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During the 2017 summertime Arctic cruise observation campaigns, we measured over 290,000 individual submicron particles and clustered them into two inorganic classes (dominated by sea salt, accounting for 38.6% by number fraction) and five organic classes (dominated by natural and anthropogenic organics, 61.4%), presenting a distinct difference in geographic distribution. In the high Arctic and marginal ice zone (81.1–84.6°N) compared with the low Arctic (Chukchi Sea, Svalbard, and Iceland, <80°N), ocean‐derived organic aerosols were more prevalent (73.6% vs. 37.1%). Specifically, we found sharp contrasts in the geographic distributions of OC‐Ca (organics internally mixed with calcium, 29.0% vs. 9.4%) and OC‐S (organics internally mixed with sulfate, 3.2% vs. 21.4%). Utilizing an explainable machine learning technique, we inferred that OC‐Ca was driven by wind‐blown sea ice and/or sea ice floes and/or bubble bursting within sea ice leads under low wind speed conditions in the high Arctic, while OC‐S tended to associate with elemental carbon, sulfate, and higher temperatures, potentially originating from combustion emissions at low latitude regions. Plain Language Summary: Knowledge of the mixing state of individual particles is essential for elucidating their sources, formation mechanisms, atmospheric processes, and assessing their climate effect in the Arctic atmosphere. Here, we investigated the origins and geographic distribution of organic aerosol types using a single‐particle aerosol mass spectrometer during the 8th Chinese Arctic Expedition Research Cruise (Chinese Research Vessel Xuelong) in the summertime over the Arctic Ocean. According to the mixing state, individual organic particles were classified into several ocean‐derived and anthropogenic types. Ocean‐derived types were prevalent in the high Arctic compared with that of anthropogenic type in the low Arctic, and their driven factors were different. Specifically, sea ice fraction was the most important driver for the generation of ocean‐derived OC‐Ca (an aerosol type of organics internally mixed with calcium). OC‐S (an aerosol type of organics internally mixed with sulfate) substantially increased in the low Arctic, most probably driven by combustion sources. Key Points: Submicron organic aerosol types show distinct geographic distributions in the summertime ArcticHigher number fraction of ocean‐derived submicron organic aerosols is observed in the high Arctic than the low ArcticThe proportion of sea ice coverage is a determining factor contributing to the spatial variability of OC‐Ca number fractions. [ABSTRACT FROM AUTHOR]

While aqueous-phase processing is known to contribute to the formation of nitrogen-containing organic compounds (NOCs), the specific pathways involved remain poorly understood. In this study, we aimed to characterize the NOCs present in both pre-fog aerosols and fog water collected at a suburban site in northern China. Fourier-transform ion cyclotron resonance mass spectrometry was utilized to analyze the molecular composition of NOCs in both negative and positive modes of electrospray ionization (ESI - and ESI +). In both pre-fog aerosols and fog water samples, NOCs constituted a significant portion, accounting for over 60 % of all assigned formulas in ESI - and more than 80 % in ESI +. By comparing the molecular composition of NOCs originating from biomass burning, coal combustion, and vehicle emissions, we identified that 72.3 % of NOCs in pre-fog aerosols were attributed to primary anthropogenic sources (pNOCs), while the remaining NOCs were categorized as secondary NOCs formed within the aerosols (saNOCs). Unique NOCs found in fog water were classified as secondary NOCs formed within the fog water (sfNOCs). Through a comprehensive "precursor–product pair" screening involving 39 reaction pathways, we observed that the nitration reaction, the amine pathway, and the intramolecular N-heterocycle pathway of NH 3 addition reactions contributed 43.6 %, 22.1 %, and 11.6 % of saNOCs, respectively. In contrast, these pathways contributed 26.8 %, 28.4 %, and 29.7 % of sfNOCs, respectively. This disparity in formation pathways is likely influenced by the diverse precursors, the aqueous acidity, and the gas-phase species partitioning. Correspondingly, saNOCs were found to contain a higher abundance of carbohydrate-like and highly oxygenated compounds with two nitrogen atoms compared to pNOCs. Conversely, sfNOCs exhibited a higher content of lipid-like compounds with fewer oxygen atoms. These results underscore the distinct secondary processes contributing to the diversity of NOCs in aerosols and fog water, which may lead to their different climate effects. [ABSTRACT FROM AUTHOR]

Although calcium is known to be enriched in sea spray aerosols (SSAs), the factors that affect its enrichment remain ambiguous. In this study, we examine how environmental factors affect the distribution of water-soluble calcium (Ca 2+) distribution in SSAs. We obtained our dataset from observations taken during the R/V Xuelong research cruise in the Ross Sea, Antarctica, from December 2017 to February 2018. Our observations showed that the enrichment of Ca 2+ in aerosol samples was enhanced under specific conditions, including lower temperatures (<-3.5 ∘ C), lower wind speeds (<7 m s -1), and the presence of sea ice. Our analysis of individual particle mass spectra revealed that a significant portion of calcium in SSAs was likely bound with organic matter (in the form of a single-particle type, OC-Ca, internally mixed organics with calcium). Our findings suggest that current estimations of Ca 2+ enrichment based solely on water-soluble Ca 2+ may be inaccurate. Our study is the first to observe a single-particle type dominated by calcium in the Antarctic atmosphere. Our findings suggest that future Antarctic atmospheric modeling should take into account the environmental behavior of individual OC-Ca particles. With the ongoing global warming and retreat of sea ice, it is essential to understand the mechanisms of calcium enrichment and the mixing state of individual particles to better comprehend the interactions between aerosols, clouds, and climate during the Antarctic summer. [ABSTRACT FROM AUTHOR]

Calcium is known to be enriched in sea spray aerosols (SSA), but its controlling factors and individual mixing states remain ambiguous. Here, we investigate the impact of various environmental factors on the water-soluble calcium (Ca2+) distribution in SSA through R/V Xuelong cruise observations over the Ross Sea, Antarctica, from December 2017 to February 2018. We observed enhanced Ca2+ enrichment in aerosol samples at lower temperatures (< -3.5 °C), lower wind speeds (< 7 m s-1) and in the presence of sea ice. Further individual particle mass spectral analysis indicated that considerable fractions of calcium in SSA likely bind with organic matter (a single-particle type, OC-Ca), which may be neglected in current water-soluble estimation of Ca2+ enrichment. Also, this is the first time that a calcium-dominated single-particle type has been observed in the Antarctic atmosphere. We suggest that a broader focus on individual OC-Ca and its subsequent environmental behavior should be included in future Antarctic atmospheric modeling. Given the context of global warming and sea ice retreat, an understanding of the mechanisms of calcium enrichment and mixing state of individual particles involved is valuable for further recognizing the aerosol-cloud-climate interactions in the Antarctica summer. [ABSTRACT FROM AUTHOR]

Atmospheric brown carbon (BrC) makes a substantial contribution to aerosol light-absorbing and thus the global radiative forcing. Although BrC may change the lifetime of the cloud and ultimately affect precipitation, little is known regarding the optical properties and formation of BrC in the cloud. In the present study, the light-absorption properties of cloud droplet residual (cloud RES) were measured by coupled a ground-based counterflow virtual impactor (GCVI) and an Aethalometer (AE-33), in addition to the cloud interstitial (cloud INT) and ambient (cloud-free) particles by PM2.5 inlet-AE-33, at Mt. Tianjing (1690 m a.s.l.), a remote mountain site in southern China, from November to December 2020. Meanwhile, the light-absorption and fluorescence properties of water-soluble organic carbon (WSOC) in the collected cloud water and PM2.5 samples were also obtained, associated with the concentration of water-soluble ions. The mean light-absorption coefficient (Abs370) of the cloud RES, cloud INT, and cloud-free particles were 0.25 ± 0.15, 1.16 ± 1.14, and 1.47 ± 1.23 Mm−1, respectively. The Abs365 of WSOC was 0.11 ± 0.08 Mm−1 in cloud water and 0.40 ± 0.31 Mm−1 in PM2.5, and the corresponding mass absorption efficiency (MAE365) was 0.17 ± 0.07 and 0.31 ± 0.21 m2·g−1, respectively. A comparison of the light-absorption coefficient between BrC in the cloud RES/cloud INT and WSOC in cloud water/PM2.5 indicates a considerable contribution (48-75 %) of water-insoluble BrC to total BrC light-absorption. Secondary BrC estimated by minimum R squared (MRS) method dominated the total BrC in cloud RES (67-85 %), rather than in the cloud-free (11-16 %) and cloud INT (9-23 %) particles. It may indicate the formation of secondary BrC during cloud processing. Supporting evidence includes the enhanced WSOC and dominant contribution of secondary formation/biomass burning factor (> 80 %) to Abs365 in cloud water provided by Positive Matrix Factorization (PMF) analysis. In addition, we showed that the light-absorption of BrC in cloud water was closely related to humic-like substances and tyrosine/proteins-like substances (r > 0.63, p < 0.01), whereas only humic-like substances for PM2.5, as identified by excitation-emission matrix fluorescence spectroscopy. [ABSTRACT FROM AUTHOR]

Corona virus disease 2019 (COVID-19) has exerted a profound adverse impact on human health. Studies have demonstrated that aerosol transmission is one of the major transmission routes of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). Pathogenic microorganisms such as SARS-CoV-2 can survive in the air and cause widespread infection among people. Early monitoring of pathogenic microorganism transmission in the atmosphere and accurate epidemic prediction are the frontier guarantee for preventing large-scale epidemic outbreaks. Monitoring of pathogenic microorganisms in the air, especially in densely populated areas, may raise the possibility to detect viruses before people are widely infected and contain the epidemic at an earlier stage. The multi-scale coupled accurate epidemic prediction system can provide support for governments to analyze the epidemic situation, allocate health resources, and formulate epidemic response policies. This review first elaborates on the effects of the atmospheric environment on pathogenic microorganism transmission, which lays a theoretical foundation for the monitoring and prediction of epidemic development. Secondly, the monitoring technique development and the necessity of monitoring pathogenic microorganisms in the atmosphere are summarized and emphasized. Subsequently, this review introduces the major epidemic prediction methods and highlights the significance to realize a multi-scale coupled epidemic prediction system by strengthening the multidisciplinary cooperation of epidemiology, atmospheric sciences, environmental sciences, sociology, demography, etc. By summarizing the achievements and challenges in monitoring and prediction of pathogenic microorganism transmission in the atmosphere, this review proposes suggestions for epidemic response, namely, the establishment of an integrated monitoring and prediction platform for pathogenic microorganism transmission in the atmosphere., Competing Interests: The authors declare that they have no conflicts of interest in this work., (© 2023 The Authors. Publishing Services by Elsevier B.V. on behalf of KeAi Communications Co. Ltd.)

Vehicle emissions are an important source of nitrated aromatic compounds (NACs) in particulate size smaller 2.5 μm (PM 2.5 ), which adversely affect human health and biodiversity, especially in urban areas. In this study, filter-based PM 2.5 samples were collected during October 14-19, 2019, in a busy urban tunnel (approximately 35,000 vehicles per day) in south China to identify PM 2.5 -bound NACs. Among them, 2,8-dinitrodibenzothiophene, 3-nitrodibenzofuran and 2-nitrodibenzothiophene were the most abundant nitrated polycyclic aromatic hydrocarbons (NPAHs), while 2-methyl-4-nitrophenol, 2,4-dinitrophenol, 3-methyl-4-nitrophenol and 4-nitrophenol were the most abundant nitrophenols (NPs). The observed mean fleet emission factors (EFs) of NPAHs and NPs were 2.2 ± 2.1 and 7.7 ± 4.1 μg km -1 , and were 2.9 ± 2.7 and 10.2 ± 5.4 μg km -1 if excluding electric and liquefied petroleum gas vehicles, respectively. Regression analysis revealed that diesel vehicles (DVs) had NPAH-EFs (55.3 ± 5.3 μg km -1 ) approximately 180 times higher than gasoline vehicles (GVs) (0.3 ± 0.2 μg km -1 ), and NP-EFs (120.6 ± 25.8 μg km -1 ) approximately 30 times higher than GVs (4.1 ± 0.2 μg km -1 ), and thus 89% NPAH emissions and 56% NP emissions from the onroad fleets were contributed by DVs although DVs only accounted for 3.3% in the fleets. Methanol solution-based light absorption measurements demonstrated that the mean incremental light absorption for methanol-soluble brown carbon at 365 nm was 6.8 ± 2.2 Mm -1 , of which the 44 detected NACs only contributed about 1%. The mean EF of the 7 toxic NACs was approximately 3% that of the 16 priority PAHs; However, their benzo(a)pyrene toxic equivalence quotients (TEQ BaP ) could reach over 25% that of the PAHs. Moreover, 6-nitrochrysene mainly from DVs contributed 93% of the total TEQ BaP of the NACs. This study demonstrated that enhancing DV emission control in urban areas could benefit the reduction of exposure to air toxins such as 6-nitrochrysene., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier Ltd. All rights reserved.)