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NASA NTRS2003

Distributions of Trace Gases and Aerosols during the Dry Biomass Burning Season in Southern Africa

Vertical profiles in the lower troposphere of temperature, relative humidity, sulfur dioxide (SO2), ozone (O3), condensation nuclei (CN), and carbon monoxide (CO), and horizontal distributions of twenty gaseous and particulate species, are presented for five regions of southern Africa during the dry biomass burning season of 2000. The regions are the semiarid savannas of northeast South Africa and northern Botswana, the savanna-forest mosaic of coastal Mozambique, the humid savanna of southern Zambia, and the desert of western Namibia. The highest average concentrations of carbon dioxide (CO2), CO, methane (CH4), O3, black particulate carbon, and total particulate carbon were in the Botswana and Zambia sectors (388 and 392 ppmv, 369 and 453 ppbv, 1753 and 1758 ppbv, 79 and 88 ppbv, 2.6 and 5.5 micrograms /cubic meter and 13.2 and 14.3 micrograms/cubic meter). This was due to intense biomass burning in Zambia and surrounding regions. The South Africa sector had the highest average concentrations of SO2, sulfate particles, and CN (5.1 ppbv, 8.3 micrograms/cubic meter, and per 6400 cubic meter , respectively), which derived from biomass burning and electric generation plants and mining operations within this sector. Air quality in the Mozambique sector was similar to the neighboring South Africa sector. Over the arid Namibia sector there were polluted layers aloft, in which average SO2, O3, and CO mixing ratios (1.2 ppbv, 76 ppbv, and 3 10 ppbv, respectively) were similar to those measured over the other more polluted sectors. This was due to transport of biomass smoke from regions of widespread savanna burning in southern Angola. Average concentrations over all sectors of CO2 (386 +/- 8 ppmv), CO (261 +/- 81 ppbv), SO2 (2.5 +/- 1.6 ppbv), O3 (64 +/- 13 ppbv), black particulate carbon (2.3 +/- 1.9 microgram/cubic meter), organic particulate carbon (6.2 +/- 5.2 microgram/cubic meter), total particle mass (26.0 +/- 4.7 microgram/cubic meter), and potassium particles (0.4 +- 0.1 microgram/cubic meter) were comparable to those in polluted, urban air. Since the majority of the measurements in this study were obtained in locations well removed from industrial sources of pollution, the high average concentrations of pollutants reflect the effects of widespread biomass burning. On occasions, relatively thin (-0.5 km) layers of remarkably clean air were located at -3 km above mean sea level, sandwiched between heavily polluted air. The data presented here can be used for inputs to and validation of regional and global atmospheric chemical models.

Sinha, Parikhit↗
NASA NTRS2004

Transport of Biomass Burning Emissions from Southern Africa

The transport of biomass burning emissions from southern Africa to the neighboring Atlantic and Indian Oceans during the dry season (May-October) of 2000 is characterized using ground, ozonesonde, and aircraft measurements of carbon monoxide (CO) and ozone (O3) in and around southern Africa, together with the GEOS-CHEM global model of tropospheric chemistry. The model shows a positive bias of approximately 20% for CO and a negative bias of approximately 10-25% for O3 at oceanic sites downwind of fire emissions. Near areas of active fire emissions the model shows a negative bias of approximately 60% and approximately 30% for CO and O3, respectively, likely due to the coarse spatial (2 deg. x 2.5 deg.) and temporal (monthly) resolution of the model compared to that of active fires. On average, from 1994 to 2000, approximately 60 Tg of carbon monoxide (CO) from biomass burning in southern Africa was transported eastward to the Indian Ocean across the latitude band 0 deg. -60 S during the 6 months of the dry season. Over the same time period, approximately 40 Tg of CO from southern African biomass burning was transported westward to the Atlantic Ocean over the latitudes 0 deg. -20 S during the 6-month dry season, but most of that amount was transported back eastward over higher latitudes to the south (21 deg. -60 S). Eastward transport of biomass burning emissions from southern Africa enhances CO concentrations by approximately 4- 13 ppbv per month over the southern subtropical Indian Ocean during the dry season, with peak enhancements in September. Carbon monoxide from southern African and South American biomass burning is seen in the model simulations as far away as Australia, contributing approximately 8 ppbv and approximately 12-15 ppbv CO, respectively, and thus explaining the approximately 20- 25 ppbv observed enhancement of CO over Melbourne in mid-September 2000.

Sinha, Parikhit↗
NASA NTRS2006

High Resolution Spectroscopy to Support Atmospheric Measurements

The major research activities performed during the cooperative agreement enhanced our spectroscopic knowledge of molecules of atmospheric interest such as H2O (water vapor), O3 (ozone), HCN (hydrogen cyanide), CH4 (methane), NO2 (nitrogen dioxide) and CO (carbon monoxide). The data required for the analyses were obtained from two different Fourier Transform Spectrometers (FTS); one of which is located at the National Solar Observatory (NSO) on Kitt Peak, Arizona and the other instrument is located at the Pacific Northwest National Laboratories (PNNL) at Richland, Washington. The data were analyzed using a modified multispectrum nonlinear least squares fitting algorithm developed by Dr. D. Chris Benner of the College of William and Mary. The results from these studies made significant improvements in the line positons and intensities for these molecules. The measurements of pressure broadening and pressure induced line shift coefficients and the temperature dependence of pressure broadening and pressure induced shift coefficients for hundreds of infrared transitions of HCN, CO3 CH4 and H2O were also performed during this period. Results from these studies have been used for retrievals of stratospheric gas concentration profiles from data collected by several Upper Atmospheric Research Satellite (UARS) infrared instruments as well as in the analysis of high resolution atmospheric spectra such as those acquired by space-based, ground-based, and various balloon- and aircraft-borne experiments. Our results made significant contributions in several updates of the HITRAN (HIgh resolution TRANsmission) spectral line parameters database. This database enjoys worldwide recognition in research involving diversified scientific fields. The research conducted during the period 2003-2006 has resulted in publications given in this paper. In addition to Journal publications, several oral and poster presentations were given at various Scientific conferences within the United States and abroad.

Venkataraman, Malathy Devi↗
NASA NTRS2007

Transport in the Subtropical Lowermost Stratosphere during CRYSTAL-FACE

We use in situ measurements of water vapor (H2O), ozone (O3), carbon dioxide (CO2), carbon monoxide (CO), nitric oxide (NO), and total reactive nitrogen (NO(y)) obtained during the CRYSTAL-FACE campaign in July 2002 to study summertime transport in the subtropical lowermost stratosphere. We use an objective methodology to distinguish the latitudinal origin of the sampled air masses despite the influence of convection, and we calculate backward trajectories to elucidate their recent geographical history. The methodology consists of exploring the statistical behavior of the data by performing multivariate clustering and agglomerative hierarchical clustering calculations, and projecting cluster groups onto principal component space to identify air masses of like composition and hence presumed origin. The statistically derived cluster groups are then examined in physical space using tracer-tracer correlation plots. Interpretation of the principal component analysis suggests that the variability in the data is accounted for primarily by the mean age of air in the stratosphere, followed by the age of the convective influence, and lastly by the extent of convective influence, potentially related to the latitude of convective injection [Dessler and Sherwuud, 2004]. We find that high-latitude stratospheric air is the dominant source region during the beginning of the campaign while tropical air is the dominant source region during the rest of the campaign. Influence of convection from both local and non-local events is frequently observed. The identification of air mass origin is confirmed with backward trajectories, and the behavior of the trajectories is associated with the North American monsoon circulation.

Pittman, Jasna V.↗
NASA NTRS2007

Transport in the Subtropical Lowermost Stratosphere during the Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment

We use in situ measurements of water vapor (H2O), ozone (O3), carbon dioxide (CO2), carbon monoxide (CO), nitric oxide (NO), and total reactive nitrogen (NOy) obtained during the CRYSTAL-FACE campaign in July 2002 to study summertime transport in the subtropical lowermost stratosphere. We use an objective methodology to distinguish the latitudinal origin of the sampled air masses despite the influence of convection, and we calculate backward trajectories to elucidate their recent geographical history. The methodology consists of exploring the statistical behavior of the data by performing multivariate clustering and agglomerative hierarchical clustering calculations and projecting cluster groups onto principal component space to identify air masses of like composition and hence presumed origin. The statistically derived cluster groups are then examined in physical space using tracer-tracer correlation plots. Interpretation of the principal component analysis suggests that the variability in the data is accounted for primarily by the mean age of air in the stratosphere, followed by the age of the convective influence, and last by the extent of convective influence, potentially related to the latitude of convective injection (Dessler and Sherwood, 2004). We find that high-latitude stratospheric air is the dominant source region during the beginning of the campaign while tropical air is the dominant source region during the rest of the campaign. Influence of convection from both local and nonlocal events is frequently observed. The identification of air mass origin is confirmed with backward trajectories, and the behavior of the trajectories is associated with the North American monsoon circulation.

Pittman, Jasna V.↗
NASA NTRS2006

Ozone Production from the 2004 North American Boreal Fires

We examine the ozone production from boreal forest fires based on a case study of wildfires in Alaska and Canada in summer 2004. The model simulations were performed with the chemistry transport model, MOZART-4, and were evaluated by comparison with a comprehensive set of aircraft measurements. In the analysis we use measurements and model simulations of carbon monoxide (CO) and ozone (O3) at the PICO-NARE station located in the Azores within the pathway of North American outflow. The modeled mixing ratios were used to test the robustness of the enhancement ratio deltaO3/deltaCO (defined as the excess O3 mixing ratio normalized by the increase in CO) and the feasibility for using this ratio in estimating the O3 production from the wildfires. Modeled and observed enhancement ratios are about 0.25 ppbv/ppbv which is in the range of values found in the literature, and results in a global net O3 production of 12.9 2 Tg O3 during summer 2004. This matches the net O3 production calculated in the model for a region extending from Alaska to the East Atlantic (9-11 Tg O3) indicating that observations at PICO-NARE representing photochemically well-aged plumes provide a good measure of the O3 production of North American boreal fires. However, net chemical loss of fire related O3 dominates in regions far downwind from the fires (e.g. Europe and Asia) resulting in a global net O3 production of 6 Tg O3 during the same time period. On average, the fires increased the O3 burden (surface-300 mbar) over Alaska and Canada during summer 2004 by about 7-9%, and over Europe by about 2-3%.

Pfister, G. G.↗
NASA NTRS2006

Thirty Years After: The Science of the Viking Program and the Discovery of a 'New Mars'

Viking discovered a Mars that was very different from the Mars found by Mariner 4, 6 and 7. The new, exciting, more Earth-like Mars was hinted at by the Mariner 9 orbiter and confirmed by Viking. Viking discovered some very fundamental things about Mars. Viking discovered the presence of nitrogen in the atmosphere. A key ingredient needed for life. Viking made the first measurements of the isotopic composition of carbon, oxygen, nitrogen and the noble gases in the atmosphere of Mars. The ratio of 15N to 14N suggested that Mars may have lost more than 99% of the total mass of its atmosphere. The denser atmosphere in the past may explain the presence of flowing water earlier in the history of Mars first discovered by Mariner 9 with additional and higher spatial resolution examples provided by the Viking Orbiters. Viking did not measure organics or life at the surface of Mars. But, Viking did discover a surface unlike any other on the Solar System--a surface exhibiting very high chemical reactivity, most probably formed by the deposition of chemically active atmospheric gases, like hydrogen peroxide (H2O2) and ozone (O3), onto the surface of Mars.

Levine, Joel S.↗
NASA NTRS2010

An Investigation of Widespread Ozone Damage to the Soybean Crop in the Upper Midwest Determined From Ground-Based and Satellite Measurements

Elevated concentrations of ground-level ozone (O3) are frequently measured over farmland regions in many parts of the world. While numerous experimental studies show that O3 can significantly decrease crop productivity, independent verifications of yield losses at current ambient O3 concentrations in rural locations are sparse. In this study, soybean crop yield data during a 5-year period over the Midwest of the United States were combined with ground and satellite O3 measurements to provide evidence that yield losses on the order of 10% could be estimated through the use of a multiple linear regression model. Yield loss trends based on both conventional ground-based instrumentation and satellite-derived tropospheric O3 measurements were statistically significant and were consistent with results obtained from open-top chamber experiments and an open-air experimental facility (SoyFACE, Soybean Free Air Concentration Enrichment) in central Illinois. Our analysis suggests that such losses are a relatively new phenomenon due to the increase in background tropospheric O3 levels over recent decades. Extrapolation of these findings supports previous studies that estimate the global economic loss to the farming community of more than $10 billion annually.

Fishman, Jack↗
NASA NTRS2010

Development of the Global Ozone Lidar Demonstrator (GOLD) Instrument for Deployment on the NASA Global Hawk

A compact ozone (O3) and aerosol lidar system is being developed for conducting global atmospheric investigations from the NASA Global Hawk Uninhabited Aerial Vehicle (UAV) and for enabling the development and test of a space-based O3 and aerosol lidar. GOLD incorporates advanced technologies and designs to produce a compact, autonomously operating O3 and aerosol Differential Absorption Lidar (DIAL) system for a UAV platform. The GOLD system leverages advanced Nd:YAG and optical parametric oscillator laser technologies and receiver optics, detectors, and electronics. Significant progress has been made toward the development of the GOLD system, and this paper describes the objectives of this program, basic design of the GOLD system, and results from initial ground-based atmospheric tests.

Hair, Jonathan W.↗
NASA NTRS2012

Field and Satellite Observations of the Formation and Distribution of Arctic Atmospheric Bromine Above a Rejuvenated Sea Ice Cover

Recent drastic reduction of the older perennial sea ice in the Arctic Ocean has resulted in a vast expansion of younger and saltier seasonal sea ice. This increase in the salinity of the overall ice cover could impact tropospheric chemical processes. Springtime perennial ice extent in 2008 and 2009 broke the half-century record minimum in 2007 by about one million km2. In both years seasonal ice was dominant across the Beaufort Sea extending to the Amundsen Gulf, where significant field and satellite observations of sea ice, temperature, and atmospheric chemicals have been made. Measurements at the site of the Canadian Coast Guard Ship Amundsen ice breaker in the Amundsen Gulf showed events of increased bromine monoxide (BrO), coupled with decreases of ozone (O3) and gaseous elemental mercury (GEM), during cold periods in March 2008. The timing of the main event of BrO, O3, and GEM changes was found to be consistent with BrO observed by satellites over an extensive area around the site. Furthermore, satellite sensors detected a doubling of atmospheric BrO in a vortex associated with a spiral rising air pattern. In spring 2009, excessive and widespread bromine explosions occurred in the same region while the regional air temperature was low and the extent of perennial ice was significantly reduced compared to the case in 2008. Using satellite observations together with a Rising-Air-Parcel model, we discover a topographic control on BrO distribution such that the Alaskan North Slope and the Canadian Shield region were exposed to elevated BrO, whereas the surrounding mountains isolated the Alaskan interior from bromine intrusion.

Nghiem, Son V.↗
NASA NTRS2013

Inverse Modeling of Texas NOx Emissions Using Space-Based and Ground-Based NO2 Observations

Inverse modeling of nitrogen oxide (NOx) emissions using satellite-based NO2 observations has become more prevalent in recent years, but has rarely been applied to regulatory modeling at regional scales. In this study, OMI satellite observations of NO2 column densities are used to conduct inverse modeling of NOx emission inventories for two Texas State Implementation Plan (SIP) modeling episodes. Addition of lightning, aircraft, and soil NOx emissions to the regulatory inventory narrowed but did not close the gap between modeled and satellite observed NO2 over rural regions. Satellitebased top-down emission inventories are created with the regional Comprehensive Air Quality Model with extensions (CAMx) using two techniques: the direct scaling method and discrete Kalman filter (DKF) with Decoupled Direct Method (DDM) sensitivity analysis. The simulations with satellite-inverted inventories are compared to the modeling results using the a priori inventory as well as an inventory created by a ground-level NO2 based DKF inversion. The DKF inversions yield conflicting results: the satellite based inversion scales up the a priori NOx emissions in most regions by factors of 1.02 to 1.84, leading to 3-55% increase in modeled NO2 column densities and 1-7 ppb increase in ground 8 h ozone concentrations, while the ground-based inversion indicates the a priori NOx emissions should be scaled by factors of 0.34 to 0.57 in each region. However, none of the inversions improve the model performance in simulating aircraft-observed NO2 or ground-level ozone (O3) concentrations.

Nitrogen dioxide↗
NASA NTRS2014

Variation of a Lightning NOx Indicator for National Climate Assessment

Lightning nitrogen oxides (LNOx) indirectly influences our climate since these molecules are important in controlling the concentration of ozone (O3) and hydroxyl radicals (OH) in the atmosphere [Huntrieser et al., 1998]. In support of the National Climate Assessment (NCA) program, satellite Lightning Imaging Sensor (LIS; Christian et al. [1999]; Cecil et al. [2014]) data is used to estimate LNOx production over the southern portion of the conterminous US for the 16 year period 1998-2013.

Koshak, William↗
NASA NTRS2015

Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS)

The Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS) mission will extend the SAGE data record from the ideal vantage point of the International Space Station (ISS). The ISS orbital inclination is ideal for SAGE measurements providing coverage between 70 deg north and 70 deg south latitude. The SAGE data record includes an extensively validated data set including aerosol optical depth data dating to the Stratospheric Aerosol Measurement (SAM) experiments in 1975 and 1978 and stratospheric ozone profile data dating to the Stratospheric Aerosol and Gas Experiment (SAGE) in 1979. These and subsequent data records, notably from the SAGE II experiment launched on the Earth Radiation Budget Satellite in 1984 and the SAGE III experiment launched on the Russian Meteor-3M satellite in 2001, have supported a robust, long-term assessment of key atmospheric constituents. These scientific measurements provide the basis for the analysis of five of the nine critical constituents (aerosols, ozone (O3), nitrogen dioxide (NO2), water vapor (H2O), and air density using O2) identified in the U.S. National Plan for Stratospheric Monitoring. SAGE III on ISS was originally scheduled to fly on the ISS in the same timeframe as the Meteor-3M mission, but was postponed due to delays in ISS construction. The project was re-established in 2009.

Gasbarre, Joseph↗
NASA NTRS2016

Formaldehyde Column Density Measurements as a Suitable Pathway to Estimate Near-Surface Ozone Tendencies from Space

In support of future satellite missions that aim to address the current shortcomings in measuring air quality from space, NASA's Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) field campaign was designed to enable exploration of relationships between column measurements of trace species relevant to air quality at high spatial and temporal resolution. In the DISCOVER-AQ data set, a modest correlation (r2 = 0.45) between ozone (O3) and formaldehyde (CH2O) column densities was observed. Further analysis revealed regional variability in the O3-CH2O relationship, with Maryland having a strong relationship when data were viewed temporally and Houston having a strong relationship when data were viewed spatially. These differences in regional behavior are attributed to differences in volatile organic compound (VOC) emissions. In Maryland, biogenic VOCs were responsible for approx.28% of CH2O formation within the boundary layer column, causing CH2O to, in general, increase monotonically throughout the day. In Houston, persistent anthropogenic emissions dominated the local hydrocarbon environment, and no discernable diurnal trend in CH2O was observed. Box model simulations suggested that ambient CH2O mixing ratios have a weak diurnal trend (+/-20% throughout the day) due to photochemical effects, and that larger diurnal trends are associated with changes in hydrocarbon precursors. Finally, mathematical relationships were developed from first principles and were able to replicate the different behaviors seen in Maryland and Houston. While studies would be necessary to validate these results and determine the regional applicability of the O3-CH2O relationship, the results presented here provide compelling insight into the ability of future satellite missions to aid in monitoring near-surface air quality.

Surface Conditions from Column and Vertically Reso↗
NASA NTRS2016

Tropospheric Emissions: Monitoring of Pollution (TEMPO)

TEMPO (Tropospheric Emissions: Monitoring of Pollution) was selected in 2012 by NASA as the first Earth Venture Instrument, for launch between 2018 and 2021. It will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO observes from Mexico City, Cuba, and the Bahamas to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution (approximately 2.1 kilometers N/S by 4.4 kilometers E/W at 36.5 degrees N, 100 degrees W). TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry, as well as contributing to carbon cycle knowledge. Measurements are made hourly from geostationary (GEO) orbit, to capture the high variability present in the diurnal cycle of emissions and chemistry that are unobservable from current low-Earth orbit (LEO) satellites that measure once per day. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a commercial GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve ozone (O3), nitrogen dioxide (NO2), sulfur dioxide (SO2), formaldehyde (H2CO), glyoxal (C2H2O2), bromine monoxide (BrO), IO (iodine monoxide),water vapor, aerosols, cloud parameters, ultraviolet radiation, and foliage properties. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, substantially reducing uncertainty in air quality predictions. TEMPO quantifies and tracks the evolution of aerosol loading. It provides these near-real-time air quality products that will be made publicly available. TEMPO will launch at a prime time to be the North American component of the global geostationary constellation of pollution monitoring together with the European Sentinel-4 (S4) and Korean Geostationary Environment Monitoring Spectrometer (GEMS) instruments.

tropospheric measurement suite↗
NASA NTRS2016

Agricultural Fires in the Southeastern U.S. During SEAC4RS: Emissions of Trace Gases and Particles and Evolution of Ozone, Reactive Nitrogen, and Organic Aerosol

Emissions from 15 agricultural fires in the southeastern U.S. were measured from the NASA DC-8 research aircraft during the summer 2013 Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. This study reports a detailed set of emission factors (EFs) for 25 trace gases and 6 fine particle species. The chemical evolution of the primary emissions in seven plumes was examined in detail for ~1.2 h. A Lagrangian plume cross-section model was used to simulate the evolution of ozone (O3), reactive nitrogen species, and organic aerosol (OA). Observed EFs are generally consistent with previous measurements of crop residue burning, but the fires studied here emitted high amounts of SO2 and fine particles, especially primary OA and chloride. Filter-based measurements of aerosol light absorption implied that brown carbon (BrC) was ubiquitous in the plumes. In aged plumes, rapid production of O3, peroxyacetyl nitrate (PAN), and nitrate was observed with (Delta)O3/(Delta)CO, (Delta)PAN/(Delta)NOy, and (Delta)nitrate/(Delta)NOy reaching approx. 0.1, approx. 0.3, and approx.0.3. For five selected cases, the model reasonably simulated O3 formation but underestimated PAN formation. No significant evolution of OA mass or BrC absorption was observed. However, a consistent increase in oxygen-to-carbon (O/C) ratios of OA indicated that OA oxidation in the agricultural fire plumes was much faster than in urban and forest fire plumes. Finally, total annual SO2, NOx, and CO emissions from agricultural fires in Arkansas, Louisiana, Mississippi, and Missouri were estimated (within a factor of approx. 2) to be equivalent to approx. 2% SO2 from coal combustion and approx. 1% NOx and approx. 9% CO from mobile sources.

OA mass or BrC absorption↗
NASA NTRS2017

Controlled Nitric Oxide Production via O(1D) + N2O Reactions for Use in Oxidation Flow Reactor Studies

Oxidation flow reactors that use low-pressure mercury lamps to produce hydroxyl (OH) radicals are an emerging technique for studying the oxidative aging of organic aerosols. Here, ozone (O3) is photolyzed at 254 nm to produce O(1D) radicals, which react with water vapor to produce OH. However, the need to use parts-per-million levels of O3 hinders the ability of oxidation flow reactors to simulate NOx-dependent secondary organic aerosol (SOA) formation pathways. Simple addition of nitric oxide (NO) results in fast conversion of NOx (NO+NO2) to nitric acid (HNO3), making it impossible to sustain NOx at levels that are sufficient to compete with hydroperoxy (HO2) radicals as a sink for organic peroxy (RO2) radicals. We developed a new method that is well suited to the characterization of NOx-dependent SOA formation pathways in oxidation flow reactors. NO and NO2 are produced via the reaction O(1D)+N2O->2NO, followed by the reaction NO+O3->NO2+O2. Laboratory measurements coupled with photochemical model simulations suggest that O(1D)+N2O reactions can be used to systematically vary the relative branching ratio of RO2 +NO reactions relative to RO2 +HO2 and/or RO2+RO2 reactions over a range of conditions relevant to atmospheric SOA formation. We demonstrate proof of concept using high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) measurements with nitrate (NO-3 ) reagent ion to detect gas-phase oxidation products of isoprene and -pinene previously observed in NOx-influenced environments and in laboratory chamber experiments.

Lambe, Andrew↗
NASA NTRS2016

Quantifying the Contribution of Thermally Driven Recirculation to a High-Ozone Event Along the Colorado Front Range Using Lidar

A high-ozone (O3) pollution episode was observed on 22 July 2014 during the concurrent Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) and Front Range Air Pollution and Photochemistry Experiment (FRAPPE) campaigns in northern Colorado. Surface O3 monitors at three regulatory sites exceeded the Environmental Protection Agency (EPA) 2008 National Ambient Air Quality Standard (NAAQS) daily maximum 8h average (MDA8) of 75ppbv. To further characterize the polluted air mass and assess transport throughout the event, measurements are presented from O3 and wind profilers, O3-sondes, aircraft, and surface-monitoring sites. Observations indicate that thermally driven upslope flow was established throughout the Colorado Front Range during the pollution episode. As the thermally driven flow persisted throughout the day, O3 concentrations increased and affected high-elevation Rocky Mountain sites. These observations, coupled with modeling analyses, demonstrate a westerly return flow of polluted air aloft, indicating that the mountain-plains solenoid circulation was established and impacted surface conditions within the Front Range.

Front Range Air Pollution and Photochemistry Exper↗