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Atmospheric models of secondary organic aerosol (OA) (SOA) typically rely on parameters derived from environmental chambers. Chambers are subject to experimental artifacts, including losses of (1) particles to the walls (PWL), (2) vapors to the particles on the wall (V2PWL), and (3) vapors to the wall directly (VWL). We present a method for deriving artifact-corrected SOA parameters and translating these to volatility basis set (VBS) parameters for use in chemical transport models (CTMs). Our process involves combining a box model that accounts for chamber artifacts (Statistical Oxidation Model with a TwO-Moment Aerosol Sectional model (SOM-TOMAS)) with a pseudo-atmospheric simulation to develop VBS parameters that are fit across a range of OA mass concentrations. We found that VWL led to the highest percentage change in chamber SOA mass yields (high NO

Condensable particulate matter (CPM) emitted from stationary combustion and mobile sources exhibits high emissions and a large proportion of organic components. However, CPM is not generally measured when conducting emission surveys of PM in most countries, including China. Consequently, previous emission inventories have not included emission rates for CPM. Here, we construct an emission inventory of CPM in China with a focus on organic aerosols (OAs) based on collected CPM emission information. Results show that OA emissions are enhanced twofold after the inclusion of CPM in a new inventory for China for the years 2014 and 2017. Considering organic CPM emissions and model representations of secondary OA (SOA) formation from CPM, a series of sensitivity cases have been simulated here using the three-dimensional Community Multiscale Air Quality (CMAQ) model to estimate the contributions of CPM emissions to atmospheric OA and fine PM (PM2.5, particulate matter with aerodynamic diameter not exceeding 2.5 µm) concentrations in China. Compared with observations at a Beijing site during a haze episode from 14 October to 14 November 2014, estimates of the temporal average primary OA (POA) and SOA concentrations were greatly improved after including the CPM effects. These scenarios demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to the POA (51 %–85 %​​​​​​​), SOA (42 %–58 %), and total OA concentrations (45 %–75 %). Furthermore, the contributions of CPM emissions to total OA concentrations were demonstrated over the 2 major cities and 26 other cities of the Beijing–Tianjin–Hebei region (hereafter referred to as the “BTH2 + 26 cities”) in December 2018, with average contributions of up to 49 %, 53 %, 54 %, and 50 % for Handan, Shijiazhuang, Xingtai, and Dezhou, respectively. Correspondingly, the inclusion of CPM emissions also narrowed the gap between simulated and observed PM2.5 concentrations over the BTH2 + 26 cities. These results improve the simulation performance of atmospheric OA and PM2.5 and may also provide important implications for the sources of OA.

Atmospheric simulation chambers continue to be indispensable tools for research in the atmospheric sciences. Insights from chamber studies are integrated into atmospheric chemical transport models, which are used for science-informed policy decisions. However, a centralized data management and access infrastructure for their scientific products had not been available in the United States and many parts of the world. ICARUS (Integrated Chamber Atmospheric data Repository for Unified Science) is an open access, searchable, web-based infrastructure for storing, sharing, discovering, and utilizing atmospheric chamber data [https://icarus.ucdavis.edu]. ICARUS has two parts: a data intake portal and a search and discovery portal. Data in ICARUS are curated, uniform, interactive, indexed on popular search engines, mirrored by other repositories, version-tracked, vocabulary-controlled, and citable. ICARUS hosts both legacy data and new data in compliance with open access data mandates. Targeted data discovery is available based on key experimental parameters, including organic reactants and mixtures that are managed using the PubChem chemical database, oxidant information, nitrogen oxide (NOx) content, alkylperoxy radical (RO₂) fate, seed particle information, environmental conditions, and reaction categories. A discipline-specific repository such as ICARUS with high amounts of metadata works to support the evaluation and revision of atmospheric model mechanisms, intercomparison of data and models, and the development of new model frameworks that can have more predictive power in the current and future atmosphere. The open accessibility and interactive nature of ICARUS data may also be useful for teaching, data mining, and training machine learning models.

The global methane pledge paves a fresh, critical way toward carbon neutrality. However, it remains largely invisible and highly controversial due to the fact that planet-scale and plant-level methane retrievals have rarely been coordinated. This has never been more essential within the narrow window to reach the Paris target. Here we present a two-tiered spaceborne architecture to address this issue. Using this framework, we focused on the United States, China, the Middle East, and North Africa, and simultaneously uncovered methane-abundant regions and plumes. These include new super-emitters, potential leakages, and unprecedented multiple plumes in a single source. More importantly, this framework is shown to challenge official emission reports that possibly mislead estimates from global, regional, and site scales, particularly by missing super-emitters. Our results show that, in principle, the above framework can be extended to be multi-tiered by adding upcoming stereoscopic measurements and suitable artificial intelligence, and thus it is sufficiently versatile for immediate and future monitoring of the global methane pledge.

This study describes a modeling framework, model evaluation, and source apportionment to understand the causes of Los Angeles (LA) air pollution. A few major updates are applied to the Community Multiscale Air Quality (CMAQ) Model with high spatial resolution (1 km × 1 km). The updates include dynamic traffic emissions based on real-time on-road information and recent emission factors and secondary organic aerosol (SOA) schemes to represent volatile chemical products (VCP). Meteorology is well-predicted compared to ground-based observations, and the emission rates from multiple sources (i.e., on-road, volatile chemical product, area, point, biogenic, and sea spray) are quantified. Evaluation of the CMAQ model shows that ozone is well-predicted despite inaccuracies in nitrogen oxide (NOx) predictions. Particle matter (PM) is underpredicted compared to concurrent measurements made with an aerosol mass spectrometer (AMS) in Pasadena. Inorganic aerosol is well-predicted while SOA is underpredicted. Modeled SOA consists of mostly organic nitrates and products from oxidation of alkane-like intermediate volatility organic compounds (IVOCs) and has missing components that behave like less-oxidized oxygenated organic aerosol (LO-OOA). Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated (VOC-sensitive) with the largest sensitivity of O3 to changes in VOCs in the urban core. Differing oxidative capacities in different regions impact the nonlinear chemistry leading to PM and SOA formation, which is quantified in this study.

The San Joaquin Valley is an agricultural region in California that suffers from poor air quality. Since traffic emissions are decreasing, other sources of volatile organic compounds (VOCs) are gaining importance in the formation of secondary air pollutants. Using airborne eddy covariance, we conducted direct, spatially resolved flux observations of a wide range of VOCs in the San Joaquin Valley during June 2021 at 23–36 °C. Through landcover-informed footprint disaggregation, we were able to attribute emissions to sources and identify tracers for distinct source types. VOC mass fluxes were dominated by alcohols, mainly from dairy farms, while oak isoprene and citrus monoterpenes were important sources of reactivity. Comparisons with two commonly used inventories showed that isoprene emissions in the croplands were overestimated, while dairy and highway VOC emissions were generally underestimated in the inventories, and important citrus and biofuel VOC point sources were missing from the inventories. This study thus presents unprecedented insights into the VOC sources in an intensive agricultural region and provides much needed information for the improvement of inventories, air quality predictions and regulations.

Nitrogen oxides (NOx ≡ NO + NO2) are involved in most atmospheric photochemistry, including the formation of tropospheric ozone (O3). While various methods exist to accurately measure NOx concentrations, it is still a challenge to quantify the source and flux of NOx emissions. We present airborne measurements of NOx and winds used to infer the emission of NOx across Los Angeles. The measurements were obtained during the research aircraft campaign RECAP-CA (Re-Evaluating the Chemistry of Air Pollutants in CAlifornia) in June 2021. Geographic allocations of the fluxes are compared to the NOx emission inventory from the California Air Resources Board (CARB). We find that the NOx fluxes have a pronounced weekend effect and are highest in the Eastern part of the San Bernardino valley. The comparison of the RECAP-CA and the modeled CARB NOx fluxes suggest the modeled emissions are too high near the coast and in downtown Los Angeles and too low further inland in the Eastern part of the San Bernardino valley.

Decamethylcyclopentasiloxane (D5, C10H30O5Si5) is measured at parts per trillion (ppt) levels outdoors and parts per billion (ppb) levels indoors. Primarily used in personal care products, its outdoor concentration is correlated to population density. Since understanding the aerosol formation potential of volatile chemical products is critical to understanding particulate matter in urban areas, the secondary organic aerosol yield of D5 was studied under a wide range of OH concentrations and, correspondingly, OH exposures using both batch-mode chamber and continuously run flow tube experiments. These results were comprehensively analyzed and compared to two other secondary organic aerosol (SOA) yield datasets from literature. It was found that the SOA yield from the oxidation of D5 is extremely dependent on either the OH concentration or exposure. For OH concentrations of ≲ 107 molec.cm-3 or OH exposures of ≲ 2 × 1011 molec.scm-3, the SOA yield is largely < 5 % and usually ∼ 1 %. This is significantly lower than SOA yields previously reported. Using a two-product absorptive partitioning model for the upper bound SOA yields, the stoichiometric mass fraction and absorptive partitioning coefficients are, for the first product, α1 = 0.056 and KOM,1 = 0.022 m3 µg−1; for the second product, they are α2 = 7.7 and KOM,2 = 4.3 × 10−5 m3 µg−1. Generally, there are high SOA yields (> 90 %) at OH mixing ratios of 5 × 109 molec.cm-3 or OH exposures above 1012 molec.scm-3.

Nitrogen oxides (NOx) are principle components of air pollution and serve as important ozone precursors. As the San Joaquin Valley (SJV) experiences some of the worst air quality in the United States, reducing NOx emissions is a pressing need, yet quantifying current emissions is complicated due to a mixture of mobile and agriculture sources. We performed airborne eddy covariance flux measurements during the Re-Evaluating the Chemistry of Air Pollutants in CAlifornia (RECAP-CA) field campaign in June 2021. Combining footprint calculations and land cover statistics, we disaggregate the observed fluxes into component fluxes characterized by three different land cover types. On average we find emissions of 2.95 mg m-2 h-1 over highways, 1.24 mg m-2 h-1 over urban areas and 0.79 mg m-2 h-1 over croplands. The calculated NOx emissions using flux observations are utilized to evaluate anthropogenic emission inventories and soil NOx emission schemes. We show that two anthropogenic inventories for mobile sources, EMFAC (EMssion FACtor) and FIVE (Fuel-based Inventory for Vehicle Emissions), yield similar agreement with emissions derived from measured fluxes over urban regions with 24 % and 22 % low bias, respectively. Three soil NOx schemes, including MEGAN v3 (Model of Emissions of Gases and Aerosols from Nature), BEIS v3.14 (Biogenic Emission Inventory System) and BDISNP (Berkeley Dalhousie Iowa Soil NO Parameterization), show substantial underestimates over the study domain. Compared to the cultivated soil NOx emissions derived from measured fluxes, MEGAN and BEIS are lower by more than one order of magnitude and BDISNP is lower by a factor of 2.7. Despite the low bias, observed soil NOx emissions and BDISNP present a similar spatial pattern as well as temperature dependence. We conclude that soil NOx is a key feature of the NOx emissions in the SJV and that a state-of-the-science model of these emissions is needed to simulate emissions for modeling air quality in the region.

Urban on-road vehicle emissions affect air quality and human health locally and globally. Given uneven sources, they typically exhibit distinct spatial heterogeneity, varying sharply over short distances (10 m–1 km). However, all-around observational constraints on the emission sources are limited in much of the world. Consequently, traditional emission inventories lack the spatial resolution that can characterize the on-road vehicle emission hotspots. Here we establish a bottom-up approach to reveal a unique pattern of urban on-road vehicle emissions at a spatial resolution 1–3 orders of magnitude higher than current emission inventories. We interconnect all-around traffic monitoring (including traffic fluxes, vehicle-specific categories, and speeds) via an intelligent transportation system (ITS) over Xiaoshan District in the Yangtze River Delta (YRD) region. This enables us to calculate single-vehicle-specific emissions over each fine-scale (10 m–1 km) road segment. Thus, the most hyperfine emission dataset of its type is achieved, and on-road emission hotspots appear. The resulting map shows that the hourly average on-road vehicle emissions of CO, NOx, HC, and PM2.5 are 74.01, 40.35, 8.13, and 1.68 kg, respectively. More importantly, widespread and persistent emission hotspots emerged. They are of significantly sharp small-scale variability, up to 8–15 times within individual hotspots, attributable to distinct traffic fluxes, road conditions, and vehicle categories. On this basis, we investigate the effectiveness of routine traffic control strategies on on-road vehicle emission mitigation. Our results have important implications for how the strategies should be designed and optimized. Integrating our traffic-monitoring-based approach with urban air quality measurements, we could address major data gaps between urban air pollutant emissions and concentrations.

Light-duty gasoline vehicles (LDGVs) have made up >90 % of vehicle fleets in China since 2019, moreover, with a high annual growth rate (> 10 %) since 2017. Hence, accurate estimates of air pollutant emissions of these fast-changing LDGVs are vital for air quality management, human healthcare, and ecological protection. However, this issue is poorly quantified due to insufficient reserves of timely updated LDGV emission factors, which are dependent on real-world activity levels. Here we constructed a big dataset of explicit emission profiles (e.g., emission factors and accumulated mileages) for 159,051 LDGVs based on an official I/M database by matching real-time traffic dynamics via real-world traffic monitoring (e.g., traffic volumes and speeds). Consequently, we provide robust evidence that the emission factors of these LDGVs follow a clear heavy-tailed distribution. The top 10 % emitters contributed >60 % to the total fleet emissions, while the bottom 50 % contributed 50 km/h). These empirical analyses enabled us to propose future traffic scenarios that could harmonize emission standards and traffic congestion. Practical approaches on vehicle emission controls under realistic conditions are proposed, which would provide new insights for future urban vehicle emission management.

Increased wildfire events constitute a significant threat to life and property in the United States. Wildfire impact on severe storms and weather hazards is another pathway that threatens society, and our understanding of which is very limited. Here, we use unique modeling developments to explore the effects of wildfires in the western US (mainly California and Oregon) on precipitation and hail in the central US. We find that the western US wildfires notably increase the occurrences of heavy precipitation rates by 38% and significant severe hail (≥2 in.) by 34% in the central United States. Both heat and aerosols from wildfires play an important role. By enhancing surface high pressure and increasing westerly and southwesterly winds, wildfires in the western United States produce (1) stronger moisture and aerosol transport to the central United States and (2) larger wind shear and storm-relative helicity in the central United States. Both the meteorological environment more conducive to severe convective storms and increased aerosols contribute to the enhancements of heavy precipitation rates and large hail. Moreover, the local wildfires in the central US also enhance the severity of storms, but their impact is notably smaller than the impact of remote wildfires in California and Oregon because of the lessened severity of the local wildfires. As wildfires are projected to be more frequent and severe in a warmer climate, the influence of wildfires on severe weather in downwind regions may become increasingly important.

International audience; Rising air pollution by surface ozone (O 3) in China has induced extensive efforts to control ozone generation in major urban and industrial areas, yet mechanisms ruling the ozone production and loss are not well understood. In particular, ozone levels are strongly influenced by meteorological factors such as relative humidity, but this has been explored only in local situations, and the effect of relative humidity on ozone levels in warm seasons on a large scale in China is still unknown. Here we studied surface ozone, relative humidity, temperature, and other meteorological variables in 74 major cities in China during 2017-2018, focusing on the warm seasons in seven regions. Results show that ozone levels decrease with increasing relative humidity in all cities, with an average correlation coefficient of − 0.58, ranging from − 0.17 in Zhangjiakou to − 0.84 in Hengshui. At high relative humidity levels, above 75%, average ozone levels ranged from 44.6 to 122.5 μg m −3 , which is lower than Chinese quality threshold of hourly average ozone level of 200 μg m −3. The decreases of ozone with relative humidity were more pronounced at high temperature, above 30 °C, than below 25 °C. The increases of ozone with temperature were more pronounced at low relative humidity, below 40%. Overall, our findings reveal that mechanisms ruling surface ozone levels are similar on a large scale. This is promising to design common methods of climate engineering to protect human health.

Summary Transportation contributes to around one-fifth of global greenhouse gas emissions, while also causing severe air pollution. The conversion to electric vehicles (EVs) represents a major path to decarbonize the transport sector, with potentially significant co-benefits for human health. However, the scale of such co-benefits largely remains an empirical question and lacks observational evidence. The full lockdown in China during the coronavirus disease 2019 (COVID-19) pandemic provides an unprecedented real-world experiment to evaluate emission reduction potentials of a large-scale transition to EVs. Here, we utilize ground and satellite observations of air quality during the full lockdown to constrain predictions of a comprehensive chemical transport model and find that the substantial traffic reductions are near-linearly linked to reductions of PM2.5 (particles with an aerodynamic diameter ≤2.5 μm) and NO2. A further extrapolation of a full conversion to EVs shows a significant reduction of PM2.5 (30%–70%) and NO2 (30%–80%) in most of China. Our findings provide fact-based evidence of potential environmental benefits generated by fully switching to EVs.

Photooxidation of volatile organic compounds (VOCs) produces secondary organic aerosol (SOA) and light-absorbing brown carbon (BrC) via multiple reaction steps/pathways, reflecting significant chemical complexity relevant to gaseous oxidation and subsequent gas-to-particle conversion. Toluene is an important VOC under urban conditions, but the fundamental chemical mechanism leading to SOA formation remains uncertain. Here, we elucidate multigeneration SOA production from toluene by simultaneously tracking the evolutions of gas-phase oxidation and aerosol formation in a reaction chamber. Large size increase and browning of monodisperse sub-micrometer seed particles occur shortly after initiating oxidation by hydroxyl radical (OH) at 10–90% relative humidity (RH). The evolution in gaseous products and aerosol properties (size/density/optical properties) and chemical speciation of aerosol-phase products indicate that the aerosol growth and browning result from earlier generation products consisting dominantly of dicarbonyl and carboxylic functional groups. While volatile dicarbonyls engage in aqueous reactions to yield nonvolatile oligomers and light-absorbing nitrogen heterocycles/heterochains (in the presence of NH₃) at high RH, organic acids contribute to aerosol carboxylates via ionic dissociation or acid–base reaction in a wide RH range. We conclude that toluene contributes importantly to SOA/BrC formation from dicarbonyls and organic acids because of their prompt and high yields from photooxidation and unique functionalities for participation in aerosol-phase reactions.

The gas-phase formation of new particles less than 1 nm in size and their subsequent growth significantly alters the availability of cloud condensation nuclei (CCN, >30–50 nm), leading to impacts on cloud reflectance and the global radiative budget. However, this growth cannot be accounted for by condensation of typical species driving the initial nucleation. Here, we present evidence that nucleated iodine oxide clusters provide unique sites for the accelerated growth of organic vapors to overcome the coagulation sink. Heterogeneous reactions form low-volatility organic acids and alkylaminium salts in the particle phase, while further oligomerization of small α-dicarbonyls (e.g., glyoxal) drives the particle growth. This identified heterogeneous mechanism explains the occurrence of particle production events at organic vapor concentrations almost an order of magnitude lower than those required for growth via condensation alone. A notable fraction of iodine associated with these growing particles is recycled back into the gas phase, suggesting an effective transport mechanism for iodine to remote regions, acting as a “catalyst” for nucleation and subsequent new particle production in marine air.

Large amounts of small α-dicarbonyls (glyoxal and methylglyoxal) are produced in the atmosphere from photochemical oxidation of biogenic isoprene and anthropogenic aromatics, but the fundamental mechanisms leading to secondary organic aerosol (SOA) and brown carbon (BrC) formation remain elusive. Methylglyoxal is commonly believed to be less reactive than glyoxal because of unreactive methyl substitution, and available laboratory measurements showed negligible aerosol growth from methylglyoxal. Herein, we present experimental results to demonstrate striking oligomerization of small α-dicarbonyls leading to SOA and BrC formation on sub-micrometer aerosols. Significantly more efficient growth and browning of aerosols occur upon exposure to methylglyoxal than glyoxal under atmospherically relevant concentrations and in the absence/presence of gas-phase ammonia and formaldehyde, and nonvolatile oligomers and light-absorbing nitrogen-heterocycles are identified as the dominant particle-phase products. The distinct aerosol growth and light absorption are attributed to carbenium ion-mediated nucleophilic addition, interfacial electric field-induced attraction, and synergetic oligomerization involving organic/inorganic species, leading to surface- or volume-limited reactions that are dependent on the reactivity and gaseous concentrations. Our findings resolve an outstanding discrepancy concerning the multiphase chemistry of small α-dicarbonyls and unravel a new avenue for SOA and BrC formation from atmospherically abundant, ubiquitous carbonyls and ammonia/ammonium sulfate.

Nitrogen oxides (NO

Secondary organic aerosols (SOA) constitute an important fraction of fine-mode atmospheric aerosol mass. Frameworks used to develop SOA parameters from laboratory experiments and subsequently used to simulate SOA formation in atmospheric models make many simplifying assumptions about the processes that lead to SOA formation in the interest of computational efficiency. These assumptions can limit the ability of the model to predict the mass, composition, and properties of SOA accurately. In this work, we developed a computationally efficient, process-level model named simpleSOM to represent the chemistry, thermodynamic properties, and microphysics of SOA. simpleSOM simulates multigenerational gas-phase chemistry, phase-state-influenced kinetic gas/particle partitioning, heterogeneous chemistry, oligomerization reactions, and vapor losses to the walls of Teflon chambers. As a case study, we used simpleSOM to simulate SOA formation from the photooxidation of α-pinene. This was done to demonstrate the ability of the model to develop parameters that can reproduce environmental chamber data, to highlight the chemical and microphysical processes within simpleSOM, and discuss implications for SOA formation in chambers and in the real atmosphere. SOA parameters developed from experiments performed in the chamber at the California Institute of Technology (Caltech) reproduced observations of SOA mass yield, O : C, and volatility distribution gathered from other experiments. Sensitivity simulations suggested that multigenerational gas-phase aging contributed to nearly half of all SOA and that in the absence of vapor wall losses, SOA production in the Caltech chamber could be nearly 50% higher. Heterogeneous chemistry did not seem to affect SOA formation over the short timescales for oxidation experienced in the chamber experiments. Simulations performed under atmospherically relevant conditions indicated that the SOA mass yields were sensitive to whether and how oligomerization reactions and the particle phase state were represented in the chamber experiment from which the parameters were developed. simpleSOM provides a comprehensive, process-based framework to consistently model the SOA formation and evolution in box and 3D models.

Ambient fine particulate matter (PM2.5) mitigation relies strongly on anthropogenic emission control measures, the actual effectiveness of which is challenging to pinpoint owing to the complex synergies between anthropogenic emissions and meteorology. Here, observational constraints on model simulations allow us to derive not only reliable PM2.5 evolution but also accurate meteorological fields. In this study, we isolate meteorological factors to achieve reliable estimates of surface PM2.5 responses to both long-term and emergency emission control measures from 2016 to 2019 over the Yangtze River Delta (YRD), China. The results show that long-term emission control strategies play a crucial role in curbing PM2.5 levels (> 14 μg/m3, 19 %), especially in the megacities and other areas with abundant anthropogenic emissions. The G20 summit hosted in Hangzhou in 2016 provides a unique and ideal opportunity involving the most stringent, even unsustainable, emergency emission control measures. For the winter time periods from 2016 to 2019, the most substantial declines in PM2.5 concentrations (~ 35 μg/m3, ~ 59 %) are thus achieved in Hangzhou and its surrounding areas. The following hotspots also emerge in megacities, especially in Shanghai (32 μg/m3, 51 %), Nanjing (27 μg/m3, 55 %), and Hefei (24 μg/m3, 44 %). Compared to the long-term policies from 2016 to 2019, the emergency emission control measures implemented during the G20 Summit achieve more significant decreases in PM2.5 concentrations (17 μg/m3 and 41 %) over most of the whole domain, especially in Hangzhou (24 μg/m3, 48 %) and Shanghai (21 μg/m3, 45 %). By extrapolation, we derive insight into the magnitude and spatial distributions of PM2.5 mitigation potentials across the YRD, revealing significantly additional rooms for curbing PM2.5 levels.

Secondary organic aerosol (SOA) data gathered in environmental chambers (ECs) have been used extensively to develop parameters to represent SOA formation and evolution. The EC-based parameters are usually constrained to less than one day of photochemical aging but extrapolated to predict SOA aging over much longer timescales in atmospheric models. Recently, SOA has been increasingly studied in oxidation flow reactors (OFRs) over aging timescales of one to multiple days. However, these OFR data have been rarely used to validate or update the EC-based parameters. The simultaneous use of EC and OFR data is challenging because the processes relevant to SOA formation and evolution proceed over very different timescales, and both reactor types exhibit distinct experimental artifacts. In this work, we show that a kinetic SOA chemistry and microphysics model that accounts for various processes, including wall losses, aerosol phase state, heterogeneous oxidation, oligomerization, and new particle formation, can simultaneously explain SOA evolution in EC and OFR experiments, using a single consistent set of SOA parameters. With α-pinene as an example, we first developed parameters by fitting the model output to the measured SOA mass concentration and oxygen-to-carbon (O:C) ratio from an EC experiment (

The outbreak of coronavirus named COVID-19, initially identified in Wuhan, China in December 2019, has spread rapidly at the global scale. Most countries have rapidly stopped almost all activities including industry, services and transportation of goods and people, thus decreasing air pollution in an unprecedented way, and providing a unique opportunity to study air pollutants. While satellite data have provided visual evidence for the global reduction in air pollution such as nitrogen dioxide (NO2) worldwide, precise and quantitative information is missing at the local scale. Here we studied changes in particulate matter (PM2.5, PM10), carbon monoxide (CO), NO2, sulfur dioxide (SO2) and ozone (O3) at 10 urban sites in Hangzhou, a city of 7.03 million inhabitants, and at 1 rural site, before city lockdown, January 1–23, during city lockdown, January 24-February 15, and during resumption, February 16–28, in 2020. Results show that city lockdown induced a sharp decrease in PM2.5, PM10, CO, and NO2 concentrations at both urban and rural sites. The NO2 decrease is explained by reduction in traffic emissions in the urban areas, and by lower regional transport in rural areas during lockdown, as expected. SO2 concentrations decreased from 6.3 to 5.3 μg m−3 in the city, but increased surprisingly from 4.7 to 5.8 μg m−3 at the rural site: this increase is attributed both to higher coal consumption for heating and emissions from traditional fireworks of the Spring Eve and Lantern Festivals during lockdown. Unexpectedly, O3 concentrations increased by 145% from 24.6 to 60.6 μg m−3 in the urban area, and from 42.0 to 62.9 μg m−3 in the rural area during the lockdown. This finding is explained by the weakening of chemical titration of O3 by NO due to reductions of NOx fresh emissions during the non-photochemical reaction period from 20:00 PM to 9:00 AM (local time). During the lockdown, compared to the same period in 2019, the daily average concentrations in the city decreased by 42.7% for PM2.5, 47.9% for PM10, 28.6% for SO2, 22.3% for CO and 58.4% for NO2, which is obviously explained by the absence of city activities. Overall, we observed not only the expected reduction in some atmospheric pollutants (PM, SO2, CO, NO2), but also unexpected increases in SO2 in the rural areas and of ozone (O3) in both urban and rural areas, the latter being paradoxically due to the reduction in nitrogen oxide levels. In other words, the city lockdown has improved air quality by reducing PM2.5, PM10, CO, and NO2, but has also decreased air quality by augmenting O3 and SO2. Electronic supplementary material The online version of this article (10.1007/s10311-020-01028-3) contains supplementary material, which is available to authorized users.

Filter-based thermal desorption (F-TD) techniques, such as the filter inlet for gases and aerosols, are widely employed to investigate the molecular composition and physicochemical properties of secondary organic aerosol (SOA). Here, we introduce an enhanced capability of F-TD through the combination of a customized F-TD inlet with chemical ionization mass spectrometry (CIMS) and ultraperformance liquid chromatography/electrospray ionization mass spectrometry (UPLC/ESI-MS). The utility of F-TD/CIMS + UPLC/ESI-MS is demonstrated by application to α-pinene ozonolysis SOA for which increased filter aerosol mass loading is shown to slow the evaporation rates of deposited compounds. Evidence for oligomer decomposition producing multimode F-TD/CIMS thermograms is provided by the measurement of the mass fraction remaining of monomeric and dimeric α-pinene oxidation products on the filter via UPLC/ESI-MS. In situ evaporation of aerosol particles suggests that α-pinene-derived hydroperoxides are thermally labile; thus, analysis of particle-phase (hydro)peroxides via F-TD may not be appropriate. A synthesized pinene-derived dimer ester (C₂₀H₃₂O₅) is found to be thermally stable up to 200 °C, whereas particle-phase dimers (C₁₉H₃₀O₅) are observed to form during F-TD analysis via thermally induced condensation of synthesized pinene-derived alcohols and diacids. The complementary F-TD/CIMS + UPLC/ESI-MS method offers previously inaccessible insight into the molecular composition and thermal desorption behavior of SOA that both clarifies and expands on analysis via traditional F-TD techniques.

A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog1,2, but how it occurs in cities is often puzzling3. If the growth rates of urban particles are similar to those found in cleaner environments (1–10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below −15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid–base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms4,5., Measurements in the CLOUD chamber at CERN show that the rapid condensation of ammonia and nitric acid vapours could be important for the formation and survival of new particles in wintertime urban conditions, contributing to urban smog.

Open biomass burning (OBB) has a high potential to trigger local and regional severe haze with elevated fine particulate matter (PM2.5) concentrations and could thus deteriorate ambient air quality and threaten human health. Open crop straw burning (OCSB), as a critical part of OBB, emits abundant gaseous and particulate pollutants, especially in fields with intensive agriculture, such as in central and eastern China (CEC). This region includes nine provinces, i.e., Hubei, Anhui, Henan, Hunan, Jiangxi, Shandong, Jiangsu, Shanghai, and Fujian. The first four ones are located inland, while the others are on the eastern coast. However, uncertainties in current OCSB and other types of OBB emissions in chemical transport models (CTMs) lead to inaccuracies in evaluating their impacts on haze formations. Satellite retrievals provide an alternative that can be used to simultaneously quantify emissions of OCSB and other types of OBB, such as the Fire INventory from NCAR version 1.5 (FINNv1.5), which, nevertheless, generally underestimates their magnitudes due to unresolved small fires. In this study, we selected June 2014 as our study period, which exhibited a complete evolution process of OBB (from 1 to 19 June) over CEC. During this period, OBB was dominated by OCSB in terms of the number of fire hotspots and associated emissions (74 %–94 %), most of which were located at Henan and Anhui (> 60 %) with intensive enhancements from 5 to 14 June (> 80 %). OCSB generally exhibits a spatiotemporal correlation with regional haze over the central part of CEC (Henan, Anhui, Hubei, and Hunan), while other types of OBB emissions had influences on Jiangxi, Zhejiang, and Fujian. Based on these analyses, we establish a constraining method that integrates ground-level PM2.5 measurements with a state-of-art fully coupled regional meteorological and chemical transport model (the two-way coupled WRF-CMAQ) in order to derive optimal OBB emissions based on FINNv1.5. It is demonstrated that these emissions allow the model to reproduce meteorological and chemical fields over CEC during the study period, whereas the original FINNv1.5 underestimated OBB emissions by 2–7 times, depending on specific spatiotemporal scales. The results show that OBB had substantial impacts on surface PM2.5 concentrations over CEC. Most of the OBB contributions were dominated by OCSB, especially in Henan, Anhui, Hubei, and Hunan, while other types of OBB emissions also exerted an influence in Jiangxi, Zhejiang, and Fujian. With the concentration-weighted trajectory (CWT) method, potential OCSB sources leading to severe haze in Henan, Anhui, Hubei, and Hunan were pinpointed. The results show that the OCSB emissions in Henan and Anhui can cause haze not only locally but also regionally through regional transport. Combining with meteorological analyses, we can find that surface weather patterns played a cardinal role in reshaping spatial and temporal characteristics of PM2.5 concentrations. Stationary high-pressure systems over CEC enhanced local PM2.5 concentrations in Henan and Anhui. Then, with the evolution of meteorological patterns, Hubei and Hunan in the low-pressure system were impacted by areas (i.e., Henan and Anhui) enveloped in the high-pressure system. These results suggest that policymakers should strictly undertake interprovincial joint enforcement actions to prohibit irregular OBB, especially OCSB over CEC. Constrained OBB emissions can, to a large extent, supplement estimations derived from satellite retrievals as well as reduce overestimates of bottom-up methods.

Winter extreme weather events receive major public attention due to their serious impacts1, but the dominant factors regulating their interdecadal trends have not been clearly established2,3. Here, we show that the radiative forcing due to geospatially redistributed anthropogenic aerosols mainly determined the spatial variations of winter extreme weather in the Northern Hemisphere during 1970–2005, a unique transition period for global aerosol forcing4. Over this period, the local Rossby wave activity and extreme events (top 10% in wave amplitude) exhibited marked declining trends at high latitudes, mainly in northern Eurasia. The combination of long-term observational data and a state-of-the-art climate model revealed the unambiguous signature of anthropogenic aerosols on the wintertime jet stream, planetary wave activity and surface temperature variability on interdecadal timescales. In particular, warming due to aerosol reductions in Europe enhanced the meridional temperature gradient on the jet’s poleward flank and strengthened the zonal wind, resulting in significant suppression in extreme events over northern Eurasia. These results exemplify how aerosol forcing can impact large-scale extratropical atmospheric dynamics, and illustrate the importance of anthropogenic aerosols and their spatiotemporal variability in assessing the drivers of extreme weather in historical and future climate. Anthropogenic aerosol emissions decreased over North America and Europe but increased over Asia since the 1970s. This caused jet stream winds to shift poleward over the Atlantic, decreasing planetary wave activity and partially inhibiting extreme winter weather over northern Eurasia.

Water soluble inorganic ions (WSIIs) are important components in PM2.5 and could strongly affect the acidity and hygroscopicity of PM2.5. In order to achieve the seasonal characteristics and determine the potential sources of WSIIs in PM2.5 in Hangzhou, online systems were used to measure hourly mass concentrations of WSIIs (SO42−, NO3−, NH4+, Cl−, Na+, K+, Ca2+ and Mg2+) as well as PM2.5, NO2 and SO2 at an urban site for one month each season (May, August, October, December) in 2017. Results showed that the hourly mass concentrations of PM2.5 during the whole campaign varied from 1 to 292 μg·m−3 with the mean of 56.03 μg·m−3. The mean mass concentration of WSIIs was 26.49 ± 20.78 μg·m−3, which contributed 48.28% to averaged PM2.5 mass. SNA (SO42−, NO3− and NH4+) were the most abundant ions in PM2.5 and on average, they comprised 41.57% of PM2.5 mass. PM2.5, NO2, SO2 and WSIIs showed higher mass concentrations in December, possibly due to higher energy consumption emissions, unfavorable meteorological factors (e.g., lower wind speed and temperature) and regional transport. Results from PCA models showed that secondary aerosols and vehicle emissions were the dominant sources of WSIIs in the observations. Our findings highlight the importance of stronger controls on precursor (e.g., SO2 and NO2) emissions in Hangzhou, and show that industrial areas should be controlled at local and regional scales in the future.

Volatile organic compounds (VOCs) were measured in the Los Angeles (LA) Basin from mid-April to mid-July 2020 during the COVID-19 pandemic, as a part of the Los Angeles Air Quality Campaign (LAAQC). VOCs were quantified in over 450 samples using one- and two-dimensional gas chromatography with different detectors;mixing ratios were determined for 150 compounds associated with on- and off-road mobile, volatile chemical product, and biogenic sources. During the sampling period, traffic counts increased from ∼55% to ∼80% of pre-COVID levels. While the average afternoon combustion-derived VOCs and carbon monoxide (CO) mixing ratios did not change significantly between April-May and June-July, there was a shift in the distribution to higher mixing ratios in June-July, particularly for VOCs associated with gasoline evaporation. Compared to observations made in the last major air quality campaign in the LA Basin (CalNex-2010), emission ratios for 40 compounds relative to acetylene (VOC/acetylene) have remained similar, while emission ratios relative to CO (VOC/CO) have dropped to ∼60% of their 2010 values. This divergence in trends suggests that whereas mobile sources are still the dominant source of the combustion-derived VOCs measured in the LA Basin, there has been a shift in the mobile source sectors, with a growing contribution from sources that have lower CO/acetylene emission ratios, including off-road equipment and vehicles. In addition to the observed shift in source sector contributions, estimated OH exposure was 70-120% higher than in 2010. © 2021 American Chemical Society.