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.
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.
Biomass burning is a major source of carbonaceous aerosols that significantly influences the Earth's radiation balance. However, the spectral light absorption properties of biomass burning aerosols (BBAs), particularly the contribution of brown carbon (BrC), remain poorly constrained due to reliance on laboratory measurements that may not accurately represent real-world atmospheric conditions. To address this limitation, we developed an unmanned aerial vehicle (UAV) based-platform for direct in-situ measurements of BBAs in the ambient atmosphere over the rural North China Plain. This approach reduces biases inherent to laboratory chamber experiments and enables a more realistic characterization of BBAs absorption properties. Our measurements revealed that the absorption & Aring;ngstr & ouml;m exponent (AAE) for typical residential biomass burning was 3.70 +/- 0.04 under smoldering conditions and 1.50 +/- 0.08 under flaming conditions. Variations in AAE were driven primarily by combustion conditions and smoke humidity rather than fuel type. Additionally, field-observed OC/EC ratios were up to ten times higher than those reported in laboratory chamber studies, resulting in systematically lower mass absorption cross-sections. This finding suggests that the BBAs light absorption and radiative forcing estimates in the North China Plain may be systematically overestimated by chamber-based studies. Notably, under smoldering conditions, BrC absorption at 375 nm was up to 6.6 times greater than that of black carbon (BC) once mass emissions are considered, emphasizing that strategies aiming at reducing smoldering combustion could be particularly effective in mitigating the ultraviolet radiative effects of BBAs. Our results demonstrate that ambient atmospheric measurements are essential for accurately constraining BBAs absorption properties and their climate impacts.
The present study performed classification global aerosols based on particle linear depolarization ratio (PLDR) and single scattering albedo (SSA) provided from AErosol RObotic NETwork (AERONET) Version 3.0 and Level 2.0 inversion products of 171 AERONET sites located in six continents. Current methodology could distinguish effectively between dust and non-dust aerosols using PLDR and SSA. These selected sites include dominant aerosol types such as, pure dust (PD), dust dominated mixture (DDM), pollution dominated mixture (PDM), very weakly absorbing (VWA), strongly absorbing (SA), moderately absorbing(MA), and weakly absorbing (WA). Biomass-burning aerosols which are associated with black carbon are assigned as combinations of WA, MA and SA. The key important findings show the sites in the Northern African region are predominantly influenced by PD, while south Asian sites are characterized by DDM as well as mixture of dust and pollution aerosols. Urban and industrialized regions located in Europe and North American sites are characterized by VWA, WA, and MA aerosols. Tropical regions, including South America, South-east-Asia and southern African sites which prone to forest and biomass-burning, are dominated by SA aerosols. The study further examined the impacts by radiative forcing for different aerosol types. Among the aerosol types, SA and VWA contribute with the highest (30.14 +/- 8.04 Wm-2) and lowest (7.83 +/- 4.12 Wm-2) atmospheric forcing, respectively. Consequently, atmospheric heating rates are found to be highest by SA (0.85 K day-1) and lowest by VWA aerosols (0.22 Kday-1). The current study provides a comprehensive report on aerosol optical, micro-physical and radiative properties for different aerosol types across six continents.
This study investigates the inter-annual variability of carbonaceous aerosols (CA) over Kolkata, a megacity in eastern India, using dual carbon isotopes (C-14 and C-13) alongside measurements of the optical properties of brown carbon (BrC). Sampling was conducted during the post-monsoon, winter, and spring seasons over two consecutive years (2020-21 and 2021-22). The analysis reveals that PM2.5 and CA concentrations were higher in 2020-21 (194 +/- 40 and 54 +/- 15 mu g m(-3), respectively) compared to 2021-22 (141 +/- 31 and 44 +/- 21 mu g m(-3)), likely due to higher precipitation in 2021-22. The contribution of biomass burning and biogenic sources to CA (f(bio_TC)) was slightly higher in 2020-21 (70 +/- 3 %) than in 2021-22 (68 +/- 3 %), with both years exhibiting a consistent decreasing trend from post-monsoon to spring. Observed lower values for oxidised CA proxies, such as the WSOC/OC ratio (0.41 +/- 0.08) and AMS-derived f(44) (0.13 +/- 0.02), throughout the study period suggest that surface CA over Kolkata primarily originates from local sources rather than long-range transport. The relative radiative forcing (RRF) also showed a clear reduction in the subsequent year; however, on average, the RRF of methanol-soluble BrC (16 +/- 6 %) was approximately three times higher than that of the water-soluble fraction (5.5 +/- 2.2 %), highlighting the substantial role of BrC in influencing regional radiative forcing. These findings underscore the substantial impact of local emissions over transported pollutants on Kolkata's ground-level air quality.
The direct radiative impact of atmospheric aerosols remains more uncertain than that of greenhouse gases, largely due to the complex transformations' aerosols undergo during atmospheric aging. Sulfate aerosols have been the subject of considerable research, with a robust body of literature characterising their cooling effect. In contrast, the light-absorbing properties and warming potential of black carbon and related products remain less well understood, with limited research available to date. The present study examines the iron-catalyzed reaction of catechol in levitated microdroplets, tracked in situ using elastic light scattering spectroscopy. The reaction forms water-insoluble polycatechol aggregates, which drive a transition from homogeneous spheres to heterogeneous droplets with internal inclusions. To interpret the evolving optical behaviour, the Multiple Sphere T-Matrix (MSTM) model is employed, a method which overcomes the limitations of Mie theory by accounting for internal morphological complexity. The model provides realistic complex refractive indices and fractal parameters, though it should be noted that its solutions are not unique due to sensitivity to input assumptions and droplet variability. This underscores the necessity for supplementary measurements and more comprehensive models incorporating evaporation, chemical dynamics, and phase transitions. These findings emphasise the potential of elastic scattering spectroscopy for real-time monitoring of multiphase chemistry and offer new constraints for improving aerosol aging schemes in climate models, thereby contributing to reduced uncertainties in aerosol radiative forcing.
Light-absorbing impurities (LAIs), such as mineral dust (MD), organic carbon (OC), and black carbon (BC), deposited in snow, can reduce snow albedo and accelerate snowmelt. The Ili Basin, influenced by its unique geography and westerly atmospheric circulation, is a critical region for LAI deposition. However, quantitative assessments on the impact of LAIs on snow in this region remain limited. This study investigated the spatial distribution of LAIs in snow and provided a quantitative evaluation of the effects of MD and BC on snow albedo, radiative forcing, and snowmelt duration through sampling analysis and model simulations. The results revealed that the Kunes River Basin in the eastern Ili Basin exhibited relatively high concentrations of MD. In contrast, the southwestern Tekes River Basin showed relatively high concentrations of OC and BC. Among the impurities, MD plays a dominant role in the reduction of snow albedo and has a greater effect on the absorption of solar radiation by snow than BC, while MD is the most important light-absorbing impurity responsible for the reduction in the number of snow-melting days in the Ili Basin. Under the combined influence of MD and BC, the snowmelt period in the Ili Basin was reduced by 2.19 +/- 1.43 to 7.31 +/- 4.76 days. This study provides an initial understanding of the characteristics of LAIs in snow and their effects on snowmelt within the Ili Basin, offering essential basic data for future research on the influence of LAIs on snowmelt runoff and hydrological processes in this region.
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.
This study investigates aerosol characteristics using ground-based measurements at two distinct regions, MohalKullu (31.9 degrees N, 77.12 degrees E; 1154 m amsl) and Kosi-Katarmal (29.64 degrees N, 79.62 degrees E; 1225 m amsl), from July 2019 to June 2022. The average Black Carbon (BC) concentrations were 1.5 f 1.0 mu g m- 3 at Mohal and 1.1 f 1.4 mu g m-3 at Katarmal. BC showed strong seasonal variability, with maxima during post-monsoon (2.6 f 1.0 mu g m- 3) and pre-monsoon (1.8 f 0.5 mu g m-3) seasons. The diurnal variation displayed distinct morning and evening peaks in all the seasons. High pre-monsoon AOD500 (0.30 f 0.06 to 0.54 f 0.08) and low values of & Aring;ngstrom exponent (0.67 f 0.10 to 0.95 f 0.30) indicated dominance of large particles, whereas lower AOD500 (0.21 f 0.07 to 0.25 f 0.03) in post-monsoon and winter, along with larger & Aring;ngstrom exponent (1.05 f 0.74 to 1.13 f 0.11), indicated smaller particles. Satellite-derived (OMI and MAIAC) AOD500 showed weak to moderate correlation with ground-based measurements at Mohal (R = 0.4639 for MAIAC, R = 0.1402 for OMI) and Katarmal (R = 0.3976 for MAIAC, R = 0.2980 for OMI). Using optical properties of aerosols and clouds (OPAC) and Santa Barbara discrete ordinate radiative transfer (SBDART) models, the short-wave aerosol radiative forcing (SWARF) was found negative at the surface and top of the atmosphere but positive in the atmosphere, suggesting significant surface cooling and atmospheric warming leading to high heating rates, respectively. Annual mean atmospheric radiative forcing was 27.36 f 6.00 Wm- 2 at Mohal and 21.87 f 7.26 Wm- 2 at Katarmal. These findings may have consequences for planning air pollution strategies and understanding the effects of regional climate change.
Under environment with various water contents, the variations in the mixing state and particle size of coated black carbon (BC) aerosols cause changes in optical and radiative effects. In this study, fractal models for thinly, partially, and thickly coated BC under six relative humidities (RHs 1/4 0-95%) are constructed and optically simulated at 1064 and 532 nm. Differential scattering cross-sections are selected to retrieve the mixing state (Dp/Dc) of BC to investigate the possible retrieval errors caused by the nonspherical morphology when using the single-particle soot photometer (SP2). Furthermore, the radiative forcing of BC aerosols at different RHs are analyzed. Results showed that the retrieval errors (REs) of Dp/Dc are negative for coated particles with BC volume fraction smaller than 0.10, indicating that the mixing states of coated fractal BC are underestimated during the hygroscopic growth. The partiallycoated BC has the best retrieval accuracy of the mixing state, followed by the closed-cell and coatedaggregate model, judging from averaged REs. Radiative forcing enhancements for partially-coated aerosols with different BC volume fractions exponentially increase to opposite values, resulting in a warming or cooling effect. This study helps understand the uncertainties in Dp/Dcof BC aerosols retrieved by SP2 and their radiative forcing at different RHs. (c) 2025 Chinese Society of Particuology and Institute of Process Engineering, Chinese Academy of Sciences. Published by Elsevier B.V. All rights are reserved, including those for text and data mining, AI training, and similar technologies.