Effects of Fire Diurnal Variation and Plume Rise on U.S. Air Quality During FIREX‐AQ and WE‐CAN Based on the Multi‐Scale Infrastructure for Chemistry and Aerosols (MUSICAv0)

Journal of Geophysical Research Atmospheres, Journal Year: 2022, Volume and Issue: 127(16)

Published: Aug. 12, 2022

Abstract We analyze the effects of diurnal cycle fire emissions (DCFE) and plume rise on U.S. air quality using MUSICAv0 (Multi‐Scale Infrastructure for Chemistry Aerosols Version 0) model during FIREX‐AQ (Fire Influence Regional to Global Environments Air Quality) WE‐CAN (Western wildfire Experiment Cloud chemistry, Aerosol absorption Nitrogen) field campaigns. To include DCFE in model, we employ two approaches: a climatology derived from satellite radiative power product. also implemented sets plume‐rise climatologies, parameterizations. evaluate performance with airborne measurements, EPA Quality System surface products. Overall, including improves agreement observations such as aircraft CO NO x WE‐CAN. Applying performance, PM 2.5 fire‐impacted regions. The impact is larger than DCFE. Plume can greatly enhance modeled long‐range transport fire‐emitted pollutants. simulations parameterizations generally perform better climatologies FIREX‐AQ, but not 2019 Williams Flats Fire case study demonstrates that change impacts because are subject different meteorology chemistry when emitted at times day altitudes. Moreover, local‐to‐regional chemical reaction rates. will be included future MUSICA versions.

Language: Английский

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Evaluating the Impact of Chemical Complexity and Horizontal Resolution on Tropospheric Ozone Over the Conterminous US With a Global Variable Resolution Chemistry Model

Journal of Advances in Modeling Earth Systems, Journal Year: 2022, Volume and Issue: 14(6)

Published: May 21, 2022

A new configuration of the Community Earth System Model (CESM)/Community Atmosphere with full chemistry (CAM-chem) supporting capability horizontal mesh refinement through use spectral element (SE) dynamical core is developed and called CESM/CAM-chem-SE. Horizontal in CESM/CAM-chem-SE unique novel that pollutants such as ozone are accurately represented at human exposure relevant scales while also directly including global feedbacks. down to ∼14 km over conterminous US (CONUS) beginning Multi-Scale Infrastructure for Chemistry Aerosols (MUSICAv0). Here, MUSICAv0 evaluated used better understand how resolution chemical complexity impact precursors CONUS compared measurements from five aircraft campaigns, which occurred 2013. This field campaign analysis demonstrates importance using finer simulate nitrogen oxides carbon monoxide. In general, more complex on other oxidation products pronounced when where a larger number regimes resolved. Large model biases near surface remain Southeast observations even updated resolution. suggests need adding replacing sections emission inventories regional inventories, increasing vertical planetary boundary layer, reducing meteorological variables temperature clouds.

Language: Английский

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Nitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO₂ measurements

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(2), P. 1227 - 1257

Published: Jan. 24, 2023

Abstract. Satellite-based retrievals of tropospheric NO2 columns are widely used to infer NOx (≡ NO + NO2) emissions. These rely on model information for the vertical distribution NO2. The free background above 2 km is particularly important because sensitivity increases with altitude. Free also has a strong effect OH and ozone concentrations. Here we use observations from three aircraft campaigns (SEAC4RS, DC3, ATom) four atmospheric chemistry models (GEOS-Chem, GMI, TM5, CAMS) evaluate capabilities simulating in troposphere attribute it sources. measurements during Studies Emissions Atmospheric Composition, Clouds, Climate Coupling by Regional Surveys (SEAC4RS) Deep Convective Clouds Chemistry (DC3) over southeastern U.S. summer show increasing concentrations upper 10 km, which not replicated GEOS-Chem, although consistent measurements. Using concurrent NO, NO2, DC3 flight thunderstorm outflow, that biased high, plausibly due interference thermally labile reservoirs such as peroxynitric acid (HNO4) methyl peroxy nitrate (MPN). We find calculated NO–NO2 photochemical steady state (PSS) more reliable profiles models. GEOS-Chem reproduces shape PSS-inferred throughout SEAC4RS but overestimates about factor 2. underestimates MPN alkyl concentrations, suggesting missing organic chemistry. On other hand, standard Tomography Mission (ATom) Pacific Atlantic oceans, indicating source oceans. can account this including photolysis particulate sea salt aerosols at rates inferred laboratory studies field nitrous (HONO) Atlantic. median column density ATom campaign 1.7 ± 0.44 × 1014 molec. cm−2, simulated range 1.4–2.4 implying uncertainty using modeled clean areas stratosphere–troposphere separation 1 cm−2. lightning main primary tropics southern midlatitudes, emissions dominate northern midlatitudes winter Particulate up 5 ppbv (parts per billion volume) extratropics model, would largely correct low bias relative ozonesonde observations. Global increase 19 %. contribution observed satellites contiguous 25 11 % 65 9 summer, according profiles. This needs be accounted when deriving satellite

Language: Английский

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One-third of global population at cancer risk due to elevated volatile organic compounds levels

npj Climate and Atmospheric Science, Journal Year: 2024, Volume and Issue: 7(1)

Published: March 1, 2024

Abstract Outdoor air pollution, particularly volatile organic compounds (VOCs), significantly contributes to the global health burden. Previous analyses of VOC exposure have typically focused on regional and national scales, thereby limiting burden assessments. In this study, we utilized a chemistry-climate model simulate distributions estimate related cancer risks from 2000 2019. Our findings indicated 10.2% rise in emissions during period, with substantial increases Sub-Saharan Africa, Rest Asia, China, but decreases U.S. Europe due reductions transportation residential sectors. Carcinogenic VOCs such as benzene, formaldehyde, acetaldehyde contributed lifetime affecting 0.60 [95% confidence interval (95CI): 0.40–0.81] 0.85 [95CI: 0.56–1.14] million individuals globally. We projected that between 36.4% 39.7% population was exposed harmful levels, highest rates found China (82.8–84.3%) considerably lower (1.7–5.8%). Open agricultural burning less-developed regions amplified VOC-induced burdens. Significant disparities burdens high-income low-to-middle-income countries were identified throughout study primarily unequal growth emissions. These underscore among different income nations emphasize persistent need address environmental injustice pollution exposure.

Language: Английский

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Evaluating NO_x emissions and their effect on O₃ production in Texas using TROPOMI NO₂ and HCHO

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(16), P. 10875 - 10900

Published: Aug. 26, 2022

Abstract. The Tropospheric Monitoring Instrument (TROPOMI) on the Sentinel-5 Precursor (S5P) satellite is a valuable source of information to monitor NOx emissions that adversely affect air quality. We conduct series experiments using 4×4 km2 Comprehensive Air Quality Model with Extensions (CAMx) simulation during April–September 2019 in eastern Texas evaluate multiple challenges arise from reconciling model simulations TROPOMI. find an increase NO2 (+17 % urban areas) when transitioning TROPOMI version 1.3 algorithm 2.3.1 Texas, greatest difference (+25 %) city centers and smaller differences (+5 less polluted areas. lightning contribute up 24 column areas over Gulf Mexico 8% inventories, locally resolved inputs, agree derived within 20 most circumstances, small underestimate Dallas–Fort Worth (−13 Houston (−20 %). In vicinity large power plant plumes (e.g., Martin Lake Limestone) we larger disagreements, i.e., consistently by 40 %–60 than modeled NO2, which incorporates measured stack emissions. having difficulty distinguishing attributed plants background concentrations – area atmospheric conditions cause short lifetimes. Second, NOx/NO2 ratio may be underestimated due 4 km grid cell size. To understand ozone formation regimes area, combine formaldehyde (HCHO) information. modest low biases relative HCHO, −9 −21 central lower biogenic volatile organic compound (VOC) Ozone at time early afternoon overpass are limited almost everywhere domain, except along Ship Channel, near Dallas/Fort International airport, presence undiluted plumes. There likely NOx-saturated morning hours cannot observe would well-suited for analysis HCHO upcoming TEMPO (Tropospheric Emissions: Pollution) mission. This study highlights measurements offer means validate inventories regimes, important limitations.

Language: Английский

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Ozone in the Desert Southwest of the United States: A Synthesis of Past Work and Steps Ahead

ACS ES&T Air, Journal Year: 2024, Volume and Issue: 1(2), P. 62 - 79

Published: Jan. 24, 2024

A region often neglected in the grander scale of general atmospheric chemistry studies and model evaluation for gas-phase is desert southwest U.S. Despite regulatory progress, challenges meeting National Ambient Air Quality Standard ozone motivate a re-examination unique meteorological conditions, interactions between desert, agricultural, built environmental landscapes, emissions across natural anthropogenic sources, regional transport precursors that govern formation Southwest. Arizona includes multiple nonattainment counties with situation terms its environment (e.g., vegetation, meteorology, fire prone areas), complex terrain, urban growth, vulnerability, limited knowledge base. Here we summarize past works investigating over Arizona, including 61 peer-reviewed publications found since first one 1996, determine significant gaps to guide future research aim improving policy. more in-depth focus placed here on Maricopa County, which Phoenix Metropolitan area, where population growth recent decades coupled extreme high temperatures surrounding terrain creates poorly understood airshed chemistry, thereby complicating decisions. We suggest paths forward, improved monitoring, assessment, modeling tools region, better leveraging archived data, engagement public, government, This Review highly relevant as well other semiarid arid regions, represent most common land type globally, warranting attention.

Language: Английский

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Reducing Long‐Standing Surface Ozone Overestimation in Earth System Modeling by High‐Resolution Simulation and Dry Deposition Improvement

Journal of Advances in Modeling Earth Systems, Journal Year: 2025, Volume and Issue: 17(3)

Published: March 1, 2025

Abstract The overestimation of surface ozone concentration in low‐resolution global atmospheric chemistry and climate models has been a long‐standing issue. We first update the dry deposition scheme both high‐ (0.25°) (1°) Community Earth System Model (CESM) version 1.3 runs, by adding effects leaf area index correcting sunlit shaded fractions stomatal resistances. With this update, 5‐year‐long summer simulations (2015–2019) using CESM still exhibit substantial (by 6.0–16.2 ppbv) over U.S., Europe, eastern China, pollution hotspots. is further improved adjusting cuticle conductance, reducing mean bias 19%, increasing model resolution reduces 43%. elucidate mechanism which grid spacing influences simulated ozone, revealing distinctive pathways urban versus rural areas. In areas, mainly affects daytime levels, where additional NO x emissions from nearby areas result an boost simulations. contrast, follows similar due to influence volatile organic compounds surrounding However, nighttime closely linked weakened titration owing redistribution Additionally, stratosphere‐troposphere exchange may also contribute high‐resolution simulations, warranting investigation. This optimized enhance understanding formation mechanisms, sources, changes warming climate.

Language: Английский

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Comparison of Urban Air Quality Simulations During the KORUS‐AQ Campaign With Regionally Refined Versus Global Uniform Grids in the Multi‐Scale Infrastructure for Chemistry and Aerosols (MUSICA) Version 0

Journal of Advances in Modeling Earth Systems, Journal Year: 2023, Volume and Issue: 15(7)

Published: July 1, 2023

Abstract Model intercomparison studies often report a large spread in simulation results, but quantifying the causes of these differences is hindered by fact that several processes contribute to model simultaneously. Here we use Multi‐Scale Infrastructure for Chemistry and Aerosols (MUSICA) version 0 investigate resolution dependencies simulated chemical species, with focus on between global uniform grid regional refinement simulations same modeling framework. We construct two (ne30 [∼112 km] ne60 [∼56 km]) grids over Korea (ne30x8 [∼14 ne30x16 [∼7 km]). The can change concentrations an order magnitude boundary layer, importance increases as species' reactivity (e.g., up 50% 1,000% changes ethane xylenes, respectively). diurnal cycle oxidants (OH, O 3 , NO ) also varies resolution, which leads different oxidation pathways volatile organic compounds fraction monoterpenes reacting Seoul around midnight 90% ne30, 65% ne30x16). models high‐resolution usually do better job at reproducing aircraft observations during KORUS‐AQ campaign, not always, implying compensating errors coarse simulations. For example, ozone reproduced due artificial mixing x . When developing new mechanisms evaluating urban areas, uncertainties associated should be considered.

Language: Английский

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Impacts of changes in climate, land use, and emissions on global ozone air quality by mid-21st century following selected Shared Socioeconomic Pathways

The Science of The Total Environment, Journal Year: 2023, Volume and Issue: 906, P. 167759 - 167759

Published: Oct. 11, 2023

Surface ozone (O

Language: Английский

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Global Health and Climate Effects of Organic Aerosols from Different Sources

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(37), P. 13793 - 13807

Published: Sept. 6, 2023

The impact of aerosols on human health and climate is well-recognized, yet many studies have only focused total PM2.5 or changes from anthropogenic activities. This study quantifies the effects organic (OA) anthropogenic, biomass burning, biogenic sources. Using two atmospheric chemistry models, CAM-chem GEOS-Chem, our findings reveal that primary OA (POA) has highest efficiency for but lowest direct radiative due to spatial temporal variations associated with population surface albedo. treatment POA as nonvolatile semivolatile also influences these efficiencies through different chemical processes. Biogenic shows moderate indirect reduced high cloud, caused by stabilized temperature profiles aerosol-radiation interactions in OA-rich regions. Biomass burning important cloud effect remote atmospheres its ability be transported further than other OAs. highlights importance not characteristics such toxicity refractive index processes transport determining efficiencies.

Language: Английский

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