Carbonaceous aerosols (CA) strongly impact regional and global climate through their light-absorbing and scattering properties, yet their effects remain uncertain in dust-influenced regions. We investigated the optical properties, source contributions, and radiative impacts of CA at two climatically distinct regions in northwestern India: an arid region (AR, Jodhpur; post-monsoon) and a semi-arid region (SAR, Kota; winter). Mean absorption & Aring;ngstr & ouml;m exponent (AAE) values were comparable between the two regions (AR: 1.416 +/- 0.173; SAR: 1.395 +/- 0.069), but temporal cluster analysis revealed source-specific variability, with lower AAE during traffic-dominated periods (similar to 1.30) and elevated AAE during solid fuel and biomass combustion (1.68 in AR and 1.52 in SAR). While equivalent BC (eBC) levels were higher in AR with a relatively uniform liquid-fuel contribution (BClf = 80.06 +/- 1.98 %), the mass absorption cross- of BC (MAC(BC)) in SAR was similar to 4.5X greater, driven by local solid fuel combustion and transported biomass burning emissions (BCsf = 34.61 +/- 6.88 %). Mie modelling indicated higher SSA in AR due to higher contribution of mineral dust, in contrast to SAR, where carbonaceous aerosols caused stronger absorption, forward scattering, and higher imaginary refractive index (k(OBD)). Although absorption enhancement (E-lambda) was slightly higher in AR (similar to 1.11 vs. similar to 0.99), SAR aerosols nearly doubled the warming potential (Delta RFE), with RFE values of similar to 0.87 W/m(2) in SAR versus similar to 0.43 W/m(2) in AR. These findings highlight strong source-specific and site-specific variability in aerosol absorption and radiative, emphasizing the need to integrate region-specific parameters into climate models and air quality assessments for data-scarce arid and semi-arid South Asian environments.
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.
The long-term trend for aerosol optical properties and climate impact sensitivity in terms of radiative forcing efficiency were analyzed at a suburban station in Athens, Southeast Mediterranean, using an extensive dataset from 2008 to 2022. The study examined scattering (nsc) and absorption (nap) coefficients, scattering & Aring;ngstrom exponent (SAE), absorption & Aring;ngstrom exponent (AAE), single scattering albedo (SSA), asymmetry parameter (g), and radiative forcing efficiency (RFE). Seasonal variability was linked to meteorological conditions and human activities. Single Scattering Albedo (SSA) was lowest (0.86), and Radiative Forcing Efficiency (RFE) was highest (-61 W/m2) in winter, confirming enhanced contributions from traffic and biomass burning. Lower SAE values (1.5) in spring indicate a greater presence of coarse particles due to frequent Saharan dust events (SDEs). Daily patterns of nap and SSA reflect local emissions, with pronounced traffic-related peaks. Aerosol classification revealed that Black Carbon (BC) dominates the suburban aerosol (51 %), with mixed BrC-BC (16 %) peaking in winter and dust-pollution mixtures (13 %) increasing in spring. The presence of large particles mixed with BC (11 %) was more frequent in spring, further highlighting seasonal variability. Trend analysis showed statistically significant (ss) decreases in nsc (-0.611) and SSA (-0.003), alongside increases in nap (+0.027) and RFE (+0.270) at a 95 % confidence level, suggesting a shift toward more absorbing aerosols. The findings provide new insights and reveal a new aerosol regime, where a reduction in anthropogenic emissions is affecting the scattering rather than the absorbing aerosol component, while the impact from forest fires as a climate feedback mechanism has a significant effect in the Eastern Mediterranean. It is important for future studies and climate modelling to account for the regionally observed changes of the state of mixing of ambient aerosol leading to a shift in radiative forcing efficiency through the reduction in SSA. This is evident in the long term for the east Mediterranean region and must be accounted for in radiative forcing estimates and future climate projections.
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 hygroscopic phase transition (HPT) latent heat of black carbon (BC) particles can affect the atmospheric energy budget. However, the source-dependent characteristics and underlying mechanisms remain poorly understood. Herein, three representative BCs (Corn Cob BC, Camphor Wood BC, and Coal BC) were systematically analyzed to quantify HPT latent heat and reveal component-specific contributions. By combining component-resolved analysis with differential scanning calorimetry, it was found that Coal BC exhibited the highest HPT latent heat at 97% RH (Delta H = 93.77 J g-1), which was approximately 253 times higher than that at 11% RH (Delta H = 0.37 J g-1). This was primarily driven by its inorganic component, including the water-extractable fraction (WEBC) and water-extractable minerals (WEM). The corresponding spectral shifts of WEBC (85-100 cm-1 blueshift) and WEM (100-105 cm-1 redshift) in O-H stretching bands under 97% RH indicate strong hydrogen-bonding and solvent effects. These inorganic-rich fractions, although accounting for only 10.1-18.0 wt % in Coal BC, controlled water uptake and latent-heat release, highlighting their pivotal role in BC's nonlinear thermodynamic behavior. This is the first study to quantitatively resolve BC's HPT latent heat and attribute it to specific components, providing thermodynamic insights for improving the parametrization of BC radiative effects in atmospheric models.
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.
Objective Absorbing aerosols, particularly black carbon (BC), exerts significant influence on the Earth's radiation budget by modifying both the amount and vertical distribution of solar radiation. Their climatic effects are especially pronounced in regions characterized by concentrated fossil fuel activities, such as large-scale coal mining areas. However, the spatial and temporal variability of their microphysical and optical properties introduces considerable uncertainty into regional radiative forcing assessments. The Zhundong Coalfield, located in eastern Xinjiang, China, is one such region where BC emissions from coal extraction and associated industrial activity are persistent yet under-characterized from a radiative perspective. This study aims to construct a rapid estimation framework for aerosol radiative forcing (ARF) over this region by integrating multi-band satellite observations with physically based scattering and radiative transfer models. The primary goal is to evaluate how aerosol optical depth (AOD), single scattering albedo (SSA), and particle size influence shortwave ARF at the top of the atmosphere (TOA), bottom of the atmosphere (BOA), and within the atmospheric column (ATM), and how ultraviolet-band data enhances the reliability of this estimation. Methods The research adopts a modular approach comprising aerosol property inversion and radiative transfer modeling. The aerosol inversion is based on a Mie scattering model incorporating a core-shell structure assumption, where BC forms the absorbing core and is coated by non-absorbing substances such as sulfate and nitrate. Satellite-derived aerosol products are used to constrain the model: MODIS provides AOD and SSA at visible wavelengths, while OMI contributes ultraviolet (UV) -band SSA and AOD information. Two experimental configurations are established-one based solely on MODIS data, and another integrating both MODIS and OMI-to assess the role of UV spectral information in constraining aerosol characteristics. Following inversion, the retrieved aerosol size and optical parameters are used as input to the SBDART (Santa Barbara DISORT Atmospheric Radiative Transfer) model to simulate instantaneous ARF at TOA, BOA, and ATM under clear-sky conditions. Radiative forcing is calculated as the difference in net shortwave flux with and without aerosols. Multiple linear regression models are then constructed using different combinations of AOD, SSA, and core radius to quantify the relationship between these parameters and simulated ARF. Regression performance is evaluated using R (2) and RMSE statistics across both single-source and combined-source scenarios. Results and Discussions First, the inclusion of OMI UV-band data significantly improves the inversion accuracy of aerosol particle size characteristics. When only MODIS data are used, the retrieved BC core sizes are relatively narrow, mostly centered around 120 nm, and the shell diameters exhibit limited variation. However, when OMI UV observations are incorporated, the core size distribution broadens, capturing particles ranging from 90 to 160 nm, while the shell diameter spans a wider interval of 300?700 nm. This improved resolution stems from the stronger sensitivity of UVs to absorption by fine-mode particles, which enhances the model's ability to distinguish subtle differences in particle morphology. The resulting total particle size distributions-core plus shell-are more consistent with reported field measurements in coal-intensive regions. These results confirm that UV data not only improve inversion detail but also reduce the uncertainty in the wavelength in the representation of aerosol mixing states. Second, the quantitative relationship between optical parameters and ARF demonstrates clear physical consistency across TOA, BOA, and ATM layers. In both MODIS-only and MODIS-OMI configurations, AOD exhibits a strong negative correlation with TOA and BOA radiative forcing (R=-0.77 and -0.78, respectively), indicating a cooling effect due to enhanced scattering and absorption of incoming solar radiation. SSA also shows a strong negative correlation with TOA and BOA forcing (R=-0.78 and -0.62, respectively), suggesting that as the aerosol becomes more scattering-dominant, its net radiative cooling effect intensifies. Conversely, AOD shows weaker but positive correlations with ATM forcing (R=0.43), suggesting an increase in atmospheric heating when aerosol loading or absorption increases. This pattern aligns with physical expectations: absorbing aerosols like BC trap energy in the atmosphere, contributing to vertical energy redistribution. The analysis confirms that SSA has a stronger explanatory power than AOD, emphasizing its role as a key driver of radiative uncertainty forcing. Third, regression model performance improves markedly with the inclusion of SSA and core size as input parameters. Under the MODIS-only scenario, models using AOD alone yield limited explanatory power, withR (2) values of 0.59 (TOA), 0.61 (BOA), and 0.18 (ATM). Adding SSA improves the fits substantially, increasingR (2) to 0.78 (TOA) and 0.67 (BOA), and to 0.21 in the ATM. Incorporating core radius into the model yields additional gains, raisingR (2) in the ATM layer to 0.23 and lowering RMSE values across all layers. In the MODIS-OMI fusion scenario, even though the number of valid observation days decreases significantly (eg, from 2589 to 954 days at the Wucaiwan site), model performance continues to improve. For example,R (2) for ATM forcing increases from 0.18 to 0.29, and RMSE decreases from 2.04 to 1.85. These results suggest that high-spectral-resolution UV data provide greater constraint on aerosol absorption properties, thereby enabling more physically consistent radiative forcing estimates, even with reduced samples. This finding supports the robustness of UV-enhanced satellite inversion strategies in regional ARF modeling. Conclusions This study presents a data-model integration framework for estimating ARF over coal mining regions using multi-source satellite observations and physically based scattering and radiative transfer models. The combination of MODIS visible and OMI ultraviolet aerosol products improves the inversion of absorbing aerosol particle size distributions and enhances the retrieval of SSA, especially under complex mixing conditions. The constructed regression models reveal that SSA exerts a greater influence on radiative forcing than AOD, and that including particle size parameters further strengthens model reliability. Despite a reduction in observational frequency due to OMI's narrower sampling, the incorporation of UV-band information leads to consistently improved model performance across all atmospheric layers, particularly in the atmospheric column. These results highlight the critical role of spectral diversity in satellite remote sensing for accurately characterizing the radiative impacts of absorbing aerosols, and demonstrate the feasibility of applying such approaches to high-emission, data-scarce environments like the Zhundong Coalfield.
The recent large reduction in anthropogenic aerosol emissions across China has improved China's air quality but has potential consequences for climate forcing. This sharp reduction in anthropogenic emissions has occurred against a background influenced by changing regional biomass burning emissions over a similar period of time. Here, we use the UK Earth System Model (UKESM) to estimate aerosol instantaneous radiative forcing (IRF) due to changes in emissions of aerosols and precursors from biomass burning and anthropogenic sources (separately and in combination) over 2008-2016, with a focus on China and regions downwind. We also separately quantify the IRF due to changes in anthropogenic aerosol emissions inside China (CHN) and the Rest Of the World (ROW). Reductions in Chinese anthropogenic emissions of BC, SO2 and OC contributed -0.30 +/- 0.01, +1.00 +/- 0.04, and +0.05 +/- 0.01 W m-2, respectively to IRF over China, accounting for similar to 97% of the total local anthropogenic aerosol IRF. These emission changes contributed a remote regional IRF of 0.22 +/- 0.04 W m-2 over the North Pacific Ocean. The reduction in SO2 emissions from China contributed a global IRF of equal magnitude to that from SO2 emissions from ROW (similar to 0.08 W m-2). Changes in global biomass burning emissions contributed 0.03 W m-2 (equivalent to over 20% of the magnitude of anthropogenic aerosol IRF), enhancing the global anthropogenic aerosol IRF, whereas they partly offset the anthropogenic IRF over China. Meanwhile, biomass burning emissions dominated the total IRF (around 98%) over the Arctic.
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.