Rapid climate change in the Northern Hemisphere cryosphere threatens ancient permafrost carbon. Once thawed, permafrost carbon may migrate to surface waters. However, the magnitude of permafrost carbon processed by northern freshwater remains uncertain. Here, we compiled '1800 radiocarbon data of aquatic dissolved organic carbon (DOC) and particulate organic carbon (POC) in the Arctic and Qinghai -Tibet Plateau (QTP) to explore the fate of permafrost carbon under climate warming over the past 30 years. We showed that the contribution of aged carbon has significantly increased since 2015. Approximately 70 % of DOC and POC was derived from aged carbon for QTP rivers. In Arctic waters, an average of '67 % of POC was derived from aged carbon, however, '75 % of DOC was derived from modern carbon, mainly due to low temperatures and protection by vegetation limiting the export of aged DOC. For both regions, DOC 14 C age was positively correlated with the active layer thickness, whereas the POC 14 C age was positively correlated with the mean annual ground temperature, suggesting that gradual thaw accelerated the mobilization of aged DOC while abrupt thaw facilitated the export of aged POC. Furthermore, POC 14 C age was positively correlated with the soil organic carbon density, which was attributed to well-developed pore networks facilitated aged carbon output. This study suggests that permafrost carbon release is affected by both permafrost thermal properties and soil organic carbon density, which should be considered in evaluation of permafrost carbon -climate feedback.
Black carbon (BC) mixed with non-BC components strongly absorbs visible light and leads to uncertainty in assessing the absorption enhancement (Eabs) and thus radiative forcing. Traditional Single-Particle Soot Photometer (SP2) combined with the leading-edge only fitting (the only-SP2 method) derives BC's mixing states through Mie scattering calculations. However, errors exist in retrieved optical diameter (Dopt) and MR due to the assumption of the ideal spherical core-shell structure and the selection of the calculation parameters like density and refractive index (RI) of the components. Here, we employed a custom-developed tandem CPMA-SP2 system, which classifies fixed-mass BC to characterize the mixing state, then compared with the only-SP2 method in quantifying the mixing state and Eabs. The field measurements show that the SP2 demonstrates variability in assessing the mixing state of BC in different aging states. The thickly-coated particles with small core approaching the internally mixed state are more sensitive to the change of calculated RI. The Dopt decreases with the RI increasing, indicating that this method accurately measures both Dopt and Eabs when a reasonable refractive index is selected for calculation. However, for thinly-coated particles with moderate or large core, this method results in significant deviations in the computed Eabs (errors up to 15 %). These deviations may be caused by the various shapes of BC and systematic errors. Our results provide valuable insights into the accuracy of the SP2-retrieved Dopt and MR based on Mie calculations and highlight the importance of employing advanced techniques for further assessment of BC's mixing state.
Large-scale wildfires are essential sources of black carbon (BC) and brown carbon (BrC), affecting aerosol-induced radiative forcing. This study investigated the impact of two wildfire plumes (Plume 1 and 2) transported to Moscow on the optical properties of BC and BrC during August 2022. During the wildfires, the total light absorption at 370 nm (b(abs_370nm)) increased 2.3-3.4 times relative to background (17.30 +/- 13.98 Mm(-)(1)), and the BrC contribution to total absorption increased from 14 % to 42-48 %. BrC was further partitioned into primary (BrCPri) and secondary (BrCSec) components. Biomass burning accounted for similar to 83-90 % of BrCPri during the wildfires. The b(abs_370nm) of BrCPri increased 5.6 times in Plume 1 and 11.5 times in Plume 2, due to the higher prevalence of peat combustion in Plume 2. b(abs_370nm) of BrCSec increased 8.3-9.6 times, driven by aqueous-phase processing, as evidenced by strong correlations between aerosol liquid water content and b(abs_370nm) of BrCSec. Daytime b(abs_370nm) of BrCSec increased 7.6 times in Plume 1 but only 3.6 times in Plume 2, due to more extensive photobleaching, as indicated by negative correlations with oxidant concentrations and longer transport times. The radiative forcing of BrCPri relative to BC increased 1.8 times in Plume 1 and Plume 2. In contrast, this increase for BrCSec was 3.4 times in Plume 1 but only 2.3 times in Plume 2, due to differences in chemical processes, which may result in higher uncertainty in its radiative forcing. Future work should prioritize elucidating both the emissions and atmospheric processes to better quantify wildfire-derived BrC and its radiative forcing.
Soil organic matter (SOM) stability in Arctic soils is a key factor influencing carbon sequestration and greenhouse gas emissions, particularly in the context of climate change. Despite numerous studies on carbon stocks in the Arctic, a significant knowledge gap remains regarding the mechanisms of SOM stabilization and their impact on the quantity and quality of SOM across different tundra vegetation types. The main aim of this study was to determine SOM characteristics in surface horizons of permafrost-affected soils covered with different tundra vegetation types (pioneer tundra, arctic meadow, moss tundra, and heath tundra) in the central part of Spitsbergen (Svalbard). Physical fractionation was used to separate SOM into POM (particulate organic matter) and MAOM (mineral-associated organic matter) fractions, while particle-size fractionation was applied to evaluate SOM distribution and composition in sand, silt, and clay fractions. The results indicate that in topsoils under heath tundra POM fractions dominate the carbon and nitrogen pools, whereas in pioneer tundra topsoils, the majority of the carbon and nitrogen are stored in MAOM fractions. Moreover, a substantial proportion of SOM is occluded within macro-and microaggregates. Furthermore, the results obtained from FTIR analysis revealed substantial differences in the chemical properties of individual soil fractions, both concerning the degree of occlusion in aggregates and across particle size fractions. This study provides clear evidence that tundra vegetation types significantly influence both the spatial distribution and chemical composition of SOM in the topsoils of central Spitsbergen.
The critical role of light-absorbing aerosol black carbon (BC) in modifying the Earth's atmosphere and climate system warrants detailed characterization of its microphysical properties. The present study examines the BC microphysical properties (size distributions and mixing state) and their impact on the light-absorption characteristics over a semi-urban tropical coastal location in Southern Peninsular India. The measurements of refractory BC (rBC) properties, carried out using the single particle soot photometer during 2018-2021, covering four distinct air mass conditions (Marine, Continental, Mixed-1, and Mixed-2), were used for this purpose. These were supported by measurements of non-refractory submicron particulate matter (NR-PM1) mass loadings and the core-shell Mie theory model for BC-containing particles. The results suggested that the BC particles exhibited varying sizes (mass median diameters from 0.181 +/- 0.079 mu m to 0.202 +/- 0.064 mu m) and relative coating thicknesses (RCT) (1.3-1.6) under distinct air mass conditions. These characteristics reflected varying source/sink strengths, aging processes of BC, and potential condensable coating material. The aerosol system during the Marine air mass period has lower BC (similar to 0.67 +/- 0.57 mu g m(-3)) and NR-PM1 (12.06 +/- 10.81 mu g m(-3)) mass concentrations, and the lowest RCT on BC (similar to 1.34 +/- 0.14). However, the other periods with continental influence depicted significant coatings on BC (mean RCT >1.5). The coatings on BC particles exhibited daytime enhancement, driven by photochemically produced condensable material, a contrasting diurnal pattern to that of other BC properties. Interestingly, the RCT on BC increased and/or remained invariant with increasing relative humidity (RH) until RH 85 %), indicating the potential role of secondary organics as coatings. The changes in the BC mixing state resulted in a significant alteration to its light-absorption properties. The mean light-absorption enhancement of BC (compared to uncoated BC) ranged from 1.36 +/- 0.14 for the Marine air mass periods to 1.58 +/- 0.15 for the Continental air mass periods, whereas the overall mass absorption cross-sections of BC varied between 7.91 +/- 0.91 to 9.03 +/- 0.84 m(2)/g at 550 nm. The key implication of this study is that changes to the BC mixing state, caused by multiple underlying processes unique to tropical atmospheric conditions, can lead to a significant enhancement in its light-absorption characteristics, which can lead to a notable increase in the positive radiative forcing of BC.
Aerosols over the Tibetan Plateau (TP) strongly influence regional climate and hydrological cycles. Here we investigate the size-resolved microphysical and optical properties of aerosols in an urban area of the northern TP using a tandem system of a differential mobility analyzer, a condensation particle counter, and a single particle soot photometer. Under the 2021 summer conditions, the average particle number size distribution follows a lognormal pattern, peaking at similar to 70 nm. Refractory black carbon (rBC) aerosols constitute 17.7% of the total particle population in the 100-750 nm mobility diameter (D-mob) range, with their proportion rising to over 50% for D-mob > 500 nm. Most rBC particles are externally mixed, while only 12.2% are thickly coated with non-refractory materials. Externally mixed rBC particles show strong non-sphericity, with a dynamic shape factor increasing from 1.8 at 115 nm to 2.8 at 750 nm, consistent with aggregate structures. In contrast, thickly coated rBC particles are nearly spherical, with coating thickness increasing with size. The total rBC mass estimated from size-resolved measurements closely matches bulk rBC mass directly measured. rBC-free particles exhibit slight non-sphericity, with shape factor positively correlated with refractive index, likely due to dust contributions. Bulk scattering coefficients derived from size-resolved data match those estimated under the well-mixed spherical assumption. However, the later scheme-lacking observational constraints on morphology and mixing state-overestimates absorption by over a factor of three, thereby underestimating the single-scattering albedo. These results provide key constraints for improving aerosol radiative forcing estimates and advancing understanding of aerosol-climate interactions over the TP.
The Himalayan glacier valleys are encountering escalating environmental challenges. One of the contributing factors is thought to be the rising amounts of light-absorbing carbonaceous aerosols, particularly brown carbon (BrC) and black carbon (BC), that are reaching glacier valleys. The present study examines the optical and radiative characteristics of BC at Bhojbasa, near Gaumukh (similar to 3800amsl). Real-time in-situ BC data, optical characteristics, radiative forcing, heating rate, several meteorological parameters, and BC transport pathways to this high-altitude site are investigated. The daily mean concentration of equivalent black carbon (eBC) was 0.28 +/- 0.21 mu g/m(3) over the research period, and the eBC from fossil fuel (BCFF) is dominant with 78 % with a daily mean of 0.22 +/- 0.19 mu g/m(3)(,) and eBC from biomass burning (BCBB) is 22 % with a daily mean of 0.06 +/- 0.08 mu g/m(3). Meteorological data, Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) imaging, and backward air-mass trajectory analysis demonstrate the presence of BC particles and their plausible transit pathways from multiple source locations to the pristine Gangotri Glacier Valley. The estimated daily mean BC radiative forcing values are +6.71 +/- 1.80 W/m(2) in the atmosphere, +1.87 +/- 1.16 W/m(2) at the top of the atmosphere, and -4.84 +/- 1.01 W/m(2) at the surface with a corresponding atmospheric heating rate of 0.19 +/- 0.05 K/day. These findings highlight the critical role of ground-based measurements in monitoring the fluctuations of BC over such varied Himalayan terrain, as they offer important information on the localized trends and effects. Long-term measurements of glacier valleys are essential for a comprehensive evaluation of the impact of BC particles on Himalayan ecology and climate.
To achieve the goal of carbon neutrality, China is projected to significantly reduce anthropogenic aerosols in addition to greenhouse gases. Here, the future changes in East Asian summer monsoon (EASM) and weather extremes responding to the idealized local emission reductions of anthropogenic aerosols (AA) in China are investigated based on time-slice simulations in an aerosol-climate model together with a localized carbon neutral emission scenario, while greenhouse gases and other anthropogenic climate forcers are kept at the present-day (2015) levels. The AA reduction in China leads to a positive change in June-July-August (JJA) mean effective radiative forcing over eastern China in 2030 and 2060s, along with a 0.2 degrees C-0.4 degrees C warming, respectively. It intensifies the temperature difference between land and ocean, and increases the precipitation over eastern China. Multiple EASM indices show that EASM intensity in JJA is estimated to be strengthened in the future, because of the AA decline in China. The AA emissions reduction toward carbon neutrality in China also presents a potential side effect of intensifying the summertime extreme temperatures and precipitation in China. This study reveals the important role of reductions of AA emissions in influencing EASM and weather extremes, which warrants careful assessment in the emission policymaking process prior to the implementation of mitigation strategies.
Ecosystem carbon use efficiency (CUE) is a key indicator of an ecosystem's capacity to function as a carbon sink. While previous studies have predominantly focused on how climate and resource availability affect CUE through physiological processes during the growing season, the role of canopy structure in regulating carbon and energy exchange, especially its interactions with winter climate processes and nitrogen use efficiency (NUE) in shaping ecosystem CUE in semi-arid grasslands, remains insufficiently understood. Here, we conducted a 5-year snow manipulation experiment in a temperate grassland to investigate the effects of deepened snow on ecosystem CUE. We measured ecosystem carbon fluxes, soil nitrogen concentration, species biomass, plants' nitrogen concentration, canopy height and cover and species composition. We found that deepened snow increased soil nitrogen availability, while the concurrent rise in soil moisture facilitated nutrient acquisition and utilization. Together, these changes supported greater biomass accumulation per unit of nitrogen uptake, thereby enhancing NUE. In addition, deepened snow favoured the dominance of C3 grasses, which generally exhibit higher NUE and greater height than C3 forbs, providing a second pathway that further elevated community-level NUE. The enhanced NUE, through both physiological efficiency and compositional shifts, promoted biomass production and facilitated the development of larger canopy volumes. Larger canopy volumes under deepened snow increased gross primary production through improved light interception, while the associated increase in autotrophic maintenance respiration was moderated by higher NUE. Besides, denser canopies reduced understorey temperatures throughout the day, particularly at night, thereby suppressing heterotrophic respiration. Ultimately, deepened snow increased ecosystem CUE by enhancing carbon uptake while limiting respiratory carbon losses. Synthesis. These findings demonstrated the crucial role of biophysical processes associated with canopy structure and NUE in regulating ecosystem CUE, which has been largely overlooked in previous studies. We also highlight the importance of winter processes in shaping carbon sequestration dynamics and their potential to modulate future grassland responses to climate change.
Black carbon (BC) is a major short-lived climate pollutant (SLCP) with significant climate and environmentalhealth impacts. This review synthesizes critical advancements in the identification of emerging anthropogenic BC sources, updates to global warming potential (GWP) and global temperature potential (GTP) metrics, technical progress in characterization techniques, improvements in global-regional monitoring networks, emission inventory, and impact assessment methods. Notably, gas flaring, shipping, and urban waste burning have slowly emerged as dominant emission sources, especially in Asia, Eastern Europe, and Arctic regions. The updated GWP over 100 years for BC is estimated at 342 CO2-eq, compared to 658 CO2-eq in IPCC AR5. Recent CMIP6-based Earth System Models (ESMs) have improved attribution of BC's microphysics, identifying a 22 % increase in radiative forcing (RF) over hotspots like East Asia and Sub-Saharan Africa. Despite progress, challenges persist in monitoring network inter-comparability, emission inventory uncertainty, and underrepresentation of BC processes in ESMs. Future efforts could benefit from the integration of satellite data, artificial intelligence (AI)assisted methods, and harmonized protocols to improve BC assessment. Targeted mitigation strategies could avert up to four million premature deaths globally by 2030, albeit at a 17 % additional cost. These findings highlight BC's pivotal roles in near-term climate and sustainability policy.