Compositions and sources of fluorescent water-soluble and water-insoluble organic aerosols.

Brown carbon (BrC), the light-absorbing component of organic aerosols, plays a significant role in climate change and atmospheric photochemistry. However, the water-insoluble fractions of BrC have not been extensively studied, limiting the assessment of the overall climate effects of BrC. In this study, water-soluble and -insoluble organic carbon (i.e., WSOC and WIOC) in wintertime aerosols in Hefei were subsequently fractionated, and their fluorescence properties were comparatively investigated with the excitation-emission matrix method. WIOC contributing 57.1 % was the major component of organic carbon. WSOC with the largest contribution from humic-like regions exhibited a redshift compared to WIOC. Three humic-like substances (HULIS) with different oxidation degrees and one protein-like substances (PRLIS) were identified as the major fluorescent components by the parallel factor analysis. WSOC had more highly oxygenated HULIS, whereas low-oxygenated HULIS dominated WIOC. Nighttime WIOC contained more less-oxygenated species. The positive matrix factorization analysis suggested that biomass burning (43 %) was the largest source of both fluorescent WSOC and WIOC. Coal combustion contributed much more to fluorescent WIOC (40 %), whereas secondary formation contributed more to fluorescent WSOC (12 %). During aerosol pollution episodes, the increase in fluorescence efficiency was much greater for WIOC (25 %) than for WSOC (12 %), and WSOC and WIOC experienced a redshift and blueshift in emission wavelength, respectively. WSOC had more highly oxygenated HULIS, while WIOC had more less-oxygenated HULIS in aerosol episodes than the non-episodic periods. In addition, aerosol pollution was accompanied by the increased contributions of biomass burning and coal combustion to both fluorescent WSOC and WIOC, while the decreased relative contribution of secondary formation to fluorescent WSOC. Our findings highlighted the different fluorescence properties, compositions and sources of fluorescent WSOC and WIOC, providing a comprehensive view of BrC aerosols.

Peatland Wildfires Enhance Nitrogen-Containing Organic Compounds in Marine Aerosols over the Western Pacific.

Peatland wildfires contribute significantly to the atmospheric release of light-absorbing organic carbon, often referred to as brown carbon. In this study, we examine the presence of nitrogen-containing organic compounds (NOCs) within marine aerosols across the Western Pacific Ocean, which are influenced by peatland fires from Southeast Asia. Employing ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) in electrospray ionization (ESI) positive mode, we discovered that NOCs are predominantly composed of reduced nitrogenous bases, including CHN+ and CHON+ groups. Notably, the count of NOC formulas experiences a marked increase within plumes from peatland wildfires compared to those found in typical marine air masses. These NOCs, often identified as N-heterocyclic alkaloids, serve as potential light-absorbing chromophores. Furthermore, many NOCs demonstrate pyrolytic stability, engage in a variety of substitution reactions, and display enhanced hydrophilic properties, attributed to chemical processes such as methoxylation, hydroxylation, methylation, and hydrogenation that occur during emission and subsequent atmospheric aging. During the daytime atmospheric transport, aging of aromatic N-heterocyclic compounds, particularly in aliphatic amines prone to oxidation and reactions with amine, was observed. The findings underscore the critical role of peatland wildfires in augmenting nitrogen-containing organics in marine aerosols, underscoring the need for in-depth research into their effects on marine ecosystems and regional climatic conditions.

Dominant contribution of combustion-related ammonium during haze pollution in Beijing.

Aerosol ammonium (NH4+), mainly produced from the reactions of ammonia (NH3) with acids in the atmosphere, has significant impacts on air pollution, radiative forcing, and human health. Understanding the source and formation mechanism of NH4+ can provide scientific insights into air quality improvements. However, the sources of NH3 in urban areas are not well understood, and few studies focus on NH3/NH4+ at different heights within the atmospheric boundary layer, which hinders a comprehensive understanding of aerosol NH4+. In this study, we perform both field observation and modeling studies (the Community Multiscale Air Quality, CMAQ) to investigate regional NH3 emission sources and vertically resolved NH4+ formation mechanisms during the winter in Beijing. Both stable nitrogen isotope analyses and CMAQ model suggest that combustion-related NH3 emissions, including fossil fuel sources, NH3 slip, and biomass burning, are important sources of aerosol NH4+ with more than 60% contribution occurring on heavily polluted days. In contrast, volatilization-related NH3 sources (livestock breeding, N-fertilizer application, and human waste) are dominant on clean days. Combustion-related NH3 is mostly local from Beijing, and biomass burning is likely an important NH3 source (∼15%-20%) that was previously overlooked. More effective control strategies such as the two-product (e.g., reducing both SO2 and NH3) control policy should be considered to improve air quality.

Impact of battery electric vehicle usage on air quality in three Chinese first-tier cities.

China, the world leader in automobile production and sales, confronts the challenge of transportation emissions, which account for roughly 10% of its total carbon emissions. This study, utilizing real-world vehicle data from three major Chinese cities, assesses the impact of Battery Electric Vehicles (BEVs) on air quality. Our analysis reveals that BEVs, when replacing gasoline vehicles in their operational phase, significantly reduce emissions, with reductions ranging from 8.72 to 85.71 kg of CO2 per vehicle monthly. The average monthly reduction rate is 9.47%, though this effect is less pronounced during winter. Advanced BEVs, characterized by higher efficiency and newer technology, exhibit greater emission reduction benefits. While private BEVs generally contribute positively to environmental outcomes, taxi BEVs, due to their intensive usage patterns, show less environmental advantage and may sometimes worsen air quality. Looking ahead, we project substantial emission reductions from the replacement of gasoline vehicles with electric alternatives over the next decade. Policymakers are urged to adopt proactive measures, focusing on promoting medium to large electric vehicles and fostering the use of private and ride-hailing electric vehicles.

Spatial and molecular variations in forest topsoil dissolved organic matter as revealed by FT-ICR mass spectrometry.

Forest soils cover about 30 % of the Earth's land surface and play a fundamental role in the global cycle of organic matter. Dissolved organic matter (DOM), the largest active pool of terrestrial carbon, is essential for soil development, microbial metabolism and nutrient cycling. However, forest soil DOM is a highly complex mixture of tens of thousands of individual compounds, which is largely composed of organic matter from primary producers, residues from microbial process and the corresponding chemical reactions. Therefore, we need a detailed picture of molecular composition in forest soil, especially the pattern of large-scale spatial distribution, which can help us understand the role of DOM in the carbon cycle. To explore the spatial and molecular variations of DOM in forest soil, we choose six major forest reserves located in different latitudes ranging in China, which were investigated by Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS). Results show that aromatic-like molecules are preferentially enriched in DOM at high latitude forest soils, while aliphatic/peptide-like, carbohydrate-like, and unsaturated hydrocarbon molecules are preferentially enriched in DOM at low latitude forest soils, besides, lignin-like compounds account for the highest proportion in all forest soil DOM. High latitude forest soils have higher aromatic equivalents and aromatic indices than low latitude forest soils, which suggest that organic matter at higher latitude forest soils preferentially contain plant-derived ingredients and are refractory to degradation while microbially derived carbon is dominant in organic matter at low latitudes. Besides, we found that CHO and CHON compounds make up the majority in all forest soil samples. Finally, we visualized the complexity and diversity of soil organic matter molecules through network analysis. Our study provides a molecular-level understanding of forest soil organic matter at large scales, which may contribute to the conservation and utilization of forest resources.

Molecular transformation of organic nitrogen in Antarctic penguin guano-affected soil.

Organic nitrogen (ON) is an important participant in the Earth's N cycle. Previous studies have shown that penguin feces add an abundance of nutrients including N to the soil, significantly changing the eco-environment in ice-free areas in Antarctica. To explore the molecular transformation of ON in penguin guano-affected soil, we collected guano-free weathered soil, modern guano-affected soil from penguin colonies, ancient guano-affected soil from abandoned penguin colonies, and penguin feces from the Ross Sea region, Antarctica, and Fourier transform ion cyclotron mass spectrometry (FT-ICR MS) was used to investigate the chemical composition of water-extractable ON. By comparing the molecular compositions of ON among different samples, we found that the number of ON compounds (>4,000) in weathered soil is minimal, while carboxylic-rich alicyclic-like molecules (CRAM-like) are dominant. Penguin feces adds ON into the soil with > 10,000 CHON, CHONS and CHN compounds, including CRAM-like, lipid-like, aliphatic/ peptide-like molecules and amines in the guano-affected soil. After the input of penguin feces, macromolecules continue to degrade, and other ON compounds tend to be oxidized into relatively stable CRAM-like molecules, this is an important transformation process of ON in guano-affected soils. We conclude the roles of various forms of ON in the N cycle are complex and diverse. Combined with previous studies, ON eventually turns into inorganic N and is lost from the soil. The lost N ultimately returns to the ocean and the food web, thus completing the N cycle. Our study preliminarily reveals the molecular transformation of ON in penguin guano-affected soil and is important for understanding the N cycle in Antarctica.

Diurnal variations in primary and secondary organic aerosols in an eastern China coastal city: The impact of land-sea breezes.

The land-sea breeze circulation significantly impacts the atmospheric transport of organic aerosols in coastal regions. However, the links between organic aerosols and land-sea breezes remain poorly understood. In this study, organic marker compounds for biomass burning, primary biological aerosols, biogenic and anthropogenic secondary organic aerosols (SOA) in fine particles from a coastal city in East China were analysed using gas chromatography-mass spectrometry. Land-sea breeze circulations were identified to explore their potential influence on organic molecular compositions. Organic marker compounds showed obvious diurnal/seasonal patterns. Surprisingly, due to the combined influence of weakened East Asian monsoons and land-sea breezes, all detected organic markers decreased except α/ß-pinene SOA markers during land-sea breeze periods in early autumn; whereas, all the organic markers increased except α/ß-pinene SOA markers, pollen and plant debris markers during land-sea breeze periods in early spring. Furthermore, the reaction pathway and aging of biogenic SOA were also related to land-sea breezes. During the land-sea breeze periods, the ratios of 2-methylglyceric acid (2-MGA) to 2-methyltetrols increased in early autumn, indicating that more isoprene-derived SOA generated from the high-NOx (nitrogen oxides) pathway when the land-sea breezes occurred; while the ratios decreased in early spring, this may be related to the chemical transformation of 2-MGA to 2-MGA sulfates. Changes in the ratio of monoterpene SOA markers demonstrate that monoterpene SOA was relatively aged during sea breeze periods, while it was fresher when the land breeze occurred. Although boundary layer height, emissions, gas/particle partitioning, etc. are important reasons for the diurnal variations of organic aerosols, night/day ratios of molecular markers increased obviously when land-sea breezes occurred in both early autumn and early spring. Our results provide new insights into the shift in the chemical composition of organic aerosols over coastal areas that are influenced by land-sea breezes.

Accumulation of dissolved organic matter in the transition from fresh to aged seasonal snow in an industrial city in NE China.

Dissolved organic matter (DOM) plays a significant role in the reduction of snow albedo and the acceleration of snowmelt, but its accumulation in snow remains poorly understood. This study investigated the accumulation of DOM in seasonal snow including its accumulation rate, molecular characteristics, and biological and chemical processing. Sixteen snow samples of both fresh and aged snow were collected at one-day interval in Changchun, a typical industrial city in NE China. The snow DOM contents increased linearly with accumulation time at a rate of 30.3 µg L-1 d-1. The optical properties, including fluorescence intensity and optical absorption coefficient, of snowmelt increased exponentially with time owing to the rapid accumulation of terrestrial humic-like fluorophores through snow-soil exchange and deposition of soil-derived substances. Fourier transform-ion cyclotron resonance-mass spectrometry highlighted the properties of DOM at a molecular level, indicating that compounds derived from underlying soil and vascular plants make the largest contribution to DOM. Microbe-derived compounds contribute 35.5 % to the DOM pool. Degrees of saturation and oxidation increase slightly after accumulation, with the impacts of photo- and bio-chemistry on DOM molecules being non-negligible. This study provides a new perspective concerning the accumulation and fate of organic contaminants in snow ecosystems.

Stable Isotopes Reveal Photoreduction of Particle-Bound Mercury Driven by Water-Soluble Organic Carbon during Severe Haze.

Haze with high loading of particles may result in significant enrichment of particle-bound Hg (PBM), potentially impacting the atmospheric Hg transformation and transport. However, the dynamics of Hg transformation and the relative environmental effect during severe haze episodes remain unclear. Here, we report Hg isotopic compositions of atmospheric particles (PM2.5, PM10, and TSP) collected during a severe haze episode in Tianjin, China, to investigate the transformation and fate of Hg during haze events. All severe haze samples display significantly higher Δ199Hg (up to 1.50‰) than global urban PBM, which cannot be explained by primary anthropogenic emissions. The high Δ199Hg is likely caused by photoreduction of PBM promoted by water-soluble organic carbon (WSOC) during the particle accumulation period, as demonstrated by the positive correlations of Δ199Hg with WSOC and relative humidity and confirmed by our laboratory-controlled photoreduction experiment. The results show that, on average, 21% of PBM are likely photoreduced and re-emitted back to the atmosphere as Hg(0), potentially requiring revision of atmospheric Hg budgeting and modeling. This study highlights the release of large portions of PBM back to the gas phase through photoreduction, which needs to be taken into account while evaluating the atmospheric Hg cycle and the relative ecological effects.

Dwindling aromatic compounds in fine aerosols from chunk coal to honeycomb briquette combustion.

With the implementation of clean coal policy in China, the chunk coal has been gradually replaced by honeycomb briquette in domestic energies. In this study, the molecular composition of fine particles (PM2.5) from chunk coal and honeycomb briquette combustion is characterized using the Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS). More than 6000 molecular formulae were detected in each PM2.5 sample. A remarkable decrease in unsaturation and aromatic compounds was found from chunk coal to honeycomb briquette derived aerosols. Around 73.6% of the unique CHON compounds in chunk coal are considered to have aromatic structures, while it decreased to 7.3% in honeycomb briquette. Most of these nitroaromatics detected only in chunk coal are highly carcinogenic and mutagenic with 4-6 rings. Moreover, the aromatic compounds in sulfur-containing compounds also showed a significant decrease. Meanwhile, because of the perforated shape and the additives added during the production of honeycomb briquettes, there are more heteroatoms-containing molecules released from honeycomb briquette combustion, which are highly functional compounds with high molecular weight, high degree of oxidation, and low volatility. Our results provide molecular level evidence that the transformation from chunk coal to honeycomb briquette can effectively reduce the emission of aromatic compounds, which is beneficial to assessing and reducing the impacts to climate change as well as human health.

Source and formation process impact the chemodiversity of rainwater dissolved organic matter along the Yangtze River Basin in summer.

Rainwater dissolved organic matter (DOM) plays an important role in the biogeochemical cycle and evolution of organic matter in the land-atmosphere interface. To better understand their sources and molecular composition in the atmosphere, rainwater samples were collected at six different locations along the Yangtze River Basin. Based on the application of a combined approach including excitation-emission matrix (EEM) fluorescence and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), various sources (terrestrial, anthropogenic, and autochthonous sources) of rainwater DOM were revealed. Results show that the derivatives of biogenic volatile organic compounds were widely distributed and contributed to rainwater DOM along the Yangtze River Basin. In the up-river city Batang, rainwater DOM was affected by the long-range atmospheric transport due to the Indian summer monsoon. Lijiang, a city on the southeastern edge of Tibetan plateau, was related to strong local biomass burning. The industrial cities of Panzhihua and Luzhou showed large differences in organic composition due to distinct industrial types. Fuling, a district in Chongqing Municipality, was significantly contributed by aged organics from biomass burning. While rainwater DOM in Shanghai, a coastal megacity, contained a high fraction of sea spray organics. Further, more than 70% of rainwater DOM molecules are associated with 36 typical transformation mechanisms during rainwater-scavenging processes, e.g., oxidation reactions, dealkylation and decarboxylation. Our study demonstrates that local natural and anthropogenic emissions and climatic conditions strongly shaped the chemodiversity and possible precursor-product pairs of rainwater DOM along the Yangtze River Basin, which helps to better understand the biogeochemical cycles of organic matter in a large-scale watershed under the influence of human activities.

Latitudinal difference in the molecular distributions of lipid compounds in the forest atmosphere in China.

Lipids are important biogenic markers to indicate the sources and chemical process of aerosol particles in the atmosphere. To better understand the influences of biogenic and anthropogenic sources on forest aerosols, total suspended particles (TSP) were collected at Mt. Changbai, Shennongjia, and Xishuangbanna that are located at different climatic zones in northeastern, central and southwestern China. n-Alkanes, fatty acids and n-alcohols were detected in the forest aerosols based on gas chromatography-mass spectrometry. The total concentrations of aliphatic compounds ranged from 15.3 ng m-3 to 566 ng m-3, and fatty acids were the most abundant (44-95%) followed by n-alkanes and n-alcohols. Low molecular weight- (LFAs) and unsaturated fatty acids (UnFAs) showed diurnal variation with higher concentrations during the nighttime in summer, indicating the potential impact from microbial activities on forest aerosols. The differences of oleic acid (C18:1) and linoleic acid (C18:2) concentrations between daytime and nighttime increased at lower latitude, indicating more intense photochemical degradation occurred at lower latitude regions. High levels of n-alkanes during daytime in summer with higher values of carbon preference indexes, combining the strong odd carbon number predominance with a maximum at C27 or C29, implied the high contributions of biogenic sources, e.g., higher plant waxes. In contrast, higher concentrations of low molecular weight n-alkanes were detected in winter forest aerosols. Levoglucosan showed a positive correlation (R2 > 0.57) with high- and low molecular weight aliphatic compounds in Mt. Changbai, but such a correlation was not observed in Shennongjia and Xishuangbanna. These results suggest the significant influence of biomass burning in Mt. Changbai, and fossil fuel combustion might be another important anthropogenic source of forest aerosols. This study adds useful information to the current understanding of forest organic aerosols at different geographical locations in China.

Molecular characterization and spatial distribution of dicarboxylic acids and related compounds in fresh snow in China.

Low molecular weight organic compounds are ubiquitous in the atmosphere. However, knowledge on their concentrations and molecular distribution in fresh snow remains limited. Here, twelve fresh snow samples collected at eight sites in China were investigated for dicarboxylic acids and related compounds (DCRCs) including oxocarboxylic acids and α-dicarbonyls. Dissolved organic carbon (DOC) concentrations in the snow samples ranged from 0.99 to 14.6 mg C L-1. Concentrations of total dicarboxylic acids were from 225 to 1970 µg L-1 (av. 650 µg L-1), while oxoacids (28.3-173, av. 68.1 µg L-1) and dicarbonyls (12.6-69.2, av. 31.3 µg L-1) were less abundant, accounting for 4.6-8.5% (6.2%), 0.45-1.4% (0.73%), and 0.12-0.88% (0.46%) of DOC, respectively. Molecular patterns of dicarboxylic acids are characterized by a predominance of oxalic acid (C2) (95.0-1030, av. 310 µg L-1), followed by phthalic (Ph) (9.69-244, av. 69.9 µg L-1) or succinic (C4) (23.8-163, av. 63.7 µg L-1) acid. Higher concentrations of Ph in snow from Beijing and Tianjin than other urban and rural regions suggest significant emissions from vehicular exhausts and other fossil fuel combustion sources in megacities. C2 constituted 40-54% of total diacids, corresponding to 1.5-2.6% of snow DOC. The total measured DCRCs represent 5.5-10% of snow DOC, which suggests that there are large amounts of unknown organics requiring further investigations. The spatial distributions of diacids exhibited higher loadings in megacities than rural and island sites. Molecular distributions of diacids indicated that the photochemical modification was restrained under the weak solar radiation during the snow events, while anthropogenic primary sources had a more significant influence in megacities than rural areas and islands.

Variations in physicochemical properties of airborne particles during a heavy haze-to-dust episode in Beijing.

The variations in physicochemical properties of airborne particles collected during a typical transition from haze to dust were investigated using single particle analysis with transmission and scanning electron microscopes combined with online measurement of chemical compositions of airborne particles in Beijing in February 2013. The transition was divided into three phases based on the weather condition. During haze pollution (Phase 1), gaseous and particle pollutants enhanced gradually. Results from single particle analysis showed that more coatings and more anthropogenic elements (e.g., S) appeared on the surface of fine and coarse particles, which was probably caused by efficient aqueous-phase reactions under high humidity (70%) condition. Phase 2 was dust intrusion episode. PM10 reached over 1000 µg m-3. Larger fractions of mineral particles and bare-like soot particles were observed in fine particles, while the fraction of secondary particles with coatings decreased. The proportion of black carbon in submicron particles also increased. Photochemical oxidation in gas phase likely dominated in secondary formation under high O3 concentration. After the dust episode (Phase 3), secondary formation enhanced obviously. Soot aged quickly and had a larger mode of 0.45 µm than the other phases. The size modes of airborne fine particles during Phases 1 and 3 were 0.35 µm, which were a bit larger than that during Phase 2 (0.24 µm). These results indicate that dust plumes accompanied with strong wind brought mineral particles in both fine and coarse modes and freshly emitted particles with smaller sizes, and swept away pre-presence air pollutants. This study could provide detailed information on the physicochemical properties of airborne particles during typical severe pollution processes in a short time. Such short-term change should be taken into account in order to more accurately assess the environmental, climatic and health-related effects of airborne particles.

Molecular markers for fungal spores and biogenic SOA over the Antarctic Peninsula: Field measurements and modeling results.

Biogenic organic aerosols are important components of atmospheric organic aerosols and play vital roles in atmospheric chemistry, global climate, and biogeochemical cycles of carbon. However, studies on biogenic organic aerosols in the vast regions of the Southern Ocean and over the coastal waters of the Antarctic, especially Antarctic Peninsula, are still extremely limited. To understand the concentrations, molecular composition and seasonality of biogenic organic aerosols in Antarctica, atmospheric aerosols were collected at the Palmer Station on the west Antarctic Peninsula experiencing dramatic climate warming. Molecular marker compounds of fungal spores and secondary organic aerosols formed from the photooxidation of isoprene and monoterpene were analyzed using gas chromatography/mass spectrometry. Concentrations of sugar alcohols and biogenic SOA tracers both presented seasonal patterns with higher average concentrations in summer (90.7 and 122 pg m-3) than in winter (8.88 and 57.2 pg m-3). Sugar alcohols and biogenic SOA tracers were predominated by mannitol and isoprene oxidation products. Relative contributions of fungal-spore organic carbon (OC), isoprene-derived secondary OC (SOC) and monoterpene-derived SOC estimated with tracer-based methods were 26.2%, 55.6% and 18.2%, respectively. The observed seasonality of total biogenic SOA and some molecular species at the Antarctic Peninsula was further supported by the results from the global model CESM/IMPACT. Model results also suggest higher biogenic SOA in East Antarctica than that in West Antarctica, which is attributed to the influence of vertical atmospheric circulation. Our results of air-mass trajectory indicate the potential influence of marine emissions on the biogenic organic aerosols over the Antarctic Peninsula.

Summertime fluorescent bioaerosol particles in the coastal megacity Tianjin, North China.

Primary biological particles are an important subset of atmospheric aerosols. They have significant impacts on climate change and public health. Tianjin is a coastal megacity in the North China Plain, which is affected by both anthropogenic activities and marine air masses. To study the abundance and dynamic change of bioaerosols in Tianjin, fluorescent biological aerosol particles (FBAPs) in Tianjin were investigated by a wideband integrated bioaerosol sensor (WIBS-4A) in terms of number concentrations and size distributions in summer (11th -25th August 2018). Meanwhile, total suspended particles were collected and analyzed for chemical compounds to identify potential sources of bioaerosols. WIBS data showed that fluorescent biological particles exhibited two peaks at sunrise (~7:00) and in the evening (~20:00), which were probably caused by the enhancement of fungal spores and bacteria. Three rain events occurred during the observation period. Precipitation enhanced the abundance of biological particles, which were likely released from vegetation leaves, resuspended from soil surfaces, and/or carried by raindrops from high altitudes. The abundance of biological particles showed no significant correlation with Na+ (r = -0.17), indicating the air masses from marine areas carried limited biological particles compared to those from continental areas.

High daytime abundance of primary organic aerosols over Mt. Emei, Southwest China in summer.

Organic molecular composition of fine aerosols in the free troposphere is poorly understood. Here, PM2.5 (particles with aerodynamic diameters ≤ 2.5 µm) samples were collected at the summit of Mt. Emei (3080 m a.s.l.) in the Southwestern China on a daytime and nighttime basis during summer 2016 (June-July). The samples were analyzed by solvent-extraction followed by derivatization and gas chromatography/mass spectrometry (GC/MS). Four classes of organic compounds, i.e. n-alkanes, fatty acids, saccharides and lignin/resin acids were measured quantitatively. Fatty acids were found to be the most abundant species with an average concentration of 401 ±â€¯419 ng m-3 (range 25.7-1490 ng m-3) in the daytime, similar to the average concentration at night (399 ±â€¯447 ng m-3, 19.6-1970 ng m-3). However, the concentrations of biomass burning tracers (e.g., levoglucosan), primary biological aerosol tracers (e.g., mannitol and arabitol) and low molecular weight n-alkanes derived from fossil fuel combustion in daytime samples were obviously higher than those in nighttime samples. The results suggest that valley breezes transported a large number of aerosols and their precursors from the ground surface to the summit of Mt. Emei in the daytime. Estimated with tracer-based methods, the contributions of biogenic primary sources (plant debris, fungal spore, and biomass burning) to organic carbon was in the range of 3.28-83.5% (22.0 ±â€¯17.5%) in the daytime and 3.45-37.4% (10.9 ±â€¯8.97%) at night. As the largest contributor, biomass burning was an important anthropogenic/natural source of aerosol particles in the free troposphere over Mt. Emei. CAPSULE: Valley/mountain breeze is an important constraint to the temporal variations in organic aerosols over Mt. Emei.

Black carbon in Xiamen, China: Temporal variations, transport pathways and impacts of synoptic circulation.

Black carbon (BC) plays a vital role in atmospheric environment and climate change. Temporal variations and transport pathways of BC in Xiamen, China with the impacts of synoptic circulation were investigated in 2014 with Aethalometer. Annual mean BC concentration was 4270 ng m-3. BC exhibited clear diurnal (seasonal) variations, with the maximum of 6182 (4755) ng m-3 at 6:00 (in spring) and minimum of 2847 (3774) ng m-3 at 13:00 (in summer). Conditional probability function analysis indicated that high BC concentrations were associated with northwesterly winds with low wind speed. Air masses originating from the East China Sea and passing along with East China Coast had the highest BC concentrations. Potential source contribution function and concentration weighted trajectory analysis suggested that major sources for BC included the surrounding region, southwestern Fujian and eastern Guangdong to the southwest, Hubei, Hunan and Jiangxi to the northwest, the East China Sea and the South China Sea. Of the nine synoptic circulation patterns, three cyclone-related patterns were associated with low BC concentrations and small biomass burning (BCbb) contributions. Of the six anticyclone-related patterns, the three cold-high circulations around winter were associated with moderate BC concentrations and large BCbb contributions. The two cold-high patterns in spring and autumn were associated with high BC concentrations and small BCbb contributions, while the warm-high pattern was associated with moderate BC concentration and small BCbb contribution. The findings provide insights into the transport mechanisms of BC with the impacts of synoptic pattern in China.

Aerosol light absorption in a coastal city in Southeast China: Temporal variations and implications for brown carbon.

Light-absorbing carbonaceous aerosols including black carbon (BC) and brown carbon (BrC) play significant roles in atmospheric radiative properties. One-year measurements of aerosol light absorption at multi-wavelength were continuously conducted in Xiamen, southeast of China in 2014 to determine the light absorption properties including absorption coefficients (σabs) and absorption Ångström exponent (AAE) in the coastal city. Light absorptions of BC and BrC with their contributions to total light absorption were further quantified. Mean σabs at 370 nm and 880 nm were 56.6 ±â€¯34.3 and 16.5 ±â€¯11.2 Mm-1, respectively. σabs presented a double-peaks diurnal pattern with the maximum in the morning and the minimum in the afternoon. σabs was low in warm seasons and high in cold seasons. AAE ranged from 0.26 to 2.58 with the annual mean of 1.46, implying that both fossil fuel combustion and biomass burning influenced aerosol optical properties. σabs of BrC at 370 nm was 24.0 ±â€¯5.7 Mm-1, contributing 42% to the total absorption. The highest AAE (1.52 ±â€¯0.02) and largest BrC contributions (47% ±â€¯4%) in winter suggested the significant influence of biomass burning on aerosol light absorption. Long-distance air masses passing through North China Plain and the Yangtze River Delta led to high AAE and BrC contributions. High AAE value of 1.46 in July indicated that long-range transport of the air pollutants from intense biomass burning in Southeast Asia would affect aerosol light absorption in Southeast China. The study will improve the understanding of light absorption properties of aerosols and the optical impacts of BrC in China.