Characterizing Chemical, Environmental, and Stimulated Subcellular Physical Characteristics of Size-Fractionated PMs Down to PM0.1.

Air pollution, especially particulate matter (PM), is a significant environmental pollution worldwide. Studying the chemical, environmental, and life-related cellular physical characteristics of size-fractionated PMs is important because of their different degrees of harmful effects on human respiratory tracts and organ systems, causing severe diseases. This study evaluates the chemical components of size-fractionated PMs down to PM0.1 collected during a biomass-burning episode, including elemental/organic carbon and trace elements. Single particle sizes and distributions of PM0.1, PM0.5-0.1, PM1.0-0.5, and PM2.5-1.0 were analyzed by scanning electron microscopy and Zeta sizer. Two commonly used cell lines, e.g., HeLa and Cos7 cells, and two respiratory-related cell lines including lung cancer/normal cells were utilized for cell cytotoxicity experiments, revealing the key effects of particle sizes and concentrations. A high-speed scanning ion conductance microscope explored particle-stimulated subcellular physical characteristics for all cell lines in dynamics, including surface roughness (SR) and elastic modulus (E). The statistical results of SR showed distinct features among different particle sizes and cell types while a E reduction was universally found. This work provides a comprehensive understanding of the chemical, environmental, and cellular physical characteristics of size-fractionated PMs and sheds light on the necessity of controlling small-sized PM exposures.

Fossil and Nonfossil Sources of Winter Organic Aerosols in the Regional Background Atmosphere of China.

Carbonaceous aerosols (CA) from anthropogenic emissions have been significantly reduced in urban China in recent years. However, the relative contributions of fossil and nonfossil sources to CA in rural and background regions of China remain unclear. In this study, the sources of different carbonaceous fractions in fine aerosols (PM2.5) from five background sites of the China Meteorological Administration Atmosphere Watch Network during the winter of 2019 and 2020 were quantified using radiocarbon (14C) and organic markers. The results showed that nonfossil sources contributed 44-69% to total carbon at these five background sites. Fossil fuel combustion was the predominant source of elemental carbon at all sites (73 ± 12%). Nonfossil sources dominated organic carbon (OC) in these background regions (61 ± 13%), with biomass burning or biogenic-derived secondary organic carbon (SOC) as the most important contributors. However, the relative fossil fuel source to OC in China (39 ± 13%) still exceeds those at other regional/background sites in Asia, Europe, and the USA. SOC dominated the fossil fuel-derived OC, highlighting the impact of regional transport from anthropogenic sources on background aerosol levels. It is therefore imperative to develop and implement aerosol reduction policies and technologies tailored to both the anthropogenic and biogenic emissions to mitigate the environmental and health risks of aerosol pollution across China.

Comparing sources of carbonaceous aerosols during haze and nonhaze periods in two northern Chinese cities.

Radiocarbon (14C), stable carbon isotope (13C), and levoglucosan in PM2.5 were measured in two northern Chinese cities during haze events and nonhaze periods in January 2019, to ascertain the sources and their differences in carbonaceous aerosols between the two periods. The contribution of primary vehicle emissions (17.8 ± 3.7%) to total carbon in Beijing during that haze event was higher than that of primary coal combustion (7.3 ± 4.2%), and it increased significantly (7.1%) compared to the nonhaze period. The contribution of primary vehicle emissions (4.1 ± 2.8%) was close to that of primary coal combustion (4.3 ± 3.3%) during the haze event in Xi'an, and the contribution of primary vehicle emissions decreased by 5.8% compared to the nonhaze period. Primary biomass burning contributed 21.1 ± 10.5% during the haze event in Beijing and 40.9 ± 6.6% in Xi'an (with an increase of 3.3% compared with the nonhaze period). The contribution of secondary fossil fuel sources to total secondary organic carbon increased by 29.2% during the haze event in Beijing and by 18.4% in Xi'an compared to the nonhaze period. These results indicate that specific management measures for air pollution need to be strengthened in different Chinese cities in the future, that is, controlling vehicle emissions in Beijing and restricting the use of coal and biomass fuels in winter in Xi'an.

Seasonal variations of mass absorption efficiency of elemental carbon in PM2.5 in urban Guangzhou of South China.

This study investigates seasonal variations of mass absorption efficiency of elemental carbon (MAEEC) and possible influencing factors in urban Guangzhou of South China. Mass concentrations of elemental carbon (EC) and organic carbon (OC) in PM2.5 and aerosol absorption coefficient (bap) at multi-wavelengths were simultaneously measured in four seasons of 2018-2019 at hourly resolution by a semi-continuous carbon analyzer and an aethalometer. Seasonal average mass concentrations of EC were in the range of 1.36-1.70 µgC/m3 with a lower value in summer than in the other seasons, while those of OC were in the range of 4.70-6.49 µgC/m3 with the lowest value in summer and the highest in autumn. Vehicle exhaust from local traffic was identified to be the predominant source of carbonaceous aerosols. The average aerosol absorption Ångström exponents (AAE) were lower than 1.2 in four seasons, indicating EC and bap were closely related with vehicle exhaust. Seasonal MAEEC at 550 nm was 11.0, 8.5, 10.4 and 11.3 m2/g in spring, summer, autumn, and winter, respectively. High MAEEC was related with the high mass ratio of non-carbonaceous aerosols to EC and high ambient relative humidity.

Response of Indian summer monsoon rainfall to remote carbonaceous aerosols at short time scales: Teleconnections and feedbacks.

The effect of atmospheric aerosols on Indian monsoon is one of the scientifically challenging and societally relevant research issues of the recent decades. Past studies have derived inferences mostly based on local emissions and their impacts thereupon. However, more recent studies have shown that the remote effects driven by aerosols elsewhere could also impact the monsoon system on different time scales. Our study using an atmospheric general circulation model (AGCM) shows that regional carbonaceous aerosol emissions (from North America, Europe and North Africa and Asia) can significantly alter Indian summer monsoon rainfall. It is interesting to note that the effects of remote aerosols are larger and bear a resemblance to each other in comparison to local emissions. Our study reveals that the modulation of large-scale circulation induced by regional warming by carbonaceous aerosols leads to teleconnection patterns around the globe, thereby changing the precipitation depending on the phase of these disturbances. We also find that the effects of remote carbonaceous aerosols are strengthened by modulation/feedback through natural dust aerosols over the Arabian Sea with subsequent increase in rainfall over India. The results signify that the changes in the aerosol emissions in one region could lead to the change in precipitation over other regions through global teleconnection and associated feedbacks induced by regional atmospheric warming and/or cooling.

Variabilities of δ13C and carbonaceous components in ambient PM2.5 in Northeast India: Insights into sources and atmospheric processes.

A year-long sampling campaign of ambient PM2.5 (particulate matter with aerodynamic diameter ≤2.5 mm) at a regional station in the North-Eastern Region (NER) of India was performed to understand the sources and formation of carbonaceous aerosols. Mass concentration, carbon fractions (organic and elemental carbon), and stable carbon isotope ratio (δ13C) of PM2.5 were measured and studied along with cluster analysis and Potential Source Contribution Function (PSCF) modelling. PM2.5 mass concentration was observed to be highest during winter and post-monsoon seasons when the meteorological conditions were relatively stable compared to other seasons. Organic carbon (OC) concentration was more than two times higher in the post-monsoon and winter seasons than in the pre-monsoon and monsoon seasons. Air mass back trajectory cluster analysis showed the dominance of local and regional air masses during winter and post-monsoon periods. In contrast, long-range transported air masses influenced the background site in pre-monsoon and monsoon. Air mass data and PSCF analysis indicated that aerosols during winter and post-monsoon are dominated by freshly generated emissions from local sources along with the influence from regional transport of polluted aerosols. On the contrary, the long-range transported air masses containing aged aerosols were dominant during pre-monsoon. No significant variability was observed in the range of δ13C values (-28.2‰ to -26.4‰) during the sampled seasons. The δ13C of aerosols indicates major sources to be combustion of biomass/biofuels (C3 plant origin), biogenic aerosols, and secondary aerosols. The δ13C variability and cluster/PSCF modelling suggest that aged aerosols (along with enhanced photo-oxidation derived secondary aerosols) influenced the final δ13C during the pre-monsoon. On the other hand, lower δ13C in winter and post-monsoon is attributed to the freshly emitted aerosols from biomass/biofuels.

Four year long simulation of carbonaceous aerosols in India: Seasonality, sources and associated health effects.

India's air quality is in a dismal state, with many studies ascribing it to PM2.5. Most of these corroborate that carbonaceous aerosol (CA) constitute significant fraction of PM2.5. However, investigations on the effect of long-term meteorological or emission changes on PM2.5 and its components, and their associated health effects are rare. In this work, WRF-Chem simulations for three seasons over four years (2016-2019) were carried out to cogitate the spatial and temporal changes in PM2.5 and its components in India. Model predicted PM2.5 concentrations were in good agreement with the ground-based observations for 25 cities. PM2.5 was highest in winter and lowest in pre-monsoon. PM2.5 reduced by ∼8% in Indo-Gangetic Plain (IGP) but increased by ∼38% and ∼130% in south and northeast India, respectively, from 2016 to 2019. IGP witnessed three times higher average PM2.5 concentrations than south India. No significant interannual change in CA contributions was observed, however, it peaked in the winter season. Other inorganics (OIN) were the major component of PM2.5, contributing more than 40%. Primary organic aerosol (POA) fractions were higher in north India, while secondary inorganic aerosol (SIA) dominated south India. Transport and residential sectors were the chief contributors to CA across India. Biomass burning contributed up to ∼23% of PM2.5 in regions of IGP during post-monsoon, with CA fractions up to 50%. Associations between PM2.5 and its components with daily inpatient admissions from a tertiary care centre in Delhi showed that PM2.5 and OIN had lower associations with daily hospital admissions than CA. Every 10 µg/m3 increase in POA, black carbon (BC), and secondary organic aerosol (SOA) were associated with ∼1.09%, ∼3.07% and ∼4.93% increase in the risk of daily hospital admissions. This invigorates the need for more policies targeting CA rather than PM2.5 to mitigate associated health risks, in India.

A year-long study on PM2.5 and its carbonaceous components over eastern Himalaya in India: Contributions of local and transported fossil fuel and biomass burning during premonsoon.

A year-long (March 2019-February 2020) study on the characterization of fine mode carbonaceous aerosols has been conducted over a high altitude urban atmosphere, Darjeeling (27.01°N, 88.15°E, 2200 m asl) in eastern Himalaya. The fine mode aerosol (PM2.5; 41.7 ± 23.7 µgm-3), total carbonaceous aerosols (TCA; 19.8 ± 7.7 µgm-3), organic carbon (OC; 8.0 ± 3.9 µgm-3) and elemental carbon (EC; 2.0 ± 0.9 µgm-3) exhibited similar seasonal variability with the highest abundance during winter followed by premonsoon, postmonsoon and minimum in monsoon. The OC:EC varied over a range of 2.8-19.4 whereas the secondary organic carbon ranged between 1.9 and 17.1 µgm-3 respectively. Higher PM2.5 associated with higher winds and elevated mixing layer depth suggest a strong influence of regional and long-range transport. In addition to the usual morning and evening rush-hour peaks, the impact of low land plain regions driven by up-slope valley winds was observed for the carbonaceous components. A novel approach has been taken to find out the individual contributions from the local and transported fossil fuel, biomass burning, and biogenic sources to OC and EC during premonsoon. We observed that the local fossil fuel (43%) contributions dominated over the biomass burning (39%) for EC whereas the contributions of local biomass burning and the local fossil fuel were same (46%) for OC. EC exhibited a higher contribution (18%) from the regional/long-range transport compared to OC (8%). IGP and Nepal were found to be the maximum contributing long distant source regions for the carbonaceous aerosol loading over eastern Himalaya. Such individual source apportionment of carbonaceous aerosols over eastern Himalaya makes the study unique and first-ever of its kind and immensely helpful for building robust mitigation action plans.

Seasonal variations in carbonaceous species of PM2.5 aerosols at an urban location situated in Indo-Gangetic Plain and its relationship with transport pathways, including the potential sources.

The study examines the variation in organic carbon (OC) and elemental carbon (EC) in PM2.5 concentration at an urban location of Indo-Gangetic Plains (IGP) to understand the impact of seasonality and regional crop residue burning activities. Seasonal cluster analysis of backward air masses and concentration-weighted trajectory (CWT) analysis was performed to identify seasonal transport pathways and potential source regions of carbonaceous aerosols. The mean PM2.5 level during the study period was 57 ± 41.6 µgm-3 (5.0-187.3 µgm-3), whereas OC and EC concentration ranges from 2.8 µgm-3 to 28.2 µgm-3 and 1.3 µgm-3 to 15.5 µgm-3 with a mean value of 8.4 ± 5.5 µgm-3 and 5.1 ± 3.3 µgm-3 respectively. The highest mean PM2.5 concentration was found during the winter season (111.3 ± 25.5 µgm-3), which rises 3.6 times compared to the monsoon season. OC and EC also follow a similar trend having the highest levels in winter. Total carbonaceous aerosols contribute ∼38% of PM2.5 composition. The positive linear trend between OC and EC identified the key sources. HYSPLIT cluster analysis of backward air mass trajectories revealed that during the post-monsoon, winters, pre-monsoon, and monsoon, 71%, 81%, 60%, and 43% of air masses originate within the 500 km radius of IGP. CWT analysis and abundance of OC in post-monsoon and winters season establish a linkage between regional solid-biomass fuel use and crop residue burning activities, including meteorology. Moreover, the low annual average OC/EC ratio (1.75) indicates the overall influence of vehicular emissions. The current dataset of carbonaceous aerosols collated with other Indian studies could be used to validate the global aerosol models on a regional scale and aid in evidence-based air pollution reduction strategies.

Long-Term Variation in Carbonaceous Components of PM2.5 from 2012 to 2021 in Delhi.

Carbonaceous species [organic carbon (OC), elemental carbon (EC), elemental matter (EM), primary organic carbon (POC), secondary organic carbon (SOC), total carbon (TC), and total carbonaceous matter (TCM)] of PM2.5 were analyzed to study the seasonal variability and long-term trend of carbonaceous aerosols (CAs) in megacity Delhi, India from January, 2012 to April, 2021. The average concentrations (± standard deviation) of PM2.5, OC, EC, TC, EM, TCM, POC and SOC were 127 ± 77, 15.7 ± 11.6, 7.4 ± 5.1, 23.1 ± 16.5, 8.2 ± 5.6, 33.3 ± 23.9, 9.3 ± 6.3 and 6.5 ± 5.3 µg m-3, respectively during the sampling period (10-year average). The average CAs accounted for 26% of PM2.5 concentration during the entire sampling period. In addition, the seasonal variations in PM2.5, OC, EC, POC, SOC, and TCM levels were recorded with maxima in post-monsoon and minima in monsoon seasons. The linear relationship of OC and EC, OC/EC and EC/TC ratios suggested that the vehicular emissions (VE), fossil fuel combustion (FFC) and biomass burning (BB) are the major sources of CAs at megacity Delhi, India.

Nitrogenous and carbonaceous aerosols in PM2.5 and TSP during pre-monsoon: Characteristics and sources in the highly polluted mountain valley.

This study reports for the first time a comprehensive analysis of nitrogenous and carbonaceous aerosols in simultaneously collected PM2.5 and TSP during pre-monsoon (March-May 2018) from a highly polluted urban Kathmandu Valley (KV) of the Himalayan foothills. The mean mass concentration of PM2.5 (129.8 µg/m3) was only ~25% of TSP mass (558.7 µg/ m3) indicating the dominance of coarser mode aerosols. However, the mean concentration as well as fractional contributions of water-soluble total nitrogen (WSTN) and carbonaceous species reveal their predominance in find-mode aerosols. The mean mass concentration of WSTN was 17.43±4.70 µg/m3 (14%) in PM2.5 and 24.64±8.07 µg/m3 (5%) in TSP. Moreover, the fractional contribution of total carbonaceous aerosols (TCA) is much higher in PM2.5 (~34%) than that in TSP (~20%). The relatively low OC/EC ratio in PM2.5 (3.03 ± 1.47) and TSP (4.64 ± 1.73) suggests fossil fuel combustion as the major sources of carbonaceous aerosols with contributions from secondary organic aerosols. Five-day air mass back trajectories simulated with the HYSPLIT model, together with MODIS fire counts indicate the influence of local emissions as well as transported pollutants from the Indo-Gangetic Plain region to the south of the Himalayan foothills. Principal component analysis (PCA) also suggests a mixed contribution from other local anthropogenic, biomass burning, and crustal sources. Our results highlight that it is necessary to control local emissions as well as regional transport while designing mitigation measures to reduce the KV's air pollution.

High rise in carbonaceous aerosols under very low anthropogenic emissions over eastern Himalaya, India: Impact of lockdown for COVID-19 outbreak.

The present study has been conducted to investigate the relative changes of carbonaceous aerosols (CA) over a high altitude Himalayan atmosphere with and without (very low) anthropogenic emissions. Measurements of atmospheric organic (OC) and elemental carbon (EC) were conducted during the lockdown period (April 2020) due to global COVID 19 outbreak and compared with the normal period (April 2019). The interesting, unexpected and surprising observation is that OC, EC and the total CA (TCA) during the lockdown (OC: 12.1 ± 5.5 µg m-3; EC: 2.2 ± 1.1 µg m-3; TCA: 21.5 ± 10 µg m-3) were higher than the normal period (OC: 7.04 ± 2.2 µg m-3; EC: 1.9 ± 0.7 µg m-3; TCA: 13.2 ± 4.1 µg m-3). The higher values for OC/EC ratio too was observed during the lockdown (5.7 ± 0.9) compared to the normal period (4.2 ± 1.1). Much higher surface O3 during the lockdown (due to very low NO) could better promote the formation of secondary OC (SOC) through the photochemical oxidation of biogenic volatile organic compounds (BVOCs) emitted from Himalayan coniferous forest cover. SOC during the lockdown (7.6 ± 3.5 µg m-3) was double of that in normal period (3.8 ± 1.4 µg m-3). Regression analysis between SOC and O3 showed that with the same amount of increase in O3, the SOC formation increased to a larger extent when anthropogenic emissions were very low and biogenic emissions dominate (lockdown) compared to when anthropogenic emissions were high (normal). Concentration weighted trajectory (CWT) analysis showed that the anthropogenic activities over Nepal and forest fire over north-east India were the major long-distant sources of the CA over Darjeeling during the normal period. On the other hand, during lockdown, the major source regions of CA over Darjeeling were regional/local. The findings of the study indicate the immense importance of Himalayan biosphere as a major source of organic carbon.

Carbonaceous Species of PM2.5 in Megacity Delhi, India During 2012-2016.

Organic carbon (OC) and elemental carbon (EC) in PM2.5 were estimated to study the seasonal and inter-annual variability of atmospheric total carbonaceous aerosols (TCA) at an urban site of megacity Delhi, India for 5 years from January, 2012 to December, 2016. The annual average (± standard deviation) concentrations of PM2.5, OC, EC and TCA were 128 ± 81, 16.6 ± 12.2, 8.4 ± 5.8 and 34.5 ± 25.2 µg m-3, respectively. During the study, significant seasonal variations in mass concentrations of PM2.5, OC, EC and TCA were observed with maxima in winter and minima in monsoon seasons. Significant correlations between OC and EC, and OC/EC ratio suggested that vehicular emissions, fossil fuel combustion and biomass burning could be major sources of carbonaceous aerosols of PM2.5 at the sampling site of Delhi, India.

Atmospheric carbonaceous aerosols from Indo-Gangetic Plain and Central Himalaya: impact of anthropogenic sources.

In the present-day scenario of growing anthropogenic activities, carbonaceous aerosols contribute significantly (∼20-70%) to the total atmospheric particulate matter mass and, thus, have immense potential to influence the Earth's radiation budget and climate on a regional to global scale. In addition, formation of secondary organic aerosols is being increasingly recognized as an important process in contributing to the air-pollution and poor visibility over urban regions. It is, thus, essential to study atmospheric concentrations of carbonaceous species (EC, OC and WSOC), their mixing state and absorption properties on a regional scale. This paper presents the comprehensive data on emission sources, chemical characteristics and optical properties of carbonaceous aerosols from selected urban sites in the Indo-Gangetic Plain (IGP) and from a high-altitude location in the central Himalaya. The mass concentrations of OC, EC and WSOC exhibit large spatio-temporal variability in the IGP. This is attributed to seasonally varying emissions from post-harvest agricultural-waste burning, their source strength, boundary layer dynamics and secondary aerosol formation. The high concentrations of OC and SO4(2-), and their characteristic high mass scattering efficiency, contribute significantly to the aerosol optical depth and scattering coefficient. This has implications to the assessment of single scattering albedo and aerosol radiative forcing on a regional scale.

Characterization and apportionment of carbonaceous aerosol emission factors from light-duty and heavy-duty vehicle fleets in Maharashtra, India.

This study aims to investigate the characteristics of carbonaceous aerosols and estimate emission factor (EF) based on roadway tunnel measurements, from two distinct vehicular fleets: an all light-duty vehicle (LDV) fleet, and a mixed fleet of 80% LDV and 20% heavy-duty vehicle (HDV). Carbonaceous content (organic carbon: OC and elemental carbon: EC) in total fine particles (PM2.5) accounted for 41% ± 6.8% in LDV fleet and 48% ± 7.2% in mixed fleet. While higher volatile OC dominated in the LDV fleet emissions, in mixed fleet, lower volatile OC and EC emissions dominated due to the presence of higher HDV and super-emitter (SE) fractions which led to significantly higher optically active absorbing aerosols. Reconstructed HDV fleet EF was higher than LDV fleet by 36 times (PM2.5), 19 times (OC) and 51 times (EC). Our findings emphasize the significance of implementing vehicle inspection and maintenance programs, coupled with decarbonization of HDVs to mitigate on-road vehicular emissions in India.

Optical properties and radiative forcing of carbonaceous aerosols in a valley city under persistent high temperature.

Carbonaceous aerosols were collected in the valley city of Baoji city in Northern China in August 2022. The light absorption characteristics and influencing factors of black carbon (BC) and brown carbon (BrC) were analyzed, and their radiative forcing was estimated. The results showed that the light absorption of secondary brown carbon [AbsBrC,sec (370)] was 7.5 ± 2.4 Mm-1, which was 2.5 times that of primary brown carbon [AbsBrC,pri (370), 3.0 ± 1.2 Mm-1]. During the study period, the absorption Ångström exponent (AAE) of aerosol was 1.6, indicating that there was obvious secondary aerosol formation or carbonaceous aerosol aging in the valley city of Baoji. Except for secondary BrC (BrCsec), the light absorption coefficient (Abs) and mass absorption efficiency (MAE) of BC and primary BrC (BrCpri) during the persistent high temperature period (PHT) were higher than those during the normal temperature period (NT) and the precipitation period (PP), which indicated that the light absorption capacity of black carbon and primary brown carbon increased, while the light absorption capacity of secondary brown carbon decreased under persistent high temperature period. Secondary aerosols sulfide (SO42-), nitrate (NO3-) and secondary organic carbon (SOC) are important factors for promoting the light absorption enhancemen of BC and BrCpri and photobleaching of BrCsec during persistent high temperature period. The Principal Component Analysis-Multiple Linear Regression (PCA-MLR) model showed that traffic emissions was the most important source of pollution in Baoji City. Based on this, the secondary source accelerates the aging of BC and BrC, causing changes in light absorption. During PHT, the radiative forcing of BC and BrCpri were enhanced, while the radiative forcing of BrCsec was weakened, but the positive radiative forcing generated by them may aggravate the high-temperature disaster.

Contributions of fossil and non-fossil fractions to total carbon in urban aerosols in Bratislava (Slovakia).

Radiocarbon measurements of total carbon (TC) fraction of aerosol samples collected at the campus of the Comenius University in Bratislava (Slovakia) during 2022-2023 were carried out. Based on radiocarbon activity of these samples and a source apportionment model we have determined the relative proportion of fossil and non-fossil carbon in collected atmospheric aerosols. The carbon from non-fossil sources (biomass burning and biogenic emissions) was dominant in this time period, on average it formed 72% of carbon present in the aerosols from the atmosphere of Bratislava. The whole range of determined non-fossil fraction was relatively small as it varied only from 0.67 (August-September) to 0.82 (December-January). These changes do not exhibit any significant seasonal variation as was previously observed in Bratislava during 2017-2018 in the elemental carbon (EC) aerosol fraction.

Dual carbon isotope-based brown carbon aerosol characteristics at a high-altitude site in the northeastern Himalayas: Role of biomass burning.

PM2.5 samples (n = 34) were collected from January to April 2017 over Shillong (25.7°N, 91.9°E; 1064 m amsl), a high-altitude site situated in the northeastern Himalaya. The main aim was to understand the sources, characteristics, and optical properties of local vs long-range transported carbonaceous aerosols (CA) using chemical species and dual carbon isotopes (13C and 14C). Percentage biomass burning (BB)/biogenic fraction (fbio, calculated from 14C) varied from 67 to 92 % (78 ± 7) and correlated well with primary BB tracers like f60, and K+, suggesting BB as a considerable source. Rain events are shown to reduce the fbio fraction, indicating majority of BB-derived CA are transported. Further, δ13C (-26.6 ± 0.4) variability was very low over Shillong, suggesting it's limitations in source apportionment over the study region, if used alone. Average ratio of absorption coefficient of methanol-soluble BrC (BrCMS) to water-soluble BrC (BrCWS) at 365 nm was 1.8, indicating a significant part of BrC was water-insoluble. A good positive correlation between fbio and mass absorption efficiency of BrCWS and BrCMS at 365 nm with the higher slope for BrCMS suggests BB derived water-insoluble BrC was more absorbing. Relative radiative forcing (RRF, 300 to 2500 nm) of BrCWS and BrCMS with respect to EC were 11 ± 5 % and 23 ± 16 %, respectively. Further, the RRF of BrCMS was up to 60 %, and that of BrCWS was up to 22 % with respect to EC for the samples with fbio ≥ 0.85 (i.e., dominated by BB), reflecting the importance of BB in BrC RRF estimation.

Black carbon and particulate matter concentrations amid central Chile's extreme wildfires.

The increase in the frequency and severity of global wildfires has been largely influenced by climate change and land use changes. From February 2 to 6, 2024, central Chile experienced its most devastating wildland-urban interface wildfire in history, severely impacting the Valparaíso region. This catastrophic event, which led to extensive forest destruction, the loss of thousands of homes, and over a hundred human fatalities, directly impacted the area surrounding the campus of Federico Santa María Technical University. In that period, an air quality monitoring campaign was set up on the campus to measure black carbon (BC) and particulate matter (PM) during the wildfire season. The monitoring station was located directly within the smoke plume, allowing for the collection of unprecedented air quality data. Extremely high concentrations of BC at 880 nm were reported during the wildfires, with a daily mean (±σ) of 14.83 ± 19.52 µg m-3. Peak concentrations measured at 880 nm and 375 nm reached 812.89 µg m-3 and 1561.24 µg m-3, respectively. The maximum daily mean BC concentrations at these wavelengths were 55 and 99 times higher, respectively, compared to the pre-event period. The mean Ångström absorbing coefficient during the event was 1.66, indicating biomass burning as the primary BC source, while the maximum BC/PM2.5 ratio (at 375 nm) reached 57 %. From February 2 to 5, 2024, PM concentrations exceeded the Chilean air quality standard by 82 % and 198 % for coarse and fine particles, respectively. These levels are 4.7 and 6.0 times higher than the World Health Organization's recommendations. These elevated concentrations persisted for up to three days after the fire was extinguished. This study provides unique evidence of the rapid deterioration of regional air quality during a wildfire event using in situ measurements, serving as a stark reminder of the far-reaching consequences of a warming climate.

Long-term evolution of carbonaceous aerosols in PM2.5 during over a decade of atmospheric pollution outbreaks and control in polluted central China.

Against the backdrop of an uncertain evolution of carbonaceous aerosols in polluted areas over the long term amid air pollution control measures, this 11-year study (2011-2021) investigated fine particulate matter (PM2.5) and carbonaceous components in polluted central China. Organic carbon (OC) and elemental carbon (EC) averaged 16.5 and 3.4 µg/m3, constituting 16 and 3 % of PM2.5 mass. Carbonaceous aerosols dominated PM2.5 (35 and 27 %) during periods of excellent and good air quality, while polluted days witnessed other components as dominants, with a significant decrease in primary organic aerosols and increased secondary pollution. From 2011 to 2021, OC and EC decreased by 53 and 76 %, displaying a high-value oscillation phase (2011-2015) and a low-value fluctuation phase (post-2016). A substantial reduction in high OC and EC concentrations in 2016 marked a milestone in significant air quality improvement attributed to effective control measures, especially targeting OC and EC, evident from their decreased proportion in PM2.5. Primary OC (POC) in winter exhibited the most pronounced reduction (8 % per year), and the seasonal disparities in PM2.5 and carbonaceous components were reduced, showcasing the effectiveness of control measures. Contrary to the more pronounced reduction of EC, which decreased in proportion to PM2.5, secondary OC (SOC) in PM2.5 exhibited an increasing trend. Along with rising OC/EC, SOC/OC, and SOC/EC ratios, this indicates a growing prominence of secondary pollution compared to the decrease in primary pollution. SOC shows an increasing trend with NO2 rise (r = 0.53), without O3 promoting SOC. Positive correlations of SOC with SO2, CO (r = 0.41, 0.59), also highlight their influence on atmospheric conditions, oxidative capacity, and chemical reactions, indirectly impacting SOC formation. The implementation of precise precursor emission reduction measures holds the key to future efforts in mitigating SOC pollution and reducing PM2.5 concentrations, thereby contributing to improved air quality.