Anthropogenic Fingerprint Detectable in Upper Tropospheric Ozone Trends Retrieved from Satellite.

Tropospheric ozone (O3) is a strong greenhouse gas, particularly in the upper troposphere (UT). Limited observations point to a continuous increase in UT O3 in recent decades, but the attribution of UT O3 changes is complicated by large internal climate variability. We show that the anthropogenic signal ("fingerprint") in the patterns of UT O3 increases is distinguishable from the background noise of internal variability. The time-invariant fingerprint of human-caused UT O3 changes is derived from a 16-member initial-condition ensemble performed with a chemistry-climate model (CESM2-WACCM6). The fingerprint is largest between 30°S and 40°N, especially near 30°N. In contrast, the noise pattern in UT O3 is mainly associated with the El Niño-Southern Oscillation (ENSO). The UT O3 fingerprint pattern can be discerned with high confidence within only 13 years of the 2005 start of the OMI/MLS satellite record. Unlike the UT O3 fingerprint, the lower tropospheric (LT) O3 fingerprint varies significantly over time and space in response to large-scale changes in anthropogenic precursor emissions, with the highest signal-to-noise ratios near 40°N in Asia and Europe. Our analysis reveals a significant human effect on Earth's atmospheric chemistry in the UT and indicates promise for identifying fingerprints of specific sources of ozone precursors.

Ozone-related acute excess mortality projected to increase in the absence of climate and air quality controls consistent with the Paris Agreement.

Short-term exposure to ground-level ozone in cities is associated with increased mortality and is expected to worsen with climate and emission changes. However, no study has yet comprehensively assessed future ozone-related acute mortality across diverse geographic areas, various climate scenarios, and using CMIP6 multi-model ensembles, limiting our knowledge on future changes in global ozone-related acute mortality and our ability to design targeted health policies. Here, we combine CMIP6 simulations and epidemiological data from 406 cities in 20 countries or regions. We find that ozone-related deaths in 406 cities will increase by 45 to 6,200 deaths/year between 2010 and 2014 and between 2050 and 2054, with attributable fractions increasing in all climate scenarios (from 0.17% to 0.22% total deaths), except the single scenario consistent with the Paris Climate Agreement (declines from 0.17% to 0.15% total deaths). These findings stress the need for more stringent air quality regulations, as current standards in many countries are inadequate.

Space-Based Observations of Ozone Precursors within California Wildfire Plumes and the Impacts on Ozone-NOx-VOC Chemistry.

The frequency of wildfires in the western United States has escalated in recent decades. Here we examine the impacts of wildfires on ground-level ozone (O3) precursors and the O3-NOx-VOC chemistry from the source to downwind urban areas. We use satellite retrievals of nitrogen dioxide (NO2) and formaldehyde (HCHO, an indicator of VOC) from the Tropospheric Monitoring Instrument (TROPOMI) to track the evolution of O3 precursors from wildfires over California from 2018 to 2020. We improved these satellite retrievals by updating the a priori profiles and explicitly accounting for the effects of smoke aerosols. TROPOMI observations reveal that the extensive and intense fire smoke in 2020 led to an overall increase in statewide annual average HCHO and NO2 columns by 16% and 9%. The increase in the level of NO2 offsets the anthropogenic NOx emission reduction from the COVID-19 lockdown. The enhancement of NO2 within fire plumes is concentrated near the regions actively burning, whereas the enhancement of HCHO is far-reaching, extending from the source regions to urban areas downwind due to the secondary production of HCHO from longer-lived VOCs such as ethene. Consequently, a larger increase in NOx occurs in NOx-limited source regions, while a greater increase in HCHO occurs in VOC-limited urban areas, both contributing to more efficient O3 production.

An observation-based, reduced-form model for oxidation in the remote marine troposphere.

The hydroxyl radical (OH) fuels atmospheric chemical cycling as the main sink for methane and a driver of the formation and loss of many air pollutants, but direct OH observations are sparse. We develop and evaluate an observation-based proxy for short-term, spatial variations in OH (ProxyOH) in the remote marine troposphere using comprehensive measurements from the NASA Atmospheric Tomography (ATom) airborne campaign. ProxyOH is a reduced form of the OH steady-state equation representing the dominant OH production and loss pathways in the remote marine troposphere, according to box model simulations of OH constrained with ATom observations. ProxyOH comprises only eight variables that are generally observed by routine ground- or satellite-based instruments. ProxyOH scales linearly with in situ [OH] spatial variations along the ATom flight tracks (median r2 = 0.90, interquartile range = 0.80 to 0.94 across 2-km altitude by 20° latitudinal regions). We deconstruct spatial variations in ProxyOH as a first-order approximation of the sensitivity of OH variations to individual terms. Two terms modulate within-region ProxyOH variations-water vapor (H2O) and, to a lesser extent, nitric oxide (NO). This implies that a limited set of observations could offer an avenue for observation-based mapping of OH spatial variations over much of the remote marine troposphere. Both H2O and NO are expected to change with climate, while NO also varies strongly with human activities. We also illustrate the utility of ProxyOH as a process-based approach for evaluating intermodel differences in remote marine tropospheric OH.

Daily Satellite Observations of Nitrogen Dioxide Air Pollution Inequality in New York City, New York and Newark, New Jersey: Evaluation and Application.

Urban air pollution disproportionately harms communities of color and low-income communities in the U.S. Intraurban nitrogen dioxide (NO2) inequalities can be observed from space using the TROPOspheric Monitoring Instrument (TROPOMI). Past research has relied on time-averaged measurements, limiting our understanding of how neighborhood-level NO2 inequalities co-vary with urban air quality and climate. Here, we use fine-scale (250 m × 250 m) airborne NO2 remote sensing to demonstrate that daily TROPOMI observations resolve a major portion of census tract-scale NO2 inequalities in the New York City-Newark urbanized area. Spatiotemporally coincident TROPOMI and airborne inequalities are well correlated (r = 0.82-0.97), with slopes of 0.82-1.05 for relative and 0.76-0.96 for absolute inequalities for different groups. We calculate daily TROPOMI NO2 inequalities over May 2018-September 2021, reporting disparities of 25-38% with race, ethnicity, and/or household income. Mean daily inequalities agree with results based on TROPOMI measurements oversampled to 0.01° × 0.01° to within associated uncertainties. Individual and mean daily TROPOMI NO2 inequalities are largely insensitive to pixel size, at least when pixels are smaller than ∼60 km2, but are sensitive to low observational coverage. We statistically analyze daily NO2 inequalities, presenting empirical evidence of the systematic overburdening of communities of color and low-income neighborhoods with polluting sources, regulatory ozone co-benefits, and worsened NO2 inequalities and cumulative NO2 and urban heat burdens with climate change.

Investigating Changes in Ozone Formation Chemistry during Summertime Pollution Events over the Northeastern United States.

Understanding the local-scale spatial and temporal variability of ozone formation is crucial for effective mitigation. We combine tropospheric vertical column densities (VCDTrop) of formaldehyde (HCHO) and nitrogen dioxide (NO2), referred to as HCHO-VCDTrop and NO2-VCDTrop, retrieved from airborne remote sensing and the TROPOspheric Monitoring Instrument (TROPOMI) with ground-based measurements to investigate changes in ozone precursors and the inferred chemical production regime on high-ozone days in May-August 2018 over two Northeast urban domains. Over New York City (NYC) and Baltimore/Washington D.C. (BAL/DC), HCHO-VCDTrop increases across the domain, but higher NO2-VCDTrop occurs mainly in urban centers on ozone exceedance days (when maximum daily 8 h average (MDA8) ozone exceeds 70 ppb at any monitor in the region). The ratio of HCHO-VCDTrop to NO2-VCDTrop, proposed as an indicator of the sensitivity of local surface ozone production rates to its precursors, generally increases on ozone exceedance days, implying a transition toward a more NOx-sensitive ozone production regime that should lead to higher efficacy of NOx controls on the highest ozone days in NYC and BAL/DC. Warmer temperatures and enhanced influence from emissions in the local boundary layer on the high-ozone days are accompanied by slower wind speeds in BAL/DC but stronger, southwesterly winds in NYC.

Large contribution of biomass burning emissions to ozone throughout the global remote troposphere.

Ozone is the third most important anthropogenic greenhouse gas after carbon dioxide and methane but has a larger uncertainty in its radiative forcing, in part because of uncertainty in the source characteristics of ozone precursors, nitrogen oxides, and volatile organic carbon that directly affect ozone formation chemistry. Tropospheric ozone also negatively affects human and ecosystem health. Biomass burning (BB) and urban emissions are significant but uncertain sources of ozone precursors. Here, we report global-scale, in situ airborne measurements of ozone and precursor source tracers from the NASA Atmospheric Tomography mission. Measurements from the remote troposphere showed that tropospheric ozone is regularly enhanced above background in polluted air masses in all regions of the globe. Ozone enhancements in air with high BB and urban emission tracers (2.1 to 23.8 ppbv [parts per billion by volume]) were generally similar to those in BB-influenced air (2.2 to 21.0 ppbv) but larger than those in urban-influenced air (-7.7 to 6.9 ppbv). Ozone attributed to BB was 2 to 10 times higher than that from urban sources in the Southern Hemisphere and the tropical Atlantic and roughly equal to that from urban sources in the Northern Hemisphere and the tropical Pacific. Three independent global chemical transport models systematically underpredict the observed influence of BB on tropospheric ozone. Potential reasons include uncertainties in modeled BB injection heights and emission inventories, export efficiency of BB emissions to the free troposphere, and chemical mechanisms of ozone production in smoke. Accurately accounting for intermittent but large and widespread BB emissions is required to understand the global tropospheric ozone burden.

Large uncertainties in global hydroxyl projections tied to fate of reactive nitrogen and carbon.

The hydroxyl radical (OH) sets the oxidative capacity of the atmosphere and, thus, profoundly affects the removal rate of pollutants and reactive greenhouse gases. While observationally derived constraints exist for global annual mean present-day OH abundances and interannual variability, OH estimates for past and future periods rely primarily on global atmospheric chemistry models. These models disagree ± 30% in mean OH and in its changes from the preindustrial to late 21st century, even when forced with identical anthropogenic emissions. A simple steady-state relationship that accounts for ozone photolysis frequencies, water vapor, and the ratio of reactive nitrogen to carbon emissions explains temporal variability within most models, but not intermodel differences. Here, we show that departure from the expected relationship reflects the treatment of reactive oxidized nitrogen species (NO y ) and the fraction of emitted carbon that reacts within each chemical mechanism, which remain poorly known due to a lack of observational data. Our findings imply a need for additional observational constraints on NO y partitioning and lifetime, especially in the remote free troposphere, as well as the fate of carbon-containing reaction intermediates to test models, thereby reducing uncertainties in projections of OH and, hence, lifetimes of pollutants and greenhouse gases.

Satellite Monitoring for Air Quality and Health.

Data from satellite instruments provide estimates of gas and particle levels relevant to human health, even pollutants invisible to the human eye. However, the successful interpretation of satellite data requires an understanding of how satellites relate to other data sources, as well as factors affecting their application to health challenges. Drawing from the expertise and experience of the 2016-2020 NASA HAQAST (Health and Air Quality Applied Sciences Team), we present a review of satellite data for air quality and health applications. We include a discussion of satellite data for epidemiological studies and health impact assessments, as well as the use of satellite data to evaluate air quality trends, support air quality regulation, characterize smoke from wildfires, and quantify emission sources. The primary advantage of satellite data compared to in situ measurements, e.g., from air quality monitoring stations, is their spatial coverage. Satellite data can reveal where pollution levels are highest around the world, how levels have changed over daily to decadal periods, and where pollutants are transported from urban to global scales. To date, air quality and health applications have primarily utilized satellite observations and satellite-derived products relevant to near-surface particulate matter <2.5 µm in diameter (PM2.5) and nitrogen dioxide (NO2). Health and air quality communities have grown increasingly engaged in the use of satellite data, and this trend is expected to continue. From health researchers to air quality managers, and from global applications to community impacts, satellite data are transforming the way air pollution exposure is evaluated.

Short-term PM2.5 and cardiovascular admissions in NY State: assessing sensitivity to exposure model choice.

BACKGROUND: Air pollution health studies have been increasingly using prediction models for exposure assessment even in areas without monitoring stations. To date, most studies have assumed that a single exposure model is correct, but estimated effects may be sensitive to the choice of exposure model. METHODS: We obtained county-level daily cardiovascular (CVD) admissions from the New York (NY) Statewide Planning and Resources Cooperative System (SPARCS) and four sets of fine particulate matter (PM2.5) spatio-temporal predictions (2002-2012). We employed overdispersed Poisson models to investigate the relationship between daily PM2.5 and CVD, adjusting for potential confounders, separately for each state-wide PM2.5 dataset. RESULTS: For all PM2.5 datasets, we observed positive associations between PM2.5 and CVD. Across the modeled exposure estimates, effect estimates ranged from 0.23% (95%CI: -0.06, 0.53%) to 0.88% (95%CI: 0.68, 1.08%) per 10 µg/m3 increase in daily PM2.5. We observed the highest estimates using monitored concentrations 0.96% (95%CI: 0.62, 1.30%) for the subset of counties where these data were available. CONCLUSIONS: Effect estimates varied by a factor of almost four across methods to model exposures, likely due to varying degrees of exposure measurement error. Nonetheless, we observed a consistently harmful association between PM2.5 and CVD admissions, regardless of model choice.

Role of emission controls in reducing the 2050 climate change penalty for PM2.5 in China.

Previous studies demonstrated that global warming can lead to deteriorated air quality even when anthropogenic emissions were kept constant, which has been called a climate change penalty on air quality. It is expected that anthropogenic emissions will decrease significantly in the future considering the aggressive emission control actions in China. However, the dependence of climate change penalty on the choice of emission scenario is still uncertain. To fill this gap, we conducted multiple independent model simulations to investigate the response of PM2.5 to future (2050) climate warming (RCP8.5) in China but with different emission scenarios, including the constant 2015 emissions, the 2050 CLE emissions (based on Current Legislation), and the 2050 MTFR emissions (based on Maximum Technically Feasible Reduction). For each set of emissions, we estimate climate change penalty as the difference in PM2.5 between a pair of simulations with either 2015 or 2050 meteorology. Under 2015 emissions, we find a PM2.5 climate change penalty of 1.43 µg m-3 in Eastern China, leading to an additional 35,000 PM2.5-related premature deaths [95% confidence interval (CI), 21,000-40,000] by 2050. However, the PM2.5 climate change penalty weakens to 0.24 µg m-3 with strict anthropogenic emission controls under the 2050 MTFR emissions, which decreases the associated PM2.5-related deaths to 17,000. The smaller MTFR climate change penalty contributes 14% of the total PM2.5 decrease when both emissions and meteorology are changed from 2015 to 2050, and 24% of total health benefits associated with this PM2.5 decrease in Eastern China. This finding suggests that controlling anthropogenic emissions can effectively reduce the climate change penalty on PM2.5 and its associated premature deaths, even though a climate change penalty still occurs even under MTFR. Strengthened controls on anthropogenic emissions are key to attaining air quality targets and protecting human health in the context of future global climate change.

Evaluating Drought Responses of Surface Ozone Precursor Proxies: Variations With Land Cover Type, Precipitation, and Temperature.

Prior work suggests drought exacerbates US air quality by increasing surface ozone concentrations. We analyze 2005-2015 tropospheric column concentrations of two trace gases that serve as proxies for surface ozone precursors retrieved from the OMI/Aura satellite: Nitrogen dioxide (ΩNO2; NOx proxy) and formaldehyde (ΩHCHO; VOC proxy). We find 3.5% and 7.7% summer drought enhancements (classified by SPEI) for ΩNO2 and ΩHCHO, respectively, corroborating signals previously extracted from ground-level observations. When we subset by land cover type, the strongest ΩHCHO drought enhancement (10%) occurs in the woody savannas of the Southeast US. By isolating the influences of precipitation and temperature, we infer that enhanced biogenic VOC emissions in this region increase ΩHCHO independently with both high temperature and low precipitation during drought. The strongest ΩNO2 drought enhancement (6.0%) occurs over Midwest US croplands and grasslands, which we infer to reflect the sensitivity of soil NOx emissions to temperature.

Using Satellites to Track Indicators of Global Air Pollution and Climate Change Impacts: Lessons Learned From a NASA-Supported Science-Stakeholder Collaborative.

The 2018 NASA Health and Air Quality Applied Science Team (HAQAST) "Indicators" Tiger Team collaboration between NASA-supported scientists and civil society stakeholders aimed to develop satellite-derived global air pollution and climate indicators. This Commentary shares our experience and lessons learned. Together, the team developed methods to track wildfires, dust storms, pollen counts, urban green space, nitrogen dioxide concentrations and asthma burdens, tropospheric ozone concentrations, and urban particulate matter mortality. Participatory knowledge production can lead to more actionable information but requires time, flexibility, and continuous engagement. Ground measurements are still needed for ground truthing, and sustained collaboration over time remains a challenge.

Dry Deposition of Ozone over Land: Processes, Measurement, and Modeling.

Dry deposition of ozone is an important sink of ozone in near surface air. When dry deposition occurs through plant stomata, ozone can injure the plant, altering water and carbon cycling and reducing crop yields. Quantifying both stomatal and nonstomatal uptake accurately is relevant for understanding ozone's impact on human health as an air pollutant and on climate as a potent short-lived greenhouse gas and primary control on the removal of several reactive greenhouse gases and air pollutants. Robust ozone dry deposition estimates require knowledge of the relative importance of individual deposition pathways, but spatiotemporal variability in nonstomatal deposition is poorly understood. Here we integrate understanding of ozone deposition processes by synthesizing research from fields such as atmospheric chemistry, ecology, and meteorology. We critically review methods for measurements and modeling, highlighting the empiricism that underpins modeling and thus the interpretation of observations. Our unprecedented synthesis of knowledge on deposition pathways, particularly soil and leaf cuticles, reveals process understanding not yet included in widely-used models. If coordinated with short-term field intensives, laboratory studies, and mechanistic modeling, measurements from a few long-term sites would bridge the molecular to ecosystem scales necessary to establish the relative importance of individual deposition pathways and the extent to which they vary in space and time. Our recommended approaches seek to close knowledge gaps that currently limit quantifying the impact of ozone dry deposition on air quality, ecosystems, and climate.

Methods, availability, and applications of PM2.5 exposure estimates derived from ground measurements, satellite, and atmospheric models.

Fine particulate matter (PM2.5) is a well-established risk factor for public health. To support both health risk assessment and epidemiological studies, data are needed on spatial and temporal patterns of PM2.5 exposures. This review article surveys publicly available exposure datasets for surface PM2.5 mass concentrations over the contiguous U.S., summarizes their applications and limitations, and provides suggestions on future research needs. The complex landscape of satellite instruments, model capabilities, monitor networks, and data synthesis methods offers opportunities for research development, but would benefit from guidance for new users. Guidance is provided to access publicly available PM2.5 datasets, to explain and compare different approaches for dataset generation, and to identify sources of uncertainties associated with various types of datasets. Three main sources used to create PM2.5 exposure data are ground-based measurements (especially regulatory monitoring), satellite retrievals (especially aerosol optical depth, AOD), and atmospheric chemistry models. We find inconsistencies among several publicly available PM2.5 estimates, highlighting uncertainties in the exposure datasets that are often overlooked in health effects analyses. Major differences among PM2.5 estimates emerge from the choice of data (ground-based, satellite, and/or model), the spatiotemporal resolutions, and the algorithms used to fuse data sources.Implications: Fine particulate matter (PM2.5) has large impacts on human morbidity and mortality. Even though the methods for generating the PM2.5 exposure estimates have been significantly improved in recent years, there is a lack of review articles that document PM2.5 exposure datasets that are publicly available and easily accessible by the health and air quality communities. In this article, we discuss the main methods that generate PM2.5 data, compare several publicly available datasets, and show the applications of various data fusion approaches. Guidance to access and critique these datasets are provided for stakeholders in public health sectors.

Scientific assessment of background ozone over the U.S.: Implications for air quality management.

Ozone (O3) is a key air pollutant that is produced from precursor emissions and has adverse impacts on human health and ecosystems. In the U.S., the Clean Air Act (CAA) regulates O3 levels to protect public health and welfare, but unraveling the origins of surface O3 is complicated by the presence of contributions from multiple sources including background sources like stratospheric transport, wildfies, biogenic precursors, and international anthropogenic pollution, in addition to U.S. anthropogenic sources. In this report, we consider more than 100 published studies and assess current knowledge on the spatial and temporal distribution, trends, and sources of background O3 over the continental U.S., and evaluate how it inflattainment of the air quality standards. We conclude that spring and summer seasonal mean U.S. background O3 (USB O3), or O3 formed from natural sources plus anthropogenic sources in countries outside the U.S., is greatest at high elevation locations in the western U.S., with monthly mean maximum daily 8-hour average (MDA8) mole fractions approaching 50 parts per billion (ppb) and annual 4th highest MDA8s exceeding 60 ppb, at some locations. At lower elevation sites, e.g., along the West and East Coasts, seasonal mean MDA8 USB O3 is in the range of 20-40 ppb, with generally smaller contributions on the highest O3 days. The uncertainty in U.S. background O3 is around ±10 ppb for seasonal mean values and higher for individual days. Noncontrollable O3 sources, such as stratospheric intrusions or precursors from wildfires, can make significant contributions to O3 on some days, but it is challenging to quantify accurately these contributions. We recommend enhanced routine observations, focused fi studies, process-oriented modeling studies, and greater emphasis on the complex photochemistry in smoke plumes as key steps to reduce the uncertainty associated with background O3 in the U.S.

Future ozone-related acute excess mortality under climate and population change scenarios in China: A modeling study.

BACKGROUND: Climate change is likely to further worsen ozone pollution in already heavily polluted areas, leading to increased ozone-related health burdens. However, little evidence exists in China, the world's largest greenhouse gas emitter and most populated country. As China is embracing an aging population with changing population size and falling age-standardized mortality rates, the potential impact of population change on ozone-related health burdens is unclear. Moreover, little is known about the seasonal variation of ozone-related health burdens under climate change. We aimed to assess near-term (mid-21st century) future annual and seasonal excess mortality from short-term exposure to ambient ozone in 104 Chinese cities under 2 climate and emission change scenarios and 6 population change scenarios. METHODS AND FINDINGS: We collected historical ambient ozone observations, population change projections, and baseline mortality rates in 104 cities across China during April 27, 2013, to October 31, 2015 (2013-2015), which included approximately 13% of the total population of mainland China. Using historical ozone monitoring data, we performed bias correction and spatially downscaled future ozone projections at a coarse spatial resolution (2.0° × 2.5°) for the period April 27, 2053, to October 31, 2055 (2053-2055), from a global chemistry-climate model to a fine spatial resolution (0.25° × 0.25°) under 2 Intergovernmental Panel on Climate Change Representative Concentration Pathways (RCPs): RCP4.5, a moderate global warming and emission scenario where global warming is between 1.5°C and 2.0°C, and RCP8.5, a high global warming and emission scenario where global warming exceeds 2.0°C. We then estimated the future annual and seasonal ozone-related acute excess mortality attributable to both climate and population changes using cause-specific, age-group-specific, and season-specific concentration-response functions (CRFs). We used Monte Carlo simulations to obtain empirical confidence intervals (eCIs), quantifying the uncertainty in CRFs and the variability across ensemble members (i.e., 3 predictions of future climate and air quality from slightly different starting conditions) of the global model. Estimates of future changes in annual ozone-related mortality are sensitive to the choice of global warming and emission scenario, decreasing under RCP4.5 (-24.0%) due to declining ozone precursor emissions but increasing under RCP8.5 (10.7%) due to warming climate in 2053-2055 relative to 2013-2015. Higher ambient ozone occurs under the high global warming and emission scenario (RCP8.5), leading to an excess 1,476 (95% eCI: 898 to 2,977) non-accidental deaths per year in 2053-2055 relative to 2013-2015. Future ozone-related acute excess mortality from cardiovascular diseases was 5-8 times greater than that from respiratory diseases. Ozone concentrations increase by 15.1 parts per billion (10-9) in colder months (November to April), contributing to a net yearly increase of 22.3% (95% eCI: 7.7% to 35.4%) in ozone-related mortality under RCP8.5. An aging population, with the proportion of the population aged 65 years and above increased from 8% in 2010 to 24%-33% in 2050, will substantially amplify future ozone-related mortality, leading to a net increase of 23,838 to 78,560 deaths (110% to 363%). Our analysis was mainly limited by using a single global chemistry-climate model and the statistical downscaling approach to project ozone changes under climate change. CONCLUSIONS: Our analysis shows increased future ozone-related acute excess mortality under the high global warming and emission scenario RCP8.5 for an aging population in China. Comparison with the lower global warming and emission scenario RCP4.5 suggests that climate change mitigation measures are needed to prevent a rising health burden from exposure to ambient ozone pollution in China.

Investigating the causes of increased 20th-century fall precipitation over the southeastern United States.

Much of the eastern United States (US) experienced increased precipitation over the 20th century. Characterizing these trends and their causes is critical for assessing future hydroclimate risks. Here, US precipitation trends are analyzed during 1895-2016, revealing that fall precipitation in the southeastern region north of the Gulf of Mexico (SE-Gulf) increased by nearly 40%, primarily increasing after the mid-1900s. As fall is the climatological dry season in the SE-Gulf and precipitation in other seasons changed insignificantly, the seasonal precipitation cycle diminished substantially. The increase in SE-Gulf fall precipitation was caused by increased southerly moisture transport from the Gulf of Mexico, which was almost entirely driven by stronger winds associated with enhanced anticyclonic circulation west of the North Atlantic Subtropical High (NASH) and not by increases in specific humidity. Atmospheric models forced by observed SSTs and fully-coupled models forced by historical anthropogenic forcing do not robustly simulate 20th-century fall wetting in the SE-Gulf. SST-forced atmospheric models do simulate an intensified anticyclonic low-level circulation around the NASH, but the modeled intensification occurred farther west than observed. CMIP5 analyses suggest an increased likelihood of positive SE-Gulf fall precipitation trends given historical and future GHG forcing. Nevertheless, individual model simulations (both SST-forced and fully-coupled) only very rarely produce the observed magnitude of the SE-Gulf fall precipitation trend. Further research into model representation of the western ridge of the fall NASH is needed, which will help us better predict whether 20th-century increases in SE-Gulf fall precipitation will persist into the future.

Evaluating a Space-Based Indicator of Surface Ozone-NO x -VOC Sensitivity Over Midlatitude Source Regions and Application to Decadal Trends.

Determining effective strategies for mitigating surface ozone (O3) pollution requires knowledge of the relative ambient concentrations of its precursors, NO x , and VOCs. The space-based tropospheric column ratio of formaldehyde to NO2 (FNR) has been used as an indicator to identify NO x -limited versus NO x -saturated O3 formation regimes. Quantitative use of this indicator ratio is subject to three major uncertainties: (1) the split between NO x -limited and NO x -saturated conditions may shift in space and time, (2) the ratio of the vertically integrated column may not represent the near-surface environment, and (3) satellite products contain errors. We use the GEOS-Chem global chemical transport model to evaluate the quantitative utility of FNR observed from the Ozone Monitoring Instrument over three northern midlatitude source regions. We find that FNR in the model surface layer is a robust predictor of the simulated near-surface O3 production regime. Extending this surface-based predictor to a column-based FNR requires accounting for differences in the HCHO and NO2 vertical profiles. We compare four combinations of two OMI HCHO and NO2 retrievals with modeled FNR. The spatial and temporal correlations between the modeled and satellite-derived FNR vary with the choice of NO2 product, while the mean offset depends on the choice of HCHO product. Space-based FNR indicates that the spring transition to NO x -limited regimes has shifted at least a month earlier over major cities (e.g., New York, London, and Seoul) between 2005 and 2015. This increase in NO x sensitivity implies that NO x emission controls will improve O3 air quality more now than it would have a decade ago.

Air quality and climate connections.

UNLABELLED: Multiple linkages connect air quality and climate change. Many air pollutant sources also emit carbon dioxide (CO2), the dominant anthropogenic greenhouse gas (GHG). The two main contributors to non-attainment of U.S. ambient air quality standards, ozone (O3) and particulate matter (PM), interact with radiation, forcing climate change. PM warms by absorbing sunlight (e.g., black carbon) or cools by scattering sunlight (e.g., sulfates) and interacts with clouds; these radiative and microphysical interactions can induce changes in precipitation and regional circulation patterns. Climate change is expected to degrade air quality in many polluted regions by changing air pollution meteorology (ventilation and dilution), precipitation and other removal processes, and by triggering some amplifying responses in atmospheric chemistry and in anthropogenic and natural sources. Together, these processes shape distributions and extreme episodes of O3 and PM. Global modeling indicates that as air pollution programs reduce SO2 to meet health and other air quality goals, near-term warming accelerates due to "unmasking" of warming induced by rising CO2. Air pollutant controls on CH4, a potent GHG and precursor to global O3 levels, and on sources with high black carbon (BC) to organic carbon (OC) ratios could offset near-term warming induced by SO2 emission reductions, while reducing global background O3 and regionally high levels of PM. Lowering peak warming requires decreasing atmospheric CO2, which for some source categories would also reduce co-emitted air pollutants or their precursors. Model projections for alternative climate and air quality scenarios indicate a wide range for U.S. surface O3 and fine PM, although regional projections may be confounded by interannual to decadal natural climate variability. Continued implementation of U.S. NOx emission controls guards against rising pollution levels triggered either by climate change or by global emission growth. Improved accuracy and trends in emission inventories are critical for accountability analyses of historical and projected air pollution and climate mitigation policies. IMPLICATIONS: The expansion of U.S. air pollution policy to protect climate provides an opportunity for joint mitigation, with CH4 a prime target. BC reductions in developing nations would lower the global health burden, and for BC-rich sources (e.g., diesel) may lessen warming. Controls on these emissions could offset near-term warming induced by health-motivated reductions of sulfate (cooling). Wildfires, dust, and other natural PM and O3 sources may increase with climate warming, posing challenges to implementing and attaining air quality standards. Accountability analyses for recent and projected air pollution and climate control strategies should underpin estimated benefits and trade-offs of future policies.