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​​​​​​​This study compares aerosol mixing-state parameters obtained via simultaneous measurements using DMA–CCNC, H(/V)TDMA, and DMA–SP2, shedding light on the impacts of primary aerosol emissions and secondary aerosol (SA) formation. The analysis reveals significant variations in mixing-state parameters among different techniques, with VTDMA and DMA–SP2 indicating that non-volatile particles mainly stem from black carbon (BC)-containing aerosols, while a substantial proportion of nearly hydrophobic aerosols originates from fossil fuel combustion and biomass-burning emissions. Synthesizing the results, some nearly hydrophobic BC-free particles were found to be cloud condensation nuclei (CCN)-inactive under the measured supersaturated conditions, likely from fossil fuel combustion emissions, while others were CCN-active, linked to biomass-burning emissions. Moreover, BC-containing aerosols emitted from fossil fuel combustion exhibit more external mixing with other aerosol components compared to those from biomass burning. Secondary nitrate and organic aerosol formation significantly affect aerosol mixing states, enhancing aerosol hygroscopicity and volatility while reducing heterogeneity among techniques. The study also highlights distinct physical properties of two resolved secondary organic aerosol factors, hinting at their formation through different mechanisms. These findings underscore the importance of comparing aerosol mixing states from different techniques as a tool for understanding aerosol physical properties from different sources and their responses to SA formation, as well as aiding in the exploration of SA formation mechanisms. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is one of the most important climate forcers with severe health effects. Large uncertainties in radiative forcing estimation and health impact assessment arise from the fact that there is no standardized method to measure BC mass concentration. This study presents a 2-year comparison of three state-of-the-art BC measurement techniques at the high-altitude research station Pic du Midi (PDM) located in the French Pyrenees at an altitude of 2877 m above sea level. A recently upgraded Aethalometer AE33, a thermal-optical analyser Sunset and a single-particle soot photometer SP2 were deployed to measure simultaneously the mass concentration of equivalent black carbon (MeBC), elemental carbon (MEC) and refractory black carbon (MrBC), respectively. Significant deviations in the response of the instruments were observed. All techniques responded to seasonal variations in the atmospheric changes in BC levels and exhibited good correlation during the whole study period. This indicates that the different instruments quantified the same particle type despite the fact that they are based on different physical principles. However the slopes and correlation coefficients varied between instrument pairs. The largest biases were observed for the AE33 with MeBC values that were around 2 times greater than MrBC and MEC values. The principal reasons of such large discrepancy were explained by the mass absorption cross section (MAC) that was too low and C values recommended by the AE33 manufacturer and applied to the absorption coefficients measured by the AE33. In addition, the long-range transport of dust particles at PDM in spring caused significant increases in the bias between AE33 and SP2 by up to a factor 8. The Sunset MEC measurements agreed within around 17 % with the SP2 MrBC values. The largest overestimations of MEC were observed when the total carbon concentrations were below 25 µgCcm-2 , which is probably linked to the incorrect determination of the organic carbon (OC)–EC split point. Another cause of the discrepancy between instruments was found to be the limited detection range of the SP2, which did not allow for the total detection of fine rBC particles. The procedure used to estimate the missing mass fraction of rBC not covered by the measurement range of the SP2 was found to be critical. We found that a time-dependent correction based on fitting the observed rBC size distribution with a multimodal lognormal distribution is needed to accurately estimate MrBC over a larger size range. [ABSTRACT FROM AUTHOR]

Anthropogenic aerosols play a major role in the Earth–atmosphere system by influencing the Earth's radiative budget and precipitation and consequently the climate. The perturbation induced by changes in anthropogenic aerosols on the Earth's energy balance is quantified in terms of the effective radiative forcing (ERF). In this work, the present-day shortwave (SW), longwave (LW), and total (i.e., SW plus LW) ERF of anthropogenic aerosols is quantified using two different sets of experiments with prescribed sea surface temperatures (SSTs) from Earth system models (ESMs) participating in the Coupled Model Intercomparison Project Phase 6 (CMIP6): (a) time-slice pre-industrial perturbation simulations with fixed SSTs (piClim) and (b) transient historical simulations with time-evolving SSTs (histSST) over the historical period (1850–2014). ERF is decomposed into three components for both piClim and histSST experiments: (a) ERFARI , representing aerosol–radiation interactions; (b) ERFACI , accounting for aerosol–cloud interactions (including the semi-direct effect); and (c) ERFALB , which is due to temperature, humidity, and surface albedo changes caused by anthropogenic aerosols. We present spatial patterns at the top-of-atmosphere (TOA) and global weighted field means along with inter-model variability (1 standard deviation) for all SW, LW, and total ERF components (ERFARI , ERFACI , and ERFALB) and for every experiment used in this study. Moreover, the inter-model agreement and the robustness of our results are assessed using a comprehensive method as utilized in the IPCC Sixth Assessment Report. Based on piClim experiments, the total present-day (2014) ERF from anthropogenic aerosol and precursor emissions is estimated to be - 1.11 ± 0.26 Wm-2 , mostly due to the large contribution of ERFACI to the global mean and to the inter-model variability. Based on the histSST experiments for the present-day period (1995–2014), similar results are derived, with a global mean total aerosol ERF of - 1.28 ± 0.37 Wm-2 and dominating contributions from ERFACI. The spatial patterns for total ERF and its components are similar in both the piClim and histSST experiments. Furthermore, implementing a novel approach to determine geographically the driving factor of ERF, we show that ERFACI dominates over the largest part of the Earth and that ERFALB dominates mainly over the poles, while ERFARI dominates over certain reflective surfaces. Analysis of the inter-model variability in total aerosol ERF shows that SW ERFACI is the main source of uncertainty predominantly over land regions with significant changes in aerosol optical depth (AOD), with eastern Asia contributing mostly to the inter-model spread of both ERFARI and ERFACI. The global spatial patterns of total ERF and its components from individual aerosol species, such as sulfates, organic carbon (OC), and black carbon (BC), are also calculated based on piClim experiments. The total ERF caused by sulfates (piClim- SO2) is estimated at - 1.11 ± 0.31 Wm-2 , and the OC ERF (piClim-OC) is - 0.35 ± 0.21 Wm-2 , while the ERF due to BC (piClim-BC) is 0.19 ± 0.18 Wm-2. For sulfates and OC perturbation experiments, ERFACI dominates over the globe, whereas for BC perturbation experiments ERFARI dominates over land in the Northern Hemisphere and especially in the Arctic. Generally, sulfates dominate ERF spatial patterns, exerting a strongly negative ERF especially over industrialized regions of the Northern Hemisphere (NH), such as North America, Europe, and eastern and southern Asia. Our analysis of the temporal evolution of ERF over the historical period (1850–2014) reveals that ERFACI clearly dominates over ERFARI and ERFALB for driving the total ERF temporal evolution. Moreover, since the mid-1980s, total ERF has become less negative over eastern North America and western and central Europe, while over eastern and southern Asia there is a steady increase in ERF magnitude towards more negative values until 2014. [ABSTRACT FROM AUTHOR]

Earth system models (ESMs) participating in the latest Coupled Model Intercomparison Project Phase 6 (CMIP6) simulate various components of fine particulate matter (PM2.5) as major climate forcers. Yet the model performance for PM2.5 components remains little evaluated due in part to a lack of observational data. Here, we evaluate near-surface concentrations of PM2.5 and its five main components over China as simulated by 14 CMIP6 models, including organic carbon (OC; available in 14 models), black carbon (BC; 14 models), sulfate (14 models), nitrate (4 models), and ammonium (5 models). For this purpose, we collect observational data between 2000 and 2014 from a satellite-based dataset for total PM2.5 and from 2469 measurement records in the literature for PM2.5 components. Seven models output total PM2.5 concentrations, and they all underestimate the observed total PM2.5 over eastern China, with GFDL-ESM4 (- 1.5 %) and MPI-ESM-1-2-HAM (- 1.1 %) exhibiting the smallest biases averaged over the whole country. The other seven models, for which we recalculate total PM2.5 from the available component output, underestimate the total PM2.5 concentrations partly because of the missing model representations of nitrate and ammonium. Concentrations of the five individual components are underestimated in almost all models, except that sulfate is overestimated in MPI-ESM-1-2-HAM by 12.6 % and in MRI-ESM2-0 by 24.5 %. The underestimation is the largest for OC (by - 71.2 % to - 37.8 % across the 14 models) and the smallest for BC (- 47.9 % to - 12.1 %). The multi-model mean (MMM) reproduces the observed spatial pattern for OC (R = 0.51), sulfate (R = 0.57), nitrate (R = 0.70) and ammonium (R = 0.74) fairly well, yet the agreement is poorer for BC (R = 0.39). The varying performances of ESMs on total PM2.5 and its components have important implications for the modeled magnitude and spatial pattern of aerosol radiative forcing. [ABSTRACT FROM AUTHOR]

Black carbon (BC) plays an important role in air quality, public health, and climate, but its long-term variations in emissions and health effects have been insufficiently understood for China. Here, we present the spatiotemporal evolution of BC emissions and the associated premature mortality in China during 2000–2020 based on an integrated framework combining satellite observations from the Ozone Monitoring Instrument (OMI), an extreme gradient boosting (XGBoost) algorithm, a "top-down" inversion approach, and an exposure–response model. We found that the "bottom-up" approach most likely underestimated BC emissions, particularly in less developed western and remote areas. Pollution controls were estimated to reduce the annual BC emissions by 26 % during 2010–2020, reversing the 8 % growth during 2000–2010. BC emissions in the main coal-producing provinces declined by 2010 but rebounded afterwards. By contrast, provinces with higher economic and urbanization levels experienced emission growth (0.05–0.10 Mg km -2 yr -1) by 2010 and declined greatly (0.07–0.23 Mg km -2 yr -1) during 2010–2020. The national annual BC-associated premature mortality ranged between 733 910 (95 % confidence interval: 676 790–800 250) and 937 980 cases (864 510–1 023 400) for different years. The changing BC emissions contributed to an increase of 78 590 cases (72 520–85 600) during 2000–2005 and a decrease of 133 360 cases (123 150–145 180) during 2010–2015. Strategies differentiated by region are needed for further reducing BC emissions and their health and climate impacts. [ABSTRACT FROM AUTHOR]

Black carbon (BC) aerosol is considered one of the most important contributors to rapid climate warming as well as snow and sea ice melting in the Arctic, yet the observations of BC aerosols in the Arctic Ocean have been limited due to infrastructural and logistical difficulties. We observed BC mass concentrations (mBC) using light absorption methods on board the icebreaker R/V Araon in the Arctic Ocean (< 80° N and 166° E to 156° W) as well as the North Pacific Ocean in summer and early autumn of 2016–2020. The levels, interannual variations, and pollution episodes of mBC in the Arctic were examined, and the emission sources responsible for the high-BC episodes were analyzed with global chemistry-transport-model simulations. The average mBC in the surface air over the Arctic Ocean (72–80° N) observed by the 2019 cruise exceeded 70 ng m -3 , which was substantially higher than that observed by cruises in other years (approximately 10 ng m -3). The much higher mBC observed in 2019 was perhaps due to more frequent wildfires occurring in the Arctic region than in other years. The model suggested that biomass burning contributed most to the observed BC by mass in the western Arctic Ocean and the marginal seas. For these 5 years, we identified 10 high-BC episodes north of 65° N, including one in 2018 that was associated with co-enhancements of CO and CH 4 but not CO 2 and O 3. The model analysis indicated that certain episodes were attributed to BC-containing air masses transported from boreal fire regions to the Arctic Ocean, with some transport occurring near the surface and others in the mid-troposphere. This study provides crucial datasets on BC mass concentrations and the mixing ratios of O 3 , CH 4 , CO, and CO 2 in the western Arctic Ocean regions, and it highlights the significant impact of boreal fires on the observed Arctic BC during the summer and early autumn months. [ABSTRACT FROM AUTHOR]

The Aethalometer is a widely used instrument for black carbon (BC) mass concentration and light absorption coefficient (babs) measurements around the world. However, field intercomparison of the two popular models, dual-spot (AE33) and single-spot (AE31) Aethalometers, remains limited; in addition, the difference in secondary brown carbon (BrCsec) light absorption estimation between the two models is largely unknown. We performed full-year collocated AE33 and AE31 measurements in a megacity in southern China – Guangzhou. The babs values agree well between the two Aethalometers (R2 > 0.95), with AE33 / AE31 slopes ranging from 0.87 to 1.04 for seven wavelengths. AE33 consistently exhibits lower limits of detection (LODs) than AE31 for time resolutions of 2 to 60 min. The AE33 / AE31 slope for equivalent BC (eBC) was 1.2, implying the need for site-specific post-correction. The absorption Ångström exponent (AAE) obtained from different approaches does not agree very well between the two models, with the biggest discrepancy found in AAE880/950. The estimated BrCsec light absorption at 370 nm (babs370_BrCsec) was calculated using the minimum- R -squared (MRS) method for both Aethalometers. The babs370_BrCsec comparison yields a slope of 0.78 and an R2 of 0.72 between the two models, implying a non-negligible inter-instrument difference. This study highlights the high consistency in babs but less so in AAE between AE31 and AE33 and reveals site-specific correction for eBC estimation and non-negligible difference in BrCsec estimation. The results are valuable for data continuity in long-term Aethalometer measurements when transitioning from the older (AE31) to the newer (AE33) model, as anticipated in permanent global-climate and air-quality stations. [ABSTRACT FROM AUTHOR]

Currently, emissions from internal combustion vehicles are not properly monitored throughout their life cycle. In particular, a small share of vehicles (< 20 %) with malfunctioning after-treatment systems and old vehicles with outdated engine technology are responsible for the majority (60 %–90 %) of traffic-related emissions. Remote emission sensing (RES) is a method used for screening emissions from a large number of in-use vehicles. Commercial open-path RES systems are capable of providing emission factors for many gaseous compounds, but they are less accurate and reliable for particulate matter (PM). Point sampling (PS) is an extractive RES method where a portion of the exhaust is sampled and then analyzed. So far, PS studies have been predominantly conducted on a rather small scale and have mainly analyzed heavy-duty vehicles (HDVs), which have high exhaust flow rates. In this work, we present a comprehensive PS system that can be used for large-scale screening of PM and gas emissions, largely independent of the vehicle type. The data analysis framework developed here is capable of processing data from thousands of vehicles. The core of the data analysis is our peak detection algorithm (TUG-PDA), which determines and separates emissions down to a spacing of just a few seconds between vehicles. We present a detailed evaluation of the main influencing factors on PS measurements by using about 100 000 vehicle records collected from several measurement locations, mainly in urban areas. We show the capability of the emission screening by providing real-world black carbon (BC), particle number (PN) and nitrogen oxide (NOx) emission trends for various vehicle categories such as diesel and petrol passenger cars or HDVs. Comparisons with open-path RES and PS studies show overall good agreement and demonstrate the applicability even for the latest Euro emission standards, where current open-path RES systems reach their limits. [ABSTRACT FROM AUTHOR]

An enhanced formation of brown carbon (BrC) with a non-negligible warming effect at the tropopause has recently been found. However, its formation mechanism is unclear. Here we report a BrC formation process that happens during air mass upward transport by conducting simultaneously a 4-hour time resolution of measurement on atmospheric BrC at the mountain foot (MF, 400 m a.s.l.) and mountainside (MS, 1120 m a.s.l.) of Mt. Hua, China in 2016 summer. Our results showed that the daytime light-absorption (Abs365nm) of BrC at MS is approximately 60 % lower than that at MF due to a dilution effect caused by the planetary boundary layer expansion, but the daytime light-absorption of BrC relative to black carbon at MS is about 30 % higher than that at MF, suggesting a significant formation of secondary BrC in the lifting process of air mass from MF to MS. Such a secondary formation accounted for >50 % of BrC at MS but only 27 % of BrC at MF. Moreover, N:C elemental ratio of the daytime BrC was 15 % higher at MS than that at MF, mainly due to an aerosol aqueous phase formation of water-soluble organic nitrogen (WSON) compounds. Stable nitrogen isotope composition further indicated that such light-absorbing WSON compounds were produced from the aerosol aqueous-phase reaction of carbonyls with NH4+. Our work for the first time revealed that ammonia-induced aerosol aqueous reactions can significantly promote BrC formation during the air mass lifting process, which is probably responsible for an enhanced light absorption of BrC in the upper troposphere. [ABSTRACT FROM AUTHOR]

The cloud condensation nuclei (CCN) activity of black carbon (BC) particles importantly determines their impacts on cloud microphysics and atmospheric lifetime. This process is crucially influenced by the number of hygroscopic coating materials that BC acquire during the ageing process. It remains a challenge for ambient measurements to capture this process and link this with CCN activity of BC. Here, we directly measured the droplet activation diameter (D50) and activation fraction of BC-containing (BCc) particles (Fact,BC) in suburban Beijing using coupled measurements of size-resolved number concentrations of CCN at configured water supersaturation (SS) and BCc particles. The number concentration of BCc particles was found to peak at diameter 180–210 nm after acquiring coatings, larger than that for all particles (50–150 nm). Consequently, the initially smaller BC particles become enlarged and more hygroscopic, thereby exhibiting CCN activities than other particles. The Fact,BC increased from 42 % to 69 % in number and from 67 % to 85 % in mass as SS increased from 0.1 % to 0.2 % but tended to reach a plateau when SS > 0.2 %. Notably, Fact,BC and D50 linearly correlated with equivalent photochemical age, at a rate of +2 % h -1 and -3 nm h -1 , respectively. The results suggest BCc particles from anthropogenic sources can readily serve as CCN at a relatively low SS, and more than half of the BC population can be activated within a few hours, indicating that the surface-sourced BC can efficiently incorporate into clouds and potentially exert important indirect radiative impacts. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is a major component of sub-micron particulate matter (PM) with significant health and climate impacts. Many cities in emerging countries lack comprehensive knowledge about BC emissions and exposure levels. This study investigates BC concentration levels, identify its emission sources, and characterize the optical properties of BC at urban background sites of the two largest high-altitude Bolivian cities: La Paz (LP) (3600 m above sea level) and El Alto (EA) (4050 m a.s.l.) where atmospheric oxygen levels and intense radiation may affect BC production. The study relies on concurrent measurements of equivalent black carbon (eBC), elemental carbon (EC), and refractory black carbon (rBC), and their comparison with analogous data collected at the nearby Global Atmosphere Watch-Chacaltaya station (5240 m a.s.l). The performance of two independent source-apportionment techniques was compared: a bilinear model and a least squares multilinear regression (MLR). Maximum eBC concentrations were observed during the local dry season (LP: eBC=1.5±1.6 μg m-3; EA: 1.9±2.0 μg m-3). While eBC concentrations are lower at the mountain station, daily transport from urban areas is evident. Average mass absorption cross sections of 6.6-8.2 m2 g-1 were found in the urban area at 637 nm. Both source apportionment methods exhibited a reasonable level of agreement in the contribution of biomass burning (BB) to absorption. The MLR method allowed the estimation of the contribution and the source-specific optical properties for multiple sources including open waste burning. [ABSTRACT FROM AUTHOR]

Recent years have seen an increase in the use of wood for energy production of over 30 %, and this trend is expected to continue due to the current energy crisis and geopolitical instability. At present, residential wood burning (RWB) is one of the most important sources of organic aerosols (OAs) and black carbon (BC), posing a significant risk to air quality and health. Simultaneously, as a substantial aerosol source, RWB also holds relevance in the context of aerosol radiative effects and climate. While BC is recognized for its large light absorption cross-section, the role of OAs in light absorption is still under evaluation due to their heterogeneous composition and source-dependent optical properties. Existing studies that characterize wood-burning aerosol emissions in Europe primarily concentrate on urban and background sites and focus on BC properties. Despite the significant RWB emissions in rural areas, these locations have received comparatively less attention. The present scenario underscores the imperative for an improved understanding of RWB pollution, aerosol optical properties, and their subsequent connection to climate impacts, particularly in rural areas. We have characterized atmospheric aerosol particles from a central European rural site during wintertime in the village of Retje in Loški Potok, Slovenia, from 1 December 2017 to 7 March 2018. The village experienced extremely high aerosol concentrations produced by RWB and near-ground temperature inversion. The isolated location of the site and the substantial local emissions made it an ideal laboratory-like place for characterizing RWB aerosols with low influence from non-RWB sources under ambient conditions. The mean mass concentrations of OA and BC were 35 µgm-3 (max⁡=270 µgm-3) and 3.1 µgm-3 (max⁡=24 µgm-3), respectively. The mean total particle number concentration (10–600 nm) was 9.9×103 particles cm -3 (max⁡=59×103 particles cm -3). The mean total light absorption coefficients at 370 and 880 nm measured by an AE33 Aethalometer were 120 and 22 Mm -1 and had maximum values of 1100 and 180 Mm -1 , respectively. The aerosol concentrations and absorption coefficients measured during the campaign in Loški Potok were significantly larger than reported values for several urban areas in the region with larger populations and a larger extent of aerosol sources. Here, considerable contributions from brown carbon (BrC) to the total light absorption were identified, reaching up to 60 % and 48 % in the near-UV (370 nm) and blue (470 nm) wavelengths. These contributions are up to 3 times higher than values reported for other sites impacted by wood-burning emissions. The calculated mass absorption cross-section and the absorption Ångström exponent for RWB OA were MAC OA,370nm=2.4 m 2 g -1 , and AAE BrC,370-590nm=3.9 , respectively. Simple-forcing-efficiency (SFE) calculations were performed as a sensitivity analysis to evaluate the climate impact of the RWB aerosols produced at the study site by integrating the optical properties measured during the campaign. The SFE results show a considerable forcing capacity from the local RWB aerosols, with a high sensitivity to OA absorption properties and a more substantial impact over bright surfaces like snow, typical during the coldest season with higher OA emissions from RWB. Our study's results are highly significant regarding air pollution, optical properties, and climate impact. The findings suggest that there may be an underestimation of RWB emissions in rural Europe and that further investigation is necessary. [ABSTRACT FROM AUTHOR]

Speed restrictions for ships have been introduced locally to reduce the waves and turbulence causing erosion, and safety hazards, and to mitigate the air and underwater noise emissions. Ship speed restrictions could be used to minimise the climate impact of maritime transport since many air pollutants in ship exhaust gas are reduced when travelling at lower speeds. However, for example, methane and black carbon emissions do not linearly correlate with the load of internal combustion engines. Therefore, the effect of speed restrictions may not be trivial. Black carbon concentrations from ship plumes were examined at the remote marine site in the Finnish Southwestern archipelago. Ships with service speeds over 15 knots and equipped with an exhaust gas cleaning system were analysed for black carbon emissions as a function of speed. Both unadjusted and weather-adjusted main engine loads were modelled to determine load-based emission factors. Black carbon concentration per kilogram of fuel decreased as a function of engine load. However, as calculated per hour the black carbon emission increased as a function of ship speed except around a constant emission area, which was roughly 15–20 knots. In terms of local air quality, total black carbon emission per nautical mile was the highest around the halved speeds, 10–13 knots, or when the speed was higher than 20–23 knots. From a climate warming perspective, the CO2 emissions dominated the exhaust gas and reducing the speed decreased the global warming potential in CO2 equivalent both per hour and per nautical mile. [ABSTRACT FROM AUTHOR]

Understanding black carbon (BC) levels and their sources in urban environments is of paramount importance due to their far-reaching health, climate and air quality implications. While several recent studies have assessed BC concentrations at specific fixed urban locations, there is a notable lack of knowledge in the existing literature on spatially resolved data alongside source estimation methods. This study aims to fill this gap by conducting a comprehensive investigation of BC levels and sources in Modena (Po Valley, Italy), which serves as a representative example of a medium-sized urban area in Europe. Using a combination of multi-wavelength micro-aethalometer measurements and a hybrid Eulerian-Lagrangian modelling system, we studied two consecutive winter seasons (February–March 2020 and December 2020–January 2021). Leveraging the multi-wavelength absorption analyser (MWAA) model, we differentiate sources (fossil fuel combustion, FF, and biomass burning, BB) and components (BC vs. brown carbon, BrC) from micro-aethalometer measurements. The analysis reveals consistent, minimal diurnal variability in BrC absorption, in contrast to FF-related sources, which exhibit distinctive diurnal peaks during rush hours, while BB sources show less diurnal variation. The city itself contributes significantly to BC concentrations (52 % ± 10 %), with BB and FF playing a prominent role (35 % ± 15 % and 9 % ± 4 %, respectively). Long-distance transport also influences BC concentrations, especially in the case of BB and FF emissions, with 28 % ± 1 % and 15 % ± 2 %, respectively. When analysing the traffic related concentrations, Euro 4 diesel passenger cars considerably contribute to the exhaust emissions. These results provide valuable insights for policy makers and urban planners to manage BC levels in medium-sized urban areas, taking into account local and long-distance sources. [ABSTRACT FROM AUTHOR]

Black-carbon-containing particles strongly absorb light, causing substantial radiative heating of the atmosphere. The climate-relevant properties of black carbon (BC) are poorly constrained in high-altitude mountain regions, where many complex interactions between BC, radiation, clouds and snow have important climate implications. This study presents 2-year measurements of BC microphysical and optical properties at the Pic du Midi (PDM) research station, a high-altitude observatory located at 2877 m above sea level in the French Pyrenees. Among the long-term monitoring sites in the world, PDM is subject to limited influence from the planetary boundary layer (PBL), making it a suitable site for characterizing the BC in the free troposphere (FT). The classification of the dominant aerosol type using aerosol spectral optical properties indicates that BC is the predominant aerosol absorption component at PDM and controls the variation in single-scattering albedo (SSA) throughout the 2 years. Single-particle soot photometer (SP2) measurements of refractory BC (rBC) show a mean mass concentration (MrBC) of 35 ngm-3 and a relatively constant rBC core mass-equivalent diameter of about 180 nm, which are typical values for remote mountain sites. Combining the MrBC with in situ absorption measurements, a rBC mass absorption cross-section (MAC rBC) of 9.2 ± 3.7 m2g-1 at λ=880 nm has been obtained, which corresponds to an absorption enhancement (Eabs) of ∼2.2 compared to that of bare rBC particles with equal rBC core size distribution. A significant reduction in the ΔMrBC/ΔCO ratio when precipitation occurred along the air mass transport suggests wet removal of rBC. However we found that the wet removal process did not affect the rBC size, resulting in unchanged Eabs. We observed a large seasonal contrast in rBC properties with higher MrBC and Eabs in summer than in winter. In winter a high diurnal variability in MrBC (Eabs) with higher (lower) values in the middle of the day was linked to the injection of rBC originating from the PBL. On the contrary, in summer, MrBC showed no diurnal variation despite more frequent PBL conditions, implying that MrBC fluctuations are rather dominated by regional and long-range transport in the FT. Combining the ΔMrBC/ΔCO ratio with air mass transport analysis, we observed additional sources from biomass burning in summer leading to an increase in MrBC and Eabs. The diurnal pattern of Eabs in summer was opposite to that observed in winter with maximum values of ∼2.9 observed at midday. We suggest that this daily variation may result from a photochemical process driving the rBC mixing state rather than a change in BC emission sources. Such direct 2-year observations of BC properties provide quantitative constraints for both regional and global climate models and have the potential to close the gap between model-predicted and observed effects of BC on the regional radiation budget and climate. The results demonstrate the complex influence of BC emission sources, transport pathways, atmospheric dynamics and chemical reactivity in driving the light absorption of BC. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is one of the most important climate forcer with severe health effects. Large uncertainties in radiative forcing estimation and health impact assessment arise from the fact that there is no standardized method to measure BC mass concentration. This study presents a two-year comparison of three state-of-the-art BC measurement techniques at the high-altitude research station Pic du Midi located in the French Pyrenees at an altitude of 2877 m above sea level. A recently upgraded aethalometer AE33, a thermal-optical analyzer Sunset and a single-particle soot photometer SP2 were deployed to measure simultaneously the mass concentration of equivalent black carbon (MeBC), elemental carbon (MEC) and refractory black carbon (MrBC), respectively. Significant deviations in the response of the instruments were observed. All techniques responded to seasonal variations of the atmospheric changes in BC levels and exhibited good correlation during the whole study period. This indicates that the different instruments quantified the same particle type, despite the fact that they are based on different physical principles. However the slopes and correlation coefficients varied between instrument pairs. The largest biases were observed for the AE33 with MeBC values that were around 2 times greater than MrBC and MEC values. The principal reasons of such large discrepancy was explained by the too low MAC and C values recommended by the AE33 manufacturer and applied to the absorption coefficients measured by the AE33. In addition, the long-range transport of dust particles at PDM in spring caused significant increases in the bias between AE33 and SP2 by up to a factor 8. The Sunset MEC measurements agreed within around 17 % with the SP2 MrBC values. The largest overestimations of MEC were observed when the total carbon concentration were below 25 µ gC cm−2 , which is probably linked to the incorrect determination of the OC-EC split point. Another cause of the discrepancy between instruments was found to be the limited detection range of the SP2, which did not allow the total detection of fine rBC particles. The procedure used to estimate the missing mass fraction of rBC not covered by the measurement range of the SP2 was found to be critical. We found that a time-dependent correction based on fitting the observed rBC size distribution with a multimodal lognormal distribution are needed to accurately estimate MrBC over a larger size range. [ABSTRACT FROM AUTHOR]

Atmospheric aerosols strongly influence the global climate by their light absorption (e.g., black carbon, BC, brown carbon, BrC) and scattering (e.g., sulfate) properties. This study presents simultaneous measurements of ambient aerosol light absorption properties and chemical composition from three large-footprint South Asian receptor sites during the South Asian Pollution Experiment (SAPOEX) in December-March 2018. The BC mass absorption cross-section (BC-MAC678) values increased from 3.5 ± 1.3 at the Bhola Climate Observatory-Bangladesh (i.e., located at exit outflow of Indo-Gangetic Plain) to 6.4 ± 1.3 at the two regional receptor observatories at Maldives Climate Observatory-Hanimaadhoo (MCOH) and Maldives Climate Observatory-Gan (MCOG). This likely reflects a coating-enhancement effect due to ageing of the aerosols during long-range transport. At the same time, the BrC-MAC365 decreased by a factor of three from the IGP exit to the equatorial Indian Ocean, likely due to photochemical bleaching of organic chromophores. The high chlorine-to-sodium ratio at the near-source-region BCOB suggests a significant contribution of chorine from anthropogenic activities. This particulate Cl- has the potential to convert into Cl-radicals that can affect the oxidation capacity of the polluted air. Moreover, Cl- is shown to be near-fully consumed during the long-range transport. The results of this synoptic study over the large South Asian scale have significance for understanding the ageing effect of the optical and chemical properties of aerosols as the pollution from the Indo-Gangetic Plain disperses over regional scales. [ABSTRACT FROM AUTHOR]

Black carbon (BC) exerts potential effects on climate, especially in the Tibetan Plateau (TP), where the cryosphere and environment are very sensitive to climate change. The TP saw a record-breaking aerosol pollution event during the period from 20 April to 10 May 2016. This paper investigates the meteorological causes of the severe aerosol pollution event, the transboundary transport flux of BC, the aerosol–meteorology feedback, and its effect on the transboundary transport flux of BC during the severe aerosol pollution event using observational and reanalysis datasets as well as simulation based on a coupled meteorology and aerosol/chemistry model, Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). By analyzing weather maps derived from the reanalysis dataset, it is found that the plateau vortex and southerly winds were key factors that contributed to the severe aerosol pollution event. Subsequently, due to the good performance of the WRF-Chem model for the spatiotemporal characteristics of meteorological conditions and aerosols, the transboundary transport flux of BC during the pollution event was investigated. The results show that the vertically integrated cross-Himalayan transport flux of BC decreases from west to east, with the largest transport flux of 20.8 mg m -2 s -1 occurring at the deepest mountain valley in southwestern TP. Results from simulations with and without aerosol–meteorology feedback show that aerosols induce significant changes in meteorological conditions in the southern TP and the Indo-Gangetic Plain (IGP), with the atmospheric stratification being more stable and the planetary boundary layer height decreasing in both regions, and the 10 m wind speed increasing in the southern TP but decreasing in the IGP. Changes in meteorological conditions in turn lead to a decrease in the surface BC concentration in the southern TP of up to 0.16 µ g m -3 (50 %) and an increase in the surface BC concentration in the IGP of up to 2.2 µ g m -3 (75 %). In addition, it is found that the aerosol–meteorology feedback decreases the vertically integrated transboundary transport flux of BC from the central and western Himalayas towards the TP. This study not only provides crucial policy implications for mitigating glacier melt caused by aerosols over the TP but is also of great significance for the protection of the ecological environment of the TP. [ABSTRACT FROM AUTHOR]

Methods based on the absorption Ångström exponent (AAE) are widely used to estimate the absorption by brown carbon (BrC), and the estimated absorption by BrC can be significantly different from 0, even for pure black carbon (BC). However, few studies have systematically quantified the effects of BC microphysical properties. Moreover, the conditions under which AAE-based methods are applicable are still unclear. In this work, we used BC models partially coated with non-absorbing materials to calculate the total absorption. Since the total absorption is entirely due to BC, the estimated BrC absorption should be 0 if the retrieval methods are accurate. Thus, the ratio of the estimated BrC absorption to BC absorption (ABS BrC) should be the proportion of the BC absorption that is incorrectly attributed to BrC. The results show that a BC AAE of 1 can generally provide reasonable estimates for freshly emitted BC, since ABS BrC is generally in the range of -4.8 % to 2.7 % during that period. However, when BC aerosols are aged, ABS BrC can sometimes reach about 38.7 %. The wavelength dependence of the AAE (WDA) method does not necessarily improve the estimates; sometimes a negative ABSBrC of about -40.8 % is found for partially coated BC. By combining simulations of a global chemical transport model, this work also quantified the effects of BC microphysical properties on BrC global aerosol absorption optical depth (AAOD) estimates. The AAE = 1 method sometimes leads to a misassigned global mean AAOD of about - 0.43– 0.46×10-3 if the BC aerosols have a complex morphology. The WDA method does not necessarily improve the estimates. In our cases, the WDA methods based on spherical models could lead to a global-mean misassigned AAOD range of about -0.87 – 0.04×10-3. At the regional scale, the AAE = 1 method sometimes leads to a distributed AAOD of about -7.3 to 5.7×10-3 in some specific regions. Mie-theory-based WDA methods lead to an estimated AAOD error of about -22×10-3 in some regions (e.g., East Asia). This work also showed that the misattributed BrC absorption would lead to substantial uncertainties in the estimation of the global direct radiative forcing (DRF) of absorbing aerosols from different sources. [ABSTRACT FROM AUTHOR]

Forest wildfires in interior Alaska represent an important black carbon (BC) source for the Arctic and sub-Arctic. However, BC observations in interior Alaska have not been sufficient to constrain the range of existing emissions. Here, we show our observations of BC mass concentrations and carbon monoxide (CO) mixing ratios in the Poker Flat Research Range (65.12° N, 147.43° W), located in central Alaska, since April 2016. The medians of the hourly BC mass concentration and CO mixing ratio throughout the observation period were 13 ng m-3 and 124.7 ppb, respectively. Significant peaks in the BC mass concentration and CO mixing ratio were observed at the same time, indicating influences from common sources. These BC peaks coincided with peaks at other comparative sites in Alaska, indicating large BC emissions in interior Alaska. Source estimation by FLEXPART-WRF confirmed a contribution of forest wildfires in Alaska when high BC mass concentrations were observed. For these cases, we found a positive correlation (r = 0.44) between the observed BC/∆CO ratio and fire radiative power (FRP) observed in Alaska and Canada. This finding indicates that the BC and CO emission ratio is controlled by the intensity and time progress of forest wildfires and suggests the BC emission factor or/and inventory could be potentially improved by FRP. We recommend that FRP be integrated into future bottom-up emission inventories to achieve a better understanding of the dynamics of pollutants from frequently occurred forest wildfires under the rapidly changing climate in the Arctic. [ABSTRACT FROM AUTHOR]

Black carbon (BC) plays an important role in air quality, public health, and climate, while its long-term variations in emissions and health effect were insufficiently understood for China. Here, we present the spatiotemporal evolution of BC emissions and the associated premature mortality in China during 2000–2020 based on an integrated framework combining satellite observations, a machine learning technique, a "top-down" inversion approach, and an exposure-response model. We found that the "bottom-up" approach likely underestimated BC emissions, particularly in less developed western and remote areas. Pollution controls were estimated to reduce the annual BC emissions by 26 % during 2010–2020, reversing the 8 % growth during 2000–2010. BC emissions in the main coal-producing provinces declined by 2010 but rebounded afterwards. By contrast, provinces with higher economic and urbanization levels experienced emission growth (0.05–0.10 Mg/km2/yr) by 2010 and declined greatly (0.07–0.23 Mg/km2/yr) during 2010–2020. The national annual BC-associated premature mortality ranged between 733,910 (95 % confidence interval: 676,790–800,250) and 937,980 cases (864,510–1,023,400) for different years. The changing BC emissions contributed 78,590 cases (72,520–85,600) growth within 2000–2005 and 133,360 (123,150–145,180) reduction within 2010–2015. Strategies differentiated by region are needed for further reducing BC emissions and its health and climate impacts. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is a short-lived climate forcer affecting the Arctic climate through multiple mechanisms, which vary substantially from winter to summer. Several models still fail in reproducing BC seasonal variability, limiting the ability to fully describe BC climate implications. This study aims at gaining insights into the mechanisms controlling BC transport from lower latitudes to the Arctic lower troposphere. Here we investigate the drivers controlling black carbon daily and seasonal variability in the Arctic using generalized additive models (GAMs). We analysed equivalent black carbon (eBC) concentrations measured at the Gruvebadet Atmospheric Laboratory (GAL – Svalbard archipelago) from March 2018 to December 2021. The eBC showed a marked seasonality with higher values in winter and early spring. The eBC concentration averaged 22 ± 20 ngm-3 in the cold season (November–April) and 11 ± 11 ngm-3 in the warm season (May–October). The seasonal and interannual variability was mainly modulated by the efficiency of wet scavenging removal during transport towards higher latitudes. Conversely, the short-term variability was controlled by boundary layer dynamics as well as local-scale and synoptic-scale circulation patterns. During both the cold and warm seasons, the transport of air masses from Europe and northern Russia was an effective pathway for the transport of pollution to the European Arctic. Finally, in the warm season we observed a link between the intrusion of warm air from lower latitudes and the increase in eBC concentration. Changes in the synoptic-scale circulation system and precipitation rate in the Northern Hemisphere, linked to climate change, are expected to modify the BC burden in the Arctic. [ABSTRACT FROM AUTHOR]

Aethalometer is a widely used instrument for black carbon (BC) mass concentration and light absorption coefficient (babs) measurements around the world. However, field intercomparison of the two popular models, dual-spot (AE33) and single-spot (AE31) aethalometers, remain limited; in addition, the difference in secondary brown carbon (BrCsec) light absorption estimation between the two models is largely unknown. We performed full-year collocated AE33 and AE31 measurements in a megacity in southern China – Guangzhou. The babs values agree well between the two aethalometers (R² > 0.95), with AE33/AE31 slopes ranging from 0.87 to 1.04 for 7 wavelengths. AE33 consistently exhibits lower limits of detection (LOD) than AE31 for time resolutions of 2 to 60 min. The AE33/AE31 slope for equivalent BC (eBC) was 1.2, implying the need for site-specific post-correction. The Ångström exponent (AAE) obtained from different approaches agrees not very well between the two models, with the biggest discrepancy found in AAE880/950. The estimated BrCsec light absorption at 370 nm (babs370_BrCsec) was calculated using the minimum R squared method (MRS) for both Aethalometers. The babs370_BrCsec comparison yields a slope of 0.78 and an R² of 0.72 between the two models, implying a non-negligible inter-instrument difference. This study highlights the high consistency in babs but less so in AAE between AE31 and AE33, and reveals site-specific correction for eBC estimation and non-negligible difference in BrCsec estimation. The results are valuable for data continuity in long-term aethalometer measurements when transiting from the older (AE31) to the newer (AE33) model, as anticipated in permanent global-climate and air-quality stations. [ABSTRACT FROM AUTHOR]

The cloud condensation nuclei (CCN) activity of black carbon particles (BC) importantly determines their impacts on cloud microphysics and atmospheric lifetime. This process is crucially determined by the amount of more hygroscopic coating materials BC can acquire during aging process. It remains a challenge for ambient measurements to capture this process and link this with CCN activity of BC. Here by using coupled measurements of size-resolved number concentrations of CCN at configured water supersaturation (SS) and BC-containing particles (BCc), we are able to directly monitor the droplet activation diameter (D50) and activation fraction of BCc (Fact,BC) in ambient environment. The number concentration of BCc was found to peak at diameter 180–210 nm after acquiring coatings, larger than that for all particles (50–150 nm). This led to that the initially smaller BC can be enlarged and become larger and more hygroscopic, even having higher CCN activities than other particles. The Fact,BC increased from 42 % to 69 % in number and from 67 % to 85 % in mass, as SS increased from 0.1 % to 0.2 %, but tended to reach a plateau when SS>0.2 %.Notably, Fact,BC and D50 linearly correlated with equivalent photochemical age, at a rate of +2 % per hour and -3 nm per hour, respectively. The results suggest BCc from anthropogenic sources can readily serve as CCN at a relatively low SS, and over half of the BC population can be activated in a few hours. This means the surface-sourced BC can efficiently incorporate into clouds and may exert important indirect radiative impacts. [ABSTRACT FROM AUTHOR]

The impacts of soot particles on climate and human health depend on the concentration of black carbon (BC) as well as the thickness and composition of the coating material, i.e., organic and inorganic compounds internally mixed with BC. In this study, the size-resolved chemical composition of BC-containing aerosol was measured using a high-resolution soot particle aerosol mass spectrometer (SP-AMS) during wintertime in Fresno, California, a location influenced by abundant combustion emissions and frequent fog events. Concurrently, particle optical properties were measured to investigate the BC absorption enhancement. Positive matrix factorization (PMF) analysis was performed on the SP-AMS mass spectral measurements to explore the sources of soot particles and the atmospheric processes affecting the properties of BC coatings. The analysis revealed that residential woodburning and traffic are the dominant sources of soot particles. Alongside primary soot particles originating from biomass burning (BBOA BC) and vehicles (HOA BC) two distinct types of processed BC-containing aerosol were identified: fog-related oxidized organic aerosol (FOOA BC) and winter-background OOA BC (WOOA BC). Both types of OOA BC showed evidence of having undergone aqueous processing, albeit with differences. The concentration of FOOA BC was substantially elevated during fog events, indicating the formation of aqueous secondary organic aerosol (aqSOA) within fog droplets. On the other hand, WOOA BC was present at a relatively consistent concentration throughout the winter and was likely related to the formation of secondary organic aerosol (SOA) in both the gas phase and aerosol liquid water. By comparing the chemical properties and temporal variations in FOOA BC and WOOA BC , we gain insights into the key aging processes of BC aerosol. It was found that aqueous-phase reactions facilitated by fog droplets had a significant impact on the thickness and chemical composition of BC coatings, thereby affecting the light absorption and hygroscopic properties of soot particles. These findings underscore the important role of chemical reactions occurring within clouds and fogs and influencing the climate forcing of BC aerosol in the atmosphere. [ABSTRACT FROM AUTHOR]

Black carbon (BC) mass size distribution (BCMSD) is crucial in both the environment and the climate system due to BC's intense size-dependent absorption of solar radiation. BC-containing particles larger than 700 nm (BC >700) could contribute to more than half of bulk BC mass concentration. Unfortunately, previous methods concentrated on BC-containing particles of less than 700 nm because of technical limitations. The contribution of BC to absorption and the radiative effect might be underestimated without consideration of BC >700. In this study, equivalent BCMSD (eBCMSD) from 150 nm up to 1.5 µm was measured at high time resolution of 1 h for the first time by an aerodynamic aerosol classifier in tandem with an aethalometer in two field campaigns over eastern China, namely Changzhou located in the Yangtze River Delta and Beijing located in the North China Plain. The results revealed that the pattern of eBCMSD in Changzhou (Beijing) was mostly bimodal (unimodal) peaking at 240 and 1249 nm (427 nm). The peak diameter of eBCMSD in Changzhou did not shift significantly with increasing pollution (240 to 289 nm). In contrast, the peak diameter of eBCMSD in Beijing shifted towards larger sizes, from 347 to 527 nm, with increasing pollution, indicating that the aging process at the urban site was different from that at the regional background site. eBCMSD in both Changzhou and Beijing had a significant diurnal cycle with a smaller (larger) value of eBCMSD during daytime (nighttime). Equivalent BC >700 (eBC >700) was ubiquitous and varied significantly with different locations and pollution levels. The campaign-averaged contribution of eBC >700 to bulk eBC mass concentration (meBC,bulk), bulk absorption coefficient (σab,bulk) and estimated direct radiative forcing of eBC (DRF eBC) in Changzhou and Beijing were 27.8 % (20.9 %–36.5 %) and 24.1 % (17.5 %–34.2 %), 19.6 % (15.8 %–24.6 %) and 25.9 % (19.6 %–33.7 %) and 20.5 % (18.4 %–22.2 %) and 21.0 % (16.3 %–26.1 %), respectively. meBC,bulk , σab,bulk and DRF eBC of eBC >700 in Changzhou (Beijing) increased by a factor of 3.6 (5.1) from 0.11 (0.07) to 0.40 (0.36) µgm-3 , by a factor of 3.2 (5.5) from 0.54 (0.63) to 1.75 (3.45) Mm -1 and by a factor of 2.4 (4.7) from 0.1 (0.1) to 0.24 (0.47) W m -2 , respectively, with the aggravation of pollution. The contribution of eBC >700 to meBC,bulk and σab,bulk had a significant diurnal cycle with a higher (lower) fraction during daytime (nighttime) in both Changzhou and Beijing. A case study indicated that the contribution of eBC >700 to meBC,bulk , σab,bulk and DRF eBC could reach up to 50 %, 50 % and 40 %, respectively. It was highly recommended to consider the whole size range of BC-containing particles in model estimation of the BC radiative effect. [ABSTRACT FROM AUTHOR]

Anthropogenic emissions of aerosols and precursor compounds are known to significantly affect the energy balance of the Earth–atmosphere system, alter the formation of clouds and precipitation, and have a substantial impact on human health and the environment. Global models are an essential tool for examining the impacts of these emissions. In this study, we examine the sensitivity of model results to the assumed height of SO 2 injection, seasonality of SO 2 and black carbon (BC) particulate emissions, and the assumed fraction of SO 2 emissions that is injected into the atmosphere as particulate phase sulfate (SO 4) in 11 climate and chemistry models, including both chemical transport models and the atmospheric component of Earth system models. We find large variation in atmospheric lifetime across models for SO 2 , SO 4 , and BC, with a particularly large relative variation for SO 2 , which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO 2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of - 0.35 W m -2), SO 2 lifetime over Northern Hemisphere land (maximum difference of 0.8 d), surface SO 2 concentration (up to 59 % decrease), and surface sulfate concentration (up to 23 % increase). Emitting SO 2 at height consistently increased SO 2 and SO 4 column burdens and shortwave cooling, with varying magnitudes, but had inconsistent effects across models on the sign of the change in implied cloud forcing. The assumed SO 4 emission fraction also had a significant impact on net radiative flux and surface sulfate concentration. Because these properties are not standardized across models this is a source of inter-model diversity typically neglected in model intercomparisons. These results imply a need to ensure that anthropogenic emission injection height and SO 4 emission fraction are accurately and consistently represented in global models. [ABSTRACT FROM AUTHOR]

Anthropogenic aerosols play a major role for the Earth-Atmosphere system by influencing the Earth's radiative budget and climate. The effect of the perturbation induced by changes in anthropogenic aerosols on the Earth's energy balance is quantified in terms of the effective radiative forcing (ERF) which is the recommended metric for perturbations affecting the Earth's top-of-atmosphere energy budget since it is a better way to link this perturbation to subsequent global mean surface temperature change. In this work, the present-day ERF of anthropogenic aerosols is quantified using simulations from Earth system models (ESMs) participating in the Coupled Model Intercomparison Project Phase 6 (CMIP6). The ERFs of individual aerosol species, such as sulphates, organic carbon (OC), and black carbon (BC) are calculated along with the ERF due to all anthropogenic aerosols and the transient ERF over the historical period (1850–2014). Additionally, ERF is analyzed into three components: (a) ERFARI, representing aerosol-radiation interactions, (b) ERFACI, accounting for aerosol-cloud interactions, and (c) ERFALB, which is mainly due to the contribution of surface albedo changes caused by anthropogenic aerosols. Here, the total anthropogenic aerosol ERF (calculated using the piClim-aer experiment) is estimated to be -1.11 ± 0.26 W m-2, mostly due to the large contribution of ERFACI (-1.14 ± 0.33 W m-2), compared to ERFARI (-0.02 ± 0.20 W m-2) and ERFALB (0.05 ± 0.07 W m-2). The total ERF caused by sulphates (piClim-SO2) is estimated at -1.11 ± 0.31 W m-2, the OC ERF (piClim-OC) is -0.35 ± 0.21 W m-2, whereas the ERF exerted by BC (piClim-BC) is 0.19 ± 0.18 W m-2. On top of that, our analysis reveals that ERFACI clearly prevails over the largest part of the Earth except for the BC experiment where ERFARI prevails over land. By the end of the historical period (1995–2014), the global mean total aerosol ERF is estimated at -1.28 ± 0.37 W m-2 (calculated using the histSST experiment). We find that sulphates dominate both present-day and transient ERF spatial patterns at the top of the atmosphere, exerting a strongly negative ERF especially over industrialized regions of the Northern Hemisphere, such as North America, Europe, East and South Asia. Since the mid-1980s ERF has become less negative over Eastern North America and Western and Central Europe, while over East and South Asia there is a steady increase in ERF magnitude towards more negative values until 2014. [ABSTRACT FROM AUTHOR]

Earth system models (ESMs) participating in the latest Coupled Model Intercomparison Project Phase 6 (CMIP6) simulate various components of fine particulate matter (PM2.5) as major climate forcers. Yet the model performance for PM2.5 components remains little evaluated due in part to lack of observational data. Here, we evaluate near-surface concentrations of PM2.5 and its five main components over China as simulated by fourteen CMIP6 models, including organic carbon (OC, available in 14 models), black carbon (BC, 14 models), sulfate (14 models), nitrate (4 models), and ammonium (5 models). For this purpose, we collect observational data between 2000 and 2014 from a satellite-based dataset for total PM2.5 and from 2469 measurement records in the literature for PM2.5 components. Seven models output total PM2.5 concentrations, and they all underestimate the observed total PM2.5 over eastern China, with GFDL-ESM4 (–1.5 %) and MPI-ESM-1-2-HAM (–1.1 %) exhibiting the smallest biases averaged over the whole country. The other seven models, for which we recalculate total PM2.5 from the available components output, underestimate the total PM2.5 concentrations, partly because of the missing model representations of nitrate and ammonium. Concentrations of the five individual components are underestimated in almost all models, except that sulfate is overestimated in MPI-ESM-1-2-HAM by 12.6 % and in MRI-ESM2-0 by 24.5 %. The underestimation is the largest for OC (by –71.2 % to –37.8 % across the 14 models) and the smallest for BC (–47.9 % to –12.1 %). The multi-model mean (MMM) reproduces fairly well the observed spatial pattern for OC (R = 0.51), sulfate (R = 0.57), nitrate (R = 0.70) and ammonium (R = 0.75), yet the agreement is poorer for BC (R = 0.39). The varying performances of ESMs on total PM2.5 and its components have important implications for the modeled magnitude and spatial pattern of aerosol radiative forcing. [ABSTRACT FROM AUTHOR]

Earth system models (ESMs) participating in the latest Coupled Model Intercomparison Project Phase 6 (CMIP6) simulate various components of fine particulate matter (PM2.5) as major climate forcers. Yet the model performance for PM2.5 components remains little evaluated due in part to lack of observational data. Here, we evaluate near-surface concentrations of PM2.5 and its five main components over China as simulated by fourteen CMIP6 models, including organic carbon (OC, available in 14 models), black carbon (BC, 14 models), sulfate (14 models), nitrate (4 models), and ammonium (5 models). For this purpose, we collect observational data between 2000 and 2014 from a satellite-based dataset for total PM2.5 and from 2469 measurement records in the literature for PM2.5 components. Seven models output total PM2.5 concentrations, and they all underestimate the observed total PM2.5 over eastern China, with GFDL-ESM4 (–1.5 %) and MPI-ESM-1-2-HAM (–1.1 %) exhibiting the smallest biases averaged over the whole country. The other seven models, for which we recalculate total PM2.5 from the available components output, underestimate the total PM2.5 concentrations, partly because of the missing model representations of nitrate and ammonium. Concentrations of the five individual components are underestimated in almost all models, except that sulfate is overestimated in MPI-ESM-1-2-HAM by 12.6 % and in MRI-ESM2-0 by 24.5 %. The underestimation is the largest for OC (by –71.2 % to –37.8 % across the 14 models) and the smallest for BC (–47.9 % to –12.1 %). The multi-model mean (MMM) reproduces fairly well the observed spatial pattern for OC (R = 0.51), sulfate (R = 0.57), nitrate (R = 0.70) and ammonium (R = 0.75), yet the agreement is poorer for BC (R = 0.39). The varying performances of ESMs on total PM2.5 and its components have important implications for the modeled magnitude and spatial pattern of aerosol radiative forcing. [ABSTRACT FROM AUTHOR]

Brown carbon (BrC) is an absorbing organic aerosol, primarily emitted through biomass burning, that exhibits light absorption unique from both black carbon (BC) and other organic aerosols (OA). Despite many field and laboratory studies seeking to constrain BrC properties, the radiative forcing of BrC is still highly uncertain. To better understand it's climate impact, we introduced BrC to the One-Moment Aerosol (OMA) module of the GISS ModelE Earth system model (ESM). We assessed ModelE sensitivity to primary BrC processed through a novel chemical aging scheme, as well as secondary BrC formed from biogenic volatile organic compounds (BVOCs). Initial results show BrC typically contributes a top of the atmosphere (TOA) radiative effect of 0.04 W m-2. Sensitivity tests indicate that explicitly simulating BrC (separating it from other OA), including secondary BrC, and simulating chemical bleaching of BrC all contribute distinguishable radiative effects and should be accounted for in BrC schemes. This addition of prognostic BrC to ModelE allows for greater physical and chemical complexity in OA representation with no apparent trade-off in model performance as evaluation of ModelE aerosol optical depth, with and without the BrC scheme, against AERONET and MODIS retrieval data reveals similar skill in both cases. Thus, BrC should be explicitly simulated to allow for more physically based chemical composition, which is crucial for more detailed OA study like comparisons to in-situ measurement campaigns. We include additional recommendations for BrC representation within ESMs at the end of this paper. [ABSTRACT FROM AUTHOR]

It is necessary to accurately determine the optical properties of highly absorbing black carbon (BC) aerosols to estimate their climate impact. In the past, there has been hesitation about using realistic fractal morphologies when simulating BC optical properties due to the complexity involved in the simulations and the cost of the computations. In this work, we demonstrate that the predictions of optical properties like single scattering albedo (ω) and mass absorption cross-section (MAC) can be improved compared to the conventional Mie-based predictions using a highly accurate benchmark machine learning algorithm. Unlike the computationally intensive simulations of complex scattering models, the ML-based approach accurately predicts optical properties in a fraction of a second. There has been an extensive evaluation procedure carried out in this study. Based on comparisons with laboratory measurements, it was demonstrated that incorporating realistic morphologies of BC significantly improved their optical properties. The results indicate that it is possible to generate optical properties in the visible spectrum using BC fractal aggregates with any desired physicochemical properties, such as size, morphology, or organic coating. Based on these findings, climate models can improve their radiative forcing estimates using such comprehensive parameterizations for the optical properties of BC based on their aging stages. [ABSTRACT FROM AUTHOR]

Black carbon (BC) aerosol is considered one of the important contributors to the fast climate warming and snow and sea ice melting in the Arctic. Yet the observations of BC in the Arctic Ocean have been limited due to infrastructural and logistical difficulties. We observed BC mass concentrations (m BC) using light absorption methods on board the icebreaker R/V Araon in the Arctic Ocean (166° E–156° W and <80° N) as well as the North Pacific Ocean in summer and early Autumn of 2016 to 2020. The levels, interannual variations and pollution episodes of m BC in the Arctic were examined, and the emission sources responsible for the high-BC episodes were analyzed with global chemistry-transport model simulations. The average m BC in the surface air over the Arctic Ocean (72–80° N) observed in 2019 was over 70 ng m–3, which was substantially higher than in other years (approximately 10 ng m–3). The much higher m BC observed in 2019 was perhaps due to more frequent wildfires occurred in the Arctic region than in other years. The model suggested that biomass burning composed the largest contribution to the observed BC in the western Arctic Ocean and the marginal seas. For these five years, we identified 10 elevated-BC episodes, including one in 2018 that was associated with co-enhancements of CO and CH4 but not CO2 and O3. The model analysis indicated that most episodes were attributed to the airmasses transported from boreal fires to the Arctic Ocean, with some near-surface and others in the mid-troposphere. This study provides crucial datasets on BC mass concentrations and the mixing ratios of O3, CH4, CO, and CO2 in the western Arctic Ocean regions and highlights the significant impact of boreal fires on the observed Arctic BC during the summer and early autumn months. [ABSTRACT FROM AUTHOR]

The mixing state of black carbon (BC) aerosols, which is the diameter ratio of coated particle to BC core (Dp/Dc), can be retrieved by the single-particle soot photometer (SP2). However, the retrieved Dp/Dc contains errors, because the core–shell model and Mie scattering calculation are normally employed in the retrieval principle of SP2 and the spherical core–shell structure seriously deviated from the real morphology of coated BC. In this study, fractal models are constructed to represent thinly and thickly coated BC particles for optical simulations, the differential scattering cross-sections are selected as references to conduct optical retrieval of particle diameter (Dp) based on Mie theory, just like the retrieval principle of SP2, and the volume equivalent diameter of BC core (Dc) is the same for fractal and spherical models. Then, the retrieval errors of the mixing state (Dp/Dc) of BC are investigated from numerical aspects, and the estimation accuracy of BC radiative forcing is analyzed through the simple forcing efficiency (SFE) equation with SP2 retrieval results taken into consideration. Results show that SP2 retrieved Dp/Dc based on Mie theory underestimates the realistic Dp/Dc of coated BC at most particle sizes. The retrieval errors of Dp/Dc of thinly coated BC for both single particles and particle groups are larger than those of thickly coated BC. In addition, evaluation errors of radiative forcing of coated BC caused by retrieval errors of SP2 are up to about 55 % and 95 % at 1064 and 532 nm , respectively. This study provides meaningful referential understandings of the retrieved Dp/Dc of SP2 based on Mie scattering. [ABSTRACT FROM AUTHOR]

A three-dimensional (spatial and vertical) gridded data set of black carbon (BC) aerosols has been developed for the first time over the Indian mainland using data from a dense ground-based network, aircraft- and balloon-based measurements from multiple campaigns, and multi-satellite observations, following statistical assimilation techniques. The assimilated data reveal that the satellite products tend to underestimate (overestimate) the aerosol absorption at lower (higher) altitudes with possible climate implications. The regional maps of BC-induced atmospheric heating derived using this data set capture the elevated aerosol heating layers over the Indian region along with the spatial high over the Indo-Gangetic Plain. It is shown that, over most of the Indian region, the incorporation of realistic profiles of aerosol absorption/extinction coefficients and single scattering albedo into the radiative transfer calculations leads to enhanced high-altitude warming. This could strongly influence the upper-tropospheric and lower-stratospheric processes, including the vertical transport of BC to higher altitudes, and thus have larger implications for atmospheric stability than what would be predicted using satellite observations alone. This will have larger implications for atmospheric stability than what would be predicted using satellite observations alone and could strongly influence the upper-tropospheric and lower-stratospheric processes, including increased vertical transport of BC to higher altitudes. The 3D assimilated BC data set will be helpful in reducing the uncertainty in aerosol radiative effects in climate model simulations over the Indian region. [ABSTRACT FROM AUTHOR]

Recent years have seen an increase in the use of wood for energy production of over 30 %, and this trend is expected to continue due to the current energy crisis and geopolitical instability. At present, residential wood burning (RWB) is one of the most important sources of organic aerosols (OA) and black carbon (BC). While BC is recognized for its large light absorption cross-section, the role of OA in light absorption is still under evaluation due to their heterogeneous composition and source-dependent optical properties. Studies that characterize wood-burning aerosol emissions in Europe typically focus on urban and background sites and only cover BC properties. However, RWB is more prevalent in rural areas, and the present scenario indicates that an improved understanding of the RWB aerosol optical properties and their subsequent connection to climate impacts is necessary for rural areas. We have characterized atmospheric aerosol particles from a central European rural site during wintertime in the village of Retje in Loški Potok, Slovenia, from 01.12.2017 to 07.03.2018. The village experienced extremely high aerosol concentrations produced by RWB and near-ground temperature inversion. The isolated location of the site and the substantial local emissions made it an ideal laboratory-like place for characterizing RWB aerosols with low influence from non-RWB sources under ambient conditions. The mean mass concentrations of OA and BC were 34.8 µg m-3 (max = 271.8 µg m-3) and 3.1 µg m-3 (max = 24.3 µg m-3), respectively. The mean total particle number concentration (10–600 nm) was 9.9 x 103 particles cm-3 (max = 53.5 x 103 particles cm-3). The mean total light absorption coefficient at 370 nm and 880 nm measured by an Aethalometer AE33 were 122.8 Mm-1 and 15.3 Mm-1 and had maximum values of 1103.9 Mm-1 and 179.1 Mm-1, respectively. The aerosol concentrations and absorption coefficients measured during the campaign in Loški Potok were significantly larger than those reported values for several urban areas in the region with larger populations and extent of aerosol sources. Here, considerable contributions from brown carbon (BrC) to the total light absorption were identified, reaching up to 60 % and 48 % in the near UV (370 nm) and blue (470 nm) wavelengths. These contributions are up to three times higher than values reported for other sites impacted by wood-burning emissions. The calculated mass absorption cross-section and the absorption Ångström exponent for RWB OA were MACOA, 370 nm= 2.4 m2 g-1, and AAEBrC, 370–590 nm= 3.9, respectively. Simple forcing efficiency (SFE) calculations were performed as a sensitivity analysis to evaluate the climate impact of the RWB aerosols produced at the study site by integrating the optical properties measured during the campaign. The SFE results show a considerable forcing capacity from the local RWB aerosols, with a high sensitivity to OA absorption properties and a more substantial impact over bright surfaces like snow, typical during the coldest season with higher OA emissions from RWB. Our study's results are highly significant regarding air pollution, optical properties, and climate impact. The findings suggest that there may be an underestimation of RWB emissions in rural Europe and that further investigation is necessary. [ABSTRACT FROM AUTHOR]

Aerosol particles have both natural and anthropogenic origins and are ubiquitous in the atmosphere. One particularly important type is carbonaceous aerosol, including a specific subset often termed "elemental carbon" chemically or "black carbon" (BC) radiatively. Carbonaceous aerosol particles have implications for atmospheric chemistry, human health, and climate, both directly and via their ability to act as sites of cloud droplet or ice crystal formation. Laboratory experiments and theory are needed to better understand these particles, specifically their radiative impact. Here we present laboratory measurements of scattering of visible radiation by analogs of atmospheric BC aggregates at scattering angles of 135±20 ∘ obtained using a depolarizing optical particle counter and accompanying theoretical calculations of scattering by compact and fractal theoretical BC aggregates. We show that, with random orientation, the theoretical calculations reproduce the qualitative behavior of the measurements but are unable to reproduce the highest values of the linear depolarization ratio; we are only able to obtain high values of the linear depolarization ratio using fixed orientation. Both our measurements and our theoretical calculations point to the possibility that fresh, unaged, bare, or uncoated BC aggregates, as opposed to the aged or coated BC or soot that was investigated in previous studies, can exhibit a higher back-scattering linear depolarization than previously assumed. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is a crucial component of aerosols in the atmosphere. Understanding the hygroscopicity of BC particles is important for studying their role as cloud condensation nuclei (CCN) and ice nuclei (IN), as well as their chemical behavior and atmospheric lifetime. However, there is still a lack of comprehensive understanding regarding the factors that determine the hygroscopic properties of fresh BC. In this work, the hygroscopic behavior of BC particles generated from different types of fuel and aged with SO2 for varying durations were measured by a vapor sorption analyzer while various characterizations of BC were conducted to understand the key factors that influence the hygroscopic properties of BC. It was found that the presence of water-soluble substances in BC facilitates the completion of monolayer water adsorption at low relative humidity, while also increasing the number of water adsorption layers at high relative humidity. On the other hand, BC prepared by burning organic fuels, which typically lacks water-soluble inorganic ions, primarily exhibits hygroscopicity characteristics influenced by organic carbon (OC) and microstructure. Furthermore, the hygroscopicity of BC can be enhanced by the formation of sulfate ions due to heterogeneous oxidation of SO2. This finding sheds light on the critical factors that affect BC hygroscopicity during water adsorption and allows for estimating the interaction between water molecules and BC particles in a humid atmosphere. [ABSTRACT FROM AUTHOR]

Global precipitation change in response to climate change is closely related to surface temperature, the forcing agent, and the atmospheric dry energy budget, but regional precipitation change is more complex. In this study, we use experiments from the Precipitation Driver and Response Model Intercomparison Project (PDRMIP) wherein carbon dioxide, sulfate aerosols, and black carbon aerosols are perturbed to study the global precipitation response in contrast with the regional response over India. The response to global warming from carbon dioxide increases precipitation both globally and regionally, whereas the cooling response to sulfate aerosol leads to a reduction in precipitation in both cases. The response to black carbon aerosols, however, is a global decrease but a regional increase of precipitation over India. The mechanism is increased atmospheric heating driving a stronger monsoon circulation and stronger low-level winds. This intensification of the Indian monsoon is, somewhat surprisingly, stronger for global black carbon emissions than when the emissions are limited to those from the Asian region. Overall, our study presents heterogeneity in precipitation responses at both global and regional levels and the potential underlying physical processes under a variety of climate forcings that would be useful in designing further model experiments with higher spatial resolution. [ABSTRACT FROM AUTHOR]

We apply a local ensemble transform Kalman smoother (LETKS) in combination with the global aerosol–climate model ECHAM–HAM to estimate aerosol emissions from POLDER-3/PARASOL (POLarization and Directionality of the Earth's Reflectances) observations for the year 2006. We assimilate aerosol optical depth at 550 mnm (AOD550), the Ångström exponent at 550 and 865 nm (AE550–865), and single-scattering albedo at 550 nm (SSA550) in order to improve modeled aerosol mass, size and absorption simultaneously. The new global aerosol emissions increase to 1419 Tgyr-1 (+ 28 %) for dust, 1850 Tgyr-1 (+ 75 %) for sea salt, 215 Tgyr-1 (+ 143 %) for organic aerosol and 13.3 Tgyr-1 (+ 75 %) for black carbon, while the sulfur dioxide emissions increase to 198 Tgyr-1 (+ 42 %) and the total deposition of sulfates to 293 Tgyr-1 (+ 39 %). Organic and black carbon emissions are much higher than their prior values from bottom-up inventories, with a stronger increase in biomass burning sources (+ 193 % and + 90 %) than in anthropogenic sources (115 % and 70 %). The evaluation of the experiments with POLDER (assimilated) and AERONET as well as MODIS Dark Target (independent) observations shows a clear improvement compared with the ECHAM–HAM control run. Specifically based on AERONET, the global mean error in AOD550 improves from - 0.094 to - 0.006, while absorption aerosol optical depth at 550 nm (AAOD550) improves from - 0.009 to - 0.004 after the assimilation. A smaller improvement is also observed in the AE550–865 mean absolute error (from 0.428 to 0.393), with a considerably higher improvement over isolated island sites at the ocean. The new dust emissions are closer to the ensemble median of AEROCOM I, AEROCOM III and CMIP5 as well as some of the previous assimilation studies. The new sea salt emissions have become closer to the reported emissions from previous studies. Indications of a missing fraction of coarse dust and sea salt particles are discussed. The biomass burning changes (based on POLDER) can be used as alternative biomass burning scaling factors for the Global Fire Assimilation System (GFAS) inventory distinctively estimated for organic carbon (2.93) and black carbon (1.90) instead of the recommended scaling of 3.4 (Kaiser et al., 2012). The estimated emissions are highly sensitive to the relative humidity due to aerosol water uptake, especially in the case of sulfates. We found that ECHAM–HAM, like most of the global climate models (GCMs) that participated in AEROCOM and CMIP6, overestimated the relative humidity compared with ERA5 and as a result the water uptake by aerosols, assuming the kappa values are not underestimated. If we use the ERA5 relative humidity, sulfate emissions must be further increased, as modeled sulfate AOD is lowered. Specifically, over East Asia, the lower AOD can be attributed to the underestimated precipitation and the lack of simulated nitrates in the model. [ABSTRACT FROM AUTHOR]

The light-absorbing organic aerosol (OA), known as brown carbon (BrC), has important radiative impacts; however, its sources and evolution after emission remain to be elucidated. In this study, the light absorption at multiple wavelengths, mass spectra of OA and microphysical properties of black carbon (BC) were characterized at a typical suburban environment in Beijing. The absorption of BC is constrained by its size distribution and mixing state, and the BrC absorption is obtained by subtracting the BC absorption from the total aerosol absorption. Aerosol absorption was further apportioned to BC, primary BrC and secondary BrC by applying the least correlation between secondary BrC and BC. The multilinear regression analysis on the factorized OA mass spectra indicated that the OA from traffic and biomass burning emission contributed to primary BrC. Importantly, the moderately oxygenated OA (O / C = 0.62) was revealed to highly correlate with secondary BrC. These OA had higher nitrogen content, in line with the nitrogen-containing functional groups detected by the Fourier transform infrared spectrometer. The photochemical processes were found to reduce the mass absorption cross section (MAC) of primary OA, reducing its contribution to total absorption by 20 %, at the same time increasing MAC for secondary OA, which showed a 30 % enhancement in contribution to total absorbance, implying the concurrent whitening and darkening of BrC. This provides field evidence that the photochemically produced secondary nitrogen-containing OA can considerably compensate for some bleaching effect on the primary BrC, hereby causing radiative impacts. [ABSTRACT FROM AUTHOR]

Black carbon (BC; i.e. soot) absorbs radiation and contributes to glacier retreat over the Tibetan Plateau (TP). A lack of comprehensive understanding of the actual mixing state leads to large controversies in the climatic simulation of soot over the TP. In this study, ground-based sampling, electron microscopy analyses, and theoretical calculations were used to investigate the interactions among the liquid–liquid phase separation (LLPS), soot redistribution in secondary particles, and fractal dimension (Df) of soot particles on the eastern rim of the TP. We found that more than half of the total analysed particles were soot-containing particles. One-third of soot-containing particles showed a core shell structure that probably formed the LLPS phenomenon after long-range transport. Particle size and the ratio of organic coating thickness to soot size are two of the major possible factors that likely induce soot redistribution between organic matter and inorganic aerosols in individual particles. The Df sequence is ranked as externally mixed soot (1.79±0.09)< sulfate-coated soot (1.84±0.07)< organic-coated soot (1.95±0.06). We concluded that the soot redistribution process promoted the morphological compaction of soot particles. This study indicates that soot-containing particles experienced consistent ageing processes that induced a more compact morphology and soot redistribution in the LLPS particles on the remote eastern rim of the TP. Understanding the microscopic changes in aged soot particles could further improve the current climate models and evaluations of BC's radiative impacts on the eastern TP and similar remote air. [ABSTRACT FROM AUTHOR]

Currently, emissions from internal combustion vehicles are not properly monitored throughout their life cycle. In particular, a small share (< 20 %) of poorly maintained or tampered vehicles are responsible for the majority (60-90 %) of traffic-related emissions. Remote emission sensing (RES) is a method used for screening emissions from a large number of in-use vehicles. Commercial open-path RES systems are capable of providing emission factors for many gaseous compounds, but they are less accurate and reliable for particulate matter (PM). Point sampling (PS) is an extractive RES method where a 5 portion of the exhaust is sampled and then analyzed. So far, PS studies have been conducted predominantly on a rather small scale and have mainly analyzed heavy duty vehicles (HDV), which have high exhaust flow rates. In this work, we present a comprehensive PS system that can be used for large-scale screening of PM and gas emissions, largely independent of the vehicle type. The developed data analysis framework is capable of processing data from 1,000s of vehicles. The core of the data analysis is our peak detection algorithm (TUG-PDA), which determines and separates emissions down to a spacing of just 10 a few seconds between vehicles.We present a detailed evaluation of the main influencing factors on PS measurements by using about 100,000 vehicle records collected from several measurement locations, mainly in urban areas.We show the capability of the emission screening by providing real-world black carbon (BC), particle number (PN) and NOx emission trends for various vehicle categories such as diesel and petrol passenger cars or HDVs. Comparisons with open-path RES and PS studies show overall good agreement and demonstrate the applicability even for the latest Euro emission standards, where current open-path 15 RES systems reach their limits. [ABSTRACT FROM AUTHOR]

Ice–albedo feedbacks in the ablation region of the Greenland Ice Sheet (GrIS) are difficult to constrain and model due, in part, to our limited understanding of the seasonal evolution of the bare-ice region. To help fill observational gaps, 13 surface samples were collected on the GrIS across the 2014 summer melt season from patches of snow and ice that were visibly light, medium, and dark colored. These samples were analyzed for their refractory black carbon (rBC) concentrations and size distributions with a single-particle soot photometer coupled to a characterized nebulizer. We present a size distribution of rBC in fresh snow on the GrIS and from the weathering crust in the bare-ice dark zone of the GrIS. The size distributions from the weathering crust samples appear unimodal and were overall smaller than the fresh snow sample, with a peak around 0.3 µm. The fresh snow sample contained very large rBC particles that had a pronounced bimodality in the peak size distributions, with peaks around 0.2 and 2 µm. rBC concentrations ranged from a minimum of 3 µg-rBC/L-H2O in light-colored patches at the beginning and end of the melt season to a maximum of 32 µg-rBC/L-H2O in a dark patch in early August. On average, the rBC concentrations were higher (20 ± 10 µg-rBC/L-H2O) in patches that were visibly dark, compared to medium patches (7 ± 2 µg-rBC/L-H2O) and light patches (4 ± 1 µg-rBC/L-H2O), suggesting that BC aggregation contributed to snow aging on the GrIS, and vice versa. Additionally, concentrations peaked in light and dark patches in early August, which is likely due to smoke transport from wildfires in northern Canada and Alaska, as supported by the Navy Aerosol Analysis and Prediction System (NAAPS) reanalysis model. According to the model output, 26 mgm-3 of biomass-burning-derived smoke was deposited between 1 April and 30 August, of which 85 % came from wet deposition, and 67 % was deposited during our sample collection time frame. The increase in the rBC concentration and size distributions immediately after the modeled smoke deposition fluxes suggest that biomass burning smoke is a source of BC to the dark zone of the GrIS. Thus, the role of BC in the seasonal evolution of the ice–albedo feedbacks should continue to be investigated in the weathering crust of the bare-ice zone of the GrIS. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is a short-lived climate forcer affecting Arctic climate through multiple mechanisms, which vary substantially from winter to summer. Several models still fail in reproducing BC seasonal variability, limiting the ability to fully describe BC climate implications. This study aims at gaining insights into the mechanisms controlling BC transport from lower latitudes to the Arctic lower troposphere. Here we investigate the drivers controlling black carbon daily and seasonal variability in the Arctic using Generalized Additive Models (GAM). We analysed equivalent black carbon (eBC) concentration measured at the Gruvebadet Atmospheric Laboratory (GAL - Svalbard archipelago) from March 2018 to December 2021. The eBC showed a marked seasonality with higher values in winter and early spring. The eBC concentration averaged 22 ± 20 ng m-3 in the cold season (November–April) and 11 ± 11 ng m-3 in the warm season (May–October). The seasonal and interannual variability was mainly modulated by the efficiency of wet scavenging removal during transport towards the higher latitudes. Conversely, the short-term variability was controlled by boundary layer dynamics, local-scale, and synoptic-scale circulation patterns. During both the cold and the warm season, the transport of air masses from western Europe and northern Russia was an effective pathway for the convey of pollution to the European Arctic. Finally, in the warm season we observed a link between the intrusion of warm air from lower latitudes and the increase in eBC concentration. Changes in synoptic scale circulation system and precipitation rate in the northern hemisphere, linked to climate change, are expected to modify BC burden in the Arctic. [ABSTRACT FROM AUTHOR]

The absorption Ångström exponent (AAE)-based methods are widely used to estimate brown carbon (BrC) absorption, and the estimated BrC absorption can be significantly different from 0 even for pure black carbon (BC). However, few studies have systematically quantified the effects of BC microphysical properties. Moreover, it is still unclear under which conditions the AAE-based method is applicable. In this work, we used BC models partially coated with non-absorbing materials to calculate the total absorption. Since the total absorption is entirely from BC, the estimated BrC absorption should be 0 if the retrieval methods are accurate. Thus, the estimated BrC absorption (ABSBrC) should be the absorption from BC that is incorrectly attributed to BrC. The results show that a BC AAE of 1 can generally provide reasonable estimates for freshly emitted BC, since at this time ABSBrC is generally in the range of -3 % to 4.5 %. However, when BC aerosols are aged, ABSBrC of about 35 % could be observed. The WDA method does not necessarily improve the estimates, sometimes a negative ABSBrC of -40 % can be found for partially coated BC. By combining simulations of a global chemical transport model, this work also quantified the effects of BC microphysical properties on BrC global optical absorption aerosol depth (AAOD) estimates. The AAE = 1 method could sometimes lead to a misassigned global mean AAOD of about -0.4 – 0.5 × 10-3 if BC aerosols have a complex morphology, leading to a global mean direct radiation factor (DRF) of about -0.068 ± 0.0172 to +0.085 ± 0.0215 W/m2 from BC, which is incorrectly assigned to BrC. The WDA method does not necessarily improve the estimates. In our cases, the WDA methods based on the spherical models can lead to a range of about -0.9 – 0.05 × 10-3 of misassigned AAOD, which could lead to a global mean DRF error range of -0.153 ± 0.0387 to +0.0085 ± 0.0022 W/m2. At the regional scale, the AAE = 1 method in East Asia sometimes leads to a distributed AAOD of over 3 × 10-3, resulting in a BC DRF of about +0.51 ± 0.129 W/m2, which is incorrectly attributed to BrC. Mie theory-based WDA methods would lead to an estimated AAOD error of more than 6 × 10-3 in some regions (e.g., East Asia), resulting in an estimated misattributed DRF of +1.0 ± 0.258 W/m2. [ABSTRACT FROM AUTHOR]

The vertical distribution of black carbon (BC), as well as its mixing state, is of great concern due to BC's strong regional climatic and environmental effects. In this study, vertical measurements were conducted through a moveable container based on a meteorological tower in the Beijing urban area during June and July. A total of 112 vertical profiles (0–240 m), including the concentrations of BC, O 3 , NO x and the optical properties of aerosols, were obtained. Based on BC concentration, the vertical profiles could be classified into four categories: uniform, gradual decrease, sharp decrease and sudden increase. The uniform type indicates strong vertical mixing with similar pollutant concentrations along the vertical direction. The gradual and sharp decrease types indicate stable vertical conditions with higher pollutant concentrations on the ground and lower concentrations at higher altitudes. Due to the strong radiation in summer, the vertical profiles exhibited a clear diurnal variation in which ∼ 80 % of profiles were uniform during the daytime and ∼ 40 %–90 % of profiles were of the gradual and sharp decrease types at night. O 3 is an exception, and its concentration generally increases with height, even under strong vertical mixing conditions. The size distribution of the BC core varied slightly along the vertical direction, and the coating thickness, denoted by the diameter ratio between the BC-containing particle and BC core (Dp/Dc), of BC increased with height under stable conditions. Although the coating thickness could increase the absorption ability with an average absorption enhancement of 1.25 at 23:00 LT (local time: UTC + 8), the vertical difference of Dp/Dc (2 %) was much lower than that of BC concentration (∼ 35 %). The vertical variation in absorption ability was mainly caused by the variation in BC concentration. In addition, O 3 and Dp/Dc occasionally increased during 06:00–08:00 but remained stable during 08:00–10:00. Vertical mixing and transportation from upper heights, such as the residual layer, could significantly influence the pollutant properties on the surface during early mornings. This study exhibits a continuous vertical picture of BC and its mixing state in urban areas, which would be helpful for understanding BC's regional environmental effect. [ABSTRACT FROM AUTHOR]

Both the size and mixing state of black carbon (BC)-containing aerosols are crucial in estimating the environmental, health and climate impacts of BC. Traffic emissions are a major global source of BC; however, parameterization of BC mass size distributions and mixing states associated with traffic remains lacking due to its dependence on vehicle types and driving conditions. To investigate BC mass size distributions and mixing states associated with traffic emissions, a field campaign was conducted in the Guangzhou urban area during winter, which used a system coupling a differential mobility analyzer (DMA) and a single-particle soot photometer (SP2) to measure BC mass size distributions in the range of 100 to 700 nm. The resolved primary organic aerosols were hydrocarbon-like organic aerosols (HOA) and cooking-like organic aerosols (COA), as well as refractory BC (rBC), which was detected by the DMA–SP2 and correlated highly with HOA (R2=0.88), confirming that traffic emissions are the dominant source of atmospheric BC during the observations. The BC mass size distribution was found to be best fitted by a lognormal distribution, with a geometric mean (Dg,BC) of 258±16 nm, varying between 200 and 300 nm. During daytime, active formation of secondary nitrate and organic aerosols was observed, but it had little effect on the variations of BC mass size distributions. Further analyses revealed that Dg,BC was moderately correlated with rBC / HOA (R2=0.41) in a linear form of Dg,BC=34×rBC/HOA+177 , demonstrating that the BC content of traffic emissions significantly impacts the BC mass size distributions. In addition, the size-dependent fractions of BC-containing aerosols in all types of aerosols (fBCc) and the fraction of identified externally mixed (bare/thinly coated) BC particles in all BC-containing aerosols (fext) were also characterized. It was found that the daytime secondary aerosol formation reduced both fBCc and fext , with the decrease in fext being more pronounced for larger particles, possibly due to the higher relative coating thickness. Variations in fext during nighttime were mainly controlled by the emission conditions. For example, fext for 600 nm particles decreased from 0.82 to 0.46 as rBC / HOA increased from 1 to 3.5, while the mass ratios of secondary aerosols to rBC varied little, demonstrating that the BC content also significantly affects the mixing states of freshly emitted BC from traffic emissions. This study suggests that BC content can be used as the key factor to parameterize both the BC mass size distribution and mixing states from traffic emissions, which warrants future comprehensive investigation. In addition, other sources such as biomass burning and coal combustion also contribute substantially to BC emissions, and it was important to investigate whether BC content of other major BC sources than traffic is also important in determining BC mass size distributions and mixing states. Overall, results of this study have significant implications for accurate representation of BC from different sources when modeling the impacts of BC. [ABSTRACT FROM AUTHOR]

The mixing state of black carbon (BC) aerosols can be measured by the single-particle soot photometer (SP2). However, the measured mixing state contains errors, because the core-shell model and Mie scattering calculation are employed in the measurement principle of SP2, and the spherical core-shell structure seriously deviated the real morphology of coated BC. In this study, fractal models are constructed to represent thinly and heavily coated BC particles for optical simulations, the scattering cross-section are selected as reference to conduct optical retrieval of particle diameter (Dp) based on Mie theory, just like the measurement principle of SP2, and the diameter of BC core (Dc) are the same for fractal and spherical models. Then, the measurement errors of mixing state (Dp/Dc) of BC are investigated from numerical aspect, and the estimation accuracy of BC radiative forcing is analyzed through the simple forcing efficiency (SFE) equation with SP2 measurement results taken into consideration. Results show that SP2 measured Dp/Dc based on Mie theory underestimates the realistic mixing state of coated BC for most particle sizes, and the largest relative error for single-particle can be about 42%. The retrieval errors of mixing state of thinly coated BC for both single-particle and particle groups are larger than these of heavily coated BC. In addition, evaluation errors of radiative forcing of coated BC caused by measurement errors of SP2 are up to about 76% and 43% at 1064 and 532 nm, respectively. This study provides meaningful referential understandings of the measured Dp/Dc of SP2. [ABSTRACT FROM AUTHOR]

Black carbon (BC), the most efficient atmospheric aerosol for absorbing light in the visible spectrum, exerts a warming effect on a region undergoing unprecedented climatic changes. Here, BC is studied indirectly using filter-based methods to ascertain aerosol light absorption parameters. We investigated long-term changes using a harmonised 21-year data set of light absorption measurements, in conjunction with air mass source analysis. The measurements were performed at Zeppelin Observatory (ZEP), Svalbard, from 2002 to 2022. We report a statistically significant (s.s.) decreasing long-term trend for the light absorption coefficient, measured at the site for the entirety of the data set. However, the last 7 years, 2016–2022, showed a slightly increasing s.s. trend for the haze season. In addition, we observed an increasing trend in the single scattering albedo from 2002 to 2022. Five distinct source regions were identified; the trends involving air masses from the five regions showed decreasing absorption coefficients, except for the air masses influenced by emissions from Eurasia. We show that the changes in the occurrences of each transport pathway cannot explain the reductions in the absorption coefficient observed at the Zeppelin station; an increase in contributions of air masses from more marine regions, with lower absorption coefficients, is compensated by the influence from high-emission regions. Along with aerosol optical properties, we also show an increasing trend in accumulated surface precipitation experienced by air masses en route to the Zeppelin Observatory. We argue that rainfall, as a sink of aerosol, plays a role in the long-term trends in the absorption coefficient, explaining approximately a quarter of the overall trend. A decreasing trend in the scavenging ratio further suggests an increase in the aerosol removal processes. We note that there is an increasing potential influence from active forest fires, particularly in the last few summers (i.e. 2015–2022). Active fires have been shown to have a significant impact on the mean seasonal absorption coefficient especially during northern hemispheric summer. However, no noticeable alteration in annual long-term trends can be observed. [ABSTRACT FROM AUTHOR]