The San Joaquin Valley (SJV) of California has suffered persistent particulate matter (PM) pollution despite many years of control efforts. To further understand the chemical drivers of this problem and to support the development of State Implementation Plan for PM, a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) outfitted with a PM₂.₅ lens and a capture vaporizer has been deployed at the Fresno-Garland air monitoring site of the California Air Resource Board (CARB) since Oct. 2018. The instrument measured non-refractory species in PM₂.₅ continuously at 10-min resolution. In this study, the data acquired from Oct. 2018 to May 2019 were analyzed to investigate the chemical characteristics, sources and atmospheric processes of PM₂.₅ in the SJV. Comparisons of the ToF-ACSM measurement with various co-located aerosol instruments show good agreements. The inter-comparisons indicated that PM₂.₅ in Fresno was dominated by submicron particles during the winter whereas refractory species accounted for a major fraction of PM₂.₅ mass during the autumn associated with elevated PM₁₀ loadings. A rolling window positive matrix factorization analysis was applied to the organic aerosol (OA) mass spectra using the Multilinear Engine (ME-2) algorithm. Three distinct OA sources were identified, including vehicle emissions, local and regional biomass burning, and formation of oxygenated species. There were significant seasonal variations in PM₂.₅ composition and sources. During the winter, residential wood burning and oxidation of nitrogen oxides were major contributors to the occurrence of haze episodes with PM₂.₅ dominated by biomass burning OA and nitrate. In autumn, agricultural activities and wildfires were found to be the main cause of PM pollution. PM₂.₅ concentrations decreased significantly after spring and were dominated by oxygenated OA during March to May. Our results highlight the importance of using seasonally dependent control strategies to mitigate PM pollution in the SJV.

The influence of regional transport on aerosol pollution has been explored in previous studies based on numerical simulation or surface observation. Nevertheless, owing to inhomogeneous vertical distribution of air pollutants, vertical observations should be conducted for a comprehensive understanding of regional transport. Here we obtained the vertical profiles of aerosol and its precursors using ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) at the Nancheng site in suburban Beijing on the southwest transport pathway of the Beijing-Tianjin-Hebei (BTH) region, China, and then estimated the vertical profiles of transport fluxes in the southwest-northeast direction. The maximum net transport fluxes per unit cross-sectional area, calculated as pollutant concentration multiply by wind speed, of aerosol extinction coefficient (AEC), NO₂, SO₂ and HCHO were 0.98 km⁻¹ m s⁻¹, 24, 14 and 8.0 μg m⁻² s⁻¹ from southwest to northeast, which occurred in the 200–300 m, 100–200 m, 500–600 m and 500–600 m layers, respectively, due to much higher pollutant concentrations during southwest transport than during northeast transport in these layers. The average net column transport fluxes were 1200 km⁻¹ m² s⁻¹, 38, 26 and 15 mg m⁻¹ s⁻¹ from southwest to northeast for AEC, NO₂, SO₂ and HCHO, respectively, in which the fluxes in the surface layer (0–100 m) accounted for only 2.3%–4.2%. Evaluation only based on surface observation would underestimate the influence of the transport from southwest cities to Beijing. Northeast or weak southwest transports dominated in clean conditions with PM₂.₅ <75 μg m⁻³ and intense southwest transport dominated in polluted conditions with PM₂.₅ >75 μg m⁻³. Southwest transport through the middle boundary layer was a trigger factor for aerosol pollution events in urban Beijing, because it not only directly bringing air pollutants, but also induced an inverse structure of aerosols, which resulted in stronger atmospheric stability and aggravated air pollution in urban Beijing.

PM₂.₅ (particulate matter having aerodynamic diameter ≤2.5 μm) samples were collected during wintertime from two polluted urban sites (Allahabad and Kanpur) in the central Indo-Gangetic Plain (IGP) to comprehend the sources and atmospheric transformations of light-absorbing water-soluble organic aerosol (WSOA). The aqueous extract of each filter was atomized and analyzed in a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Water-soluble organic carbon (WSOC) and WSOA concentrations at Kanpur were ∼1.2 and ∼1.5 times higher than that at Allahabad. The fractions of WSOC and secondary organic carbon (SOC) to total organic carbon (OC) were also significantly higher ∼53% and 38%, respectively at Kanpur compared to Allahabad. This indicates a higher abundance of oxidized WSOA at Kanpur. The absorption coefficient (bₐbₛ₋₃₆₅) of light-absorbing WSOA measured at 365 nm was 46.5 ± 15.5 Mm⁻¹ and 73.2 ± 21.6 Mm⁻¹ in Allahabad and Kanpur, respectively, indicating the dominance of more light-absorbing fractions in WSOC at Kanpur. The absorption properties such as mass absorption efficiency (MAE₃₆₅) and imaginary component of refractive index (kₐbₛ₋₃₆₅) at 365 nm at Kanpur were also comparatively higher than Allahabad. The absorption forcing efficiency (Abs SFE; indicates warming effect) of WSOA at Kanpur was ∼1.4 times higher than Allahabad. Enhancement in light absorption capacity was observed with the increase in f44/f43 (fraction of m/z 44 (f44) to 43 (f43) in organic mass spectra) and O/C (oxygen to carbon) ratio of WSOA at Kanpur while no such trend was observed for the Allahabad site. Moreover, the correlation between carbon fractions and light absorption properties suggested the influence of low-volatile organic compounds (OC3 + OC4 fraction obtained from thermal/optical carbon analyzer) in increasing the light absorption capacity of WSOA in Kanpur.

To elucidate the molecular composition and sources of organic aerosols in Central Asia, carbonaceous compounds, major ions, and 15 organic molecular tracers of total suspended particulates (TSP) were analyzed from September 2018 to August 2019 in Dushanbe, Tajikistan. Extremely high TSP concentrations (annual mean ± std: 211 ± 131 μg m⁻³) were observed, particularly during summer (seasonal mean ± std: 333 ± 183 μg m⁻³). Organic carbon (OC: 11.9 ± 7.0 μg m⁻³) and elemental carbon (EC: 5.1 ± 2.2 μg m⁻³) exhibited distinct seasonal variations from TSP, with the highest values occurring in winter. A high concentration of Ca²⁺ was observed (11.9 ± 9.2 μg m⁻³), accounting for 50.8% of the total ions and reflecting the considerable influence of dust on aerosols. Among the measured organic molecular tracers, levoglucosan was the predominant compound (632 ± 770 ng m⁻³), and its concentration correlated significantly with OC and EC during the study period. These findings highlight biomass burning (BB) as an important contributor to the particulate air pollution in Dushanbe. High ratios of levoglucosan to mannosan, and syringic acid to vanillic acid suggest that mixed hardwood and herbaceous plants were the main burning materials in the area, with softwood being a minor one. According to the diagnostic tracer ratio, OC derived from BB constituted a large fraction of the primary OC (POC) in ambient aerosols, accounting for an annual mean of nearly 30% and reaching 63% in winter. The annual contribution of fungal spores to POC was 10%, with a maximum of 16% in spring. Measurements of plant debris, accounting for 3% of POC, divulged that these have the same variation as fungal spores.

Black carbon (BC) aerosol negatively affects air quality and contributes to climate warming globally. However, little is known about the relative contributions of different source control measures to BC reduction owing to the lack of powerful source-diagnostic tools. We combine the fingerprints of dual-carbon isotope using an optimized Bayesian Markov chain Monte Carlo (MCMC) scheme and for the first time to study the key sources of BC in megacity Guangzhou of the Pearl River Delta (PRD) region, China in 2018 autumn season. The MCMC model-derived source apportionment of BC shows that the dominant contributor is petroleum combustion (39%), followed by coal combustion (34%) and biomass burning (27%). It should be noted that the BC source pattern is highly sensitive to the variations of air masses transported with an enhanced contribution of fossil source from the eastern area, suggesting the important impact of regional atmospheric transportation on the BC source profile in the PRD region. Also, we further found that fossil fuel combustion BC contributed 84% to the total BC reduction during 2013–2018. The response of PM₂.₅ concentration to the ¹⁴C-derived BC source apportionment is successfully fitted (r = 0.90) and the results predicted that it would take ∼6 years to reach the WHO PM₂.₅ guideline value (10 μg m⁻³) for the PRD region if the emission control measures keep same as they are at present. Taken together, our findings suggest that dual-carbon isotope is a powerful tool in constraining the source apportionment of BC for the evaluations of air pollution control and carbon emission measures.

Air pollution has become a major issue in China, especially for traffic-related pollutants such as nitrogen dioxide (NO₂). Current studies in China at the national scale were less focused on NO₂ exposure and consequent health effects than fine particulate exposure, mainly due to a lack of high-quality exposure models for accurate NO₂ predictions over a long period. We developed an advanced modeling framework that incorporated multisource, high-quality predictor data (e.g., satellite observations [Ozone Monitoring Instrument NO₂, TROPOspheric Monitoring Instrument NO₂, and Multi-Angle Implementation of Atmospheric Correction aerosol optical depth], chemical transport model simulations, high-resolution geographical variables) and three independent machine learning algorithms into an ensemble model. The model contains three stages: (1) filling missing satellite data; (2) building an ensemble model and predicting daily NO₂ concentrations from 2013 to 2019 across China at 1×1 km² resolution; (3) downscaling the predictions to finer resolution (100 m) at the urban scale. Our model achieves a high performance in terms of cross-validation to assess the agreement of the overall (R² = 0.72) and the spatial (R² = 0.85) variations of the NO₂ predictions over the observations. The model performance remains moderately good when the predictions are extrapolated to the previous years without any monitoring data (CV R² > 0.68) or regions far away from monitors (CV R² > 0.63). We identified a clear decreasing trend of NO₂ exposure from 2013 to 2019 across the country with the largest reduction in suburban and rural areas. Our downscaled model further improved the prediction ability by 4%–14% in some megacities and captured substantial NO₂ variations within 1-km grids in the urban areas, especially near major roads. Our model provides flexibility at both temporal and spatial scales and can be applied to exposure assessment and epidemiological studies with various study domains (e.g., national or citywide) and settings (e.g., long-term and short-term).

The spatial distributions, fluxes, and environmental effects of non-methane hydrocarbons (NMHCs) were investigated in the Yellow Sea (YS) and the East China Sea (ECS) in spring. The average concentrations of ethane, propane, i-/n-butane, ethylene, propylene and isoprene in the seawater were 18.1 ± 6.4, 15.4 ± 4.7, 6.8 ± 2.9, 6.4 ± 3.2, 67.1 ± 26.7, 20.5 ± 8.7 and 17.1 ± 11.1 pmol L⁻¹, respectively. The alkenes in the surface seawater were more abundant than their saturated homologs and NMHCs concentrations (with the exception of isoprene) decreased with carbon number. The spatial variations of isoprene were consistent with the distributions of chlorophyll a (Chl-a) and Chaetoceros, Skeletonema, Nitzschia mainly contributed to the production of isoprene, while the others’ distributions might be related to their photochemical production. Observations in atmospheric NMHCs indicated alkanes in the marine atmosphere decreased from inshore to offshore due to influence of the continental emissions, while alkenes were largely derived from the oceanic source. In addition, no apparent diurnal discrepancy of atmospheric NMHCs (except for isoprene) were found between daytime and night. As the main sink of NMHCs in seawater, the average sea-to-air fluxes of ethane, propane, i-/n-butane, ethylene and propylene were 31.70, 29.75, 18.49, 15.89, 239.6, 67.94 and 52.41 nmol m⁻² d⁻¹, respectively. The average annual emissions of isoprene accounted for 0.1–1.3% of the global ocean emissions, which indicated that the coastal and shelf areas might be significant sources of isoprene. Furthermore, this study represents the first effort to estimate the environmental effects caused by NMHCs over the YS and the ECS and the results demonstrated contributions of alkanes to ozone and secondary organic aerosol (SOA) formation were lower than those of the alkenes and the largest contributor was isoprene.

The co-occurrence of enhancement in aerosol concentration, temperatures, and ozone mixing ratio was observed between June 29 and July 4, 2018 (enhanced period, EP) on Long Island (LI) and the greater NYC metropolitan area during part of the 2018 Long Island Sound Tropospheric Ozone Study (LISTOS). Two aerosol formation pathways were identified during the EP, the first being the condensation of semi- and intermediate volatility oxidation products of anthropogenic volatile organic compounds (AVOCs) under stagnant synoptic flow conditions, high temperatures and afternoon sea-breeze circulation. While this first pathway was prevalent, the most abundant organic aerosol factor was less oxidized oxygenated organic aerosol or LO-OOA. The second formation pathway occurred during a period of more persistent (synoptic) on-shore flow transporting more aged aerosol which consisted of an internal mixture of more oxidized oxygenated organic aerosol (MO-OOA), methanesulfonic acid (MSA) and sulfate. It was estimated that 35% of the sulfate observed during the mature period (an average of about 1.2 μg m⁻³) originated from oceanic dimethyl sulfide (DMS) emissions. These two formation pathways helped elucidate the sources of fine particle pollution, highlighted the interaction between human emissions and natural DMS emission, and will help our understanding of pollution affecting other urban areas adjacent to large bodies of water during hot and stagnant periods.

The space-borne measured fine-mode aerosol optical depth (fAOD) is a gross index of column-integrated anthropogenic particulate pollutants, especially over the populated land. The fAOD is the product of the AOD and the fine-mode fraction (FMF). While there exist numerous global AOD products derived from many different satellite sensors, there have been much fewer, if any, global FMF products with a quality good enough to understand their spatiotemporal variations. This is key to understanding the global distribution and spatiotemporal variations of air pollutants, as well as their impacts on global environmental and climate changes. Modifying our newly developed retrieval algorithm to the latest global-scale Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol product (Collection 6.1), a global 10-year FMF product is generated and analyzed here. We first validate the product through comparisons with the FMF derived from Aerosol Robotic Network (AERONET) measurements. Among our 169,313 samples, the satellite-derived FMFs agreed with the AERONET spectral deconvolution algorithm (SDA)-retrieved FMFs with a root-mean-square error (RMSE) of 0.22. Analyzed using this new product are the global patterns and interannual and seasonal variations of the FMF over land. In general, the FMF is large (>0.80) over Mexico, Myanmar, Laos, southern China, and Africa and less than 0.5 in the Sahelian and Sudanian zones of northern Africa. Seasonally, higher FMF values occur in summer and autumn. The linear trend in the satellite-derived and AERONET FMFs for different countries was explored. The upward trend in the FMFs was particularly strong over Australia since 2008. This study provides a new global view of changes in FMFs using a new satellite product that could help improve our understanding of air pollution around the world.

High particulate matter (PM) and ozone (O₃) concentration in Hong Kong are frequently observed during the summertime typhoon season. Despite the critical effect of a typhoon on air pollution, contributions of vertical wind profile and cloud movement during transboundary air pollution (TAP) on surface PM and O₃ concentration have yet to be fully understood. This work is the first study to apply a network of Doppler light detection and ranging (LiDAR) as well as back trajectory analysis to comprehensively analyze the effect of a weak Typhoon (Danas) occurring during 16–19 July 2019 on different variations in PM and O₃ concentration. During the typhoon Danas, three types of surface air pollution with five episodes were identified: (1) low PM and high O₃ concentration; (2) co-occurring high PM and O₃ concentration and (3) high PM and low O₃ concentration. Employing our 3D Real-Time Atmospheric Monitoring System (3DREAMs) along with surface observations, we found the important role of TAP in the increases in surface PM and O₃ concentration with significant vertical wind shear that transported air pollutants at upper levels, and strong vertical mixing that brought air pollutants to the ground level. Cloud movement related to typhoon periphery, as well as high solar radiation due to sinking motion and remote transport by continental wind, have an impact on local O₃ concentration. For the substantial difference in O₃ concentration between two air quality measurement sites, the similar vertical aerosol distributions and wind profiles suggest the comparable TAP contributions at the two sites and thus infer the critical role of local O₃ photochemical process in the O₃ difference. This work comprehensively reveals the influences of a weak typhoon on variations in PM and O₃ during the five episodes, providing important references for air quality monitoring and forecast in regions under the influence of typhoon.