Precursor Emissions Research Articles

Contrasting changes in ozone during 2019–2021 between eastern and the other regions of China attributed to anthropogenic emissions and meteorological conditions

Ozone pollution is one of the most severe air quality issues in China that poses a serious threat to human health and ecosystems. During 2019–2021, the maximum daily 8-h average ozone concentrations in eastern China (110–122.5°E, 26–42°N) and the rest of China (ROC) show different decreasing patterns, with ozone concentrations in eastern China decreasing by 14.9 μg/m3, which is much larger than 4.8 μg/m3 in ROC. Here, based on two independent methods, the atmospheric chemical transport model (GEOS-Chem) simulations and the machine learning (ML) model (LightGBM) predictions, the reasons for the differences in ozone changes between eastern China and ROC during the warm season (April to September) are investigated. According to the GEOS-Chem (LightGBM) results, changes in the meteorological conditions contributed to an ozone decrease by 7.3 (6.8) μg/m3 in eastern China due to decreased chemical production and an ozone decrease by 6.8 (7.0) μg/m3 in ROC attributed to the weakened horizontal and vertical advection. With the influence of meteorological factors excluded, the observations show that changes in anthropogenic emissions resulted in an ozone decrease by 7.6 (8.1) μg/m3 in eastern China and an ozone increase by 2.0 (2.2) μg/m3 in ROC, which is primarily induced by the changes in NOx emissions. The surface measurements and satellite retrievals also indicate that the reduction in NOx emissions in ROC is less efficient than that in the more developed eastern China, leading to contrasting changes in ozone concentrations between eastern China and ROC during 2019–2021. Our results highlight the critical need to reduce ozone precursor emissions in the rest regions of China apart from eastern China.

Opinion: Establishing a science-into-policy process for tropospheric ozone assessment

Abstract. Elevated tropospheric ozone concentrations driven by anthropogenic precursor emissions are an environmental hazard scientifically similar to the depletion of the stratospheric ozone layer and global climate change; however, the tropospheric ozone issue lacks the generally accepted, international assessment efforts that have greatly informed our understanding of the other two. Here, we briefly review those successful science-into-policy approaches and outline the elements required to conduct a similar process for tropospheric ozone. Particular emphasis is placed on the need to establish a conceptual model to fully understand the underpinning science, useful policy metrics, and motivating international policy forums for regulating anthropogenic ozone production over the hemispheric and global scales, thereby expanding beyond the traditional regional, air basin approach that has dominated air quality regulatory philosophy to date.

Estimating the transboundary budget of sulfate aerosols in Northeast Asia with NASA MERRA aerosol reanalysis data

Using the Modern-Era Retrospective Analysis for Research and Applications Aerosol (MERRAero) reanalysis data, we conducted an estimation of the impact of transboundary-transported sulfate aerosols from China, specifically the Beijing–Tianjin–Hebei (BTH) region and Shandong province, on the sulfate concentrations in Korea between 2004 and 2020. Our analysis revealed that the ground-level sulfate concentration at six sites in Korea experienced a significant decrease of over 40%, from 7.16 μg m−3 to 3.7 μg m−3 after 2013. The MERRAero reanalysis data provided insights into a yearly reduction of 0.8 μg m−3 in sulfate concentration for the BTH and Shandong regions, while Korea showed an annual decrease of 0.2 μg m−3. Notably, the BTH and Shandong regions and Korea displayed the strongest correlation in sulfate concentrations with a one-day lag, particularly during the winter season. With the exception of summer, approximately 49.79 ton km−2 month−1 of sulfate was transported from the BTH and Shandong regions of China to Korea, resulting in a net increase of 9.8 ton km−2 month−1. The highest influx of sulfate occurred in spring at 70.06 ton km−2 month−1. Despite the clear declining trend in sulfate concentrations across the study region, the transboundary transport of sulfate from the BTH and Shandong regions of China to Korea did not exhibit a decreasing trend. This underscores the importance of thoroughly investigating the formation process of these aerosols through photochemical reactions during their long-distance transportation over northeast Asia, in addition to conducting a comprehensive examination of precursor emissions related to secondary aerosols.

Aerosol high water contents favor sulfate and secondary organic aerosol formation from fossil fuel combustion emissions

Fine-particle pollution associated with high sulfate and secondary organic aerosol (SOA) contents still occurs in winter, despite considerable reductions in precursor emissions in China. The chemical mechanisms involved are consistently acknowledged to be linked with aerosol water but remain poorly understood. Here, we present findings demonstrating that the synergistic effect of elevated aerosol water content and particles originating from fossil fuel combustion significantly enhanced the rapid formation of sulfate and SOAs under high humidity conditions during winter in northern China. The presence of high aerosol water content promoted the aging process of particles containing elemental carbon (EC) and facilitated the formation of SOAs. Evidence from single particles reveals an increased potential for SOA formation from primary organic aerosols (POAs) originating from fossil fuel combustion, in the presence of increasing aerosol water. Under conditions of relative humidity exceeding 85%, the multiphase oxidation of SO2 by in-particle nitrite/nitrous acid, generated through reactions involving aged EC-containing and iron-rich particles, as well as aqueous-phase formation of hydroxymethanesulfonate (HMS), led to a substantial increase in sulfate production. This study emphasizes the critical role of aerosol water in the aerosol chemistry concerning sulfate and SOAs, highlighting the urgent necessity to mitigate primary emissions from fossil fuel combustion.

A Comprehensive Optical Search for Pre-explosion Outbursts from the Quiescent Progenitor of SN 2023ixf

We perform a comprehensive search for optical precursor emission at the position of SN 2023ixf using data from the DLT40, ZTF, and ATLAS surveys. By comparing the current data set with precursor outburst hydrodynamical model light curves, we find that the probability of a significant outburst within 5 yr of explosion is low, and the circumstellar material (CSM) ejected during any possible precursor outburst is likely smaller than ∼0.015M ⊙. By comparing to a set of toy models, we find that, if there was a precursor outburst, the duration must have been shorter than ∼100 days for a typical brightness of M r ≃ −9 mag or shorter than 200 days for M r ≃ −8 mag; brighter, longer outbursts would have been discovered. Precursor activity like that observed in the normal Type II SN 2020tlf (M r ≃ −11.5) can be excluded in SN 2023ixf. If the dense CSM inferred by early flash spectroscopy and other studies is related to one or more precursor outbursts, then our observations indicate that any such outburst would have to be faint and only last for days to months, or it occurred more than 5 yr prior to the explosion. Alternatively, any dense, confined CSM may not be due to eruptive mass loss from a single red supergiant progenitor. Taken together, the results of SN 2023ixf and SN 2020tlf indicate that there may be more than one physical mechanism behind the dense CSM inferred around some normal Type II supernovae.

Response of the ozone-related health burden in Europe to changes in local anthropogenic emissions of ozone precursors

Exposure to ozone (O3) is associated with many human health problems, resulting in tens of thousands of premature deaths annually in Europe. This study quantifies the impact of changes in anthropogenic emissions of O3 precursors on premature deaths from long-term O3 exposure in Europe and the impact of emissions changes during 2005–2015 using the nested-grid chemical transport model Goddard Earth Observing System (GEOS)-Chem and its adjoint. In 2015, it is estimated that a 20% decrease in total anthropogenic emissions in our modeled European domain could prevent 1576 (467–3252) premature deaths from respiratory disease (30 years of age), 70% of which is owing to the decrease in nitrogen oxides (NO x ) emissions. Underlying this aggregate effect is substantial spatial variation. In most of Europe, O3 formation is NO x -limited so that NO x emission reductions help to decrease premature deaths. Yet where O3 formation is NO x -saturated (as in parts of the United Kingdom, Benelux and Germany) emission reductions cause more premature deaths through increased ozone exposure. Despite the overall decreases in anthropogenic emissions, the marginal benefit, expressed as the avoided premature deaths per 1 kg km−2 yr−1 reduction in NO x emissions, is found to generally increase during 2005–2015, with a mean value more than doubling over Europe. This highlights the general trend that O3 formation becomes less sensitive to volatile organic compound emissions and more limited by NO x emissions. An important policy implication of increasing marginal benefits is that more costly regulations of NO x emissions are economically justified even as total anthropogenic emission are declining. NO x contributions from road transport, industry, energy, and residential sectors are most affected by the change in the O3 production regime. Consequently, European regulations of NO x emissions targeted at those sectors will yield the highest health benefits per unit NO x emission of all sources.

Historical (1960–2014) lightning and LNOx trends and their controlling factors in a chemistry–climate model

Abstract. Lightning can cause natural hazards that result in human and animal injuries and fatalities, infrastructure destruction, and wildfire ignition. Lightning-produced NOx (LNOx), a major NOx (NOx=NO+NO2) source, plays a vital role in atmospheric chemistry and global climate. The Earth has experienced marked global warming and changes in aerosol and aerosol precursor emissions (AeroPEs) since the 1960s. Investigating long-term historical (1960–2014) lightning and LNOx trends can provide important indicators for all lightning-related phenomena and for LNOx effects on atmospheric chemistry and global climate. Understanding how global warming and changes in AeroPEs influence historical lightning and LNOx trends can be helpful in providing a scientific basis for assessing future lightning and LNOx trends. Moreover, global lightning activities' responses to large volcanic eruptions such as the 1991 Pinatubo eruption are not well elucidated and are worth exploring. This study employed the widely used cloud top height lightning scheme (CTH scheme) and the newly developed ice-based ECMWF-McCAUL lightning scheme to investigate historical (1960–2014) lightning and LNOx trends and variations as well as their influencing factors (global warming, increases in AeroPEs, and the Pinatubo eruption) in the framework of the CHASER (MIROC) chemistry–climate model. The results of the sensitivity experiments indicate that both lightning schemes simulated almost flat global mean lightning flash rate anomaly trends during 1960–2014 in CHASER (the Mann–Kendall trend test (significance inferred as 5 %) shows no trend for the ECMWF-McCAUL scheme, but a 0.03 % yr−1 significant increasing trend is detected for the CTH scheme). Moreover, both lightning schemes suggest that past global warming enhances historical trends for global mean lightning density and global LNOx emissions in a positive direction (around 0.03 % yr−1 or 3 % K−1). However, past increases in AeroPEs exert an opposite effect on the lightning and LNOx trends (−0.07 % to −0.04 % yr−1 for lightning and −0.08 % to −0.03 % yr−1 for LNOx) when one considers only the aerosol radiative effects in the cumulus convection scheme. Additionally, effects of past global warming and increases in AeroPEs in lightning trends were found to be heterogeneous across different regions when analyzing lightning trends on the global map. Lastly, this paper is the first of study results suggesting that global lightning activities were markedly suppressed during the first year after the Pinatubo eruption as shown in both lightning schemes (global lightning activities decreased by as much as 18.10 % as simulated by the ECMWF-McCAUL scheme). Based on the simulated suppressed lightning activities after the Pinatubo eruption, the findings also indicate that global LNOx emissions decreased after the 2- to 3-year Pinatubo eruption (1.99 %–8.47 % for the annual percentage reduction). Model intercomparisons of lightning flash rate trends and variations between our study (CHASER) and other Coupled Model Intercomparison Project Phase 6 (CMIP6) models indicate great uncertainties in historical (1960–2014) global lightning trend simulations. Such uncertainties must be investigated further.

Summer Ozone Mechanism and Control Strategy in Beijing-Tianjin-Hebei Region Using Brute-Force Method

In recent years, the ozone (O3) volume fraction in the Beijing-Tianjin-Hebei Region in summer have remained high, light to moderate pollution occurs frequently, and research on related response mechanisms is urgently needed. This study applied the WRF-Chem model to simulate the change in ozone volume fraction in this region by setting 13 precursor emission scenarios in a representative month in the summer of 2018. The results revealed that VOC-sensitivity and no-sensitivity regimes commonly occurred in the Beijing-Tianjin-Hebei Region in July, and the VOC-sensitivity regimes were mainly accumulated in the central Beijing-Tianjin-Hebei Region, with a north-to-south zonal distribution and an area share of 15.60%-26.59%. The relative response intensity (RRI) of O3 volume fraction to precursor emissions in urban areas had large spatial variability, with RRI_VOC and RRI_NOx in the ranges of 0.03-0.16 and -0.40-0.03, respectively. The higher the latitude of urban areas, the more dramatic were the RRI values, indicating a more significant regional transport influence. The lower RRI_NOx values in urban areas with high intensity of precursor emissions implied a negative dependence of RRI_NOx on local NO2 concentrations; however, RRI_VOC was not significantly correlated with NO2levels and was more dependent on the relative abundance of precursors (VOCs:NOx). The ratio of RRI_VOC to RRI_NOx showed negative values in majority of the cities; therefore, collaborative VOCs emission reduction is necessary to suppress the deterioration of O3 volume fraction. The absolute value of this ratio was much lower in cities with high industrialization and urbanization than in ordinary small and medium-sized cities, implying that the demand for collaborative VOCs emission reduction in these cities will be higher. However, even under 50% reduction of precursors, the improvement in O3 volume fraction was limited in regional cities, and the combined prevention in neighboring cities remains important.

Climate responses in China to domestic and foreign aerosol changes due to clean air actions during 2013–2019

In recent years, to improve air quality, significant efforts have been made to reduce regional aerosols including China, Europe and North America, which have potential impacts on climate. In this study, fast and slow climate responses in China to changes in domestic and foreign anthropogenic emissions of aerosols and precursors from 2013 to 2019 are investigated using the Community Earth System Model version 1 (CESM1). Aerosol emissions changes, especially reductions in China, North America and Europe, during 2013–2019 resulted in surface air temperature increases across the Northern Hemisphere. Global aerosol changes induce a regional warming of 0.2 °C in China, equally contributed by domestic and foreign emissions changes. China’s domestic emission reductions lead to a regional average temperature rise of 0.1°C, primarily driven by rapid atmospheric adjustments over eastern China. Foreign aerosol changes, particularly reductions in North America and Europe, also contributed to a 0.1°C warming in China through slow oceanic processes. This warming in China induced by foreign aerosol changes is due to a teleconnection between the aerosol-induced anomalous regional warming in Eastern U.S.-North Atlantic Ocean-Europe and the downstream East Asian climate through anomalous wave trains propagation. The comparable influence of domestic and foreign aerosol changes on climate in China underscores the importance of international collaboration in climate mitigation endeavors.

Impact of spatial scales of control measures on the effectiveness of ozone pollution mitigation in eastern China

Ozone (O3) pollution is becoming the primary air pollution issue with the large decrease in fine particulate concentrations in eastern China. The development of widely recognized policies for controlling O3 pollution episodes is urgent. This study aims to provide actionable and comprehensive suggestions for O3 control policy development, with an emphasis on the precursor emission reductions.Here, we compared the impacts of different spatial scale reductions on a widespread O3 pollution episode in eastern China by a state-of-the-art regional air quality model. We find that region-scale joint control (in >30 cities) is much more effective than city-scale sporadic reduction in reducing O3 concentration. Sporadic controls only reduce the maximum daily 8-h average (MDA8) O3 by ∼1 μg/m3 in the controlled city, whereas regional controls lead to a MDA8 O3 decrease of ∼8 μg/m3 in the controlled region. In addition, the emission reduction effectiveness increased by 2.6 times from <5 cities to >30 cities. Continuous reductions have a cumulative effect on the decrease of MDA8 O3, showing the strongest effects within 24 h and diminishing after 48 h, which underscores the importance of reducing emissions 24 h prior to an episode. Moreover, the effect of control measures on MDA8 O3 varies spatially depending on the ratio of volatile organic compounds (VOCs) to nitrogen oxides (NOx) (VOCs/NOx). Both the reductions of VOC and NOx emissions have a positive effect on the decrease of MDA8 O3 in summer, but the effects of VOC reductions are 1.2 to 1.7 times higher than those of NOx reductions. The residential sector, due to its high VOCs/NOx emission ratio, exhibits the highest efficiency in the reduction of O3 concentrations. Our results highlight the importance of regional joint control and synergistic reduction of VOCs and NOx in eastern China.

Impact of Legislated and Best Available Emission Control Measures on UK Particulate Matter Pollution, Premature Mortality, and Nitrogen-Sensitive Habitats.

Past emission controls in the UK have substantially reduced precursor emissions of health-hazardous fine particles (PM2.5) and nitrogen pollution detrimental to ecosystems. Still, 79% of the UK exceeds the World Health Organization (WHO) guideline for annual mean PM2.5 of 5μgm-3 and there is no enforcement of controls on agricultural sources of ammonia (NH3). NH3 is a phytotoxin and an increasingly large contributor to PM2.5 and nitrogen deposited to sensitive habitats. Here we use emissions projections, the GEOS-Chem model, high-resolution data sets, and contemporary exposure-risk relationships to assess potential human and ecosystem health co-benefits in 2030 relative to the present day of adopting legislated or best available emission control measures. We estimate that present-day annual adult premature mortality attributable to exposure to PM2.5 is 48,625 (95% confidence interval: 45,188-52,595), that harmful amounts of reactive nitrogen deposit to almost all (95%) sensitive habitat areas, and that 75% of ambient NH3 exceeds levels safe for bryophytes and lichens. Legal measures decrease the extent of the UK above the WHO guideline to 58% and avoid 6,800 premature deaths by 2030. This improves with best available measures to 36% of the UK and 13,300 avoided deaths. Both legal and best available measures are insufficient at reducing the extent of damage of nitrogen pollution to sensitive habitats. Far more ambitious reductions in nitrogen emissions (>80%) than is achievable with best available measures (34%) are required to halve the amount of excess nitrogen deposited to sensitive habitats.

Modelling the impacts of emission changes on O3 sensitivity, atmospheric oxidation capacity, and pollution transport over the Catalonia region

Abstract. Tropospheric ozone (O3) is an important surface pollutant in urban areas, and it has complex formation mechanisms that depend on the atmospheric chemistry and on meteorological factors. The severe reductions observed in anthropogenic emissions during the COVID-19 pandemic can further our understanding of the photochemical mechanisms leading to O3 formation and provide guidance for policies aimed at reducing air pollution. In this study, we use the Weather Research and Forecasting model with Chemistry (WRF-Chem) coupled with the urban canopy building effect parameterization and building energy model (BEP + BEM) to investigate changes in the ozone chemistry over the metropolitan area of Barcelona (AMB) and its atmospheric plume moving northwards, which is responsible for the highest number of hourly O3 exceedances in Spain. The trajectories of the air masses from the AMB to the Pyrenees are studied with the Lagrangian FLEXible PARTicle dispersion model with WRF (FLEXPART-WRF). The aim is to investigate the response of ozone chemistry to reduction in precursor emissions (NOx – nitrogen oxides; VOCs – volatile organic compounds). The results show that, with the reduction in emissions, (1) the ozone chemistry tends to enter the NOx-limited or transition regimes, but highly polluted urban areas are still in the VOC-limited regime; (2) the reduced O3 production is overwhelmed by reduced nitric oxide (NO) titration, resulting in a net increase in the O3 concentration (up to 20 %) in the evening; (3) the increase in the maximum O3 level (up to 6 %) during the highest emission-reduction period could be attributed to an enhancement in the atmospheric oxidants hydroxyl and nitrate radical (OH and NO3) given their strong link with O3 loss or production chemistry; (4) the daily maximum levels of ozone and odd oxygen species (Ox) generally decreased (4 %) in May – a period with intense radiation which favours ozone production – with the reduced atmospheric OH and NO3 oxidants, indicating an improvement in the air quality; and (5) ozone precursor concentration changes in the urban plume of Barcelona contribute significantly to the level of pollution along the 150 km south-to-north valley in the Pyrenees. Our results indicate that O3 abatement strategies cannot rely only on NOx emission control but must include a significant reduction in anthropogenic sources of VOCs. In addition, our results show that mitigation strategies intended to reduce O3 should be designed according to the local meteorology, air transport, particular ozone regimes, and oxidation capacity of the atmosphere of the urban area.

Improving photochemical indicators for attributing ozone sensitivities in source apportionment analysis

Comprehensive Air Quality Model with extensions (CAMx)–Decoupled Direct Method (DDM) simulations of first-order ozone (O3) sensitivity to nitrogen oxides (NOx) and volatile organic compounds (VOCs) emissions were performed and combined with modelled PH2O2/PHNO3 ratios to obtain a range of thresholds for determining O3-sensitivity regimes for different areas of China. Utilising the new threshold ranges for photochemical indicators, the method for determining O3 formation in the Ozone Source Apportionment Technology (OSAT) module within CAMx was improved by a dynamically varied threshold of PH2O2/PHNO3 ratio. The O3 concentration contributions in the newly added transition regime were apportioned to NOx and VOCs emissions in proportion to the relationship between the PH2O2/PHNO3 ratio and first-order O3 sensitivity. The source contributions of O3 concentrations from different emission sectors from June to September 2019 were compared using the original and improved CAMx-OSAT. The results showed that the O3 concentration contributions changed significantly in the NOx-limited regime, with a maximum decrease of 21.89%, while the contributions increased by up to 7.57% in the VOC-limited regime, and were within 15 µg/m3 in the transition regime. The modified OSAT module enabled a more sophisticated attribution of O3 to precursor emissions and may have far-reaching implications for informing O3 pollution control policy.

Meteorology-driven PM2.5 interannual variability over East Asia

Atmospheric fine particulate matter (PM2.5) is a human health risk factor, but its ambient concentration depends on both precursor emissions and meteorology. While emission reductions are used to set PM2.5-related health policies, the effect of meteorology is often overlooked. To explore this aspect, we examined PM2.5 interannual variability (IAV) associated with meteorological parameters using the long-term simulation from the Community Earth System Model (CESM1), a global climate-chemistry model, with fixed emissions. The results are subsequently contrasted with the MERRA-2 reanalysis dataset, which inherently considers emission and meteorology effects. Over continental East Asia, the CESM1 domain-average PM2.5 IAV is 6.7 %, mainly attributed to humidity, precipitation, and ventilation variation. The grid-cell PM2.5 IAVs over southern East China are larger, up to 12 % due to the more substantial influence of El Niño-induced meteorological anomalies. Under such climate extreme, sub-regional PM2.5 concentration may occasionally exceed WHO air quality guideline levels despite the compliance of the long-term mean. The simulated PM2.5 IAV over continental East Asia is ~25 % of that derived from the MERRA-2 data, which highlights the influence of both emission and meteorology-driven variations and trends inherent in the latter. Although emission-driven variability is significant to PM2.5 IAV, in remote areas downwind of major source regions in East Asia, North America, and Western Europe, the MERRA-2 data revealed that meteorological variations contributed more to PM2.5 IAV than emission variations. Thus, when setting policies for complying with the WHO PM2.5-related air quality guideline levels, the highest annual PM2.5 associated with climate extremes should be considered instead of that based on average climate conditions.

Exploring ozone formation rules and concentration response to the change of precursors based on artificial neural network simulation in a typical industrial park

Industrial parks have more complex O3 formation mechanisms due to a higher concentration and more dense emission of precursors. This study establishes an artificial neural network (ANN) model with good performance by expanding the moment and concentration changes of pollutants into general variables of meteorological factors and concentrations of pollutants. Finally, the O3 formation rules and concentration response to the changes of volatile organic compounds (VOCs) and nitrogen oxides (NOx) was explored. The results showed that the studied area belonged to the NOx-sensitive regime and the sensitivity was strongly affected by relative humidity (RH) and pressure (P). The concentration of O3 tends to decrease with a higher P, lower temperature (Temp), and medium to low RH when nitric oxide (NO) is added. Conversely, at medium P, high Temp, and high RH, the addition of nitrogen dioxide (NO2) leads to a larger decrease capacity in O3 concentration. More importantly, there is a local reachable maximum incremental reactivity (MIRL) at each certain VOCs concentration level which linearly increased with VOCs. The general maximum incremental reactivity (MIR) may lead to a significant overestimation of the attainable O3 concentration in NOx-sensitive regimes. The results can significantly support the local management strategies for O3 and the precursors control.

Source apportionment of anthropogenic and biogenic organic aerosol over the Tokyo metropolitan area from forward and receptor models

Organic aerosol (OA) is a dominant component of PM2.5, and accurate knowledge of its sources is critical for identification of cost-effective measures to reduce PM2.5. For accurate source apportionment of OA, we conducted field measurements of organic tracers at three sites (one urban, one suburban, and one forest) in the Tokyo Metropolitan Area and numerical simulations of forward and receptor models. We estimated the source contributions of OA by calculating three receptor models (positive matrix factorization, chemical mass balance, and secondary organic aerosol (SOA)-tracer method) using the ambient concentrations, source profiles, and production yields of OA tracers. Sensitivity simulations of the forward model (chemical transport model) for precursor emissions and SOA formation pathways were conducted. Cross-validation between the receptor and forward models demonstrated that biogenic and anthropogenic SOA were better reproduced by the forward model with updated modules for emissions of biogenic volatile organic compounds (VOC) and for SOA formation from biogenic VOC and intermediate-volatility organic compounds than by the default setup. The source contributions estimated by the forward model generally agreed with those of the receptor models for the major OA sources: mobile sources, biomass combustion, biogenic SOA, and anthropogenic SOA. The contributions of anthropogenic SOA, which are the main focus of this study, were estimated by the forward and receptor models to have been between 9 % and 15 % in summer 2019. The observed percent modern carbon data indicate that the amounts of anthropogenic SOA produced during daytime have substantially declined from 2007 to 2019. This trend is consistent with the decreasing trend of anthropogenic VOC, suggesting that reduction of anthropogenic VOC has been effective in reducing anthropogenic SOA in the atmosphere.

Response of PM2.5 and O3 to Emission Reductions in Nanjing Based on Random Forest Algorithm

High levels of fine particulate matter (PM2.5) and ozone (O3) in ambient air affect climate change and also endanger human health and ecosystems. Air pollution in Nanjing has been improving since the implementation of the "Air Pollution Prevention and Control Action Plan" in 2013. However, Nanjing still faces PM2.5 and O3 pollution. Evaluating the response of pollutant concentrations to the reductions in precursor emissions is helpful to obtain effective strategies of emission reduction to improve pollution levels. The sensitive simulations of emission perturbation in atmospheric chemistry models directly demonstrate the response of pollution to the reductions in emissions. Nevertheless, these sensitive simulations are limited in computing time and resources. The random forest algorithm was trained by using the simulation results of the atmospheric chemical transport model (GEOS-Chem) in 2015. The changes in daily PM2.5 and daily maximum eight-hour O3 (MDA8 O3) concentrations in Nanjing in 2019 were efficiently predicted under different reduction scenarios of anthropogenic emissions. The simulations showed that the seasonal average of ρ(PM2.5) in Nanjing would decrease by 2-4 μg·m-3 with the reduction in anthropogenic emissions of 10% in 2019 in China. In the case of controlling only local emissions in Nanjing, the concentrations of PM2.5 in Nanjing decreased significantly without local anthropogenic emissions. Additionally, the simulations showed that the annual average of ρ(PM2.5) in Nanjing could be lower than the national secondary limit (35 μg·m-3) when the anthropogenic emission reduction in China was higher than 20% in 2019. For ozone, the equal proportional emission reductions in nitrogen oxides (NOx) and volatile organic pollutants (VOCs) of O3 precursors in China likely led to the increase in seasonal average concentrations of O3 in Nanjing. For the proportional reduction of anthropogenic emissions by 10%-50% in China, the seasonal average of ρ(MDA8 O3) in Nanjing in 2019 would increase by 1-3 μg·m-3 in spring, 1-4 μg·m-3 in autumn, and 3-11 μg·m-3 in winter, respectively, compared with that in the base simulation. With the reduction in anthropogenic NOx emission by 10% and VOCs by 20%, the seasonal average of ρ(MDA8 O3) in Nanjing would decrease by 3-6 μg·m-3. On this basis, further increasing the proportion (30%) of VOCs emission reduction could reduce the annual average of ρ(MDA8 O3) in Nanjing by 7 μg·m-3. However, the annual average of ρ(MDA8 O3) of Nanjing in 2019 increased by 1 μg·m-3, with the local emission reduction of NOx by 10% and VOCs by 30%. Therefore, this showed that the key to alleviate ozone pollution in Nanjing is a reasonable control ratio of ozone precursor emissions and the implementation of regional joint prevention and control. In order to effectively reduce the O3 pollution in Nanjing, the emission reduction ratio of NOx and VOCs in China should be less than 1:2. The response of pollutant concentrations to reductions in precursor emissions were efficiently obtained by the random forest algorithm and GEOS-Chem model. The simulations would provide the scientific basis for the emission control strategy to alleviate air pollution.

Changes in Ozone Pollution Trend Characteristics and Sensitivity in Jinan from 2015 to 2020

The surface ozone (O3) spatiotemporal distribution, variations, and its causes in Ji'nan from 2015 to 2020 were revealed based on the air quality monitoring network data and satellite retrievals from the Ozone Monitoring Instrument (OMI). The results showed that the ozone concentration in Ji'nan gradually increased from 2015 to 2020. The annual 90th percentile of the daily maximum 8-h average (MDA8) O3(namely the annual evaluation value) and the MDA8 O3(April-September) increased by 4.8 μg·(m3·a)-1 and 3.8 μg·(m3·a)-1, respectively. The trend of the ozone levels in the high-concentration range increased faster than that in the low-concentration range. The MDA8 in June increased by 7.4 μg·(m3·a)-1, and the rate range of increases was 2.6-3.9 μg·(m3·a)-1 in the cool seasons (December-February); thus, the O3 control in winter cannot be ignored. It is apparent from the diurnal variations in ozone from 2015 to 2020 in April-September that the average ozone levels have risen in recent years. The growth rate in the daytime was higher than that at night. The capacity of photochemical production has been increasing, especially in recent years. Additionally, it is noteworthy that the peak time for ozone levels occurred approximately 1-2 h earlier. The disparity of ozone concentrations among different stations gradually decreased in recent years. Compared with that in 2015, the range of areas with high O3 concentrations in 2019-2020 was further expanded. The significant positive trends in MDA8-90th and MDA8 (April-September) were observed in 16.1% and 22.6% of the monitoring sites in Ji'nan (P<0.05), most of which were located in urban areas and the suburbs close to urban areas. The temporal and spatial changes in ozone in Jinan had been affected by the changes in VOCs and NOx emissions since 2015. Satellite remote sensing data from 2015 to 2020 revealed that the NO2 tropospheric columns (April-September) showed reductions of 20.6%, with a decreasing rate of 0.3×1015 mole·(cm2·a)-1, especially in the urban areas and suburbs. The detected variation trends of tropospheric HCHO were weak and insignificant, which suggested that the decrease in NOx emissions was much greater than the decrease in VOCs emissions, and the gap had become more obvious in the urban areas. With responses to precursor emissions, the chemical sensitivity of O3 formation had been changing. The VOCs-limited regimes continuously decreased, and the mixed NOx/VOCs-sensitive regimes and NOx-limited regimes increased. In general, such an extremely inappropriate control ratio of ozone precursor NOx/VOCs led to an overall trend of slow increasing fluctuations of O3 in Ji'nan. The findings clearly indicate that the reduction of VOCs in Ji'nan was far from sufficient, and strengthening the current control of VOCs emissions is an effective measure to control the growth trend of O3 pollution in Ji'nan in the near future, especially in urban and surrounding suburban areas.

Shock Cooling and Possible Precursor Emission in the Early Light Curve of the Type II SN 2023ixf

We present the densely sampled early light curve of the Type II supernova (SN) 2023ixf, first observed within hours of explosion in the nearby Pinwheel Galaxy (Messier 101; 6.7 Mpc). Comparing these data to recently updated models of shock-cooling emission, we find that the progenitor likely had a radius of 410 ± 10 R ⊙. Our estimate is model dependent but consistent with a red supergiant. These models provide a good fit to the data starting about 1 day after the explosion, despite the fact that the classification spectrum shows signatures of circumstellar material around SN 2023ixf during that time. Photometry during the first day after the explosion, provided almost entirely by amateur astronomers, does not agree with the shock-cooling models or a simple power-law rise fit to data after 1 day. We consider the possible causes of this discrepancy, including precursor activity from the progenitor star, circumstellar interaction, and emission from the shock before or after it breaks out of the stellar surface. The very low luminosity (−11 mag > M > −14 mag) and short duration of the initial excess lead us to prefer a scenario related to prolonged emission from the SN shock traveling through the progenitor system.

Meteorologically normalised long-term trends of atmospheric ammonia (NH3) in Switzerland/Liechtenstein and the explanatory role of gas-aerosol partitioning

Ammonia (NH3) is an important atmospheric pollutant and despite significant management efforts, trends of NH3 concentrations have not shown progressive decreases over the last few decades across much of Europe. To investigate this issue, long-term NH3 concentrations from passive sampling tubes were analysed at 32 locations across Switzerland and Liechtenstein. A trend analysis controlling for changes in meteorology employing generalised additive models (GAMs) between 2000 and 2021 showed that 29 of the 32 (91 %) sites experienced no significant change or increasing NH3 concentrations with the greatest trend being 0.17 μgm−3y−1. These results conflict with an indicated 13 % reduction in NH3 emissions from the Swiss emission inventory. The sensitivity of the NH3 -ammonium (NH4+) system to reductions of NH3 ‘s acidic sinks (mostly in the form of nitric and sulfuric acids) was investigated with thermodynamic equilibrium modelling to explain this disconnect. The simulations indicated that the reductions in NH3 ‘s acidic sinks resulted in less NH4+ transformation, thus increasing the NH3/NHx ratio and this process has compensated for the reduction in NH3 emissions. The average effect of the sink reductions was an increase of 0.9 μgm−3 in NH3 between 2004 and 2021. Increases in the NH3/NHx ratio have likely occurred in many European countries due to reductions of acidic precursor emissions and will have consequences for reactive nitrogen deposition and alter import-export budgets among neighbouring regions and countries.