable insights into the impact of interactions between climatic variables on hydrological processes, enhancing our understanding of the interactive roles of hydrometeorological variables.

Changing precipitation patterns and global warming have greatly changed winter snow cover, which can affect litter decomposition process by altering soil microenvironment or microbial biomass and activity. However, it remains unknown how and to what extent snow cover affects litter decomposition during winter and over longer periods of time. Here, we conducted a meta-analysis to synthesize litter decomposition studies under different levels of snow cover. Overall, deepened snow significantly enhanced litter decomposition rate and mass loss by 17% and 3%, respectively. Deepened snow enhanced litter carbon loss by 7% but did not impact the loss of litter nitrogen or phosphorus. Deepened snow increased soil temperature, decreased the frequency of freeze-thaw cycles, and stimulated microbial biomass carbon and bacterial biomass during winter, but had no effect on these parameters in summer. The promoting effect of deepened snow cover on litter decomposition in winter is mainly due to its positive effect on microbial decomposition by increasing soil temperature and reducing freezethaw cycles exceeded its negative effect on physical fragmentation of litter by reducing freeze-thaw cycles. Our findings indicate that the changes in winter snow cover under global change scenarios can greatly impact winter litter decomposition and the associated carbon cycling, which should be taken into consideration when assessing the global carbon budget in modeling.

Aerosol chemical components such as black carbon (BC) and brown carbon (BrC) regulate aerosol optical properties, which in turn drive the atmospheric radiative forcing estimations due to aerosols. In this study, we used the long-term measurements from AERONET (Aerosol Robotic Network) to better understand the aerosol types and composition with respect to their seasonal and spatial variabilities in peninsular Southeast Asia (PSEA, here defined as Vietnam, Cambodia, Thailand, Laos, and Myanmar). Two methods (i.e., aerosol type cluster and aerosol component retrieval) were applied to determine the aerosol type and chemical composition during the biomass-burning (BB) season. AERONET sites in northern PSEA showed a higher AOD (aerosol optical depth) compared to that of southern PSEA. Differences in land use pattern, geographic location, and weather regime caused much of the aerosol variability over PSEA. Lower single-scattering albedo (SSA) and higher fine-mode fraction (FMF) values were observed in February and March, suggesting the predominance of BB type aerosols with finer and stronger absorbing particles during the dry season. However, we also found that the peak BB month (i.e., March) in northern PSEA may not coincide with the lowest SSA once dust particles have mixed with the other aerosols. Furthermore, we investigated two severe BB events in March of 2014 and 2015, revealing a significant BrC fraction during BB event days. On high AOD days, although the BC fraction was high, the BrC fraction remained low due to lack of aerosol aging. This study highlights the dominance of carbonaceous aerosols in the PSEA atmosphere during the BB season, while also revealing that transported dust particles and BrC aerosol aging may introduce uncertainties into the aerosol radiative forcing calculation.

Litter decomposition represents a major path for atmospheric carbon influx into Arctic soils, thereby controlling below-ground carbon accumulation. Yet, little is known about how tundra litter decomposition varies with microenvironmental conditions, hindering accurate projections of tundra soil carbon dynamics with future climate change. Over 14 months, we measured landscape-scale decomposition of two contrasting standard litter types (Green tea and Rooibos tea) in 90 plots covering gradients of micro-climate and -topography, vegetation cover and traits, and soil characteristics in Western Greenland. We used the tea bag index (TBI) protocol to estimate relative variation in litter mass loss, decomposition rate (k) and stabilisation factor (S) across space, and structural equation modelling (SEM) to identify relationships among environmental factors and decomposition. Contrasting our expectations, microenvironmental factors explained little of the observed variation in both litter mass loss, as well as k and S, suggesting that the variables included in our study were not the major controls of decomposer activity in the soil across the studied tundra landscape. We use these unexpected findings of our study combined with findings from the current literature to discuss future avenues for improving our understanding of the drivers of tundra decomposition and, ultimately, carbon cycling across the warming Arctic.

Permafrost soils in the northern hemisphere are known to harbor large amounts of soil organic matter (SOM). Global climate warming endangers this stable soil organic carbon (SOC) pool by triggering permafrost thaw and deepening the active layer, while at the same time progressing soil formation. But depending, e.g., on ice content or drainage, conditions in the degraded permafrost can range from water-saturated/anoxic to dry/oxic, with concomitant shifts in SOM stabilizing mechanisms. In this field study in Interior Alaska, we investigated two sites featuring degraded permafrost, one water-saturated and the other well-drained, alongside a third site with intact permafrost. Soil aggregate- and density fractions highlighted that permafrost thaw promoted macroaggregate formation, amplified by the incorporation of particulate organic matter, in topsoils of both degradation sites, thus potentially counteracting a decrease in topsoil SOC induced by the permafrost thawing. However, the subsoils were found to store notably less SOC than the intact permafrost in all fractions of both degradation sites. Our investigations revealed up to net 75% smaller SOC storage in the upper 100 cm of degraded permafrost soils as compared to the intact one, predominantly related to the subsoils, while differences between soils of wet and dry degraded landscapes were minor. This study provides evidence that the consideration of different permafrost degradation landscapes and the employment of soil fractionation techniques is a useful combination to investigate soil development and SOM stabilization processes in this sensitive ecosystem.