From 2008 to mid-2016, there was more than a 7-fold increase in oil production and nearly a tripling of natural gas production in the Colorado Denver–Julesburg Basin (DJB). This study utilized air samples collected at the Boulder Atmospheric Observatory (BAO) tower in southwestern Weld County in the DJB to investigate atmospheric mole fraction trends of methane and volatile organic compounds (VOCs). Elevated methane and propane mole fractions and low values (<1) in the ratio of i-pentane to n-pentane at BAO were found to be associated with flow patterns that transport air from the northeast (NE) to east (E) sector to the site, the direction where the primary locations of oil and natural gas (O&NG) extraction and processing activities are located. Median mole fractions of the O&NG tracer propane at BAO were 10 times higher than background values when winds came from the NE quadrant. This contrasts with lower mole fractions of O&NG-related constituents in air parcels arriving at BAO from the south, the direction of the major urban area of Denver. None of O&NG tracers, for example, methane and propane, show statistically significant trends in mole fraction (relative to the background) over the study period in air transported from the DJB. Also, longer term acetylene mole fraction changes were not seen in NE quadrant or south sector samples. A significant decline in the mole fraction ratio of i-pentane to n-pentane in the NE sector data provides evidence of an increasing influence of O&NG on the overall composition of VOCs measured at BAO, a change not seen in measurements from the south (urban) sector. These results suggest that O&NG emissions and resulting atmospheric mole fractions have remained relatively constant over 2008–2016. The behavior in the observations is in contrast to the most recent VOC emissions inventory. While the inventory projects O&NG total VOC emission reductions between 2011 and 2020, of –6.5% per year despite the large production increases, the best estimate of the propane emission rate of change for the DJB-filtered data during 2008–2016 is much smaller, that is, –1.5% per year.

In this article, we examine atmospheric and river discharge conditions within the Hudson Bay Complex for the BaySys 2016–2018 field program time frame. Investigated in particular is a subset of European Centre for Medium-Range Weather Forecasts (ECMWF) Re-Analysis - Interim (ERA-Interim) atmospheric forcing variables, namely 2-m surface temperature, 10-m surface winds, precipitation, and sea-level pressure, in addition to river discharge. Results from this assessment show that 2016 was characterized by unusually warm conditions (terrestrial and marine) throughout the annual cycle; 2017 by strong cyclone activity in March and high precipitation in January, October, and November; and 2018 by cold and windy conditions throughout the annual cycle. Evaluation of terrestrial conditions showed higher than normal land surface temperatures (the Hudson Bay physical watershed) for all of the 2016–2018 period (excluding a colder than normal spell August–November 2018), particularly in January (2016 and 2017), higher than normal precipitation in October (2016 and 2017), and higher than normal terrestrial discharge to the Hudson Bay Complex in March (2016 and 2017), with drier than average June through October (2016–2018).

Advanced leak detection (ALD) to survey local natural gas distribution systems has reached a point in technological maturity where new federal regulations will require its use in compliance surveys. Because most of these deployments are conducted by commercial providers, there has been little publicly available data documenting characteristics of the underlying methane (CH 4 ) plumes that are the core features measured in ALD surveys. Here, we document key features of CH 4 plumes measured in ALD surveys of 15 U.S. metropolitan areas where we had deployed high-sensitivity CH 4 analyzers on Google Street View cars. Our analysis reveals that CH 4 concentration enhancements from CH 4 sources exhibit high temporal variability, often differing by more than 10-fold among repeated observations. This variability introduces challenges for estimating source emission rates because the same source can appear to be large on one drive-by and small on the next. Additionally, the frequency distribution of CH 4 enhancements from a given source generally has a strong positive skew that can lead to overestimation of leak size. The magnitude of CH 4 enhancements from a source measured with a mobile sensor can also change quickly over time, as indicated by decreasing temporal correlation between mobile measurements longer than an approximately hourly time scale. To manage the uncertainty, we demonstrate how additional survey effort can help overcome this variability and instability to allow discrimination among the wide range of leak sizes. We quantify the probability of source detection, finding that it increases with estimated leak size. Combining these results, we develop a simulation that demonstrates the potential for ALD to detect leaks and quantify emissions as a function of sampling (driving) effort. Our results suggest that five to eight drives of each roadway in a target area would detect >90% of leaks and provide adequate emissions quantification for repair/replacement prioritization.

Methane is a powerful greenhouse gas and a key player in atmospheric chemistry. Important uncertainties remain in the global atmospheric methane budget, with natural geologic emissions being one of the particularly uncertain terms. In recent bottom-up studies, geologic emissions have been estimated to comprise up to 10% of the global budget (40–60 Teragrams of methane per year, Tg CH 4 yr –1 ). In contrast, top-down constraints from 14 C of methane in preindustrial air extracted from ice cores indicate that the geologic methane source is approximately an order of magnitude lower. Recent bottom-up inventories propose microseepage (diffuse low-level flux of methane through soils over large areas) as the largest single component of the geologic methane flux. In this study, we present new measurements of methane microseepage from the Appalachian Basin (Western New York State) and compare these with prior microseepage measurements from other regions and with predicted values from the most recent bottom-up inventory. Our results show lower microseepage values than most prior data sets and indicate that positive microseepage fluxes in this region are not as widespread as previously assumed. A statistical analysis of our results indicates that mean microseepage flux in this region has very likely been overestimated by the bottom-up inventory, even though our measurements more likely than not underestimate the true mean flux. However, this is a small data set from a single region and as such cannot be used to evaluate the validity of the microseepage emissions inventory as a whole. Instead, the results demonstrate the need for a more extensive network of direct geologic emission measurements in support of improved bottom-up inventories.

The Copernicus Atmosphere Monitoring Service (CAMS) is operationally providing forecast and reanalysis products of air quality and atmospheric composition. In this article, we present an extended evaluation of the CAMS global reanalysis data set of four reactive gases, namely, ozone (O 3 ), carbon monoxide (CO), nitrogen dioxide (NO 2 ), and formaldehyde (HCHO), using multiple independent observations. Our results show that the CAMS model system mostly provides a stable and accurate representation of the global distribution of reactive gases over time. Our findings highlight the crucial impact of satellite data assimilation and emissions, investigated through comparison with a model run without assimilated data. Stratospheric and tropospheric O 3 are mostly well constrained by the data assimilation, except over Antarctica after 2012/2013 due to changes in the assimilated data. Challenges remain for O 3 in the Tropics and high-latitude regions during winter and spring. At the surface and for short-lived species (NO 2 ), data assimilation is less effective. Total column CO in the CAMS reanalysis is well constrained by the assimilated satellite data. The control run, however, shows large overestimations of total column CO in the Southern Hemisphere and larger year-to-year variability in all regions. Concerning the long-term stability of the CAMS model, we note drifts in the time series of biases for surface O 3 and CO in the Northern midlatitudes and Tropics and for NO 2 over East Asia, which point to biased emissions. Compared to the previous Monitoring Atmospheric Composition and Climate reanalysis, changes in the CAMS chemistry module and assimilation system helped to reduce biases and enhance the long-term temporal consistency of model results for the CAMS reanalysis.

Summertime ozone in the Western United States presents a unique public health challenge. Changes in population, background ozone, wildland fire, and local precursor emissions combined with terrain-induced meteorology can affect surface ozone levels and compliance with the National Ambient Air Quality Standards (NAAQS). While there is considerable research on ozone in the Northern Front Range Metropolitan Area of Colorado, United States, less is known about the Southern Front Range. In Colorado Springs, approximately 100 km south of Denver, summertime maximum daily 8-h average (MDA8) ozone shows no significant ( p < .05) trend at the 5th, 50th, or 95th percentile over the past 20 years. However, the region is at risk of nonattainment with the NAAQS based on observations from 2018 to 2020. From June through September 2018, the Colorado Department of Public Health and Environment measured hourly ozone at eight sites to characterize the spatial distribution of ozone in Colorado Springs. Mean ozone (±1σ) ranged from 34 ± 19 to 60 ± 9 ppb. The 95th percentile of hourly ozone increased approximately 1.1 ppb per 100 m of elevation, while the amplitudes of mean diurnal profiles decreased with elevation and distance from the interstate. MDA8 ozone was also highly correlated across all sites, and there is little evidence of local photochemical production or ozone transport from Denver. Further, results from generalized additive modeling show that summertime MDA8 in this region is strongly influenced by regional background air and wildfire, with smoke contributing an average of 4–5 ppb to the MDA8. Enhanced MDA8 values due to wildfires were especially pronounced in 2018 and 2020. Lastly, we find that the permanent monitoring sites represent the lower end of observed ozone in the region, suggesting that additional long-term monitoring for public health may be warranted in populated, higher elevation areas.

The Korea–United States Air Quality (KORUS-AQ) field study was conducted during May–June 2016. The effort was jointly sponsored by the National Institute of Environmental Research of South Korea and the National Aeronautics and Space Administration of the United States. KORUS-AQ offered an unprecedented, multi-perspective view of air quality conditions in South Korea by employing observations from three aircraft, an extensive ground-based network, and three ships along with an array of air quality forecast models. Information gathered during the study is contributing to an improved understanding of the factors controlling air quality in South Korea. The study also provided a valuable test bed for future air quality–observing strategies involving geostationary satellite instruments being launched by both countries to examine air quality throughout the day over Asia and North America. This article presents details on the KORUS-AQ observational assets, study execution, data products, and air quality conditions observed during the study. High-level findings from companion papers in this special issue are also summarized and discussed in relation to the factors controlling fine particle and ozone pollution, current emissions and source apportionment, and expectations for the role of satellite observations in the future. Resulting policy recommendations and advice regarding plans going forward are summarized. These results provide an important update to early feedback previously provided in a Rapid Science Synthesis Report produced for South Korean policy makers in 2017 and form the basis for the Final Science Synthesis Report delivered in 2020.

Transport of pollution into pristine wilderness areas is of concern for both federal and state agencies. Assessing such transport in complex terrain is a challenge when relying solely on data from standard federal or state air quality monitoring networks because of the sparsity of network monitors beyond urban areas. During the Front Range air quality study, conducted in the summer of 2008 in the vicinity of Denver, CO, research-grade surface air quality data, vertical wind profiles and mixing heights obtained by radar wind profilers, and ozone profile data obtained by an airborne ozone differential absorption lidar augmented the local regulatory monitoring networks. Measurements from this study were taken on 2 successive days at the end of July 2008. On the first day, the prevailing winds were downslope westerly, advecting pollution to the east of the Front Range metropolitan areas. On this day, chemistry measurements at the mountain and foothills surface stations showed seasonal background ozone levels of approximately 55–68 ppbv (nmol mol –1 by volume). The next day, upslope winds prevailed, advecting pollution from the Plains into the Rocky Mountains and across the Continental Divide. Mountain stations measured ozone values greater than 90 ppbv, comparable to, or greater than, nearby urban measurements. The measurements show the progression of the ozone-enriched air into the mountains and tie the westward intrusion into high-elevation mountain sites to the growth of the afternoon boundary layer. Thus, under deep upslope flow conditions, ozone-enriched air can be advected into wilderness areas of the Rocky Mountains. Our findings highlight a process that is likely to be an important ozone transport mechanism in mountainous terrain adjacent to ozone source areas when the right circumstances come together, namely a deep layer of light winds toward a mountain barrier coincident with a deep regional boundary layer.

Atmospheric nitrogen oxide and nitrogen dioxide (NO + NO 2 , together termed as NO X ) estimates from annual photochemical simulations for years 2002–2016 are compared to surface network measurements of NO X and total gas-phase-oxidized reactive nitrogen (NO Y ) to evaluate the Community Multiscale Air Quality (CMAQ) modeling system performance by U.S. region, season, and time of day. In addition, aircraft measurements from 2011 Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality are used to evaluate how emissions, chemical mechanism, and measurement uncertainty each contribute to the overall model performance. We show distinct seasonal and time-of-day patterns in NO X performance. Summertime NO X is overpredicted with bimodal peaks in bias during early morning and evening hours and persisting overnight. The summertime morning NO X bias dropped from between 28% and 57% for earlier years (2002–2012) to between –2% and 7% for later years (2013–2016). Summer daytime NO X tends to be unbiased or underpredicted. In winter, the evening NO X overpredictions remain, but NO X is unbiased or underpredicted overnight, in the morning, and during the day. NO X overpredictions are most pronounced in the Midwestern and Southern United States with Western regions having more of a tendency toward model underpredictions of NO X . Modeled NO X performance has improved substantially over time, reflecting updates to the emission inputs and the CMAQ air quality model. Model performance improvements are largest for years simulated with CMAQv5.1 or later and for emission inventory years 2014 and later, coinciding with reduced onroad NO X emissions from vehicles with newer emission control technologies and improved treatment of chemistry, deposition, and vertical mixing in CMAQ. Our findings suggest that emissions temporalization of specific mobile source sectors have a small impact on model performance, while chemistry updates improve predictions of NO Y but do not improve summertime NO X bias in the Baltimore/DC area. Sensitivity runs performed for different locations across the country suggest that the improvement in summer NO X performance can be attributed to updates in vertical mixing incorporated in CMAQv5.1.

Disposable compressed gas aerosols have been a ubiquitous part of life since the mid-1950s. The signing of the Montreal Protocol in 1987 led to aerosol propellants changing from halocarbons to less damaging replacements; around 93% of current aerosol emissions by mass are volatile organic compounds (VOCs), with small contributions from compressed air (6.6%) and fluorocarbons (0.4%). The global consumption of aerosol units has increased significantly since the signing of the Montreal Protocol, increasing by an order of magnitude in some countries. In high-income countries, annual consumption increased through the 1990s and 2000s, typically reaching a plateau of approximately 10 ± 3 units person –1 year –1 dependant on product preferences. The largest contributors of both units and mass emissions are personal care products (PCPs). Consumption of aerosols in lower- and upper-middle income countries are growing rapidly, for example, Brazil, Mexico, China, Thailand, all tripling reported consumption since 2006. Based on evidence drawn from national production estimates, product specifications and formulations, and interpolation of usage between countries of similar economic status, we estimate global emissions of VOC from aerosol propellants were approximately 1.3 ± 0.23 Tg year –1 in 2018. The fraction of anthropogenic VOC emissions accounted for by aerosols has in some countries increased significantly as emissions from vehicles and fuels have declined. For example, in the UK, 6.1% of anthropogenic VOC emissions were from aerosols in 2017, more than were released from gasoline passenger cars. Should low- and middle-income economies grow consumption per capita in line with recent trends, then we project global aerosol consumption may reach approximately 4.4 ± 0.96 × 10 10 units year –1 in 2050. Should existing national and international policies on aerosol product formulation remain unchanged, and VOCs remain the dominant propellant, compressed aerosols could account for a global emission of approximately 2.2 ± 0.48 Tg year –1 in 2050.

Nonmethane volatile organic compounds (NMVOCs) result in ozone and aerosol production that adversely affects the environment and human health. For modeling purposes, anthropogenic NMVOC emissions have been typically compiled using the “bottom-up” approach. To minimize uncertainties of the bottom-up emission inventory, “top-down” NMVOC emissions can be estimated using formaldehyde (HCHO) observations. In this study, HCHO vertical column densities (VCDs) obtained from the Geostationary Trace gas and Aerosol Sensor Optimization spectrometer during the Korea–United States Air Quality campaign were used to constrain anthropogenic volatile organic compound (AVOC) emissions in South Korea. Estimated top-down AVOC emissions differed from those of the up-to-date bottom-up inventory over major anthropogenic source regions by factors of 1.0 ± 0.4 to 6.9 ± 3.9. Our evaluation using a 3D chemical transport model indicates that simulated HCHO mixing ratios using the top-down estimates were in better agreement with observations onboard the DC-8 aircraft during the campaign relative to those with the bottom-up emission, showing a decrease in model bias from –25% to –13%. The top-down analysis used in this study, however, has some limitations related to the use of HCHO yields, background HCHO columns, and AVOC speciation in the bottom-up inventory, resulting in uncertainties in the AVOC emission estimates. Our attempt to constrain diurnal variations of the AVOC emissions using the aircraft HCHO VCDs was compromised by infrequent aircraft observations over the same source regions. These limitations can be overcome with geostationary satellite observations by providing hourly HCHO VCDs.

Single particle aerosol mass spectrometers (SPAMS) have created significant interest among atmospheric scientists by virtue of their ability to provide real-time size-resolved information on the chemical composition of aerosols. The objective of this study is to evaluate the newly developed single particle analysis technique in terms of chemical characterization and source apportionment of ambient aerosols by comparing it with traditional filter-based methods. In this study, an air quality monitoring campaign was conducted over a period of 25 days at an urban area in Yulin city, southern China, by employing both SPAMS and traditional filter-based measurements to establish the performance of SPAMS. It was observed that the chemical characterization of particles based on SPAMS did not agree well with the filter-based analysis. Based on the filter analysis, sulfate was the most abundant component in PM 2.5 (23.5%), followed by OC (18.1%), while for single particle analysis (number concentration), EC-containing particles showed the largest contribution to PM 2.5 (>40%), followed by OC (15.7%). In terms of source apportionment via positive matrix factorization, six sources were identified by each of the two approaches. Both the approaches showed relatively good agreements for secondary species, traffic, and dust sources; however, discrepancies were noted for industry, fossil fuel, and biomass burning sources. Finally, investigation of diurnal profiles and two specific emission episodes monitored during the Chinese New Year and traffic activities demonstrated the relative advantage of single particle analysis over filter-based methods. Overall, single particle analysis can provide source apportionment with a high time resolution, which is helpful for policy makers to analyze and implement emergency control strategies during air pollution episodes. However, SPAMS performs quantification of number concentration rather than mass concentration and is limited to particles larger than 200 nm, which leads to discrepancies between the two methods. SPAMS measurements can therefore not simply replace traditional filter-based analyses, which needs to be carefully considered in the selection of the monitoring implementation.

The coronavirus-19 (COVID-19) pandemic led to government interventions to limit the spread of the disease which are unprecedented in recent history; for example, stay at home orders led to sudden decreases in atmospheric emissions from the transportation sector. In this review article, the current understanding of the influence of emission reductions on atmospheric pollutant concentrations and air quality is summarized for nitrogen dioxide (NO 2 ), particulate matter (PM 2.5 ), ozone (O 3 ), ammonia, sulfur dioxide, black carbon, volatile organic compounds, and carbon monoxide (CO). In the first 7 months following the onset of the pandemic, more than 200 papers were accepted by peer-reviewed journals utilizing observations from ground-based and satellite instruments. Only about one-third of this literature incorporates a specific method for meteorological correction or normalization for comparing data from the lockdown period with prior reference observations despite the importance of doing so on the interpretation of results. We use the government stringency index (SI) as an indicator for the severity of lockdown measures and show how key air pollutants change as the SI increases. The observed decrease of NO 2 with increasing SI is in general agreement with emission inventories that account for the lockdown. Other compounds such as O 3 , PM 2.5 , and CO are also broadly covered. Due to the importance of atmospheric chemistry on O 3 and PM 2.5 concentrations, their responses may not be linear with respect to primary pollutants. At most sites, we found O 3 increased, whereas PM 2.5 decreased slightly, with increasing SI. Changes of other compounds are found to be understudied. We highlight future research needs for utilizing the emerging data sets as a preview of a future state of the atmosphere in a world with targeted permanent reductions of emissions. Finally, we emphasize the need to account for the effects of meteorology, emission trends, and atmospheric chemistry when determining the lockdown effects on pollutant concentrations.

Gaseous elemental mercury observations were conducted at Churchill, Victoria, in Australia from April to July, 2013, using a Tekran 2537 analyzer. A strong diurnal variation with daytime average values of 1.2–1.3 ng m –3 and nighttime average values of 1.6–1.8 ng m –3 was observed. These values are significantly higher than the Southern Hemisphere average of 0.85–1.05 ng m –3 . Churchill is in the Latrobe Valley, approximately 150 km East of Melbourne, where approximately 80% of Victoria’s electricity is generated from low-rank brown coal from four major power stations: Loy Yang A, Loy Yang B, Hazelwood, and Yallourn. These aging generators do not have any sulfur, nitrogen oxide, or mercury air pollution controls. Mercury emitted in the 2015–2016 year in the Latrobe Valley is estimated to have had an externalized health cost of $AUD88 million. Air pollution mercury simulations were conducted using the Weather Research and Forecast model with Chemistry at 3 × 3 km resolution. Electrical power generation emissions were added using mercury emissions created from the National Energy Market’s 5-min energy distribution data. The strong diurnal cycle in the observed mercury was well simulated ( R 2 = .49 and P value = 0.00) when soil mercury emissions arising from several years of wet and dry deposition in a radius around the power generators was included in the model, as has been observed around aging lignite coal power generators elsewhere. These results indicate that long-term air and soil sampling in power generation regions, even after the closure of coal fired power stations, will have important implications to understanding the airborne mercury emissions sources.

Methane leakage from point sources in the oil and gas industry is a major contributor to global greenhouse gas emissions. The majority of such emissions come from a small fraction of “super-emitting” sources. We evaluate the emission detection and quantification capabilities of Kairos Aerospace’s airplane-based hyperspectral imaging methane emission detection system for methane fluxes of 18–1,025 kg per hour of methane (kgh(CH 4 )). In blinded controlled releases of methane conducted over 4 days in San Joaquin County, CA, Kairos detected 182 of 200 valid nonzero releases, including all 173 over 15 kgh(CH 4 ) per meter per second (mps) of wind and none of the 12 nonzero releases below 8.3 kgh(CH 4 )/mps. Nine of the 26 releases in the partial detection range of 5–15 kgh(CH 4 )/mps were detected. There were no false positives: Kairos did not detect methane during any of the 21 negative controls. Plume quantification accuracy depends on the wind measurement technique, with a parity slope of 1.15 (σ = 0.037, R 2 = 0.84, N = 185) using a cup-based wind meter and 1.45 (σ = 0.059, R 2 = 0.80, N = 157) using an ultrasonic anemometer. Performance is comparable even with only modeled wind data. For emissions above 15 kgh/mps, quantification error scales as roughly 30%–40% of emission size, even when using wind reanalysis data instead of ground-based measurements. This reflects both uncertainty in wind measurements and in Kairos’ estimates. These findings suggest that at 2 mps winds under favorable environmental conditions in the United States, Kairos could detect and quantify over 50% of total emissions by identifying super-emitting sources.

A scientific scenario paper was prepared ahead of the Gulf of Maine (GOM) 2050 International Symposium to review and summarize possible weather-related and sea-level changes within the GOM as a result of climate change. It is projected that the GOM will experience warming temperatures, continued sea-level rise, and changes to storm characteristics and related elements such as precipitation and waves in the intermediate term, by approximately 2050. Coastal communities within the GOM region are particularly vulnerable to the anticipated impacts of climate change. This article aims to provide context on some of the consequential impacts that may occur from the changes projected within the area.

Rainwater is an essential pathway to remove fine particulate matter and dissolved atmospheric pollutants (e.g., SO 2 , HNO 3 , and NH 3 ). Acid rain (pH < 5.6) has been a severe environmental issue in China since the 1970s, adversely impacting ecosystem health. This study focuses on the influence of anthropogenically induced anions (SO 4 2– and NO 3 – ) and alkaline cations (Ca 2+ and NH 4 + ) on acid rain in Chinese cities. In this review, cities with high population density east of the Hu Huanyong Line that divides China geographically according to its uneven economic development were studied. Coastal and central areas of China to the east of the line are characterized by a much faster developing economy and rapid urbanization. The observed trends and spatial variability of acidity and chemical composition in rainwater are discussed in relation to industrialization and environmental changes in China. Over the past 3½ decades, the precipitation pH in the urban regions has exhibited reduced acidity. A mixed nitric–sulfuric acid rain type has become prominent due to the significant decrease in SO 4 2– via desulfurization. Ca 2+ levels have decreased, while NH 4 + has increased slightly due to more vehicular transportation. In addition, the neutralization capacity of Ca 2+ and NH 4 + has decreased from north to south. Overall, the acid rain problem in Chinese cities has been alleviated in recent years.

The Korea-United States Air Quality (KORUS-AQ) field study was conducted during May–June 2016 to understand the factors controlling air quality in South Korea. Extensive aircraft and ground network observations from the campaign offer an opportunity to address issues in current air quality models and reduce model-observation disagreements. This study examines these issues using model evaluation against the KORUS-AQ observations and intercomparisons between models. Six regional and two global chemistry transport models using identical anthropogenic emissions participated in the model intercomparison study and were used to conduct air quality simulations focusing on ozone (O 3 ), aerosols, and their precursors for the campaign. Using the KORUSv5 emissions inventory, which has been updated from KORUSv1, the models successfully reproduced observed nitrogen oxides (NO x ) and volatile organic compounds mixing ratios in surface air, especially in the Seoul Metropolitan Area, but showed systematic low biases for carbon monoxide (CO), implying possible missing CO sources in the inventory in East Asia. Although the DC-8 aircraft-observed O 3 precursor mixing ratios were well captured by the models, simulated O 3 levels were lower than the observations in the free troposphere in part due to too low stratospheric O 3 influxes, especially in regional models. During the campaign, the synoptic meteorology played an important role in determining the observed variability of PM 2.5 (PM diameter ≤ 2.5 μm) concentrations in South Korea. The models successfully simulated the observed PM 2.5 variability with significant inorganic sulfate-nitrate-ammonium aerosols contribution, but failed to reproduce that of organic aerosols, causing a large inter-model variability. From the model evaluation, we find that an ensemble of model results, incorporating individual models with differing strengths and weaknesses, performs better than most individual models at representing observed atmospheric compositions for the campaign. Ongoing model development and evaluation, in close collaboration with emissions inventory development, are needed to improve air quality forecasting.

Using the Purdue University Airborne Laboratory for Atmospheric Research, we measured concentrations of methane and ethane emanating from seven U.S. cities (New York, NY, Philadelphia, PA, Washington, D.C./Baltimore, MD, Boston, MA, Chicago, IL, Richmond, VA, and Indianapolis, IN), in order to determine (with a median 95% CI of roughly 7%) the fraction of methane emissions attributable to natural gas (Thermogenic Methane Emission Ratio [TMER]), for both summer and winter months. New methodology is introduced to compute inflow concentrations and to accurately define the spatial domain of the sampling region, using upwind measurements coupled with Lagrangian trajectory modeling. We show discrepancies in inventory-estimated TMER from cities when the sample domain is defined using political boundaries versus urban centers encircled by the flight track and highlight this as a potential source of error common to top-down studies. We found that methane emissions of natural gas were greater than winter biogenic emissions for all cities except Richmond, where multiple landfills dominate. Biogenic emissions increased in summer, but natural gas remained important or dominant (20%–80%). National inventories should be updated to reflect the dominance of natural gas emissions for urban environments and to account for seasonal increases in biogenic methane in summer.

To understand the characteristics of air quality in the Seoul Metropolitan Area, intensive measurements were conducted under the Korea-United States Air Quality (KORUS-AQ) campaign. Trace gases such as O 3 , NO x , NO y , SO 2 , CO, and volatile organic compounds (VOCs), photochemical byproducts such as H 2 O 2 and HCHO, aerosol species, and meteorological variables including planetary boundary layer height were simultaneously measured at Olympic Park in Seoul. During the measurement period, high O 3 episodes that exceeded the 90 ppbv hourly maximum occurred on 14 days under four distinct synoptic meteorological conditions. Furthermore, local circulation such as land–sea breeze and diurnal evolution of the boundary layer were crucial in determining the concentrations of precursor gases, including NO x and VOC as well as O 3 . During such episodes, the nighttime NO x and VOC and daytime UV levels were higher compared to non-episode days. The overall precursor levels and photochemical activity were represented fairly well by variations in the HCHO, which peaked in the morning during the high O 3 episodes. This study revealed that toluene was the most abundant VOC in Seoul, and its concentration increased greatly with NO x due to the large local influence under stagnant conditions. When O 3 was highly elevated concurrently with PM 2.5 under dominant westerlies, NO x and VOCs were relatively lower and CO was noticeably higher than in other episodes. Additionally, the O 3 production efficiency was the highest due to a low NO x with the highest NO z /NO y ratio among the four episodes. When westerlies were dominant in transport-south episode, the nighttime concentration of O 3 remained as high as 40~50 ppbv due to the minimum level of NO x titration. Overall, the Seoul Metropolitan Area is at NO x -saturated and VOC-limited conditions, which was diagnosed by indicator species and VOC/NO x ratios.