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  • 1
    Publication Date: 2019-07-13
    Description: Wildfires emit significant amounts of pollutants that degrade air quality. Plumes from three wildfires in the western U.S. were measured from aircraft during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) and the Biomass Burning Observation Project (BBOP), both in summer 2013. This study reports an extensive set of emission factors (EFs) for over 80 gases and 5 components of submicron particulate matter (PM1) from these temperate wildfires. These include rarely, or never before, measured oxygenated volatile organic compounds and multifunctional organic nitrates. The observed EFs are compared with previous measurements of temperate wildfires, boreal forest fires, and temperate prescribed fires. The wildfires emitted high amounts of PM1 (with organic aerosol (OA) dominating the mass) with an average EF that is more than 2 times the EFs for prescribed fires. The measured EFs were used to estimate the annual wildfire emissions of carbon monoxide, nitrogen oxides, total non methane organic compounds, and PM1 from 11 western U.S. states. The estimated gas emissions are generally comparable with the 2011 National Emissions Inventory (NEI). However, our PM1 emission estimate (1530 +/- 570 Gg/yr) is over 3 times that of the NEI PM2.5 estimate and is also higher than the PM2.5 emitted from all other sources in these states in the NEI. This study indicates that the source of OA from biomass burning in the western states is significantly underestimated. In addition, our results indicate that prescribed burning may be an effective method to reduce fine particle emissions.
    Keywords: Environment Pollution
    Type: GSFC-E-DAA-TN44715 , Journal of Geophysical Research (ISSN 2169-897X); 122; 11; 6108-6129
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  • 2
    Publication Date: 2019-07-13
    Description: We report fluxes and dry deposition velocities for 16 atmospheric compounds above a southeastern United States forest, including: hydrogen peroxide (H2O2), nitric acid (HNO3), hydrogen cyanide (HCN), hydroxymethyl hydroperoxide, peroxyacetic acid, organic hydroxy nitrates, and other multifunctional species derived from the oxidation of isoprene and monoterpenes. The data suggest that dry deposition is the dominant daytime sink for small, saturated oxygenates. Greater than 6 wt %C emitted as isoprene by the forest was returned by dry deposition of its oxidized products. Peroxides account for a large fraction of the oxidant flux, possibly eclipsing ozone in more pristine regions. The measured organic nitrates comprise a sizable portion (15%) of the oxidized nitrogen input into the canopy, with HNO3 making up the balance. We observe that water-soluble compounds (e.g., strong acids and hydroperoxides) deposit with low surface resistance whereas compounds with moderate solubility (e.g., organic nitrates and hydroxycarbonyls) or poor solubility (e.g., HCN) exhibited reduced uptake at the surface of plants. To first order, the relative deposition velocities of water-soluble compounds are constrained by their molecular diffusivity. From resistance modeling, we infer a substantial emission flux of formic acid at the canopy level (approx. 1 nmol m(exp.2)s(exp.1)). GEOSChem, awidely used atmospheric chemical transport model, currently underestimates dry deposition for most molecules studied in this work. Reconciling GEOSChem deposition velocities with observations resulted in up to a 45% decrease in the simulated surface concentration of trace gases.
    Keywords: Environment Pollution; Meteorology and Climatology
    Type: GSFC-E-DAA-TN20692 , Proceedings of the National Academy of Science (ISSN 1091-6490); 112; 5; E392-E401
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  • 3
    Publication Date: 2019-07-13
    Description: Recent laboratory experiments have shown that a first generation isoprene oxidation product, ISOPOOH, can decompose to methyl vinyl ketone (MVK) and methacrolein (MACR) on instrument surfaces, leading to overestimates of MVK and MACR concentrations. Formaldehyde (HCHO) was suggested as a decomposition co-product, raising concern that in situ HCHO measurements may also be affected by an ISOPOOH interference. The HCHO measurement artifact from ISOPOOH for the NASA In Situ Airborne Formaldehyde instrument (ISAF) was investigated for the two major ISOPOOH isomers, (1,2)-ISOPOOH and (4,3)-ISOPOOH, under dry and humid conditions. The dry conversion of ISOPOOH to HCHO was 3+/-2% and 6+/-4% for (1,2)-ISOPOOH and (4,3)-ISOPOOH, respectively. Under humid (RH= 40-60%) conditions, conversion to HCHO was 6+/-4% for (1,2)-ISOPOOH and 10+/-5% for (4,3)-ISOPOOH. The measurement artifact caused by conversion of ISOPOOH to HCHO in the ISAF instrument was estimated for data obtained on the 2013 September 6 flight of the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. Prompt ISOPOOH conversion to HCHO was the source for 〈4% of the observed HCHO, including in the high-isoprene boundary layer. Time-delayed conversion, where previous exposure to ISOPOOH affects measured HCHO later in flight, was conservatively estimated to be 〈 10% of observed HCHO and is significant only when high ISOPOOH sampling periods immediately precede periods of low HCHO.
    Keywords: Environment Pollution
    Type: GSFC-E-DAA-TN41602 , Atmospheric Measurement Techniques (ISSN 1867-1381) (e-ISSN 1867-8548); 9; 9; 4561-4568
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  • 4
    Publication Date: 2019-07-13
    Description: A new in situ instrument for gas-phase formaldehyde (HCHO), COmpact Formaldehyde FluorescencE Experiment (COFFEE), is presented. COFFEE utilizes nonresonant laser-induced fluorescence (NR-LIF) to measure HCHO, with 300 mW of 40 kHz 355 nm laser output exciting multiple HCHO absorption features. The resulting HCHO fluorescence is collected at 5 ns resolution, and the fluorescence time profile is fit to yield the ambient HCHO mixing ratio. Typical 1 sigma precision at approximately 0 pptv HCHO is 150 pptv for 1 s data. The compact instrument was designed to operate with minimal in-flight operator interaction and infrequent maintenance (1-2 times per year). COFFEE fits in the wing pod of the Alpha Jet stationed at the NASA Ames Research Center and has successfully collected HCHO data on 27 flights through 2017 March. The frequent flights, combined with a potentially long-term data set, makes the Alpha Jet a promising platform for validation of satellite-based column HCHO.
    Keywords: Earth Resources and Remote Sensing; Geosciences (General)
    Type: GSFC-E-DAA-TN51683 , Atmospheric Measurement Techniques (ISSN 1867-1381) (e-ISSN 1867-8548); 10; 12; 4833-4844
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  • 5
    Publication Date: 2019-07-13
    Description: VOCs (Volatile Organic Compounds) related to oil and gas extraction operations in the United States were measured by H3O (sup plus) chemical ionization time-of-flight mass spectrometry (H3O (sup plus) ToFCIMS/PTR-ToF-MS (Time of Flight Chemical Ionization Mass Spectrometry/Proton Transfer Reaction-Time of Flight-Mass Spectroscopy) from aircraft during the Shale Oil and Natural Gas Nexus (SONGNEX) campaign in March-April 2015. This work presents an overview of major VOC species measured in nine oil- and gas-producing regions, and a more detailed analysis of H3O (sup plus) ToF-CIMS measurements in the Permian Basin within Texas and New Mexico. Mass spectra are dominated by small photochemically produced oxygenates and compounds typically found in crude oil: aromatics, cyclic alkanes, and alkanes. Mixing ratios of aromatics were frequently as high as those measured downwind of large urban areas. In the Permian, the H3O (sup plus) ToF-CIMS measured a number of underexplored or previously unreported species, including aromatic and cycloalkane oxidation products, nitrogen heterocycles including pyrrole (C4H5N) and pyrroline (C4H7N), H2S, and a diamondoid (adamantane) or unusual monoterpene. We additionally assess the specificity of a number of ion masses resulting from H3O (sup plus) ion chemistry previously reported in the literature, including several new or alternate interpretations.
    Keywords: Environment Pollution
    Type: GSFC-E-DAA-TN47232 , Atmospheric Measurement Techniques (e-ISSN 1867-8548); 10; 8; 2941-2968
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  • 6
    Publication Date: 2019-07-19
    Description: The Atmospheric Tomography (ATom) mission deployed an extensive gas and aerosol payload on the NASA DC-8 aircraft on four campaigns spanning each season. ATom systematically sampled the atmosphere from 0.2 to 12 kilometer altitude, from 85 degrees North Latitude to 65 degrees South Latitude, in both the Pacific and the Atlantic to provide detailed profiles of chemical composition over the remote oceans. We will present profiles of reactive trace species, such as O3, NOx, NOy, HOx, HCHO, and several other short-lived source gases. We will combine these measurements with results from a 0-D box model to show their utility in (1) evaluating gradients in latitude/season, (2) identifying contributions of pollution from long-range and convective transport, and (3) evaluating column measurements from remote sensing satellite instruments.
    Keywords: Environment Pollution
    Type: GSFC-E-DAA-TN60227 , American Geophysical Union Fall Meeting (AGU 2018) Washington, D.C.; 10-14 Dec. 2018; Washington, DC; United States
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  • 7
    Publication Date: 2019-09-11
    Description: Hydroxymethyl hydroperoxide (HMHP), formed in the reaction of the C1 Criegee intermediate with water, is among the most abundant organic peroxides in the atmosphere. Although reaction with OH is thought to represent one of the most important atmospheric removal processes for HMHP, this reaction has been largely unstudied in the laboratory. Here, we present measurements of the kinetics and products formed in the reaction of HMHP with OH. HMHP was oxidized by OH in an environmental chamber; the decay of the hydroperoxide and the formation of formic acid and formaldehyde were monitored over time using CF3O- chemical ionization mass spectrometry (CIMS) and laser induced fluorescence (LIF). The loss of HMHP by reaction with OH is measured relative to the loss of 1,2-butanediol [k1;2-butanediol+OH = (27:0 5:6) 10- exp12 cm3 molecule-1s-1]. We find that HMHP reacts with OH at 295 K with a rate coefficient of (7.1 1.5) 10-12 cm3 molecule-1s-1, with the formic acid to formaldehyde yield in a ratio of 0:880:21 and independent of NO concentration (31010 1.51013 molecule cm-3). We suggest that, exclusively, abstraction of the methyl hydrogen of HMHP results in formic acid while abstraction of the hydroperoxy hydrogen results in formaldehyde. We further evaluate the relative importance of HMHP sinks and use global simulations from GEOS-Chem to estimate that HMHP oxidation by OH contributes 1.7 Tg yr-1 (1-3%) of global annual formic acid production.
    Keywords: Inorganic, Organic and Physical Chemistry; Geosciences (General)
    Type: GSFC-E-DAA-TN68989 , Journal of Physical Chemistry A (ISSN 1089-5639) (e-ISSN 1520-5215); 122; 30; 6292-6302
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  • 8
    Publication Date: 2019-11-22
    Description: In this work, a new commercially available, laser-based, and ultra-portable formaldehyde (HCHO) gas sensor is characterized, and its usefulness for monitoring HCHO mixing ratios in both indoor and outdoor environments is assessed. Stepped calibrations and intercomparison with well-established laser-induced fluorescence (LIF) instrumentation allow a performance evaluation of the absorption-based, mid-infrared HCHO sensor from Aeris Technologies, Inc. The Aeris sensor displays linear behavior (R2 〉 0.940) when compared with LIF instruments from Harvard and NASA Goddard. A nonlinear least-squares fitting algorithm developed independently of the sensor's manufacturer to fit the sensor's raw absorption data during post-processing further improves instrument performance. The 3σ limit of detection (LOD) for 2, 15, and 60 min integration times are 2190, 690, and 420 pptv HCHO, respectively, for mixing ratios reported in real time, though the LOD improves to 1800, 570, and 300 pptv HCHO, respectively, during post-processing. Moreover, the accuracy of the sensor was found to be ± (10 % + 0.3) ppbv when compared against LIF instrumentation sampling ambient air. The aforementioned precision and level of accuracy are sufficient for most HCHO levels measured in indoor and outdoor environments. While the compact Aeris sensor is currently not a replacement for the most sensitive research-grade instrumentation available, its usefulness for monitoring HCHO is clearly demonstrated.
    Print ISSN: 1867-1381
    Electronic ISSN: 1867-8548
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 9
    Publication Date: 2016-09-16
    Description: Recent laboratory experiments have shown that a first generation isoprene oxidation product, ISOPOOH, can decompose to methyl vinyl ketone (MVK) and methacrolein (MACR) on instrument surfaces, leading to overestimates of MVK and MACR concentrations. Formaldehyde (HCHO) was suggested as a decomposition co-product, raising concern that in situ HCHO measurements may also be affected by an ISOPOOH interference. The HCHO measurement artifact from ISOPOOH for the NASA In Situ Airborne Formaldehyde instrument (ISAF) was investigated for the two major ISOPOOH isomers, (1,2)-ISOPOOH and (4,3)-ISOPOOH, under dry and humid conditions. The dry conversion of ISOPOOH to HCHO was 3±2% and 6±4% for (1,2)-ISOPOOH and (4,3)-ISOPOOH, respectively. Under humid (relative humidity of 40–60%) conditions, conversion to HCHO was 6±4% for (1,2)-ISOPOOH and 10±5% for (4,3)-ISOPOOH. The measurement artifact caused by conversion of ISOPOOH to HCHO in the ISAF instrument was estimated for data obtained on the 6 September 2013 flight of the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. Prompt ISOPOOH conversion to HCHO was the source of 〈4% of the observed HCHO, including in the high-isoprene boundary layer. Time-delayed conversion, where previous exposure to ISOPOOH affects measured HCHO later in the flight, was conservatively estimated to be 〈10% of observed HCHO, and is significant only when high ISOPOOH sampling periods immediately precede periods of low HCHO.
    Print ISSN: 1867-1381
    Electronic ISSN: 1867-8548
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 10
    Publication Date: 2016-03-16
    Description: Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NOx ≡ NO + NO2) and biogenic isoprene. Model estimates of surface ozone concentrations tend to be biased high in the region and this is of concern for designing effective emission control strategies to meet air quality standards. We use detailed chemical observations from the SEAC4RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model (CTM) at 0.25°×0.3125° horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NOx from the US Environmental Protection Agency (EPA) is too high in the Southeast and nationally by 50 %. This is demonstrated by SEAC4RS observations of NOx and its oxidation products, by surface network observations of nitrate wet deposition fluxes, and by OMI satellite observations of tropospheric NO2 columns. Upper tropospheric NO2 from lightning makes a large contribution to the satellite observations that must be accounted for when using these data to estimate surface NOx emissions. Aircraft observations of upper tropospheric NO2 are higher than simulated by GEOS-Chem or expected from NO-NO2-O3 photochemical stationary state. NOx levels in the Southeast US are sufficiently low that only half of isoprene oxidation proceeds by the high-NOx pathway to produce ozone; this fraction is only moderately sensitive to changes in NOx emissions because isoprene and NOx emissions are spatially segregated. GEOS-Chem with reduced NOx emissions provides an unbiased simulation of ozone observations from the aircraft and from ozonesondes, and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NOx oxidation products. However, the model is still biased high by 8 ± 13 ppb relative to observed surface ozone in the Southeast US. Ozonesondes launched during midday hours show a 7 ppb ozone decrease from 1.5 km to 0.2 km altitude, whereas GEOS-Chem has no such gradient because of efficient boundary layer mixing. We conclude that model biases in simulating surface ozone over the Southeast US may be due to a combination of excessive NOx emissions and excessive boundary layer vertical mixing.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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