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Thompson, Anne M.

Publications and source records attributed to Thompson, Anne M..

At least 19 records

Observational ozone datasets over the global oceans and polar regions (version 2024)

Studying tropospheric ozone over the remote areas of the planet, such as the open oceans and the polar regions, is crucial to understand the role of ozone as a global climate forcer and regulator of atmospheric oxidative capacity. A focus on the pristine oceanic and polar regions complements the available land-based datasets and provides insights into key photochemical and depositional loss processes that control the concentrations and spatiotemporal variability in ozone as well as the physicochemical mechanisms driving these patterns. However, an assessment of the role of ozone over the oceanic and polar regions has been hampered by a lack of comprehensive observational datasets. Here, we present the first comprehensive collection of ozone data over the oceans and the polar regions. The overall dataset consists of 77 ship cruises/buoy-based observations and 48 aircraft-based campaigns. The dataset, consisting of more than 630 000 independent ozone measurement data points covering the period from 1977 to 2022 and an altitude range from the surface to 5000 m (with a focus on the lowest 2000 m), allows systematic analyses of the spatiotemporal distribution and long-term trends over the 11 defined ocean/polar regions. The datasets from ships, buoys, and aircraft are complemented by ozonesonde data from 29 launch sites or field campaigns and by 21 non-polar and 17 polar ground-based station datasets. The datasets contain information on how long the observed air masses were isolated from land, as estimated by backward trajectories from the individual observation points. To extract observations representative of oceanic conditions, we recommend using a subset of the data with an isolation time of 72 h or longer, from the analysis with coincident radon observations. These filtered oceanic and polar data showed typically flat diurnal cycles at high latitudes, whereas daytime decreases in ozone (11 %–16 %) were observed at lower latitudes. The ship/buoy- and aircraft-based datasets presented here will supplement the land-based ones in the TOAR-II (Tropospheric Ozone Assessment Report Phase II) database to provide a fully global assessment of tropospheric ozone. The described dataset is available at https://doi.org/10.17596/0004044 (Kanaya et al., 2025).

Kanaya, Yugo [Japan Agency for Marine-Earth Scienc

Trends in Global Tropospheric Ozone Inferred from a Composite Record of TOMS/OMI/MLS/OMPS Satellite Measurements and the MERRA-2 GMI Simulation

Past studies have suggested that ozone in the troposphere has increased globally throughout much of the 20th century due to increases in anthropogenic emissions and transport. We show, by combining satellite measurements with a chemical transport model, that during the last four decades tropospheric ozone does indeed indicate increases that are global in nature, yet still highly regional. Satellite ozone measurements from Nimbus-7 and Earth Probe Total Ozone Mapping Spectrometer (TOMS) are merged with ozone measurements from the Aura Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) to determine trends in tropospheric ozone for 1979–2016. Both TOMS (1979–2005) and OMI/MLS (2005–2016) depict large increases in tropospheric ozone from the Near East to India and East Asia and further eastward over the Pacific Ocean. The 38-year merged satellite record shows total net change over this region of about +6 to +7 Dobson units (DU) (i.e., ∼15 %–20 % of average background ozone), with the largest increase (∼4 DU) occurring during the 2005–2016 Aura period. The Global Modeling Initiative (GMI) chemical transport model with time-varying emissions is used to aid in the interpretation of tropospheric ozone trends for 1980–2016. The GMI simulation for the combined record also depicts the greatest increases of +6 to +7 DU over India and East Asia, very similar to the satellite measurements. In regions of significant increases in tropospheric column ozone (TCO) the trends are a factor of 2–2.5 larger for the Aura record when compared to the earlier TOMS record; for India and East Asia the trends in TCO for both GMI and satellite measurements are ∼+3 DU decade(exp −1) or greater during 2005–2016 compared to about +1.2 to +1.4 DU decade(exp −1) for 1979–2005. The GMI simulation and satellite data also reveal a tropospheric ozone increases in ∼+4 to +5 DU for the 38-year record over central Africa and the tropical Atlantic Ocean. Both the GMI simulation and satellite-measured tropospheric ozone during the latter Aura time period show increases of ∼+3 DU decade−1 over the N Atlantic and NE Pacific.

Ziemke, Jerald R.

Ozonesonde Quality Assurance: JOSIE-SHADOZ (2017) and SHALLOTS (2018)

Ozonesonde data constitute a mainstay of satellite calibration and are used for climatologies and analysis of trends, especially in the lower stratosphere where satellites are most uncertain. The electrochemical-concentration cell (ECC) ozonesonde has been deployed at ~100 stations worldwide since the 1960s, with changes over time in manufacture and procedures, including details of the cell chemical solution and data processing. As a consequence, there are biases among different stations and discontinuities in profile timeseries from individual site records. Since 1996 the Jülich [Germany] Ozone Sonde Intercomparison Experiment (JOSIE) has periodically tested ozonesondes in a simulation chamber designated the World Calibration Centre for Ozonesondes by WMO. In October- November 2017 a JOSIE campaign evaluated the sondes and procedures used in SHADOZ (Southern Hemisphere Additional Ozonesondes), a 14-station tropical and subtropical network. A distinctive feature of the 2017 JOSIE was that the tests were conducted by operators from eight SHADOZ stations; Nairobi, Natal, Irene, Costa Rica, Paramaribo, Reunion, Hanoi, Kuala Lumpur. Experimental protocols and preliminary results for the SHADOZ sonde configurations, which represent most of those in use today, are described. SHADOZ stations that follow WMO-recommended protocols record total ozone within 3% of the JOSIE reference instrument. Instrument biases noted in prior JOSIE and field tests like BESOS (2004) were noted in JOSIE-2017, with maximum effect in the stratosphere. In June 2018 we organized a series of dual launches during the OWLETS II campaign in the Maryland and Chesapeake Bay area (SHALLOTS = SHADOZ-OWLETS ParaLLel Ozonesonde Test Study). Instrument and solution types were varied as in JOSIE-2017 and three radiosonde-ozonesonde variants were tested. An example of a parallel sampling in SHALLOTS, from a Greenbelt EnSCI-iMet sonde combination flown with the Wallops SPCLMS package, is illustrated in the Figure. The result was a range of biases but in general the instrument combination (EnSCI-iMet) deployed at 11 SHADOZ stations recorded ~5-10% less ozone in the stratosphere than the SPC ECC sonde flown with a Vaisala or LMS system. These 2017 and 2018 results and prior JOSIEs demonstrate that regular testing is essential to maintain best practices in ozonesonde operations and to ensure high-quality data for the ozone assessment communities.

Quality assurance

Atmospheric Trace Gas (NO2 and Ozone) Dynamics over Coastal Waters near Polluted Urban Regions

At the interface between the land, oceans, and atmosphere, coastal regions are highly dynamic environments, characterized by strong variability in both water and air quality. Variability in atmospheric composition is associated with highly variable anthropogenic emissions, as well as complex meteorological processes that influence the circulation and accumulation of atmospheric pollutants at the land-ocean interface. Assessing the spatial and temporal dynamics of atmospheric pollutants, aerosols, and absorbing trace gases in coastal areas is critical for improving modeling of coastal tropospheric air quality, developing accurate satellite retrievals of coastal ocean color and biological processes, determining impacts of atmospheric pollution on human health, and assessing the ecological implications of atmospheric pollutant deposition for coastal terrestrial and aquatic ecosystems.Here, we present new measurements of atmospheric trace gas (NO2, and ozone) dynamics across a range of estuarine and coastal waters near urban regions. Measurements were conducted from research vessels using NASA's shipboard Pandora spectrometers, as part of recent multidisciplinary, multiplatform field campaigns, including the 2016 KORUS OC/AQ field campaign in the Yellow Sea and East Sea/Sea of Japan, the 2017/2018 OLWETS field campaign in the Chesapeake Bay estuary, and the 2018 LISTOS field campaign in the Long Island Sound. Shipboard measurements over these coastal waters were integrated with measurements from a ground-based Pandora network to examine differences in air quality over the land and over the ocean. Measurements were combined with air-parcel back-trajectory simulations to determine the origin of air masses over the coastal ocean. Comparisons with satellite retrievals of atmospheric composition reveal the benefits and limitations of polar-orbit satellite observations in capturing variability in atmospheric pollution gradients over land-water boundaries.

Tzortziou, Maria

Evaluation of MERRA-2-Based Ozone Profile Simulations with the Global Ozonesonde Network

Chemical transport model (CTM) hindcasts of ozone (O3) are useful for filling in observational gaps and providing context for observed O3 variability and trends. We use global networks of ozonesonde stations to evaluate the O3 profiles in two simulations running versions of the NASA Global Modeling Initiative (GMI) chemical mechanism. Both simulations are tied to the NASA Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) meteorological reanalysis: 1) The GMI CTM, and 2) The MERRA-2 GMI Replay (M2 GMI). Both simulations start in 1980, and are compared against >50,000 ozonesonde profiles from 37 global stations from the tropics to the poles. The comparisons allow us to evaluate how the Replay technique affects modeled O3 distribution, how an updated chemical mechanism in the GMI CTM affects simulated tropospheric O3 amounts, and how observed O3 distributions compare to the full set of model output. In general, M2 GMI O3 is ~10% higher than in the GMI CTM, and shows global near-surface and tropical upper troposphere/lower stratosphere (UT/LS) high biases. The updated chemical mechanism in the GMI CTM reduces these high biases. Both simulations show similar negative biases in tropical free-tropospheric O3, especially during typical biomass burning seasons. The simulations are highly-correlated with ozonesonde measurements, particularly in the UT/LS (r > 0.8), showing the ability of MERRA-2 to capture tropopause height variations. Both simulations show improved correlations with ozonesonde data and smaller O3 biases in recent years. We expect to use the sonde/model comparisons to diagnose causes of disagreement and to gauge the feasibility of calculating multidecadal O3 trends from the model output.

Stauffer, Ryan M.

The Ozone Water-Land Environmental Transition Study: An Innovative Strategy for Understanding Chesapeake Bay Pollution Events

Coastal regions have historically represented a significant challenge for air quality investigations because of water-land boundary transition characteristics and a paucity of measurements available over water. Prior studies have identified the formation of high levels of ozone over water bodies, such as the Chesapeake Bay, that can potentially recirculate back over land to significantly impact populated areas. Earth-observing satellites and forecast models face challenges in capturing the coastal transition zone where small-scale meteorological dynamics are complex and large changes in pollutants can occur on very short spatial and temporal scales. An observation strategy is presented to synchronously measure pollutants “over land” and “over water” to provide a more complete picture of chemical gradients across coastal boundaries for both the needs of state and local environmental management and new remote sensing platforms. Intensive vertical profile information from ozone lidar systems and ozonesondes, obtained at two main sites, one over land and the other over water, are complemented by remote sensing and in situ observations of air quality from ground-based, airborne (both personned and unpersonned), and shipborne platforms. These observations, coupled with reliable chemical transport simulations, such as the National Oceanic and Atmospheric Administration (NOAA) National Air Quality Forecast Capability (NAQFC), are expected to lead to a more fully characterized and complete land–water interaction observing system that can be used to assess future geostationary air quality instruments, such as the National Aeronautics and Space Administration (NASA) Tropospheric Emissions: Monitoring of Pollution (TEMPO), and current low-Earth-orbiting satellites, such as the European Space Agency’s Sentinel-5 Precursor (S5-P) with its Tropospheric Monitoring Instrument (TROPOMI).

Forecast Models

The Network for the Detection of Atmospheric Composition Change (NDACC): History, Status and Perspectives

The Network for the Detection of Atmospheric Composition Change (NDACC) is an international global network of more than 90 stations making high-quality measurements of atmospheric composition that began official operations in 1991 after 5 years of planning. Apart from sonde measurements, all measurements in the network are performed by ground-based remote-sensing techniques. Originally named the Network for the Detection of Stratospheric Change (NDSC), the name of the network was changed to NDACC in 2005 to better reflect the expanded scope of its measurements. The primary goal of NDACC is to establish long-term databases for detecting changes and trends in the chemical and physical state of the atmosphere (mesosphere, stratosphere, and troposphere) and to assess the coupling of such changes with climate and air quality. NDACC's origins, station locations, organizational structure, and data archiving are described. NDACC is structured around categories of ground-based observational techniques (sonde, lidar, microwave radiometers, Fourier-transform infrared, UV-visible DOAS (differential optical absorption spectroscopy)-type, and Dobson-Brewer spectrometers, as well as spectral UV radiometers), timely cross-cutting themes (ozone, water vapour, measurement strategies, cross-network data integration), satellite measurement systems, and theory and analyses. Participation in NDACC requires compliance with strict measurement and data protocols to ensure that the network data are of high and consistent quality. To widen its scope, NDACC has established formal collaborative agreements with eight other cooperating networks and Global Atmosphere Watch (GAW). A brief history is provided, major accomplishments of NDACC during its first 25 years of operation are reviewed, and a forward-looking perspective is presented.

lidar

Homogenizing and Estimating the Uncertainty in NOAA's Long-Term Vertical Ozone Profile Records Measured with the Electrochemical Concentration Cell Ozonesonde

NOAA's program of long-term monitoring of the vertical distribution of ozone with electrochemical concentration cell (ECC) ozonesondes has undergone a number of changes over the 50-year record. In order to produce a homogenous data set, these changes must be documented and, where necessary, appropriate corrections applied. This is the first comprehensive and consistent reprocessing of NOAA's ozonesonde data records that corrects for these changes using the rawest form of the data (cell current and pump temperature) in native resolution as well as a point-by-point uncertainty calculation that is unique to each sounding. The reprocessing is carried out uniformly at all eight ozonesonde sites in NOAA's network with differences in sensing solution and ozonesonde types accounted for in the same way at all sites. The corrections used to homogenize the NOAA ozonesonde data records greatly improve the ozonesonde measurements with an average one sigma uncertainty of +/- 4-6% in the stratosphere and +/- 5-20% in the troposphere. A comparison of the integrated column ozone from the ozonesonde profile with co-located Dobson spectrophotometers total column ozone measurements shows agreement within +/- 5% for >70% of the profiles. Very good agreement is also found in the stratosphere between ozonesonde profiles and profiles retrieved from the Solar Backscatter Ultraviolet (SBUV) instruments.

ozonesonde

First Reprocessing of Southern Hemisphere ADditional OZonesondes (SHADOZ) Profile Records (1998-2015): 1. Methodology and Evaluation

Electrochemical concentration cell ozonesonde measurements are an important source of highly resolved vertical profiles of ozone with long-term data records for deriving ozone trends, model development, satellite validation, and air quality studies. Ozonesonde stations employ a range of operational and data processing procedures, metadata reporting, and instrument changes that have resulted in inhomogeneities within individual station data records. A major milestone is the first reprocessing of seven Southern Hemisphere ADditional OZonesondes (SHADOZ) station ozonesonde records to account for errors and biases in operating/processing procedures. Ascension Island, Hanoi, Irene, Kuala Lumpur, La Reunion, Natal, and Watukosek station records all show an overall increase in ozone after reprocessing. Watukosek shows the largest increase of 9.0 plus or minus 2.1 Dobson Units (DU) in total column ozone; Irene and Hanoi show a 5.5 plus or minus 2.5 DU increase, while remaining sites show statistically insignificant enhancements. Negligible to modest ozone enhancements are observed after reprocessing in the troposphere (up to 8%) and stratosphere (up to 6%), except at La Reunion for which the application of background currents reduces tropospheric ozone (2.1 plus or minus1.3 DU). Inhomogeneities due to ozonesonde/solution-type changes at Ascension, Natal, and La Reunion are resolved with the application of transfer functions. Comparisons with EP-TOMS, Aura's Ozone Monitoring Instrument and Microwave Limb Sounder (MLS) satellite ozone overpasses show an overall improvement in agreement after reprocessing. Most reprocessed data sets show a significant reduction in biases with MLS at the ozone maximum region (50-10 hPa). Changes in radiosonde/ozonesonde system and nonstandard solution types can account for remaining discrepancies observed at several sites when compared to satellites.

Electrochemical concentration cell ozonesonde meas

Ozone Production by Corona Discharges During a Convective Event in DISCOVER-AQ Houston

An ozonesonde launched near electrically active convection in Houston, TX on 5 September 2013 during the NASA DISCOVER-AQ project measured a large enhancement of ozone throughout the troposphere. A separate ozonesonde was launched from Smith Point, TX (approx. 58 km southeast of the Houston site) at approximately the same time as the launch from Houston and did not measure that enhancement. Furthermore, ozone profiles for the descent of both sondes agreed well with the ascending Smith Point profile, suggesting a highly localized event in both space and time in which an anomalously large enhancement of 70 - 100 ppbv appeared in the ascending Houston ozonesonde data. Compared to literature values, such an enhancement appears to be the largest observed to date. Potential sources of the localized ozone enhancement such as entrainment of urban or biomass burning emissions, downward transport from the stratosphere, photochemical production from lightning NO(sub x), and direct ozone production from corona discharges were investigated using model simulations. We conclude that the most likely explanation for the large ozone enhancement is direct ozone production by corona discharges. Integrating the enhancement seen in the Houston ozone profile and using the number of electrical discharges detected by the NLDN (or HLMA), we estimate a production of 2.48 x 10(exp. 28) molecules of ozone per flash which falls within the range of previously recorded values (9.89 x 10(exp. 26) - 9.82 x 10)exp. 28) molecules of ozone per flash). Since there is currently no parameterization for the direct production of ozone from corona discharges we propose the implementation of an equation into a chemical transport model. Ultimately, additional work is needed to further understand the occurrence and impact of corona discharges on tropospheric chemistry on short and long timescales.

ozone

Ground-Based High Spectral Resolution Lidar Observation of Aerosol Vertical Distribution in the Summertime Southeast United States

As part of the Southeast United States-based Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS), and collinear with part of the Southeast Atmosphere Study, the University of Wisconsin High Spectral Resolution Lidar system was deployed to the University of Alabama from 19 June to 4 November 2013. With a collocated Aerosol Robotic Network (AERONET) sun photometer, a nearby Chemical Speciation Network (PM2.5) measurement station, and near daily ozonesonde releases for the August-September SEAC4RS campaign, the site allowed the regions first comprehensive diurnal monitoring of aerosol particle vertical structure. A 532nm lidar ratio of 55 sr provided good closure between aerosol backscatter and AERONET (aerosol optical thickness, AOT). A principle component analysis was performed to identify key modes of variability in aerosol backscatter. ''Fair weather'' days exhibited classic planetary boundary layer structure of a mixed layer accounting for approx. 50% of AOT and an entrainment zone providing another 25%. An additional 5-15% of variance is gained from the lower free troposphere from either convective detrainment or frequent intrusions of western United States biomass burning smoke. Generally, aerosol particles were contained below the 0 C level, a common level of stability in convective regimes. However, occasional strong injections of smoke to the upper troposphere were also observed, accounting for the remaining 10-15% variability in AOT. Examples of these common modes of variability in frontal and convective regimes are presented, demonstrating why AOT often has only a weak relationship to surface PM2.5 concentration.

HSRL

Probabilistic Forecasting of Surface Ozone with a Novel Statistical Approach

The recent change in the Environmental Protection Agency's surface ozone regulation, lowering the surface ozone daily maximum 8-h average (MDA8) exceedance threshold from 75 to 70 ppbv, poses significant challenges to U.S. air quality (AQ) forecasters responsible for ozone MDA8 forecasts. The forecasters, supplied by only a few AQ model products, end up relying heavily on self-developed tools. To help U.S. AQ forecasters, this study explores a surface ozone MDA8 forecasting tool that is based solely on statistical methods and standard meteorological variables from the numerical weather prediction (NWP) models. The model combines the self-organizing map (SOM), which is a clustering technique, with a step wise weighted quadratic regression using meteorological variables as predictors for ozone MDA8. The SOM method identifies different weather regimes, to distinguish between various modes of ozone variability, and groups them according to similarity. In this way, when a regression is developed for a specific regime, data from the other regimes are also used, with weights that are based on their similarity to this specific regime. This approach, regression in SOM (REGiS), yields a distinct model for each regime taking into account both the training cases for that regime and other similar training cases. To produce probabilistic MDA8 ozone forecasts, REGiS weighs and combines all of the developed regression models on the basis of the weather patterns predicted by an NWP model. REGiS is evaluated over the San Joaquin Valley in California and the northeastern plains of Colorado. The results suggest that the model performs best when trained and adjusted separately for an individual AQ station and its corresponding meteorological site.

Ozone variables

The First Twenty Years (1994 2014) of Ozone Soundings from Rapa Nui (27 deg S, 109 deg W, 51 m a.s.l.)

Ozone (O3) soundings have been performed on Easter Island or Rapa Nui (27 8S, 109 8W, 51 m a.s.l.) since 1994 as part of the Global Atmospheric Watch Programme of the World Meteorological Organization. In this work, we analyze 260 soundings compiled over the period 19942014, and make the data available for the international community. We characterize O3 profiles over this remote area of the Pacific by means of statistical analyses that consider, on the one hand, a traditional climatology that describes the data in terms of seasonal cycles based on monthly averages and, on the other hand, a process-oriented analysis based on self-organizing maps. Our analyses show the influence of both tropical and subtropical/mid-latitude air masses at Rapa Nui. The former occurs in summer and fall when convective conditions prevail, and the latter in late winter and spring when subsiding conditions are recurrent. The occurrence of stratospheric intrusions in late winter and spring in connection with deep troughs and the presence of the subtropical jet stream is also apparent in the data set. The tropospheric ozone column is in good agreement with the corresponding data derived from satellites but with a systematic overestimate of summer and fall values. There is evidence of an upward trend in ozone near the surface, which suggests the impact of local pollution. We look forward to an enhancement of the Rapa Nui observing site, given its location that offers a privileged position to observe climate change over the sparsely sampled and vast South Pacific Ocean.

tropical and subtropical/mid-latitude air masses

Tropospheric Ozonesonde Profiles at Long-Term U.S. Monitoring Sites: 2. Links Between Trinidad Head, CA, Profile Clusters and Inland Surface Ozone Measurements

Much attention has been focused on the transport of ozone (O3) to the western U.S., particularly given the latest revision of the National Ambient Air Quality Standard to 70 parts per billion by volume (ppbv) of O3. This makes quantifying the contributions of stratosphere-to-troposphere exchange, local pollution, and pollution transport to this region essential. To evaluate free-tropospheric and surface O3 in the western U.S., we use self-organizing maps to cluster 18 years of ozonesonde profiles from Trinidad Head, CA. Three of nine O3 mixing ratio profile clusters exhibit thin laminae of high O3 above Trinidad Head. The high O3 layers are located between 1 and 6 km above mean sea level and reside above an inversion associated with a northern location of the Pacific subtropical high. Ancillary data (reanalyses, trajectories, and remotely sensed carbon monoxide) help identify the high O3 sources in one cluster, but distinguishing mixed influences on the elevated O3 in other clusters is difficult. Correlations between the elevated tropospheric O3 and surface O3 at high-altitude monitors at Lassen Volcanic and Yosemite National Parks, and Truckee, CA, are marked and long lasting. The temporal correlations likely result from a combination of transport of baseline O3 and covarying meteorological parameters. Days corresponding to the high O3 clusters exhibit hourly surface O3 anomalies of +5-10 ppbv compared to a climatology; the positive anomalies can last up to 3 days after the ozonesonde profile. The profile and surface O3 links demonstrate the importance of regular ozonesonde profiling at Trinidad Head.

STE

Spatial and Temporal Variability of Ground and Satellite Column Measurements of NO2 and O3 over the Atlantic Ocean During the Deposition of Atmospheric Nitrogen to Coastal Ecosystems Experiment

In situ measurements of O3 and nitrogen oxides (NO + NO2=NOx) and remote sensing measurements of total column NO2 and O3 were collected on a ship in the North Atlantic Ocean as part of the Deposition of Atmospheric Nitrogen to Coastal Ecosystems (DANCE) campaign in July August 2014,100 km east of the mid-Atlantic United States. Relatively clean conditions for both surface in situ mixing ratio and total column O3 and NO2 measurements were observed throughout the campaign. Increased surface and column NO2 and O3 amounts were observed when a terrestrial air mass was advected over the study region. Relative to ship-based total column measurements using a Pandora over the entire study, satellite measurements overestimated total column NO2 under these relatively clean atmospheric conditions over offshore waters by an average of 16. Differences are most likely due to proximity, or lack thereof, to surface emissions; spatial averaging due to the field of view of the satellite instrument; and the lack of sensitivity of satellite measurements to the surface concentrations of pollutants. Total column O3 measurements from the shipboard Pandora showed good correlation with the satellite measurements(r 0.96), but satellite measurements were 3 systematically higher than the ship measurements, in agreement with previous studies. Derived values of boundary layer height using the surface in situ and total column measurements of NO2 are much lower than modeled and satellite-retrieved boundary layer heights, which highlight the differences in the vertical distribution between terrestrial and marine environments.

Martins, Douglas K.

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

Tropospheric Ozone Change from 1980 to 2010 Dominated by Equatorward Redistribution of Emissions

Ozone is an important air pollutant at the surface, and the third most important anthropogenic greenhouse gas in the troposphere. Since 1980, anthropogenic emissions of ozone precursors methane, non-methane volatile organic compounds, carbon monoxide and nitrogen oxides (NOx) have shifted from developed to developing regions. Emissions have thereby been redistributed equatorwards, where they are expected to have a stronger effect on the tropospheric ozone burden due to greater convection, reaction rates and NOx sensitivity. Here we use a global chemical transport model to simulate changes in tropospheric ozone concentrations from 1980 to 2010, and to separate the influences of changes in the spatial distribution of global anthropogenic emissions of short-lived pollutants, the magnitude of these emissions, and the global atmospheric methane concentration. We estimate that the increase in ozone burden due to the spatial distribution change slightly exceeds the combined influences of the increased emission magnitude and global methane. Emission increases in Southeast, East and South Asia may be most important for the ozone change, supported by an analysis of statistically significant increases in observed ozone above these regions. The spatial distribution of emissions dominates global tropospheric ozone, suggesting that the future ozone burden will be determined mainly by emissions from low latitudes.

Zhang, Yuqiang

Why Do Models Overestimate Surface Ozone in the Southeast United States?

Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NO(x) triple bond 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 SEAC(exp 4)RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model at 0.25 deg x 0.3125 deg horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NO(x) from the US Environmental Protection Agency (EPA) is too high. This finding is based on SEAC(exp 4)RS observations of NO(x) and its oxidation products, surface network observations of nitrate wet deposition fluxes, and OMI satellite observations of tropospheric NO2 columns. Our results indicate that NEI NO(x) emissions from mobile and industrial sources must be reduced by 30-60%, dependent on the assumption of the contribution by soil NO(x) emissions. Upper-tropospheric NO2 from lightning makes a large contribution to satellite observations of tropospheric NO2 that must be accounted for when using these data to estimate surface NO(x) emissions. We find that only half of isoprene oxidation proceeds by the high-NO(x) pathway to produce ozone; this fraction is only moderately sensitive to changes in NO(x) emissions because isoprene and NO(x) emissions are spatially segregated. GEOS-Chem with reduced NO(x) emissions provides an unbiased simulation of ozone observations from the aircraft and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NO(x) oxidation products. However, the model is still biased high by 6 plus or minus 14 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 the surface that GEOS-Chem does not capture. This bias may reflect a combination of excessive vertical mixing and net ozone production in the model boundary layer.

Oxidation