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.

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.

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.

Light-absorbing carbonaceous aerosols, comprising black carbon (BC) and brown carbon (BrC), significantly influence air quality and radiative forcing. Unlike traditional approaches that use a fixed value of absorption & Aring;ngstrom exponent (AAE), this study investigated the absorption and optical properties of carbonaceous aerosols in Beijing for both local emission and regional transport events during a wintertime pollution event by using improved AAE results that employs wavelength-dependent AAE (WDA). By calculating the difference of BC AAE at different wavelengths using Mie theory and comparing the calculated results to actual measurements from an Aethalometer (AE31), a more accurate absorption coefficient of BrC can be derived. Through the analysis of air mass sources, local emission was found dominated the pollution events during this study, accounting for 81 % of all cases, while regional transport played a minor role. Carbonaceous aerosols exhibited a continuous increasing trend during midday, which may be attributed to the re-entrainment of nighttime-accumulated carbonaceous aerosols to the surface during the early planetary boundary layer (PBL) development phase, as the mixed layer rises, combined with the variation of PBL and anthropogenic activity. At night, variations in the PBL height, in addition to anthropogenic activities, effectively contributed to surface aerosol concentrations, leading to peak surface aerosol values during local pollution episodes. The diurnal variation of AAE470/880 exhibited a decreasing trend, with a total decrease of approximately 12 %. Furthermore, the BrC fraction showed a constant diurnal variation, suggesting that the declining AAE470/880 was primarily influenced by BC, possibly due to enhanced traffic contributions.

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.

Brown carbon (BrC) aerosols play a significant role in atmospheric radiative forcing, particularly in the Arctic where they could potentially contribute to surface warming. However, their regional variability and sources in the open ocean remain poorly understood. To address this, we conducted ship-based aerosol measurements aboard the R/V Mirai during the MR18-05C research cruise (October-December 2018), spanning the western North Pacific, Bering Sea, and Arctic Ocean. We examined BrC optical properties alongside PM2.5 chemical composition, trace gases, and meteorological conditions to assess its variability and sources. Our results reveal a drastic northward decline in BrC levels, with light absorption capability in the Bering Sea and the Arctic approximately 50% lower than those in the western North Pacific. The strongest BrC absorption was observed in regions influenced by crop residue burning in Northeast China. In the Arctic, BrC remained low as the main footprint is within the Arctic alongside limited BrC sources, although occasionally affected by long-range transport. Chemical composition analysis highlights biomass burning and fossil fuel emissions as dominant BrC sources in the western North Pacific. Solubility analysis indicated that BrC in the Arctic was predominantly water soluble, increasing its susceptibility to wet scavenging. A strong high-pressure system (1027 +/- 6.2 hPa) over the Arctic (November 9-17) led to aerosol accumulation, although BrC remained low. This study underscores the complex interplay between regional emissions, long-range transport, and atmospheric processing in regulating BrC distributions across latitudinal gradients. Our findings highlight the importance of source-region emissions and transport pathways in determining BrC fate in the Arctic, with implications for understanding its role in climate forcing.

Char and soot represent distinct types of elemental carbon (EC) with varying sources and physicochemical properties. However, quantitative studies in sources, atmospheric processes and light-absorbing capabilities between them remain scarce, greatly limiting the understanding of EC's climatic and environmental impacts. For in-depth analysis, concentrations, mass absorption efficiency (MAE) and stable carbon isotope were analyzed based on hourly samples collected during winter 2021 in Nanjing, China. Combining measurements, atmospheric transport model and radiative transfer model were employed to quantify the discrepancies between char-EC and soot-EC. The mass concentration ratio of char-EC to soot-EC (R-C/S) was 1.4 +/- 0.6 (mean +/- standard deviation), showing significant dependence on both source types and atmospheric processes. Case studies revealed that lower R-C/S may indicate enhanced fossil fuel contributions, and/or considerable proportions from long-range transport. Char-EC exhibited a stronger light-absorbing capability than soot-EC, as MAE(char) (7.8 +/- 6.7 m(2)g(-1)) was significantly higher than MAE(soot) (5.4 +/- 3.4 m(2)g(-1))(p < 0.001). Notably, MAE(char) was three times higher than MAE(soot) in fossil fuel emissions, while both were comparable in biomass burning emissions. Furthermore, MAE(soot) increased with aging processes, whereas MAE(char) exhibited a more complex trend due to combined effects of changes in coatings and morphology. Simulations of direct radiative forcing (DRF) for five sites indicated that neglecting the char-EC/soot-EC differentiation could cause a 10 % underestimation of EC's DRF, which further limit accurate assessments of regional air pollution and climate effects. This study underscores the necessity for separate parameterization of two types of EC for pollution mitigation and climate change evaluation.

Carbonaceous aerosols play a crucial role in air pollution and radiative forcing, though their light-absorbing and isotopic characteristics remain insufficiently understood. This study analyzes optical absorption and isotopic composition in PM10 and PM2.5 particles from primary emission sources, focusing on traffic-related and solid fuel categories. We analyzed key optical properties, including the Angstrom absorption exponent (AAE), the contributions of black carbon (BC) and brown carbon (BrC) to total light absorption and the mass absorption efficiencies (MAE) of carbonaceous aerosols. AAE values were lower for traffic emission sources (0.9 to 1.3) than solid fuel emission sources (1.5 to 3), with similar values for both particle sizes. BrC contributions were more prominent at shorter wavelengths and were notably higher in solid fuel emission sources (61% to 88%) than in traffic emission sources (8% to 40%) at 405 nm. MAE values of BC at 405 nm were 2 to 20 times higher than BrC across different emissions. Particle size significantly affect MAE(BC) with PM2.5 higher when compared to PM10. Emissions from diesel concentrate mixer and raw coal burning exhibited the highest MAE(BC) for PM2.5 and PM10, respectively. Conversely, Coke had the lowest MAE(BC) but the highest MAE(BrC) for both sizes. Traffic emissions showed more stable carbon isotope ratios (delta C-13) enrichment (-29 parts per thousand to -24 parts per thousand) than solid fuels (-31 parts per thousand to -20 parts per thousand). delta C-13 of solid fuel combustion, unlike traffic sources, is found to be independent of size variation. These findings underscore the importance of source and size-specific aerosol characterization for unregulated emission sources.

In unsaturated soil mechanics, the liquid bridge force is a significant source of soil cohesion and tensile strength. However, the classical Young-Laplace equation, which neglects the stratified nature of water at the nanoscale, fails to accurately capture the physical and mechanical behaviour of nanoscale liquid bridges. This study utilizes molecular dynamics simulations to investigate the wetting behaviour and mechanical mechanisms of liquid bridges between particles at the nanoscale. The study proposes dividing the liquid bridge force into three components: surface tension, matric suction, and adsorption force, to explain the mechanics of nanoscale liquid bridges more comprehensively. The results demonstrate that water layers within liquid bridges exhibit discrete stratified structures at the nanoscale. Moreover, the mechanical behaviour of liquid bridges is highly dependent on pore water volume and pore spacing. Specifically, the contact angle is positively correlated with the pore spacing, while the liquid bridge force increases with the pore water volume and is inversely proportional to the pore spacing. As the separation distance increases, the liquid bridge force gradually diminishes until rupture occurs. This research expands the applicability of the classical Young-Laplace equation and offers new insights into the mechanical properties of unsaturated soils, particularly clays.