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Transport-derived emissions of volatile organic compounds (VOCs) have decreased owing to stricter controls on air pollution. This means that the relative importance of chemicals in pesticides, coatings, printing inks, adhesives, cleaning agents, and personal care products has increased. McDonald et al. show that these volatile chemical products now contribute fully one-half of emitted VOCs in 33 industrialized cities (see the Perspective by Lewis). Thus, the focus of efforts to mitigate ozone formation and toxic chemical burdens need to be adjusted. Science , this issue p. 760 ; see also p. 744 Chemical products contribute as much organic air pollution as transportation emissions in many cities. A gap in emission inventories of urban volatile organic compound (VOC) sources, which contribute to regional ozone and aerosol burdens, has increased as transportation emissions in the United States and Europe have declined rapidly. A detailed mass balance demonstrates that the use of volatile chemical products (VCPs)—including pesticides, coatings, printing inks, adhesives, cleaning agents, and personal care products—now constitutes half of fossil fuel VOC emissions in industrialized cities. The high fraction of VCP emissions is consistent with observed urban outdoor and indoor air measurements. We show that human exposure to carbonaceous aerosols of fossil origin is transitioning away from transportation-related sources and toward VCPs. Existing U.S. regulations on VCPs emphasize mitigating ozone and air toxics, but they currently exempt many chemicals that lead to secondary organic aerosols.

Data from the oil- and gas-producing basin of northeastern Utah and a box model are used to assess the photochemical reactions of nitrogen oxides and volatile organic compounds that lead to excessive atmospheric ozone pollution in winter. Influence of fracking on air quality The US experience with air quality degradation from shale gas extraction presents a measurement and modelling framework relevant to similar developments in other regions projected for the near future. High ozone mixing ratios have been observed in oil and gas producing basins in the United States during winter, but the underlying chemistry involved is not fully understood. This study presents a quantitative assessment of the underlying chemistry responsible for the winter ozone pollution events based on data from an oil and gas basin in Utah and a chemical 'box model' simulation. The results show that very high volatile organic carbon concentrations optimize the ozone production efficiency of nitrogen oxides with carbonyl photolysis as a dominant oxidant source. The United States is now experiencing the most rapid expansion in oil and gas production in four decades, owing in large part to implementation of new extraction technologies such as horizontal drilling combined with hydraulic fracturing. The environmental impacts of this development, from its effect on water quality 1 to the influence of increased methane leakage on climate 2 , have been a matter of intense debate. Air quality impacts are associated with emissions of nitrogen oxides 3 , 4 (NO x = NO + NO 2 ) and volatile organic compounds 5 , 6 , 7 (VOCs), whose photochemistry leads to production of ozone, a secondary pollutant with negative health effects 8 . Recent observations in oil- and gas-producing basins in the western United States have identified ozone mixing ratios well in excess of present air quality standards, but only during winter 9 , 10 , 11 , 12 , 13 . Understanding winter ozone production in these regions is scientifically challenging. It occurs during cold periods of snow cover when meteorological inversions concentrate air pollutants from oil and gas activities, but when solar irradiance and absolute humidity, which are both required to initiate conventional photochemistry essential for ozone production, are at a minimum. Here, using data from a remote location in the oil and gas basin of northeastern Utah and a box model, we provide a quantitative assessment of the photochemistry that leads to these extreme winter ozone pollution events, and identify key factors that control ozone production in this unique environment. We find that ozone production occurs at lower NO x and much larger VOC concentrations than does its summertime urban counterpart, leading to carbonyl (oxygenated VOCs with a C = O moiety) photolysis as a dominant oxidant source. Extreme VOC concentrations optimize the ozone production efficiency of NO x . There is considerable potential for global growth in oil and gas extraction from shale. This analysis could help inform strategies to monitor and mitigate air quality impacts and provide broader insight into the response of winter ozone to primary pollutants.

Total 550 nm aerosol optical depth (AOD) retrievals from Moderate Resolution Imaging Spectroradiometer (MODIS) sensors and surface fine particulate matter (PM2.5) observations were assimilated with the National Centers for Environmental Prediction (NCEP) Gridpoint Statistical Interpolation (GSI) three‐dimensional variational (3DVAR) data assimilation (DA) system. Parallel experiments assimilated AOD and surface PM2.5observations both individually and simultaneously. New 3DVAR aerosol analyses were produced every 6 h between 0000 UTC 01 June and 1800 UTC 14 July 2010 over a domain encompassing the continental United States. The analyses initialized Weather Research and Forecasting‐Chemistry (WRF‐Chem) model forecasts. Assimilating AOD, either alone or in conjunction with PM2.5 observations, produced better AOD forecasts than a control experiment that did not perform DA. Additionally, individual assimilation of both AOD and PM2.5 improved surface PM2.5 forecasts compared to when no DA occurred. However, the best PM2.5 forecasts were produced when both AOD and PM2.5 were assimilated. Considering the goodness of both AOD and PM2.5 forecasts, the results unequivocally show that concurrent DA of PM2.5 and AOD observations produced the best overall forecasts, illustrating how simultaneous DA of different aerosol observations can work synergistically to improve aerosol forecasts. Key Points Simultaneous 3DVAR data assimilation of MODIS AOD and surface PM2.5 observations Aerosol data assimilation substantially improves aerosol forecasts Forecasts are best when both AOD and surface PM2.5 are assimilated concurrently

During the Deepwater Horizon (DWH) oil spill, a wide range of gas and aerosol species were measured from an aircraft around, downwind, and away from the DWH site. Additional hydrocarbon measurements were made from ships in the vicinity. Aerosol particles of respirable sizes were on occasions a significant air quality issue for populated areas along the Gulf Coast. Yields of organic aerosol particles and emission factors for other atmospheric pollutants were derived for the sources from the spill, recovery, and cleanup efforts. Evaporation and subsequent secondary chemistry produced organic particulate matter with a mass yield of 8 ± 4% of the oil mixture reaching the water surface. Approximately 4% by mass of oil burned on the surface was emitted as soot particles. These yields can be used to estimate the effects on air quality for similar events as well as for this spill at other times without these data. Whereas emission of soot from burning surface oil was large during the episodic burns, the mass flux of secondary organic aerosol to the atmosphere was substantially larger overall. We use a regional air quality model to show that some observed enhancements in organic aerosol concentration along the Gulf Coast were likely due to the DWH spill. In the presence of evaporating hydrocarbons from the oil, NO ₓ emissions from the recovery and cleanup operations produced ozone.

Decades of air quality improvements have substantially reduced the motor vehicle emissions of volatile organic compounds (VOCs). Today, volatile chemical products (VCPs) are responsible for half of the petrochemical VOCs emitted in major urban areas. We show that VCP emissions are ubiquitous in US and European cities and scale with population density. We report significant VCP emissions for New York City (NYC), including a monoterpene flux of 14.7 to 24.4 kg · d−1 · km−2 from fragranced VCPs and other anthropogenic sources, which is comparable to that of a summertime forest. Photochemical modeling of an extreme heat event, with ozone well in excess of US standards, illustrates the significant impact of VCPs on air quality. In the most populated regions of NYC, ozone was sensitive to anthropogenic VOCs (AVOCs), even in the presence of biogenic sources. Within this VOC-sensitive regime, AVOCs contributed upwards of ∼20 ppb to maximum 8-h average ozone. VCPs accounted for more than 50% of this total AVOC contribution. Emissions from fragranced VCPs, including personal care and cleaning products, account for at least 50% of the ozone attributed to VCPs. We show that model simulations of ozone depend foremost on the magnitude of VCP emissions and that the addition of oxygenated VCP chemistry impacts simulations of key atmospheric oxidation products. NYC is a case study for developed megacities, and the impacts of VCPs on local ozone are likely similar for other major urban regions across North America or Europe.

The Green Ocean Amazon experiment – GoAmazon 2014–2015 – explored the interactions between natural biogenic forest emissions from central Amazonia and urban air pollution from Manaus. Previous GoAmazon 2014–2015 studies showed that nitrogen oxide (NOx = NO + NO2) and sulfur oxide (SOx) emissions from Manaus strongly interact with biogenic volatile organic compounds (BVOCs), affecting secondary organic aerosol (SOA) formation. In previous studies, ground-based and aircraft measurements provided evidence of SOA formation and strong changes in aerosol composition and properties. Aerosol optical properties also evolve, and their impacts on the Amazonian ecosystem can be significant. As particles age, some processes, such as SOA production, black carbon (BC) deposition, particle growth and the BC lensing effect change the aerosol optical properties, affecting the solar radiation flux at the surface. This study analyzes data and models SOA formation using the Weather Research and Forecasting with Chemistry (WRF-Chem) model to assess the spatial variability in aerosol optical properties as the Manaus plumes interact with the natural atmosphere. The following aerosol optical properties are investigated: single scattering albedo (SSA), asymmetry parameter (gaer), absorption Ångström exponent (AAE) and scattering Ångström exponent (SAE). These simulations were validated using ground-based measurements at three experimental sites, namely the Amazon Tall Tower Observatory – ATTO (T0a), downtown Manaus (T1), Tiwa Hotel (T2) and Manacapuru (T3), as well as the U.S. Department of Energy (DOE) Gulfstream 1 (G-1) aircraft flights. WRF-Chem simulations were performed over 7 d during March 2014. Results show a mean biogenic SOA (BSOA) mass enrichment of 512 % at the T1 site, 450 % in regions downwind of Manaus, such as the T3 site, and 850 % in areas north of the T3 site in simulations with anthropogenic emissions. The SOA formation is rather fast, with about 80 % of the SOA mass produced in 3–4 h. Comparing the plume from simulations with and without anthropogenic emissions, SSA shows a downwind reduction of approximately 10 %, 11 % and 6 % at the T1, T2 and T3 sites, respectively. Other regions, such as those further downwind of the T3 site, are also affected. The gaer values increased from 0.62 to 0.74 at the T1 site and from 0.67 to 0.72 at the T3 site when anthropogenic emissions are active. During the Manaus plume-aging process, a plume tracking analysis shows an increase in SSA from 0.91 close to Manaus to 0.98 160 km downwind of Manaus as a result of SOA production and BC deposition.

The National Oceanic and Atmospheric Administration (NOAA)'s National Weather Service (NWS) is on its way to deploying various operational prediction applications using the Unified Forecast System (https://ufscommunity.org/, last access: 18 June 2022), a community-based coupled, comprehensive Earth modeling system. An aerosol model component developed in collaboration between the Global Systems Laboratory, Chemical Science Laboratory, Air Resources Laboratory, and Environmental Modeling Center (GSL, CSL, ARL, EMC) was coupled online with the FV3 Global Forecast System (FV3GFS) using the National Unified Operational Prediction Capability (NUOPC)-based NOAA Environmental Modeling System (NEMS) software framework. This aerosol prediction system replaced the NEMS GFS Aerosol Component version 2 (NGACv2) system in the National Center for Environment Prediction (NCEP) production suite in September 2020 as one of the ensemble members of the Global Ensemble Forecast System (GEFS), dubbed GEFS-Aerosols v1. The aerosol component of atmospheric composition in the GEFS is based on the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). GEFS-Aerosols includes bulk modules from the Goddard Chemistry Aerosol Radiation and Transport model (GOCART). Additionally, the biomass burning plume rise module from High-Resolution Rapid Refresh (HRRR)-Smoke based on WRF-Chem was implemented. The GOCART dust scheme was replaced by the FENGSHA dust scheme (developed by ARL). The Blended Global Biomass Burning Emissions Product (GBBEPx version 3) provides biomass burning emission and fire radiative power (FRP) data. The global anthropogenic emission inventories are derived from the Community Emissions Data System (CEDS). All sub-grid-scale transport and deposition are handled inside the atmospheric physics routines, which required consistent implementation of positive definite tracer transport and wet scavenging in the physics parameterizations used by the NCEP's operational FV3GFS. This paper describes the details of GEFS-Aerosols model development and evaluation of real-time and retrospective runs using different observations from in situ measurement and satellite and aircraft data. GEFS-Aerosols predictions demonstrate substantial improvements for both composition and variability of aerosol distributions over those from the former operational NGACv2 system with the fundamental updates (e.g., dust and fire emission) in the atmospheric and chemical transport model.

The global Flow-following finite-volume Icosahedral Model (FIM), which was developed in the Global Systems Laboratory (GSL) of NOAA, has been coupled inline with aerosol and gas-phase chemistry schemes of different complexity using the chemistry and aerosol packages from WRF-Chem v3.7, named FIM-Chem v1. The three chemistry schemes include (1) the simple aerosol modules from the Goddard Chemistry Aerosol Radiation and Transport model that includes only simplified sulfur chemistry, black carbon (BC), organic carbon (OC), and sectional dust and sea salt modules (GOCART); (2) the photochemical gas phase of the Regional Atmospheric Chemistry Mechanism (RACM) coupled to GOCART to determine the impact of more realistic gas-phase chemistry on the GOCART aerosol simulations (RACM_GOCART); and (3) a further sophistication within the aerosol modules by replacing GOCART with a modal aerosol scheme that includes secondary organic aerosols (SOAs) based on the volatility basis set (VBS) approach (RACM_SOA_VBS). FIM-Chem is able to simulate aerosol, gas-phase chemical species, and SOA at various spatial resolutions with different levels of complexity and quantify the impact of aerosol on numerical weather prediction (NWP). We compare the results of RACM_GOCART and GOCART schemes which use the default climatological model fields for OH,H2O2, and NO3. We find significant reductions of sulfate that are on the order of 40 % to 80 % over the eastern US and are up to 40 % near the Beijing region over China when using the RACM_GOCART scheme. We also evaluate the model performance by comparing it with the Atmospheric Tomography Mission (ATom-1) aircraft measurements in the summer of 2016. FIM-Chem shows good performance in capturing the aerosol and gas-phase tracers. The model-predicted vertical profiles of biomass burning plumes and dust plumes off western Africa are also reproduced reasonably well.

In September 2020, a global aerosol forecasting model was implemented as an ensemble member of the National Oceanic and Atmospheric Administration (NOAA) National Centers for Environmental Prediction (NCEP) Global Ensemble Forecasting System (GEFS) v12.0.1 (hereafter referred to as “GEFS-Aerosols”). In this study, GEFS-Aerosols simulation results from 1 September 2019 to 30 September 2020 were evaluated using an aerosol budget analysis. These results were compared with results from other global models as well as reanalysis data. From this analysis, the global average lifetimes of black carbon (BC), organic carbon (OC), dust, sea salt, and sulfate are 4.06, 4.29, 4.59, 0.34, and 3.3 d, respectively, with the annual average loads of 0.14, 1.29, 4.52, 6.80, and 0.51 Tg. Compared with the National Aeronautics and Space Administration (NASA) Goddard Earth Observing System–Goddard Chemistry Aerosol and Radiation Transport (GEOS4-GOCART) model, the aerosols in GEFS-Aerosols have a relatively short lifetime because of the faster removal processes in GEFS-Aerosols. Meanwhile, in GEFS-Aerosols, aerosol emissions are the determining factor for the mass and composition of aerosols in the atmosphere. The size (bin) distribution of aerosol emissions is as important as its total emissions, especially in simulations of dust and sea salt. Moreover, most importantly, the strong monthly and interannual variations in natural sources of aerosols in GEFS-Aerosols suggest that improving the accuracy of the prognostic concentrations of aerosols is important for applying aerosol feedback to weather and climate predictions.

In this paper, solar irradiance forecasts made by mesoscale numerical weather prediction models are compared with observations taken during three air-quality experiments in various parts of the United States. The authors evaluated the fifth-generation Pennsylvania State University–National Center for Atmospheric Research (PSU–NCAR) Mesoscale Model (MM5) and the National Centers for Environmental Prediction (NCEP) Eta Model. The observations were taken during the 2000 Texas Air Quality Experiment (TexAQS), the 2000 Central California Ozone Study (CCOS), and the New England Air Quality Study (NEAQS) 2002. The accuracy of the model forecast irradiances show a strong dependence on the aerosol optical depth. Model errors on the order of 100 W m −2 are possible when the aerosol optical depth exceeds 0.1. For smaller aerosol optical depths, the climatological attenuation used in the models yields solar irradiance estimates that are in good agreement with the observations.