Black Carbon Mass Concentration Research Articles

A 2-year intercomparison of three methods for measuring black carbon concentration at a high-altitude research station in Europe

Abstract. 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 µg C cm−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.

Characteristics and source apportionment of black carbon the urban and desert underlying surfaces

The spatial distribution of black carbon (BC) concentrations was highly variable across different underlying surfaces. Differences in meteorological conditions and emission sources led to great temporal and spatial variations in BC characteristics. As the most important absorbing aerosol, BC can affect radiation, clouds, and surface snow. BC mass concentrations were measured using a seven channel aethalometer (AE-33) in the Urumqi and Taklimakan Deserts from January to December 2022.The aethalometer data, potential source contribution function (PSCF), and concentration-weighted trajectory (CWT) models were used to analyse the variation characteristics, potential sources, and affected areas. Results showed that the BC concentrations in the Taklamakan Desert and Urumqi were in the range of 0–500 ng·m−3, accounting for 66.20 % and 59.50 % of the total, respectively. The backward trajectory simulation of BC mass concentration in the tower and Urumqi using the HYSPLIT model found that the airflow trajectories in the tower in summer corresponded to the BC concentration in the following order: trajectory 4 > trajectory 3 > trajectory 2 > trajectory 1, and trajectory 4 originated from the Turpan airflow accounting for 46.19 % of the total, which corresponded to the highest BC concentration of 621.73 ng·m−3. The trajectories of the airflow in Urumqi in summer corresponded to the BC concentration in the order of high to low, and the BC concentration in summer corresponded to the highest concentration in the Turpan airflow. BC concentrations arranged from high to low were trajectory 1 > trajectory 5 > trajectory 3 > trajectory 4 > trajectory 2. Trajectories 3, 4, and 5 airflow directions were the same, and the airflow trajectory accounted for 47.48 %, corresponding to BC concentrations of 599.82 ng·m−3, 579.99 ng·m−3, and 555.85 ng·m−3, respectively. Tower in the spring compared with other seasons of the CWT value of >400 ng·m−3 had the widest coverage, and Urumqi had more source areas contributing to moderate pollution concentration weights in winter (400 ng·m−3 < CWT < 800 ng·m−3). The conclusions of this study provide a scientific basis for regional environmental management and the formulation of air pollution measures in Xinjiang.

Spatiotemporal variations and source on black carbon over Chongqing, China: Long-term changes and observational experiments

Black carbon (BC), as a critical light-absorbing constituent within aerosols, exerts profound effects on atmospheric radiation balance, climate, air quality and human health, etc. And it is also a long-standing focus in rapidly developing megacities. So, this study primarily focuses on investigating the variation characteristics and underlying causes of BC in Chongqing (31,914,300 population), which is one of the municipalities directly under the central government of China, serving as a pivotal economic hub in southwest China. Utilizing MERRA-2 reanalysis data, we examined the long-term changes of atmospheric BC over Chongqing 20 years (from 2002 to 2021). Moreover, BC mass concentration observations were conducted using an Aethalometer (AE-33) from March 15 to June 14, 2021 in Liangping District, Chongqing. The statistical analysis over the last 20 years reveals an annual mean BC concentration in Chongqing of 3.42 ± 0.20 μg/m3, exhibiting growth from 2002 to 2008, followed by a decline from 2008 to 2021. Monthly concentration displays a “U-shaped” trend, with the lowest values occurring in summer and the highest in winter. Due to topographical and meteorological influences, local emissions primarily contribute to BC pollution, characterized by a spatial distribution pattern of high in the west and low in the east. Ground observation indicates a distinct dual-peaked pattern in the diurnal variation of BC, with peak concentrations aligning with periods of high traffic emissions. The variation in BC is significantly influenced by meteorological conditions (wind, temperature, atmospheric boundary layer) and local pollution sources (predominantly traffic). Furthermore, extreme events analysis suggests that local emissions and regional transport (with higher contributions from Chongqing and the Sichuan Basin) predominantly contributed to BC pollution. This study effectively makes up for the deficiency in analyzing the distribution and sources of BC pollution in Chongqing, providing valuable scientific insights for the atmospheric environment of megacities.

Shipborne observations of black carbon aerosols in the western Arctic Ocean during summer and autumn 2016–2020: impact of boreal fires

Abstract. 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 (&lt; 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 CH4 but not CO2 and O3. 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 O3, CH4, CO, and CO2 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.

Long term variation of microphysical properties of black carbon in Beijing derived from observation and machine learning

The microphysical attributes of black carbon (BC) can determine its absorption and hygroscopic properties. However, long-term information is difficult to obtain from the field. In this study, the BC properties including mass concentration, the coating volume ratio (VR) relative to the refractory BC (rBC), the rBC diameter and the fraction of cloud condensation nuclei (CCN), are derived from a number of field experiments using a random forest model. This model effectively derives the long-term BC microphysical properties in the Beijing region from 2013 to 2020 using continuous measurements of particulate matter, gas, BC mass concentration and meteorological parameters. The results reveal notably higher BC coatings (mean VR = 7.2) and a greater fraction of CCN-like BC (51%) in the winter compared to other seasons. Following the implementation of national air pollution control measures in 2017, BC mass exhibited a substantial reduction of 60% (29%) in the winter (summer), and VR decreased by 45% (24%). Apart from the influence of meteorological variations, these can be attributed to the declined primary emissions and the gas precursors which are associated with secondary formation of BC coatings. The reduction of both BC mass loading and coatings leads to its solar absorption decreasing by 50%, and the fraction of CCN-like BC (likely in clouds) decreasing by 23%. Environmental regulation will therefore continue to reduce both direct and indirect radiative impacts of BC in this region.

Particulate black carbon mass concentrations and the episodic source identification driven by atmospheric blocking effects in Astana, Kazakhstan

Black carbon (BC) is a component of fine particulate matter (PM2.5) that is a key contributor to adverse human health effects and climate forcing. To date, BC mass concentrations and possible sources in Kazakhstan have not been studied. Thus, understanding the temporal variations of BC for a large developing region with a complex climate is useful. In this study, measurements of fine particulate BC mass concentrations in Astana were made from June 2020 to October 2021 by measuring light absorption of PM2.5 on filters. The mean BC concentration was 2.56 ± 1.29 μg m−3 with maximum and minimum monthly mean BC concentrations being 4.56 ± 2.03 μg m−3 and 1.12 ± 0.42 μg m−3 in January 2021 and June 2020, respectively. Temporal analyses of BC, SO2, PM10, NOx, CO, meteorological and atmospheric stability parameters were performed. Aggregated pollutant ‘episodic loadings’ during the heating and non-heating periods were identified. Their relationships with blocking anticyclones and cyclones were investigated by examining the reversal of meridional gradients at 500 hPa geopotential height (GPH) maps and identifying Omega (Ω) and Rex blocking types. Astana has some of the highest BC concentrations of cities worldwide. Seasonal BC source location identification using Conditional Bivariate Probability Function (CBPF) analysis implicated combined heat and power (CHP) plant emissions as the major BC source in Astana. Significant increases in BC concentrations were observed during the cold season due to numerous sources, generally poorer atmospheric dispersion and blocking events. The Concentration Weighted Trajectory (CWT) analysis results showed that the distribution of the 75th percentile of BC during episodic periods actively controlled by blockings exceeding than the entire measurement period, which may reflect cross-border transport and adjacent countries.

Field comparison of dual- and single-spot Aethalometers: equivalent black carbon, light absorption, Ångström exponent and secondary brown carbon estimations

Abstract. 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 &gt; 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.

Source contribution of black carbon aerosol during 2020–2022 at an urban site in Indo-Gangetic Plain

The extensive emissions of black carbon (BC) from the Indo-Gangetic Plain (IGP) region of India have been well recognized. Particularly, biomass emissions from month-specific crop-residue burning (April, May, October, November) and heating activities (December–February) are considered substantial contributors to BC emissions in the IGP. However, their precise contribution to ambient BC aerosol has not been quantified yet and remains an issue of debate. Therefore, this study aims to fill this gap by quantifying the contribution of these month-specific biomass emissions to ambient BC at an urban site in IGP. This study presents the analysis of BC mass concentrations (MBC) measured for 3 years (2020−2022) in Delhi using an optical photometer i.e., continuous soot monitoring system (COSMOS). A statistical analysis of monthly mean MBC and factors affecting the MBC (ventilation coefficients, air mass back trajectories, fire counts) is performed to derive month-wise contribution due to background concentration, conventional emission, regional transport, crop-residue burning, and heating activities. The yearly mean MBC (5.3 ± 4.7, 5.6 ± 5.0, and 5.3 ± 3.5 μg m−3 during 2020, 2021, and 2022, respectively) remained relatively consistent with repetitive monthly patterns in each year. The peak concentrations were observed from November to January and low concentrations from June to September. Anthropogenic activities contributed significantly to MBC over Delhi with background concentration contributing only 30 % of observed MBC. The percentage contribution of emissions from crop-residue burning varied from 15 % (May) to 37 % (November), while the contribution from heating activities ranged from 25 % (December) to 39 % (January). This source quantification study highlights the significant impact of month-specific biomass emissions in the IGP and can play a vital role in better management and control of these emissions in the region.

Assessment of Black Carbon, optical properties and aerosol radiative forcing at Pranmati basin Himalayan critical zone observatory

The study aimed to understand the optical properties of Black Carbon (BC) and radiative forcing over a data deficient Himalayan region focusing on critical zone observatory employing ground-based measurements by Aethalometer for BC and satellite retrieval techniques for optical properties during mid-May-June 2022 and January–May 2023.BC mass concentration ranged from 0.18 to 4.43 μgm−3, exhibit a mean of 1.47 ± 0.83 μgm−3 with higher summer concentration (1.51 ± 0.94 μgm−3) than winter (1.39 ± 0.61 μgm−3). The average Absorption Ångström Exponent observed to be significantly higher than unity (1.77 ± 0.31) over the studied high-altitude Himalayan region, suggesting the dominance of biomass-burning aerosol. Higher aethalometer derived compensation parameter (K) in winter suggesting locally originated BC while, lower K value in summer suggesting aged BC transported from Indo-Gangetic Plains.Optical properties calculated from “Optical Properties of Aerosol and Cloud” (OPAC) model are used in the “Santa Barbara DISORT Atmospheric Radiative Transfer” (SBDART) model to calculate the aerosol Direct Radiative Force (DRF). The entire studied period is characterized by the predominance of absorbing aerosols, particularly BC, increasing Aerosol Optical Depth, Asymmetric Parameters and decreasing Single Scattering Albedo, leading to a considerable increase in atmospheric radiative forcing (+0.9 Wm−2, top of atmosphere) and Heating Rate (0.36 KDay−1). The mean radiative forcing within atmosphere during summer was higher (+14.29 Wm−2) relative to the winter (+12.00 Wm−2), emphasizing the impact of absorbing aerosols on regional warming and potential glacier melting in the Himalayas at a faster rate. Urgent policy consideration for the reduction of absorbing aerosols is highlighted, recognizing the critical roles of Black Carbon in the changing behaviour of Critical Zone observatory. The study's data serve as a valuable resource to understanding and addressing uncertainties in climate models, aiding effective policy implementation for Black Carbon reduction.

Significant changes in the physicochemical properties of BC-containing particles during the cold season in Beijing

The ambient air quality has improved significantly under strict emission controls in Beijing, China over the last decade. Black carbon (BC), as a short-lived climate forcer in ambient aerosols, profoundly impacts the air quality and climate. Previous studies have demonstrated a decline in the mass concentration of BC. In this study, we characterized the chemical compositions and size distributions of BC-containing particles during the cold season of 2022 in Beijing using state-of-the-art instruments capable of exclusively measuring BC-containing particles. The optical properties of BC-containing particles were further calculated based on the Mie theory. Moreover, we compared the properties of BC-containing particles in 2022 with the results of previous studies. The results showed that the diameters of BC cores became larger while the coating thickness of BC-containing particles became thinner in 2022. For the coating materials, the mass fraction of nitrate increased obviously, and even replaced organic matter as the dominant component during the peak of the pollution period. Variations in chemical compositions and size distributions resulted in lower mass absorption cross-sections (MAC) of BC-containing particles from 10.5 ± 1.1 m2/g in 2016 to 7.3 ± 0.8 m2/g in 2022, reduced by 30.5%. Our results demonstrate the synergistic benefits of air pollution control in improving air quality and mitigating climate change. Therefore, the MAC of BC adopted in climate models should vary with the changing air pollution levels. This study emphasizes that it is imperative to conduct long-term observations of BC-containing particles to better estimate BC's climate effects.

Significant contribution of fractal morphology to aerosol light absorption in polluted environments dominated by black carbon (BC)

In recent years, researchers have emphasized the use of fractal aggregate morphology instead of the core-shell morphology in global climate models for estimating black carbon (BC) forcing. This study confirms that fractal morphology plays an important role in reducing the overestimation of aerosol light absorption calculations in the case of an urban polluted environment. During periods of high anthropogenic BC emissions at Delhi, the particle light absorption is overestimated by 50 to 200% by assumptions of both external mixing and internal core-shell mixing. While incorporating the aggregate morphology model into light absorption simulations is beneficial in such cases, it comes with a high computational burden. To address this, we propose a metric known as morphology index (MI). This index distributes the weightage between the two extreme cases of core-shell and fractal aggregate to obtain accurate particle light absorption. Long-range transported aerosols were estimated to have an MI of 0.78, and fresh local emissions had an MI of 0.48. A BC-based aerosol classification approach was developed to determine the most relevant particle size mode for light absorption. The method is based on patterns found between the correlations of the BC mass concentrations and aerosol number concentrations at the different particles sizes (BC-size correlation spectra). BC-size correlation spectra are introduced as a concept that may be used (i) independently to understand the size-dependent heterogeneous distribution of aerosol light absorption and (ii) in conjunction with MI to accurately model the optical properties of aerosols in different BC regimes.

Aircraft observations of aerosol and BC during the East Asian dust storm event: Vertical profiles, size distribution and mixing state

The vertical structure of meteorological elements, black carbon (BC), and aerosols were in situ characterized by the King Air 350 aircraft measurements over the northeast of China during an East Asian dust storm event from April 10 to 13, 2023. The main causes of this dust storm event were the strong winds generated by the Mongolian cyclone, the cold front on the ground provided dynamic conditions, and the unstable atmospheric state provided thermal conditions and less precipitation in the dust source areas led to exposed the ground surface. The number concentrations of BC and aerosol had significant vertical distribution. The number concentration of aerosol in the dust storm (DS) layer increased rapidly with height, while the number and mass concentrations of BC were higher and varied slightly with height. The BC core mass median diameters (MMD) first increased with height, reaching a maximum value of 0.24 μm at 3000 m; and it rapidly decreased to 0.18 μm at 3200 m and then varied slightly with height above 3200 m. BC's bulk relative coating thickness (coated diameter divided by uncoated core diameter Dp/Dc) first decreased with height, reaching a minimum value of 1.16 at 3000 m, then increased with height, reaching a maximum of 1.38 (4250 m). A wind shear layer (7.9 m s−1 at 1850 m) with a sudden drop in temperature (the cooling rate can reach 7.4 °C·(100 m)−1) at 1900 m hinders the transportation of dust particles to the ground, allowing the dust particles to be transported at long-term distances. There were two stratifications in the dust storm layer: DS1 (1700–3000 m, the vertical wind speed was downward, the horizontal wind speed was small) and DS2 (3000–4500 m, the vertical wind speed was upward, the horizontal wind speed was large). The distinct atmospheric flow field conditions between DS1 and DS2 led to different BC and aerosol pollution characteristics. In DS2, the number concentrations of BC and aerosol were higher, the aging ratio of BC particles was higher, and the size of the core particle of BC was smaller. The concentrations of BC, aerosol, Dp/Dc, and MMD in DS2 were 1.1, 59.0, 1.02, and 0.84 times higher than those in DS1, respectively. Dust particles transported over long distances were primarily small. The number concentrations of aerosols at 0.1–0.12 μm and 0.1–0.24 μm were higher in DS1 and DS2, respectively. Still, the number concentration of aerosol at 0.12–0.28 μm in DS1 was lower than in the planetary boundary layer (PBL) and residual layer (RL).

Black carbon and PM0.49 characterization in manila north harbour port, Metro Manila, Philippines

Globalization and industrialization have increased the shipping activities in Metro Manila. This increase in economic activity has contributed to the exacerbation of atmospheric particle pollution, particularly black carbon (BC) and particulate matter (PM). In this study, PM0.49 and BC were characterized in North Harbour in Metro Manila, Philippines. Using a multiple-split high-volume cascade impactor, PM0.49 and PM2.5 were collected from December 2019 to January 2020. Equivalent BC (eBC) mass concentrations were measured using an aethalometer (AE33, Magee Scientific) while chemical analysis was also performed using ion chromatography. The PM0.49 was tested for its morphological and mineralogical characteristics. Daily analysis showed no significant difference between the weekday and weekend pollution concentration in the port, although mean concentration (70 ± 21 μg/m3) exceeds that of the 24-hr Philippine air quality guideline value of 50 μg/m3 for PM2.5 concentrations. The particle compositions of PM0.49 are mostly from Si-rich particles and Pb-rich particles. High variability was observed for Mg, Si, Ca, Fe, Cd, Zn, Mn, S, Cl, V, and Cr heavy metals. The carbonaceous species with the highest concentration was organic carbon (OC) (33 ± 9 μg/m3) followed by BC (16 ± 3 μg/m3) and eBC (12 ± 3 μg/m3). An analysis of the ionic species showed SOX and NOX emissions as the primary ions, which are mostly related to ship emissions while the mineralogical analysis showed that soot particles are the main composition of the particles. Overall, the pollution assessment showed that North Harbour is polluted with heavy metals but within the Philippine air quality pollutant standard. In brief, the results of this study suggest that atmospheric pollution in the study site was mostly caused by local anthropogenic sources, particularly vessel emissions. The researchers suggest that a longer study period be conducted to further assess the seasonal variation of atmospheric particle pollution in North Harbour, Metro Manila.

Accumulation of absorbing aerosols over the Indian Sector of Southern Ocean during the austral summer: Role of thermal inversions

Optical properties of aerosols and their direct radiative effect were analyzed from columnar Aerosol Optical Depth (AOD) and ambient Black Carbon (BC) mass concentration (MB) estimated during Indian Southern Ocean Expeditions (SOEs), conducted in the austral summers of 2016–17 (SOE-IX) and 2017–18 (SOE-X). The aforementioned observations were supplemented with concurrent vertical soundings of the lower atmosphere. Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) data aided in investigating the vertical distribution of aerosols up to 10 km altitude. The relative contribution of BC aerosols emanating from fossil fuel combustion and biomass burning showed the former to be predominant, as the latter is larger and preferentially scavenged during long-range transport to remote marine regions. The highest values of AOD at 500 nm (AOD500; 0.156 ± 0.026) and MB (90.78 ± 40.11 ng m−3) were encountered in the region between 50 and 60°S. Consequently, the atmospheric clear-sky Aerosol Direct Radiative Effect (ADRE; +3.10 ± 0.38 W m−2) and heating rate (HR; 0.087 ± 0.011 K day−1) were also observed to be the highest in the region. Multiple atmospheric inversions were detected between 40 and 69°S. Although a much lower AOD500 (0.070 ± 0.017) prevailed between 60 and 69°S, the average clear-sky ADRE (+1.56 ± 0.49 W m−2) and HR (0.044 ± 0.014 K day−1) were fairly high. The mean MB in the region was high (68.81 ± 28.40 ng m−3) for the pristine ice-covered region. Low-lying inversions prevented the vertical ventilation and dispersal of BC therein. Simulations of BC-induced atmospheric heating rates at three locations in the coastal Antarctic waters indicated a ≈ 3–5-fold increase, corresponding to an increase in ambient BC from 50 to 300 ng m−3.

Roles of water-soluble aerosol coatings for the enhanced radiative absorption of black carbon over south asia and the northern indian ocean

Black Carbon (BC), formed by incomplete combustion, absorbs solar radiation and heats the atmosphere. We investigated the enhancement in optical absorption of BC due to coatings of water-soluble (WS) species in the polluted South Asian atmosphere. The BC Mass Absorption Cross-section (MAC; 678 nm) was estimated before and after removal of the WS components. Wintertime samples were collected from three South Asian receptor observatories intercepting large-footprint outflow: Bangladesh Climate Observatory Bhola (BCOB; integrating outflow of the Indo-Gangetic Plain), Maldives Climate Observatories at Hanimaadhoo (MCOH) and at Gan (MCOG), both reflecting outflow from the South Asian region. The ambient MAC observed at BCOB, MCOH and MCOG were 4.2 ± 1.4, 7.9 ± 1.9 and 7.1 ± 1.5 m2 g−1, respectively.The average enhancement of the BC MAC due to WS coatings (i.e., ws-EMAC) was identical at all three sites (1.6 ± 0.5) indicating that the anthropogenic aerosols had already evolved to a fully coated morphology at BCOB and/or that subsequent aging involved two compensating evolution processes of the coating. Inspecting the key coating component sulfate; the sulfate-to-BC ratio increased threefold when transitioning from BCOB to MCOH and by about 1.5 times from BCOB to MCOG. Conversely, both WS organic carbon (WSOC)/BC and water-insoluble OC (WIOC)/BC ratios declined with distance: WSOC/BC diminished by 84 % from BCOB to MCOH and by 80 % from BCOB to MCOG, while WIOC/BC dropped by about 63 % and 59 %, respectively. Such declines in WSOC and WIOC reflect a combination of photochemical oxidation and more efficient washout of OC compared to BC. The observed changes in the SO42−/BC and WSOC/BC ratios across South Asia highlight the significant impact of aerosol composition on the optical properties of Black Carbon (BC). These findings emphasize the need for detailed studies on aerosol composition to improve climate models and develop effective strategies for reducing the impact of anthropogenic aerosols on the climate.

Optical properties and simple forcing efficiency of the organic aerosols and black carbon emitted by residential wood burning in rural central Europe

Abstract. 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 µg m−3 (max⁡=270 µg m−3) and 3.1 µg m−3 (max⁡=24 µg m−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 MACOA,370nm=2.4 m2 g−1, and AAEBrC,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.

Black carbon instrument responses to laboratory generated particles

Accurate measurement of black carbon (BC) particles is vital for climate models as well as air quality assessments. While the need for BC particle measurement has been recognized, standardization of instruments and procedures for ambient measurement is still underway. In this study, we used laboratory generated soot particles to assess nine instruments targeting BC mass concentration measurement. The measurement matrix included different BC concentrations (ranging from atmospheric levels to combustion emission levels), different particle coatings, two particle sources (gas burner and spark generator) and two dilution methods. The nine instruments included six different models: aethalometers AE33 and MA200, thermo-optical OC-EC analysis, multi-angle absorption photometer MAAP 5012, photoacoustic instrument MSS, and soot particle aerosol mass spectrometer SP-AMS. The main discrepancy we observed was that the SP-AMS results were systematically lower, approximately only half of the BC measured by other instruments. A portion of this is explained by particle losses in the aerodynamic lens of the SP-AMS and the parameters used in the data analysis. Some smaller discrepancies were identified for the other instruments, but overall, the median values from were within 25 % of each other. Instruments’ operation principles and covered concentration ranges need to be carefully considered especially in emission measurements where the aerosols can have high temporal variation as well as high BC concentrations. In general, the results can decrease the uncertainties in climate and air quality studies by providing tools for more accurate and comparable BC measurements and when the existing BC data is interpreted.

High-Precision Microscale Particulate Matter Prediction in Diverse Environments Using a Long Short-Term Memory Neural Network and Street View Imagery.

In this study, we propose a novel long short-term memory (LSTM) neural network model that leverages color features (HSV: hue, saturation, value) extracted from street images to estimate air quality with particulate matter (PM) in four typical European environments: urban, suburban, villages, and the harbor. To evaluate its performance, we utilize concentration data for eight parameters of ambient PM (PM1.0, PM2.5, and PM10, particle number concentration, lung-deposited surface area, equivalent mass concentrations of ultraviolet PM, black carbon, and brown carbon) collected from a mobile monitoring platform during the nonheating season in downtown Augsburg, Germany, along with synchronized street view images. Experimental comparisons were conducted between the LSTM model and other deep learning models (recurrent neural network and gated recurrent unit). The results clearly demonstrate a better performance of the LSTM model compared with other statistically based models. The LSTM-HSV model achieved impressive interpretability rates above 80%, for the eight PM metrics mentioned above, indicating the expected performance of the proposed model. Moreover, the successful application of the LSTM-HSV model in other seasons of Augsburg city and various environments (suburbs, villages, and harbor cities) demonstrates its satisfactory generalization capabilities in both temporal and spatial dimensions. The successful application of the LSTM-HSV model underscores its potential as a versatile tool for the estimation of air pollution after presampling of the studied area, with broad implications for urban planning and public health initiatives.

Physical Properties, Chemical Components, and Transport Mechanisms of Atmospheric Aerosols Over a Remote Area on the South Slope of the Tibetan Plateau

AbstractThe physicochemical properties and origins of atmospheric aerosols in the Tibetan Plateau (TP) region are a research topic of great interest, but an in‐depth understanding of this topic is challenging, partially due to a lack of intensive in situ observations. Thus, a field campaign was conducted over Yadong, a remote area on the south slope of the TP from June 11 to 31 August 2021. The aerosol loading was low, with a black carbon mass concentration of 147.4 ± 98.4 ng·m−3. Aerosol single‐scattering albedo was low (0.73 ± 0.11 at 550 nm) and increased from 450 to 700 nm wavelength. Organic matter (OM) accounting for 69.6% of the total aerosol mass and relatively high secondary organic carbon ratios, highlighting the importance of secondary formation. An interesting phenomenon observed was that the evolution of aerosols was mainly characterized by diurnal variation, which could not be explained by large‐scale atmospheric processes such as Indian summer monsoon. Instead, it was found that regional mountain‐valley winds between the Himalayas and South Asia transported polluted air masses toward the TP, especially in the afternoon when regional valley wind are expected to be the strongest and the boundary layer in South Asia is deepest. Additionally, daytime local valley wind further elevated these aerosols to higher altitudes on the TP. This paper provides insights into the transport mechanisms of aerosols from South Asia to the TP. These findings are of great importance since aerosols exhibit significant diurnal variations in the TP region.

Effects of Diesel Emissions on Black Carbon and Particle Number Concentrations in the Eastern U.S.

The effects of emissions of diesel engines on black carbon and particle number concentrations, as well as climate-relevant aerosol properties, are explored for a summertime period in the Eastern U.S. using the chemical transport model PMCAMx-UF. A 50% reduction in diesel particulate emissions results in lower (23%) black carbon mass concentrations, as expected, and similar changes both in magnitude (27–30%) and spatial pattern for the absorption coefficient. However, an average 2% increase in the total particle number concentrations is predicted due to a decrease in the coagulation and condensation sinks and, at the same time, a 2% decrease in N100 (particles larger than 100 nm) concentrations. The diesel reduction results suggest that mitigation of large diesel particles and/or particle mass emissions can reduce climate-relevant properties related to the absorption of black carbon and provide health benefits; however, the changes could also have the unintended effect of increased ultrafine particle number concentrations. Changes in cloud condensation nuclei are predicted to be significantly less than expected, assuming a proportional reduction during this photochemically active period. Doubling the diesel emissions results in a domain-averaged 3% decrease in total particle number concentrations and a 3% increase in N100 concentrations. PM2.5 BC concentrations increase on average by 46%, and similar changes (52–60%) are predicted for the absorption coefficient. Extinction coefficients for both perturbation simulations changed by only a few percent due to the dominance of scattering aerosols in the Eastern U.S. during this period characterized by high photochemical activity.