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Air pollution in megacities has severe health impacts, but its control could provide opportunities for climate change mitigation. As of 2008, over half of humanity lives in cities. The number of megacities (with populations over 10 million) grew from 3 in 1975 to 19 in 2007, and is projected to increase to 27 in 2025 ( 1 ). These megacities are the engines of growing economies, but are also very large sources of air pollutants and climate-forcing agents. The growth of megacities greatly aggravates the health impacts of polluted air, yet it may also provide an opportunity to mitigate climate change, if implemented air quality policies are designed to also reduce global warming.

Source attribution science can help areas of the U.S. west At Earth's surface, ozone is an air pollutant that causes respiratory health effects in humans and impairs plant growth and productivity ( 1 ). The Clean Air Act (CAA) of 1970 mandates that the U.S. Environmental Protection Agency (EPA) assess the ozone standard every 5 years and revise when necessary to protect human health. With a decision expected in October 2015 as to whether the standard will be toughened, we discuss limitations of ozone and precursor observations that hinder the ability of state and local air pollution–control agencies to accurately attribute sources of ozone within their jurisdictions. Attaining a lower standard may be particularly challenging in high elevations of the western United States, which are more likely to be affected by ozone that has been transported long distances or that originated in the stratosphere.

Volatile organic compounds (VOCs) were measured online at an urban site in Beijing in August–September 2010. Diurnal variations of various VOC species indicate that VOCs concentrations were influenced by photochemical removal with OH radicals for reactive species and secondary formation for oxygenated VOCs (OVOCs). A photochemical age‐based parameterization method was applied to characterize VOCs chemistry. A large part of the variability in concentrations of both hydrocarbons and OVOCs was explained by this method. The determined emission ratios of hydrocarbons to acetylene agreed within a factor of two between 2005 and 2010 measurements. However, large differences were found for emission ratios of some alkanes and C8 aromatics between Beijing and northeastern United States secondary formation from anthropogenic VOCs generally contributed higher percentages to concentrations of reactive aldehydes than those of inert ketones and alcohols. Anthropogenic primary emissions accounted for the majority of ketones and alcohols concentrations. Positive matrix factorization (PMF) was also used to identify emission sources from this VOCs data set. The four resolved factors were three anthropogenic factors and a biogenic factor. However, the anthropogenic factors are attributed here to a common source at different stages of photochemical processing rather than three independent sources. Anthropogenic and biogenic sources of VOCs concentrations were not separated completely in PMF. This study indicates that photochemistry of VOCs in the atmosphere complicates the information about separated sources that can be extracted from PMF and the influence of photochemical processing must be carefully considered in the interpretation of source apportionment studies based upon PMF. Key Points Photochemistry significantly influenced VOC concentrations VOC emission ratios and source allocations of OVOCs are determined PMF factors represent different degrees of photochemical processing of VOCs

Detailed airborne, surface, and subsurface chemical measurements, primarily obtained in May and June 2010, are used to quantify initial hydrocarbon compositions along different transport pathways (i.e., in deep subsurface plumes, in the initial surface slick, and in the atmosphere) during the Deepwater Horizon oil spill. Atmospheric measurements are consistent with a limited area of surfacing oil, with implications for leaked hydrocarbon mass transport and oil drop size distributions. The chemical data further suggest relatively little variation in leaking hydrocarbon composition over time. Although readily soluble hydrocarbons made up ~25% of the leaking mixture by mass, subsurface chemical data show these compounds made up ~69% of the deep plume mass; only ~31% of the deep plume mass was initially transported in the form of trapped oil droplets. Mass flows along individual transport pathways are also derived from atmospheric and subsurface chemical data. Subsurface hydrocarbon composition, dissolved oxygen, and dispersant data are used to assess release of hydrocarbons from the leaking well. We use the chemical measurements to estimate that (7.8 ± 1.9) × 10⁶ kg of hydrocarbons leaked on June 10, 2010, directly accounting for roughly three-quarters of the total leaked mass on that day. The average environmental release rate of (10.1 ± 2.0) × 10⁶ kg/d derived using atmospheric and subsurface chemical data agrees within uncertainties with the official average leak rate of (10.2 ± 1.0) × 10⁶ kg/d derived using physical and optical methods.

Airborne measurements of volatile organic compounds (VOCs) were performed during CalNex 2010 (California Research at the Nexus of Air Quality and Climate Change) in the Los Angeles (LA) basin in May–June 2010 and during ITCT2k2 (Intercontinental Transport and Chemical Transformation) in May 2002. While CO2 enhancements in the basin were similar between the two years, the ΔCO/ΔCO2 ratio had decreased by about a factor of two. The ΔVOC/ΔCO emission ratios stayed relatively constant between the two years. This indicates that, relative to CO2, VOCs in the LA basin also decreased by about a factor of two since 2002. These data are compared with the results from various previous field campaigns dating back as early as 1960 and from the extensive air quality monitoring system in the LA basin going back to 1980. The results show that the mixing ratios of VOCs and CO have decreased by almost two orders of magnitude during the past five decades at an average annual rate of about 7.5%. Exceptions to this trend are the small alkanes ethane and propane, which have decreased slower due to the use and production of natural gas. A comparison with trends in London, UK shows that, due to stricter regulations at the time, VOC mixing ratios in LA decreased earlier than in London, albeit at a slower rate, such that typical mixing ratios in both cities in 2008 were at about the same level. Key Points VOCs and CO have decreased by a large factor in LA since 1960s VOC emission ratios have not changed Rate of decrease in London is more rapid, but started later

Simulations by six Coupled Model Intercomparison Project Phase 6 (CMIP6) Earth system models indicate that the seasonal cycle of baseline tropospheric ozone at northern midlatitudes has been shifting since the mid-20th century. Beginning in ∼ 1940, the magnitude of the seasonal cycle increased by ∼10 ppb (measured from seasonal minimum to maximum), and the seasonal maximum shifted to later in the year by about 3 weeks. This shift maximized in the mid-1980s, followed by a reversal – the seasonal cycle decreased in amplitude and the maximum shifted back to earlier in the year. Similar changes are seen in measurements collected from the 1970s to the present. The timing of the seasonal cycle changes is generally concurrent with the rise and fall of anthropogenic emissions that followed industrialization and the subsequent implementation of air quality emission controls. A quantitative comparison of the temporal changes in the ozone seasonal cycle at sites in both Europe and North America with the temporal changes in ozone precursor emissions across the northern midlatitudes found a high degree of similarity between these two temporal patterns. We hypothesize that changing precursor emissions are responsible for the shift in the ozone seasonal cycle; this is supported by the absence of such seasonal shifts in southern midlatitudes where anthropogenic emissions are much smaller. We also suggest a mechanism by which changing emissions drive the changing seasonal cycle: increasing emissions of NOx allow summertime photochemical production of ozone to become more important than ozone transported from the stratosphere, and increasing volatile organic compounds (VOCs) lead to progressively greater photochemical ozone production in the summer months, thereby increasing the amplitude of the seasonal ozone cycle. Decreasing emissions of both precursor classes then reverse these changes. The quantitative parameter values that characterize the seasonal shifts provide useful benchmarks for evaluating model simulations, both against observations and between models.

A nonlinear change in baseline ozone concentrations at northern midlatitudes has been quantified over preceding decades. During the past few years, several studies, using linear trend analyses, report relatively small trends over selected time periods – results inconsistent with the earlier developed picture. We show that reported COVID-19-related ozone changes in the background troposphere based on the linear analysis are significantly larger than those derived considering recent long-term decreases in background ozone, which the linear trend analyses do not quantify. We further point out that the extensive loss of lower stratospheric ozone in the unprecedented 2020 springtime Arctic stratospheric ozone depletion event likely reduced the natural source to the troposphere, rendering the background anomalously low that year. Consideration of these two issues indicates that the COVID-19 restrictions had a much smaller impact on background tropospheric ozone in 2020 than previously reported. A consensus understanding of baseline ozone changes and their causes is important for formulating policies to improve ozone air quality; cooperative, international emission control efforts aimed at continuing or even accelerating the ongoing decrease in hemisphere-wide background ozone concentrations may be the most effective approach to further reducing urban and rural ozone in the more developed northern midlatitude countries, as well as improving ozone air quality in all countries within these latitudes. Analysis of baseline ozone measurements over several years following the COVID-19 impact is expected to provide a firm basis for resolving the inconsistencies between the two views of long-term northern midlatitude ozone changes and better quantifying the COVID-19 impact.

Our quantitative understanding of natural tropospheric ozone concentrations is limited by the paucity of reliable measurements before the 1980s. We utilize the existing measurements to compare the long-term ozone changes that occurred within the marine boundary layer at northern and southern midlatitudes. Since 1950 ozone concentrations have increased by a factor of 2.1 ± 0.2 in the Northern Hemisphere (NH) and are presently larger than in the Southern Hemisphere (SH), where only a much smaller increase has occurred. These changes are attributed to increased ozone production driven by anthropogenic emissions of photochemical ozone precursors that increased with industrial development. The greater ozone concentrations and increases in the NH are consistent with the predominant location of anthropogenic emission sources in that hemisphere. The available measurements indicate that this interhemispheric gradient was much smaller and was likely reversed in the pre-industrial troposphere with higher concentrations in the SH. Six Earth system model (ESM) simulations indicate similar total NH increases (1.9 with a standard deviation of 0.3), but they occurred more slowly over a longer time period, and the ESMs do not find higher pre-industrial ozone in the SH. Several uncertainties in the ESMs may cause these model–measurement disagreements: the assumed natural nitrogen oxide emissions may be too large, the relatively greater fraction of ozone injected by stratosphere–troposphere exchange to the NH may be overestimated, ozone surface deposition to ocean and land surfaces may not be accurately simulated, and model treatment of emissions of biogenic hydrocarbons and their photochemistry may not be adequate.

Air quality improvement in Los Angeles, California is reviewed with an emphasis on aspects that may inform air quality policy formulation in developing cities. In the mid-twentieth century the air quality in Los Angeles was degraded to an extent comparable to the worst found in developing cities today; ozone exceeded 600 ppb and annual average particulate matter 〈 10 μm reached -150 μg.m -3. Today＇s air quality is much better due to very effective emission controls; e.g., modem automobilcs emit about 1% of the hydrocarbons and carbon monoxide emitted by vehicles of 50 years ago. An overview is given of the emission control efforts in Los Angeles and their impact on anabient concentrations of primary and secondary pollutants： the costs and health benefits of these controls arc briefly summarized, Today＇s developing cities have new challenges that are discussed： the effects of regional pollution transport are much greater in countries with very high population densities： often very large current populations must be supplied with goods and services even while economic development and air quality concerns are addressed; and many of currently developing cities arc located in or close to the tropics where photochemical processing of pollution is expected to be more rapid than at higher latitudes. The air quality issues of Beijing are briefly compared and contrasted with those of Los Angeles, and the opportunities for co-benefits for climate and air quality improvement are pointed out.

In the past decade, ozone (O3) pollution has become a severe environmental problem in China's major cities. Here, based on available observational records, we investigated the long-term trend of O3 pollution in China during 2014–2020. The O3 concentrations were slightly higher in urban areas than in non-urban areas. During these 7 years, the highest O3 concentrations primarily occurred during summer in northern China, and during autumn or spring in southern China. Although O3 precursors, including nitrogen oxides (NOx) and carbon monoxide (CO), continuously decreased, O3 concentrations generally increased throughout the 7 years with a slower increasing rate after 2017. The long-term trend of O3 concentrations differed across seasons, especially from 2019 to 2020, when O3 concentrations decreased in summer and increased in winter. To analyse the causes of this observed trend, a photochemical box model was used to investigate the change in the O3 sensitivity regime in two representative cities – Beijing and Shanghai. Our model simulations suggest that the summertime O3 sensitivity regime in urban areas of China has changed from a VOC-limited regime to a transition regime during 2014–2020. By 2020, the urban photochemistry was in a transition regime in summer but in a VOC-limited regime in winter. This study helps to understand the distinct trends of O3 in China and provides insights into efficient future O3 control strategies in different regions and seasons.