Nitrogen oxides in the free troposphere: Implications for tropospheric oxidants and the interpretation of satellite NO2 measurements DOI Creative Commons
Viral Shah, Daniel J. Jacob, Ruijun Dang

и другие.

Опубликована: Июль 21, 2022

Abstract. Satellite-based retrievals of tropospheric NO2 columns are used to infer NOx (NO+NO2) emissions at the surface. These rely on model information for 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 attribute this sources. measurements over southeast US during SEAC4RS DC3 show increasing concentrations in upper troposphere 10 km, which not replicated by GEOS-Chem although consistent NO measurements. Using concurrent NO, 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. reproduces shape PSS-inferred throughout but overestimates about factor 2. underestimates MPN alkyl concentrations, suggesting missing organic chemistry. On other hand, standard ATom Pacific Atlantic Oceans, indicating source oceans. can account including photolysis particulate sea salt aerosols rates inferred laboratory studies field nitrous (HONO) Atlantic. average column density campaign simulation 2.4×1014 molec cm-2 1.5×1014 without, compared 1.9×1014 (using PSS NO2) 1.4–2.4×1014 TM5 CAMS lightning main primary tropics southern midlatitudes, dominate northern midlatitudes winter summer Particulate up 5 ppbv extratropics model, would largely correct low bias relative ozonesonde observations. Global increase 19 %. contribution observed satellites contiguous 25 % 65 according profiles. This needs be accounted when deriving satellite

Язык: Английский

The Fire Inventory from NCAR version 2.5: an updated global fire emissions model for climate and chemistry applications DOI Creative Commons
Christine Wiedinmyer, Yosuke Kimura,

Elena McDonald‐Buller

и другие.

Geoscientific model development, Год журнала: 2023, Номер 16(13), С. 3873 - 3891

Опубликована: Июль 12, 2023

Abstract. We present the Fire Inventory from National Center for Atmospheric Research (NCAR) version 2.5 (FINNv2.5), a fire emissions inventory that provides publicly available of trace gases and aerosols various applications, including use in global regional atmospheric chemistry modeling. FINNv2.5 includes numerous updates to FINN 1 framework better represent burned area, vegetation burned, chemicals emitted. Major changes include active detections Visible Infrared Imaging Radiometer Suite (VIIRS) at 375 m spatial resolution, which allows smaller fires be included processing. The calculation area has been updated such more rigorous approach is used aggregate detections, accounts larger enables using multiple satellite products simultaneously estimates. Fuel characterization factors have also FINNv2.5. Daily many are determined 2002–2019 (Moderate Resolution Spectroradiometer (MODIS)-only detections) 2012–2019 (MODIS + VIIRS detections). non-methane organic gas allocated species several commonly chemical mechanisms. compare against other widely inventories. performance as inputs transport model assessed with observations. Uncertainties estimates remain, particularly Africa South America during August–October southeast equatorial Asia March April. Recommendations future evaluation given.

Язык: Английский

Процитировано

95

Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) DOI Creative Commons
C. Warneke, Joshua P. Schwarz, Jack E. Dibb

и другие.

Journal of Geophysical Research Atmospheres, Год журнала: 2022, Номер 128(2)

Опубликована: Дек. 30, 2022

Abstract The NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) experiment was a multi‐agency, inter‐disciplinary research effort to: (a) obtain detailed measurements of trace gas aerosol emissions from wildfires prescribed fires using aircraft, satellites ground‐based instruments, (b) make extensive suborbital remote sensing fire dynamics, (c) assess local, regional, global modeling fires, (d) strengthen connections observables the ground such as fuels fuel consumption satellite products burned area radiative power. From Boise, ID western were studied with NASA DC‐8 two NOAA Twin Otter aircraft. high‐altitude ER‐2 deployed Palmdale, CA observe some these in conjunction overpasses other Further conducted three mobile laboratories sites, 17 different forecast analyses for fire, air quality climate implications. Salina, KS investigated 87 smaller Southeast in‐situ data collection. Sampling by all platforms designed measure gases aerosols multiple transects capture chemical transformation perform observations smoke plumes under day night conditions. linked consumed power orbital collected during overflights sampling fuels.

Язык: Английский

Процитировано

83

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) DOI Creative Commons
Wenfu Tang, L. K. Emmons, Rebecca R. Buchholz

и другие.

Journal of Geophysical Research Atmospheres, Год журнала: 2022, Номер 127(16)

Опубликована: Авг. 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.

Язык: Английский

Процитировано

77

Nitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurements DOI Creative Commons
Viral Shah, Daniel J. Jacob, Ruijun Dang

и другие.

Atmospheric chemistry and physics, Год журнала: 2023, Номер 23(2), С. 1227 - 1257

Опубликована: Янв. 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

Язык: Английский

Процитировано

62

Airborne Emission Rate Measurements Validate Remote Sensing Observations and Emission Inventories of Western U.S. Wildfires DOI
Chelsea E. Stockwell, M. M. Bela, Matthew M. Coggon

и другие.

Environmental Science & Technology, Год журнала: 2022, Номер 56(12), С. 7564 - 7577

Опубликована: Май 17, 2022

Carbonaceous emissions from wildfires are a dynamic mixture of gases and particles that have important impacts on air quality climate. Emissions feed atmospheric models estimated using burned area fire radiative power (FRP) methods rely satellite products. These approaches show wide variability large uncertainties, their accuracy is challenging to evaluate due limited aircraft ground measurements. Here, we present novel method estimate plume-integrated total carbon speciated emission rates unique combination lidar remote sensing aerosol extinction profiles in situ measured constituents. We strong agreement between these aircraft-derived detailed area-based inventory distributes time Geostationary Operational Environmental Satellite FRP observations (Fuel2Fire inventory, slope = 1.33 ± 0.04, r2 0.93, RMSE 0.27). Other more commonly used inventories strongly correlate with but wide-ranging over- under-predictions. A correlation found monoxide those derived the TROPOspheric Monitoring Instrument (TROPOMI) for five coincident sampling windows (slope 0.99 0.18; bias 28.5%). Smoke coefficients (g MJ–1) enable direct estimations primary gas observations, derive values many compounds emitted by temperate forest fuels, including several previously unreported species.

Язык: Английский

Процитировано

47

The Fire Inventory from NCAR version 2.5: an updated global fire emissions model for climate and chemistry applications DOI Creative Commons
Christine Wiedinmyer, Yosuke Kimura,

Elena McDonald‐Buller

и другие.

Опубликована: Фев. 27, 2023

Abstract. We present the Fire Inventory from NCAR version 2.5 (FINNv2.5), a fire emissions inventory that provides publicly available of trace gases and aerosols for various applications, including use in global regional atmospheric chemistry modeling. FINNv2.5 includes numerous updates to FINN 1 framework better represent burned area, vegetation burned, chemicals emitted. Major changes include active detections Visible Infrared Imaging Radiometer Suite (VIIRS) at 375 m spatial resolution, which allows smaller fires be included processing. The calculation area has been updated such more rigorous approach is used aggregate detections, accounts larger enables using multiple satellite products simultaneously emission estimates. Fuel characterization factors have also FINNv2.5. Daily many are determined 2002–2019 (the Moderate Resolution Spectroradiometer (MODIS)-only detections) 2012–2019 (MODIS+VIIRS detections). non-methane organic gas allocated species several commonly chemical mechanisms. compare against other widely inventories. performance as inputs transport model assessed with observations. Uncertainties estimates remain, recommendations future evaluation given.

Язык: Английский

Процитировано

42

An observation-based, reduced-form model for oxidation in the remote marine troposphere DOI Creative Commons
Colleen B. Baublitz, Arlene M. Fiore, S. Ludwig

и другие.

Proceedings of the National Academy of Sciences, Год журнала: 2023, Номер 120(34)

Опубликована: Авг. 14, 2023

The hydroxyl radical (OH) fuels atmospheric chemical cycling as the main sink for methane and a driver of formation loss many air pollutants, but direct OH observations are sparse. We develop evaluate an observation-based proxy short-term, spatial variations in (Proxy

Язык: Английский

Процитировано

25

In the line of fire: Analyzing burning impacts on air pollution and air quality in an Amazonian city, Brazil DOI
Fernando Rafael de Moura, Petter Djeison Witte Machado, Paula Florêncio Ramires

и другие.

Atmospheric Pollution Research, Год журнала: 2024, Номер 15(4), С. 102033 - 102033

Опубликована: Янв. 2, 2024

Язык: Английский

Процитировано

11

Comparison of airborne measurements of NO, NO2, HONO, NOy, and CO during FIREX-AQ DOI Creative Commons
Ilann Bourgeois, Jeff Peischl, J. A. Neuman

и другие.

Atmospheric measurement techniques, Год журнала: 2022, Номер 15(16), С. 4901 - 4930

Опубликована: Авг. 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.

Язык: Английский

Процитировано

38

Emissions and Atmospheric Chemistry of Furanoids from Biomass Burning: Insights from Laboratory to Atmospheric Observations DOI Creative Commons
Manolis N. Romanías, Matthew M. Coggon,

Fatima Al Ali

и другие.

ACS Earth and Space Chemistry, Год журнала: 2024, Номер 8(5), С. 857 - 899

Опубликована: Апрель 8, 2024

Furanoids are a class of reactive volatile organic compounds that major products from the pyrolysis and combustion biomass polymers, including cellulose, hemicellulose, lignin. Biomass burning is an atmospheric source furanoids increasing in frequency intensity throughout regions world. Once emitted to atmosphere, may react with oxidants form secondary pollutants hazardous human health, ozone (O3) aerosol (SOA). This review comprehensive assessment literature between 1977 present describing emissions fate wild, prescribed, domestic fires. The organized by presenting physical properties key first, followed summary biopolymer reactions lead furanoid formation. Next, factors compiled across typical fuels consumed highlight species smoke. We next available kinetic degradation mechanism data characterize reaction rates, gas-phase products, SOA formed as result OH, NO3, O3, Cl radicals. then describe studies have focused on evaluating chemistry their impacts air quality using combination field observations model simulations. conclude perspective identifies future research directions would address gaps improve understanding processes.

Язык: Английский

Процитировано

8