Biomass burning nitrogen dioxide emissions derived from space with TROPOMI: methodology and validation

Atmospheric measurement techniques, Journal Year: 2021, Volume and Issue: 14(12), P. 7929 - 7957

Published: Dec. 21, 2021

Abstract. Smoke from wildfires is a significant source of air pollution, which can adversely impact quality and ecosystems downwind. With the recently increasing intensity severity wildfires, threat to expected increase. Satellite-derived biomass burning emissions fill in gaps absence aircraft or ground-based measurement campaigns help improve online calculation as well inventories that feed models. This study focuses on satellite-derived NOx using high-spatial-resolution TROPOspheric Monitoring Instrument (TROPOMI) NO2 dataset. Advancements improvements satellite-based determination forest fire are discussed, including information plume height effects aerosol scattering absorption satellite-retrieved vertical column densities. Two common top-down emission estimation methods, (1) an exponentially modified Gaussian (EMG) (2) flux method, applied synthetic data determine accuracy sensitivity different parameters, wind fields, satellite sampling, noise, lifetime, spread. These tests show be accurately estimated single TROPOMI overpasses. The effect smoke aerosols columns (via mass factors, AMFs) estimated, these estimates compared observations four measuring plumes 2018 2019 North America. Our results indicate applying explicit correction improves agreement with (by about 10 %–25 %). aircraft- good within uncertainties. Both methods work well; however, EMG method seems output more consistent has better aircraft-derived emissions. Assuming shape for various plumes, we estimate average e-folding time 2 ±1 h observations. Based chemistry transport model simulations observations, net 1.3 1.5 times greater than A factor should thus used infer retrievals NO2.

Language: Английский

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Observations and Modeling of NO_x Photochemistry and Fate in Fresh Wildfire Plumes

ACS Earth and Space Chemistry, Journal Year: 2021, Volume and Issue: 5(10), P. 2652 - 2667

Published: Sept. 13, 2021

With large primary emissions of nitrogen-containing compounds, wildfires impact the tropospheric oxidizing capacity, ozone (O3), and formation secondary organic inorganic aerosol. The fate reactive nitrogen in daytime fresh wildfire plumes was examined using airborne measurements over western U.S. during Wildfire Experiment for Cloud chemistry, Aerosol absorption, Nitrogen (WE-CAN) campaign summer 2018 together with a photochemical box model. For four sampled pseudo-Lagrangian manner, model predicts that majority emitted NOx (96 ± 2%) is converted into peroxyacetyl nitrate (PAN) (27 8%) sum gas particulate HNO3 (29 5%) within few hours plume evolution. In two highest initial HONO, default significantly underestimates observed dilution-normalized decay rate age. We investigated several potential causes this discrepancy found likely does not accurately represent suite oxidized species such as alkyl acyl peroxynitrates these fire plumes, consistent compounds measured by chemical ionization mass spectrometry. This reservoir can be similar magnitude to PAN thus represents an important uncertain impacts on downwind O3 aerosol depending whether are (APNs), nitrates (RONO2), or nitro-aromatics.

Language: Английский

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Comparison of airborne measurements of NO, NO₂, HONO, NO_y, and CO during FIREX-AQ

Atmospheric measurement techniques, Journal Year: 2022, Volume and Issue: 15(16), P. 4901 - 4930

Published: Aug. 29, 2022

Abstract. We present a comparison of fast-response instruments installed onboard the NASA DC-8 aircraft that measured nitrogen oxides (NO and NO2), nitrous acid (HONO), total reactive odd (measured both as (NOy) from sum individually species (ΣNOy)), carbon monoxide (CO) in troposphere during 2019 Fire Influence on Regional to Global Environments Air Quality (FIREX-AQ) campaign. By targeting smoke summertime wildfires, prescribed fires, agricultural burns across continental United States, FIREX-AQ provided unique opportunity investigate measurement accuracy concentrated plumes where hundreds coexist. Here, we compare NO measurements by chemiluminescence (CL) laser-induced fluorescence (LIF); NO2 CL, LIF, cavity-enhanced spectroscopy (CES); HONO CES iodide-adduct chemical ionization mass spectrometry (CIMS); CO tunable diode laser absorption (TDLAS) integrated cavity output (ICOS). Additionally, NOy using CL instrument were compared with ΣNOy (= + nitric (HNO3) acyl peroxy nitrates (APNs) submicrometer particulate nitrate (pNO3)). Other not included they either contributed minimally it (e.g., C1–C5 alkyl nitrates, nitryl chloride (ClNO2), dinitrogen pentoxide (N2O5)) or higher oxidized (NO3), non-acyl peroxynitrates, coarse-mode aerosol nitrate). The intercomparisons demonstrate following points: (1) LIF agreed well within uncertainties but potentially reduced time response for instrument; (2) uncertainties, was average 10 % higher; (3) CIMS highly correlated each fire plume transect, correlation slope vs. all 1 Hz data 1.8, which attribute reduction sensitivity high-temperature environments; (4) budget closure demonstrated flights combined 25 %. However, used fluid dynamic flow model estimate pNO3 sampling fraction through inlet variable one flight another ranged between 0.36 0.99, meaning approximately 0 %–24 may have been unaccounted be due unmeasured such organic nitrates; (5) ICOS TDLAS systematic offset averaged 2.87 ppbv; (6) integrating followed fitting values improved independent measurements.

Language: Английский

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Analysis of reduced and oxidized nitrogen-containing organic compounds at a coastal site in summer and winter

Atmospheric chemistry and physics, Journal Year: 2022, Volume and Issue: 22(5), P. 3045 - 3065

Published: March 8, 2022

Abstract. Nitrogen-containing organic compounds, which may be directly emitted into the atmosphere or form via reactions with prevalent reactive nitrogen species (e.g., NH3, NOx, NO3), have important but uncertain effects on climate and human health. Using gas liquid chromatography soft ionization high-resolution mass spectrometry, we performed a molecular-level speciation of functionalized compounds at coastal site Long Island Sound in summer (during 2018 Tropospheric Ozone Study – LISTOS campaign) winter. This region often experiences poor air quality due to emissions anthropogenic, biogenic, marine-derived their chemical transformation products. We observed range containing oxygen, nitrogen, and/or sulfur atoms resulting from these direct transformations, including photochemical aqueous-phase processing that was more pronounced winter, respectively. In both nitrogen-containing aerosols dominated distribution particle-phase ionized by our analytical techniques, 85 % 68 total measured ion abundance atom, particles included reduced functional groups amines, imines, azoles) common NOz contributors organonitrates). Reduced particle phase were frequently paired oxygen-containing elsewhere molecule, prevalence rivaled oxidized detected methods. Supplemental gas-phase measurements, collected adsorptive samplers analyzed novel chromatography-based method, suggest are possible contributing precursors particles. Altogether, this work highlights less-studied northeastern US potentially other regions similar marine source signatures.

Language: Английский

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Reactive Nitrogen Partitioning Enhances the Contribution of Canadian Wildfire Plumes to US Ozone Air Quality

Geophysical Research Letters, Journal Year: 2024, Volume and Issue: 51(15)

Published: Aug. 6, 2024

Abstract Quantifying the variable impacts of wildfire smoke on ozone air quality is challenging. Here we use airborne measurements from 2018 Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE‐CAN) to parameterize emissions reactive nitrogen (NO y ) wildfires into peroxyacetyl nitrate (PAN; 37%), NO 3 − (27%), (36%) in a global chemistry‐climate model with 13 km spatial resolution over contiguous US. The partitioning, compared emitting all as NO, reduces bias near‐fire plumes sampled by aircraft enhances downwind 5–10 ppbv when Canadian travel Washington, Utah, Colorado, Texas. Using multi‐platform observations, identify smoke‐influenced days daily maximum 8‐hr average (MDA8) 70–88 Kennewick, Salt Lake City, Denver Dallas. On these days, enhanced MDA8 5–25 ppbv, through produced remotely during plume transport locally via interactions urban emissions.

Language: Английский

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Associations Between Wildfire‐Related PM_2.5 and Intensive Care Unit Admissions in the United States, 2006–2015

GeoHealth, Journal Year: 2021, Volume and Issue: 5(5)

Published: March 16, 2021

Abstract Wildfire smoke is a growing public health concern in the United States. Numerous studies have documented associations between ambient exposure and severe patient outcomes for single‐fire seasons or limited geographic regions. However, there are few national‐scale of wildfire States, investigating Intensive Care Unit (ICU) admissions as an outcome, specifically framed around hospital operations. This study retrospectively examined wildfire‐related PM 2.5 at ZIP code with total ICU using hospitalization data set. was characterized combination kriged monitor observations satellite‐derived plume polygons from National Oceanic Atmospheric Administration's Hazard Mapping System. were acquired Premier, Inc. encompass 15%–20% all U.S. during period. Associations estimated distributed‐lag conditional Poisson model under time‐stratified case‐crossover design. We found that 10 μg/m 3 increase daily associated 2.7% (95% CI: 1.3, 4.1; p = 0.00018) 5 days later. Under stratification, positive among patients aged 0–20 60+, living Midwest Census Region, admitted years 2013–2015, non‐Black patients, though other results mixed. Following simulated 7‐day 120 event, our predict bed utilization peaking 131% 43, 239; < −5 ) over baseline. Our work suggests hospitals may need to preposition vital critical care resources when events forecast.

Language: Английский

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Carbon Monoxide in Optically Thick Wildfire Smoke: Evaluating TROPOMI Using CU Airborne SOF Column Observations

ACS Earth and Space Chemistry, Journal Year: 2022, Volume and Issue: 6(7), P. 1799 - 1812

Published: June 16, 2022

TROPOspheric Monitoring Instrument (TROPOMI) measurements of carbon monoxide (CO) vertical column enhancements in optically thick biomass burning plumes were evaluated using from the University Colorado Airborne Solar Occultation Flux (CU AirSOF) instrument during 2018 Biomass Burning Fluxes Trace Gases and Aerosols (BB-FLUX) field campaign northwestern United States. The different temporal spatial scales measurement geometries sampled aircraft satellite are actively accounted for by (1) focusing on coincident measurements, (2) comparing integrals CO across plume transects, (3) FLEXible PARTicle (FLEXPART) dispersion model to correct atmospheric transport, (4) accounting Averaging Kernels (AVK). TROPOMI is found be systematically higher relative +36% operational product (+27% preoperational product) without geospatial corrections. Consecutive transects CU AirSOF revealed significant variations between integrated (on average 28% over 30 min) sub-pixel scale. When additional corrections applied (FLEXPART, a lesser degree also AVK), bias reduced +10% (+7.2% preoperational), which insignificant within 15% uncertainty (variability among case studies, 95% confidence level). Radiative transfer simulations synthetic indicate that multiple scattering can enhance signals 5–10% at high aerosol loads, warrants further attention. Smoke strongly reduces trace gas ultraviolet visible wavelengths (by up factor 6), highlighting importance multispectral properties smoke.

Language: Английский

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The important contribution of secondary formation and biomass burning to oxidized organic nitrogen (OON) in a polluted urban area: insights from in situ measurements of a chemical ionization mass spectrometer (CIMS)

Atmospheric chemistry and physics, Journal Year: 2023, Volume and Issue: 23(15), P. 8855 - 8877

Published: Aug. 9, 2023

Abstract. To investigate the sources and formation mechanism of oxidized organic nitrogen (OON), field measurements OON were conducted using an iodide-adduct chemical ionization mass spectrometer equipped with a Filter Inlet for Gases AEROsols (FIGAERO-CIMS) during fall 2018 in megacity Guangzhou, China. Using levoglucosan as tracer biomass burning emissions, results show that (49±23 %) secondary (51±23 accounted comparable fractions to total particle-phase (pOON) but 24±25 % 76±25 gas-phase (gOON), respectively, signifying important contribution pOON gOON this urban area. Calculations production rates indicated hydroxyl radical (42 nitrate (NO3) (49 oxidation pathways potentially dominated gOON. A high concentration NO3 radicals afternoon was observed, demonstrating daytime might be more than previous recognition. Monoterpenes, found major precursors gOON, mainly from anthropogenic emissions The ratio Ox ([Ox] = [O3] + [NO2]) increased function relative humidity aerosol surface area, indicating heterogeneous reaction pathway pOON. Finally, highly 6 11 oxygen atoms highlighting complex processes ambient air. Overall, our improve understanding dynamic variation atmosphere.

Language: Английский

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The GFDL Variable‐Resolution Global Chemistry‐Climate Model for Research at the Nexus of US Climate and Air Quality Extremes

Journal of Advances in Modeling Earth Systems, Journal Year: 2024, Volume and Issue: 16(4)

Published: April 1, 2024

Abstract We present a variable‐resolution global chemistry‐climate model (AM4VR) developed at NOAA's Geophysical Fluid Dynamics Laboratory (GFDL) for research the nexus of US climate and air quality extremes. AM4VR has horizontal resolution 13 km over US, allowing it to resolve urban‐to‐rural chemical regimes, mesoscale convective systems, land‐surface heterogeneity. With gradually reducing 100 Indian Ocean, we achieve multi‐decadal simulations driven by observed sea surface temperatures 50% computational cost 25‐km uniform‐resolution grid. In contrast with GFDL's AM4.1 contributing sixth Coupled Model Intercomparison Project resolution, features much improved mean patterns variability. particular, shows representation of: precipitation seasonal‐to‐diurnal cycles extremes, notably central dry‐and‐warm bias; western snowpack summer drought, implications wildfires; North American monsoon, affecting dust storms. exhibits excellent winter precipitation, pollution meteorology in California complex terrain, enabling skillful prediction both extreme ozone haze events Central Valley. also provides vast improvements process‐level representations biogenic volatile organic compound emissions, interactive emissions from land, removal pollutants terrestrial ecosystems. highlight value increased representing climate–air interactions through land‐biosphere feedbacks. offers novel opportunity study dimensions quality, especially role Earth system feedbacks changing climate.

Language: Английский

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Changes in South American surface ozone trends: exploring the influences of precursors and extreme events

Atmospheric chemistry and physics, Journal Year: 2024, Volume and Issue: 24(14), P. 8225 - 8242

Published: July 22, 2024

Abstract. In this study, trends of 21st-century ground-level ozone and precursors were examined across South America, a less-studied region where trend estimates have rarely been comprehensively addressed. Therefore, we provided an updated regional analysis based on validated surface observations. We tested the hypothesis that recent increasing trends, mostly in urban environments, resulted from intense wildfires driven by extreme meteorological events impacting cities preexisting volatile organic compound (VOC)-limited regimes dominate. applied quantile regression method monthly anomalies to estimate quantify their uncertainties detect change points. Additionally, maximum daily 8 h average (MDA8) peak-season metrics used assess short- long-term exposure levels, respectively, for present day (2017–2021). Our results showed lower levels tropical (Bogotá Quito), varying between 39 43 nmol mol−1 short-term 26 27 exposure. contrast, mixing ratios higher extratropical (Santiago São Paulo), with level 61 40 41 mol−1. Santiago (since 2017) Paulo 2008) exhibited positive 0.6 0.3 yr−1, very high certainty. attributed these upward or no evidence variation, such as Bogotá Quito, well-established VOC-limited regime. However, greater increase percentile (≥ 90th) heat waves and, case southwestern associated events.

Language: Английский

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