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Estimates of Lightning NOx Production Based on OMI NO2 Observations Over the Gulf of Mexico

We evaluate nitrogen oxide (NO(sub x) NO + NO2) production from lightning over the Gulf of Mexico region using data from the Ozone Monitoring Instrument (OMI) aboard NASAs Aura satellite along with detection efficiency-adjusted lightning data from the World Wide Lightning Location Network (WWLLN). A special algorithm was developed to retrieve the lightning NOx [(LNO(sub x)] signal from OMI. The algorithm in its general form takes the total slant column NO2 from OMI and removes the stratospheric contribution and tropospheric background and includes an air mass factor appropriate for the profile of lightning NO(sub x) to convert the slant column LNO2 to a vertical column of LNO(sub x). WWLLN flashes are totaled over a period of 3 h prior to OMI overpass, which is the time an air parcel is expected to remain in a 1 deg. x 1 deg. grid box. The analysis is conducted for grid cells containing flash counts greater than a threshold value of 3000 flashes that yields an expected LNO(sub x) signal greater than the background. Pixels with cloud radiance fraction greater than a criterion value (0.9) indicative of highly reflective clouds are used. Results for the summer seasons during 2007-2011 yield mean LNO(sub x) production of approximately 80 +/- 45 mol per flash over the region for the two analysis methods after accounting for biases and uncertainties in the estimation method. These results are consistent with literature estimates and more robust than many prior estimates due to the large number of storms considered but are sensitive to several substantial sources of uncertainty.

Lightning↗

The Utility of the OMI HCHO/NO2 in Air Quality Decision-Making Activities

I will discuss a novel and practical application of the OMI HCHU and NO2 data products to the "weight of evidence" in the air quality decision-making process (e.g., State Implementation Plan (SIP)) for a city, region, or state to demonstrate that it is making progress toward attainment of the National Ambient Air Quality Standard (NAAQS) for ozone. Any trend, or lack thereof, in the observed OMI HCHO/NO2 may support that an emission control strategy implemented to reduce ozone is or is not occurring for a metropolitan area. In addition, the observed OMI HCHO/NO2 may be used to define new emission control strategies as the photochemical environments of urban areas evolve over time. I will demonstrate the utility of the OMI HCHO/NO2 over the U.S. for air quality applications with support from simulations with both a regional model and a photochemical box model. These results support mission planning of an OMI-like instrument for the proposed GEO-CAPE satellite that has as one of its objectives to study air quality from space. However, I'm attending the meeting as the Aura Deputy Project Scientist, so I don't technically need to present anything to justify the travel.

Duncan, Bryan↗

A New Global Anthropogenic SO2 Emission Inventory for the Last Decade: A Mosaic of Satellite-Derived and Bottom-Up Emissions

Sulfur dioxide (SO2) measurements from the Ozone Monitoring Instrument (OMI) satellite sensor have been used to detect emissions from large point sources. Emissions from over 400 sources have been quantified individually based on OMI observations, accounting for about a half of total reported anthropogenic SO2 emissions. Here we report a newly developed emission inventory, OMI-HTAP, by combining these OMI-based emission estimates and the conventional bottom-up inventory, HTAP, for smaller sources that OMI is not able to detect. OMI-HTAP includes emissions from OMI-detected sources that are not captured in previous leading bottom-up inventories, enabling more accurate emission estimates for regions with such missing sources. In addition, our approach offers the possibility of rapid updates to emissions from large point sources that can be detected by satellites. Our methodology applied to OMI-HTAP can also be used to merge improved satellite-derived estimates with other multi-year bottom-up inventories, which may further improve the accuracy of the emission trends. OMI-HTAP SO2 emissions estimates for Persian Gulf, Mexico, and Russia are 59%, 65%, and 56% larger than HTAP estimates, respectively, in year 2010. We have evaluated the OMI-HTAP inventory by performing simulations with the Goddard Earth Observing System version 5 (GEOS-5) model. The GEOS-5 simulated SO2 concentrations driven by both HTAP and OMI-HTAP were compared against in situ measurements. We focus for the validation on year 2010 for which HTAP is most valid and for which a relatively large number of in situ measurements are available. Results show that the OMI-HTAP inventory improves the agreement between the model and observations, in particular over the US, with the normalized mean bias decreasing from 0.41 (HTAP) to -0.03 (OMI-HTAP) for year 2010. Simulations with the OMI-HTAP inventory capture the worldwide major trends of large anthropogenic SO2 emissions that are observed with OMI. Correlation coefficients of the observed and modelled surface SO2 in 2014 increase from 0.16 (HTAP) to 0.59 (OMI-HTAP) and the normalized mean bias dropped from 0.29 (HTAP) to 0.05 (OMI-HTAP), when we updated 2010 HTAP emissions with 2014 OMI-HTAP emissions in the model.

Sulfur dioxide (SO2)↗

Exploiting OMI NO2 Satellite Observations to Infer Fossil-fuel CO2 Emissions from U.S. Megacities

Fossil-fuel CO2 emissions and their trends in eight U.S. megacities during 2006–2017 are inferred by combining satellite-derived NOX emissions with bottom-up city-specific NOX-to-CO2 emission ratios. A statistical model is fit to a collection NO2 plumes observed from the Ozone Monitoring Instrument (OMI), and is used to calculate top-down NOX emissions. Decreases in OMI-derived NOX emissions are observed across the eight cities from 2006 to 2017 (−17% in Miami to −58% in Los Angeles), and are generally consistent with long-term trends of bottom-up inventories (−25% in Miami to −49% in Los Angeles), but there are some interannual discrepancies. City-specific NOX-to-CO2 emission ratios, used to calculate inferred CO2, are estimated through annual bottom-up inventories of NOX and CO2 emissions disaggregated to 1 × 1 km2 resolution. Over the study period, NOX-to-CO2 emission ratios have decreased by ~40% nationwide (−24% to −51% for our studied cities), which is attributed to a faster reduction in NOX when compared to CO2 due to policy regulations and fuel type shifts. Combining top-down NOX emissions and bottom-up NOX-to-CO2 emission ratios, annual fossil-fuel CO2 emissions are derived. Inferred OMI-based top-down CO2 emissions trends vary between +7% in Dallas to −31% in Phoenix. For 2017, we report annual fossil-fuel CO2 emissions to be: Los Angeles 113 ± 49 Tg/yr; New York City 144 ± 62 Tg/yr; and Chicago 55 ± 24 Tg/yr. A study in the Los Angeles area, using independent methods, reported a 2013–2016 average CO2 emissions rate of 104 Tg/yr and 120 Tg/yr, which suggests that the CO2 emissions from our method are in good agreement with other studies' top-down estimates. We anticipate future remote sensing instruments – with better spatial and temporal resolution – will better constrain the NOX-to-CO2 ratio and reduce the uncertainty in our method.

Ozone Monitoring Instrument (OMI)↗

Development and Testing of the New Surface LER Climatology for OMI UV Aerosol Retrievals

Ozone Monitoring Instrument (OMI) onboard Aura satellite retrieved aerosols properties using UV part of solar spectrum. The OMI near UV aerosol algorithm (OMAERUV) is a global inversion scheme which retrieves aerosol properties both over ocean and land. The current version of the algorithm makes use of TOMS derived Lambertian Equivalent Reflectance (LER) climatology. A new monthly climatology of surface LER at 354 and 388 nm have been developed. This will replace TOMS LER (380 nm and 354nm) climatology in OMI near UV aerosol retrieval algorithm. The main objectives of this study is to produce high resolution (quarter degree) surface LER sets as compared to existing one degree TOMS surface LERs, to product instrument and wavelength consistent surface climatology. Nine years of OMI observations have been used to derive monthly climatology of surface LER. MODIS derived aerosol optical depth (AOD) have been used to make aerosol corrections on OMI wavelengths. MODIS derived BRDF adjusted reflectance product has been also used to capture seasonal changes in the surface characteristics. Finally spatial and temporal averaging techniques have been used to fill the gaps around the globes, especially in the regions with consistent cloud cover such as Amazon. After implementation of new surface data in the research version of algorithm, comparisons of AOD and single scattering albedo (SSA) have been performed over global AERONET sites for year 2007. Preliminary results shows improvements in AOD retrievals globally but more significance improvement were observed over desert and bright locations. We will present methodology of deriving surface data sets and will discuss the observed changes in retrieved aerosol properties with respect to reference AERONET measurements.

Aerosol↗

Applications of OMI Tropospheric NO(Sub 2) Data: Air Quality Trends in the US and Lightning NO(x) Source Strength

This talk will be presented in two parts: 1) an analysis of tropospheric column NO2 trends in the eastern half of the United States over the period 2005 to 2009 and 2) estimation of lightning NO(x) production rates based on OMI observations and lightning flash rate data. The air quality trends in the eastern US will be determined for specific subregions using tropospheric column NO2 data from OMI for 2005 through 2008 and from GOME-2 for 2007 through 2009. This period is characterized by significant NO(x) emission reductions at power plants within most of this region. The air quality trends will be compared with those estimated from continuous emission monitoring data from the power plants compiled by the US Environmental Protection Agency. OMI NO2 data have also been used to estimate lightning NOx production per flash in selected storms near Costa Rica and Panama during the 2007 NASA TC4 field campaign and over the continental US, Gulf of Mexico, and western Atlantic during the summers of 2005 and 2006. The lightning signal is extracted from the OMI data through a custom retrieval in which an NO2 profile representative of convective outflow is used in the airmass factor calculation and the background NO2 column is subtracted from the tropospheric column. When combined with NO(x)/NO2 ratios from the NASA GMT model and observed flash rates, the resulting estimates of NO(x) production per flash are comparable to those estimated obtained from analyses of aircraft data and cloud-resolving modeling.

Pickering, Kenneth↗

The MERRA-2 Aerosol Reanalysis, 1980 Onward. Part II: Evaluation and Case Studies

The Modern-Era Retrospective Analysis for Research and Applications, Version 2 (MERRA-2) is NASA’s latest reanalysis for the satellite era (1980-present) using the Goddard Earth Observing System version 5 (GEOS-5) Earth system model. MERRA-2 provides several improvements over its predecessor (MERRA), including the inclusion of interactive aerosols for the entire period. In addition to assimilating bias-corrected Aerosol Optical Depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) on the Terra and Aqua satellites, it also includes the assimilation of bias-corrected AOD from Advanced Very High Resolution Spectroradiometer (AVHRR) instruments, Multi-angle Imaging SpectroRadiometer (MISR) AOD over bright surfaces, and ground-based Aerosol Robotic Network (AERONET) AOD. This paper is the second of a pair that summarizes our efforts to assess the quality of the MERRA-2 aerosol assimilation. In this study, we first follow previous work performed with version 1 of the MERRA Aerosol Reanalysis (MERRAero) using independent observations. The evaluation of MERRA-2 Absorption Aerosol Optical Depth (AAOD) and ultra-violet Aerosol Index (UV-AI) against the Ozone Monitoring Instrument (OMI) observations show good agreement, particularly over dusty regions where our previous efforts improved model aerosol optical properties. Next, we find that aerosol assimilation system improves the aerosol vertical structure when compared to estimates from the same version of the model without AOD assimilation. A similar conclusion is found for MERRA-2 aerosol surface fine particulate matter (PM (sub 2.5)). However, deficiencies in the forward model such as missing emissions noted during the MERRAero study still explain the MERRA-2 PM(sub 2.5) bias relative to observations over the United States. Finally, to illustrate successes and weaknesses of the AOD assimilation, we focus on the performance of the MERRA-2 aerosol system during several major aerosol events: the Mount Pinatubo eruption in 1991, a Saharan dust event and transportation over the Atlantic Ocean during April 2010, the Rim Fire of summer 2013 in California, and an extreme pollution event over China in January 2013. We conclude with a summary that points to best practices for utilizing the MERRA-2 aerosol reanalysis in future studies.

V Buchard↗

Global Distribution and 14-Year Changes in Erythemal Irradiance, UV Atmospheric Transmission, and Total Column Ozone 2005 – 2018 Estimated from OMI and EPIC Observations

Satellite data from the Ozone Measuring Instrument (OMI) and Earth Polychromatic Imaging Camera (EPIC) are used to study changes and global distribution of UV erythemal irradiance in mW/m(exp 2) E(ζ,φ,z,t) and the dimensionless UV index (E/25 mWm(exp 2)) over the Earth’s surface as a function of latitude ζ, longitude φ, altitude z, and time t. OMI time series data starting in January 2005 to December 2018 are used to estimate 14-year changes in erythemal irradiance, total column ozone TCO3, scene reflectivity LER, and aerosol absorption τA at specific land sites in the Northern and Southern Hemispheres using publicly available OMI data. Estimates of changes in atmospheric transmission ΔCτ(ζ,φ,z,t) derived from OMI measured cloud and haze reflectivity show an increase between 60°S to 45°S almost no average 14-year change from 55°S to 30°N but show an increase from 35°N to 55°N. This implies increased solar insolation at higher latitudes that suggests positive feedback for global warming. Changes in aerosol absorption of UV irradiance ΔCA(ζ,φ,z,t) derived from changes in τA are mostly in the equatorial region and at higher southern latitudes resulting in correlated changes in E. TCO3 derived from OMI data has increased at a rate of 2% per decade for the latitudes between 60°S to 10°N changing to a decrease of 1% per decade between 40°N to 60°N. The result is an average decrease in E(ζ,φ,z,t) at a rate of 2% per decade in the Southern Hemisphere and an increase between 40°N to 60°N. For some specific sites (latitudes from 55°S to 45°N) there has been little or no change in E(ζ,φ,z,t) for the period 2005 – 2018. Nearly half the sites show strong correlation effects of both short- and long-term cloud and absorbing aerosol change as well as anticorrelation with total column ozone change ΔTCO3. Synoptic EPIC data from the sunlit Earth are used to derive ozone and reflectivity needed for global images of the distribution of E(ζ,φ,z,t) from sunrise to sunset centered on the Americas, Europe-Africa, and Asia. EPIC data are used to show the latitudinal distribution of E(ζ,φ,z,t) from the equator to 75° for specific longitudes. Dangerously high amounts of erythemal irradiance (12 < UV index < 18) are found for many low latitude and high-altitude sites (e.g., San Pedro, Chile (2.45 km), La Paz, Bolivia (3.78 km). Lower UV indices at some equatorial or high-altitude sites (e.g., Quito, Ecuador) are moderated by the presence of persistent cloud effects. High UVI levels (UVI > 6) are also found at most mid-latitude sites during the summer months.

Ozone Measuring Instrument (OMI) and Earth Polychr↗

The Utility of the OMI HCHO and NO2 Data Products in Air Quality Decision- Making Activities

We will present three related air quality applications of the OMI HCHO (formaldehyde) and NO2 (nitrogen dioxide) data products, which we us to support mission planning of an OMI-like instrument for the proposed GEO-CAPE satellite that has as one of its objectives to study air quality from space. First, we will discuss a novel and practical application of the data products to the "weight of evidence" in the air quality decision-making process (e.g., State Implementation Plan (SIP)) for a city, region, or state to demonstrate that it is making progress toward attainment of the National Ambient Air Quality Standard (NAAQS) for ozone. Any trend, or lack thereof, in the observed OMI HCHO/NO2, which we use as an air quality indicator, may support that an emission control strategy implemented to reduce ozone is or is not occurring for a metropolitan area. Second, we will discuss how we use variations in the OMI HCHO product as a proxy for variability in the biogenic hydrocarbon, isoprene, which is an important player for the formation of high levels of ozone and the dominant source of HCHO in the eastern U.S. Third, we will discuss the variability of NO2 in the U.S. as indicated by the OMI NO2 product. In addition, we will show the impact of the 2005 hurricanes on pollutant emissions, including those associated with the intensive oil extraction and refining activities, in the Gulf of Mexico region using the OMI NO2 product. The variability of HCHO and NO2 as indicated by OMI helps us to understand changes in the OMI HCHO/NO2 and the implications for ozone formation.

Duncan, Bryan N.↗

Impact of the Ozone Monitoring Instrument Row Anomaly on the Long-Term Record of Aerosol Products

Since about three years after the launch the Ozone Monitoring Instrument (OMI) on the EOS-Aura satellite, the sensor's viewing capability has been affected by what is believed to be an internal obstruction that has reduced OMI's spatial coverage. It currently affects about half of the instrument's 60 viewing positions. In this work we carry out an analysis to assess the effect of the reduced spatial coverage on the monthly average values of retrieved aerosol optical depth (AOD), single scattering albedo (SSA) and the UV Aerosol Index (UVAI) using the 2005-2007 three-year period prior to the onset of the row anomaly. Regional monthly average values calculated using viewing positions 1 through 30 were compared to similarly obtained values using positions 31 through 60, with the expectation of finding close agreement between the two calculations. As expected, mean monthly values of AOD and SSA obtained with these two scattering-angle dependent subsets of OMI observations agreed over regions where carbonaceous or sulphate aerosol particles are the predominant aerosol type. However, over arid regions, where desert dust is the main aerosol type, significant differences between the two sets of calculated regional mean values of AOD were observed. As it turned out, the difference in retrieved desert dust AOD between the scattering-angle dependent observation subsets was due to the incorrect representation of desert dust scattering phase function. A sensitivity analysis using radiative transfer calculations demonstrated that the source of the observed AOD bias was the spherical shape assumption of desert dust particles. A similar analysis in terms of UVAI yielded large differences in the monthly mean values for the two sets of calculations over cloudy regions. On the contrary, in arid regions with minimum cloud presence, the resulting UVAI monthly average values for the two sets of observations were in very close agreement. The discrepancy under cloudy conditions was found to be caused by the parameterization of clouds as opaque Lambertian reflectors. When properly accounting for cloud scattering effects using Mie theory, the observed UVAI angular bias was significantly reduced. The analysis discussed here has uncovered important algorithmic deficiencies associated with the model representation of the angular dependence of scattering effects of desert dust aerosols and cloud droplets. The resulting improvements in the handling of desert dust and cloud scattering have been incorporated in an improved version of the OMAERUV algorithm.

Atmospheric Chemistry↗

SO2 Emission Estimates Using OMI SO2 Retrievals for 2005-2017

SO2 column densities from OMI provide important information on emission trends and missing sources, but there are discrepancies between different retrieval products. We employ three OMI SO2 retrieval products (NASA standard (SP), NASA prototype, and BIRA) to study the magnitude and trend of SO2 emissions. SO2 column densities from these retrievals are most consistent when viewing angles and solar zenith angles are small, suggesting more robust emission estimates in summer and at low latitudes. We then apply a hybrid 4DVar/mass balance emission inversion to derive monthly SO2 emissions from the NASA SP and BIRA products. Compared to HTAPv2 emissions in 2010, both posterior emission estimates are lower in US, India and Southeast China, but show different changes of emissions in North China Plain. The discrepancies between monthly NASA and BIRA posterior emissions in 2010 are less than or equal to 17% in China and 34% in India. SO2 emissions increase from 2005 to 2016 by 35% (NASA) 48% (BIRA) in India, but decrease in China by 23% (NASA) 33% (BIRA) since 2008. Compared to insitu measurements, the posterior GEOSChem surface SO2 concentrations have reduced NMB in China, the US, and India but not in South Korea in 2010. BIRA posteriors have better consistency with the annual growth rate of surface SO2 measurement in China and spatial variability of SO2 concentration in China, South Korea and India, whereas NASA SP posteriors have better seasonality. These evaluations demonstrate the capability to recover SO2 emissions using OMI observations.

Data assimilation↗

High resolution assimilation of multiple satellite retrievals with emissions adjustment to improve air quality forecasting with WRF-Chem/DART

We will present results from medium (15km, 6hr cycling) and high (4 km, 6 hr cycling) spatiotemporal resolution applications of the WRF-Chem/DART ensemble, regional, air quality (AQ) forecast/assimilation system.The medium-resolution setup is applied to the Discover AQ/Front Range Air Pollution and Photochemistry Experiment (FRAPPE) domain from July 14 to July 29, 2014. The high-resolution setup is applied to a Colorado domain from July 14 to July 29, 2020. For the FRAPPE application, we assimilate MOPITT CO; IASI CO;MODIS AOD; OMI O3, NO2; and AirNow CO, O3, NO2, SO2, PM10, and PM2.5. For the Colorado application, we assimilate the same MOPITT, MODIS, and AirNow constituents as in the FRAPPE application and TROPOMI CO, O3, NO2; and synthetic TEMPO O3and NO2. WRF-Chem/DART integrates the Weather Research and Forecast (WRF) model with on-line chemistry (WRF-Chem) into the Data Assimilation Research Testbed (DART). It assimilates AirNow CO, O3, NO2, SO2, PM10, and PM2.5 measurements, MOPITT CO; IASI CO, O3; OMI O3, NO2, SO2; TROPOMI CO, O3, NO2, SO2; MODIS AOD; and synthetic TEMPO O3 and NO2 total/partial column and/or profile retrievals.WRF-Chem/DART uses: (i) the state augmentation method for adjusting emissions; (ii) state-space localization; and (iii) a near-real time scripting system. We use the medium-resolution FRAPPE application to demonstrate the incremental benefits from assimilating OMI observations with emissions adjustment and the high-resolution Colorado application to demonstrate the incremental benefits from assimilating syntheticTEMPO observations with emissions adjustment. For both applications, we expect that: (i) assimilating chemical observations will increaseAQ forecast skill; (ii) including emissions adjustment will increase forecast skill/predictability; and (iii) including assimilation of synthetic TEMPO observations will further increase forecast skill/predictability.

High resolution↗

Interpreting the Ultraviolet Aerosol Index Observed with the OMI Satellite Instrument to Understand Absorption by Organic Aerosols: Implications for Atmospheric Oxidation and Direct Radiative Effects

Satellite observations of the ultraviolet aerosol index (UVAI) are sensitive to absorption of solar radiation by aerosols; this absorption affects photolysis frequencies and radiative forcing. We develop a global simulation of the UVAI using the 3-D chemical transport model GEOSChem coupled with the Vector Linearized Discrete Ordinate Radiative Transfer model (VLIDORT). The simulation is applied to interpret UVAI observations from the Ozone Monitoring Instrument (OMI) for the year 2007. Simulated and observed values are highly consistent in regions where mineral dust dominates the UVAI, but a large negative bias (-0.32 to -0.97) exists between simulated and observed values in biomass burning regions. We determine effective optical properties for absorbing organic aerosol, known as brown carbon (BrC), and implement them into GEOS-Chem to better represent observed UVAI values over biomass burning regions. The inclusion of absorbing BrC decreases the mean bias between simulated and OMI UVAI values from -0.57 to -0.09 over West Africa in January, from -0.32 to +0.0002 over South Asia in April, from -0.97 to -0.22 over southern Africa in July, and from -0.50 to +0.33 over South America in September. The spectral dependence of absorption after including BrC in the model is broadly consistent with reported observations for biomass burning aerosol, with absorbing Angstrom exponent (AAE) values ranging from 2.9 in the ultraviolet (UV) to 1.3 across the UV-Near IR spectrum. We assess the effect of the additional UV absorption by BrC on atmospheric photochemistry by examining tropospheric hydroxyl radical (OH) concentrations in GEOS-Chem. The inclusion of BrC decreases OH by up to 30% over South America in September, up to 20% over southern Africa in July, and up to 15% over other biomass burning regions. Global annual mean OH concentrations in GEOS-Chem decrease due to the presence of absorbing BrC, increasing the methyl chloroform lifetime from 5.62 to 5.68 years, thus reducing the bias against observed values. We calculate the direct radiative effect (DRE) of BrC using GEOS-Chem coupled with the radiative transfer model RRTMG (GC-RT). Treating organic aerosol as containing more strongly absorbing BrC changes the global annual mean all-sky top of atmosphere (TOA) DRE by +0.03Wm(exp -2) and all-sky surface DRE by -0.08Wm(exp -2). Regional changes of up to +0.3Wm(exp -2) at TOA and down to -1.5Wm(exp -2) at the surface are found over major biomass burning regions.

Air Pollution↗

Nitrogen Oxides in the Global Upper Troposphere: Interpreting Cloud-Sliced NO2 Observations from the OMI Satellite Instrument

Nitrogen oxides (NOx≡NO+NO2) in the upper troposphere (UT) have a large impact on global tropospheric ozone and OH (the main atmospheric oxidant). New cloud-sliced observations of UT NO2 at 450–280 hPa (∼6–9 km) from the Ozone Monitoring Instrument (OMI) produced by NASA and the Royal Netherlands Meteorological Institute (KNMI) provide global coverage to test our understanding of the factors controlling UT NOx. We find that these products offer useful information when averaged over coarse scales (20°×32°, seasonal), and that the NASA product is more consistent with aircraft observations of UT NO2. Correlation with Lightning Imaging Sensor (LIS) and Optical Transient Detector (OTD) satellite observations of lightning flash frequencies suggests that lightning is the dominant source of NOx to the upper troposphere except for extratropical latitudes in winter. The NO2 background in the absence of lightning is 10–20 pptv. We infer a global mean NOx yield of 280±80 moles per lightning flash, with no significant difference between the tropics and midlatitudes, and a global lightning NOx source of 5.9±1.7 Tg N a(exp −1). There is indication that the NOx yield per flash increases with lightning flash footprint and with flash energy.

Marais, Eloise A.↗

Glyoxal Yield from Isoprene Oxidation and Relation to Formaldehyde: Chemical Mechanism, Constraints from SENEX Aircraft Observations, and Interpretation of OMI Satellite Data

Glyoxal (CHOCHO) is produced in the atmosphere by the oxidation of volatile organic compounds(VOCs). Like formaldehyde (HCHO), another VOC oxidation product, it is measurable from space by solar backscatter. Isoprene emitted by vegetation is the dominant source of CHOCHO and HCHO in most of the world. We use aircraft observations of CHOCHO and HCHO from the Southeast Nexus (SENEX) campaign over the southeast US in summer 2013 to better understand the CHOCHO time-dependent yield from isoprene oxidation, its dependence on nitrogen oxides (NO (sub x) triple bonded to NO plus NO2), the behavior of the CHOCHO-HCHO relationship, the quality of Ozone Monitoring Instrument (OMI) CHOCHO satellite observations, and the implications for using CHOCHO observations from space as constraints on isoprene emissions. We simulate the SENEX and OMI observations with the Goddard Earth Observing System chemical transport model (GEOSChem) featuring a new chemical mechanism for CHOCHO formation from isoprene. The mechanism includes prompt CHOCHO formation under low-NO (sub x) conditions following the isomerization of the isoprene peroxy radical (ISOPO2).The SENEX observations provide support for this prompt CHOCHO formation pathway, and are generally consistent with the GEOS-Chem mechanism. Boundary layer CHOCHO and HCHO are strongly correlated in the observations and the model, with some departure under low-NO (sub x) conditions due to prompt CHOCHO formation. SENEX vertical profiles indicate a free-tropospheric CHOCHO background that is absent from the model. The OMI CHOCHO data provide some support for this free-tropospheric background and show southeast US enhancements consistent with the isoprene source but a factor of 2 too low. Part of this OMI bias is due to excessive surface reflectivities assumed in the retrieval. The OMI CHOCHO and HCHO seasonal data over the southeast US are tightly correlated and provide redundant proxies of isoprene emissions. Higher temporal resolution in future geostationary satellite observations may enable detection of the prompt CHOCHO production under low-NO (sub x) conditions apparent in the SENEX data.

OMI↗

Intercomparison of SCIAMACHY and OMI Tropospheric NO2 Columns: Observing the Diurnal Evolution of Chemistry and Emissions from Space

Concurrent (August 2006) measurements of tropospheric NO2 columns from OMI aboard Aura (1330 local overpass time) and SCIAMACHY aboard Envisat (1000 local overpass time) offer an opportunity to examine the consistency between the two instruments under tropospheric background conditions and the effect of different observing times. For scenes with tropospheric NO 2 columns <5.0 x 10(exp 15) molecules cm 2, SCIAMACHY and OMI agree within 1.0-2.0 x 10(exp 15) molecules cm 2, consistent with the detection limits of both instruments. We find evidence for a low bias of 0.2 x 10(exp 15) molecules cm 2 in OMI observations over remote oceans. Over the fossil fuel source regions at northern midlatitudes, we find that SCIAMACHY observes up to 40% higher NO2 at 1000 local time (LT) than OMI at 1330 LT. Over biomass burning regions in the tropics, SCIAMACHY observes up to 40% lower NO 2 columns than OMI. These differences are present in the spectral fitting of the data (slant column) and are augmented in the fossil fuel regions and dampened in the tropical biomass burning regions by the expected increase in air mass factor as the mixing depth rises from 1000 to 1330 LT. Using a global 3-D chemical transport model (GEOS-Chem), we show that the 1000-1330 LT decrease in tropospheric NO2 column over fossil fuel source regions can be explained by photochemical loss, dampened by the diurnal cycle of anthropogenic emissions that has a broad daytime maximum. The observed 1000-1330 LT NO2 column increase over tropical biomass burning regions points to a sharp midday peak in emissions and is consistent with a diurnal cycle of emissions derived from geostationary satellite fire counts.

Boersma, K. Folkert↗

Highlights from a Decade of OMI-TOMS Total Ozone Observations on EOS Aura

Total ozone measurements from OMI have been instrumental in meeting Aura science objectives. In the last decade, OMI has extended the length of the TOMS total ozone record to over 35 years to monitor stratospheric ozone recovery. OMI-TOMS total ozone measurements have also been combined synergistically with measurements from other Aura instruments and MLS in particular, which provides vertically resolved information that complements the total O3 mapping capability of OMI. With this combined approach, the EOS Aura platform has produced more accurate and detailed measurements of tropospheric ozone. This has led in turn to greater understanding of the sources and transport of tropospheric ozone as well as its radiative forcing effect. The combined use of OMI and MLS data was also vital to the analysis of the severe Arctic ozone depletion event of 2011. The quality of OMI-TOMS total O3 data used in these studies is the result of several factors: a mature and well-validated algorithm, the striking stability of the OMI instrument, and OMI's hyperspectral capabilities used to derive cloud pressures. The latter has changed how we think about the effects of clouds on total ozone retrievals. We will discuss the evolution of the operational V8.5 algorithm and provide an overview and motivation for V9. After reviewing results and developments of the past decade, we finally highlight how ozone observations from EOS Aura are playing an important role in new ozone mapping missions.

Ozone↗

An Optimal-Estimation-Based Aerosol Retrieval Algorithm Using OMI Near-UV Observations

An optimal-estimation(OE)-based aerosol retrieval algorithm using the OMI (Ozone Monitoring Instrument) near-ultraviolet observation was developed in this study. The OE-based algorithm has the merit of providing useful estimates of errors simultaneously with the inversion products. Furthermore, instead of using the traditional lookup tables for inversion, it performs online radiative transfer calculations with the VLIDORT (linearized pseudo-spherical vector discrete ordinate radiative transfer code) to eliminate interpolation errors and improve stability. The measurements and inversion products of the Distributed Regional Aerosol Gridded Observation Network campaign in northeast Asia (DRAGON NE-Asia 2012) were used to validate the retrieved aerosol optical thickness (AOT) and single scattering albedo (SSA). The retrieved AOT and SSA at 388 nm have a correlation with the Aerosol Robotic Network (AERONET) products that is comparable to or better than the correlation with the operational product during the campaign. The OEbased estimated error represented the variance of actual biases of AOT at 388 nm between the retrieval and AERONET measurements better than the operational error estimates. The forward model parameter errors were analyzed separately for both AOT and SSA retrievals. The surface reflectance at 388 nm, the imaginary part of the refractive index at 354 nm, and the number fine-mode fraction (FMF) were found to be the most important parameters affecting the retrieval accuracy of AOT, while FMF was the most important parameter for the SSA retrieval. The additional information provided with the retrievals, including the estimated error and degrees of freedom, is expected to be valuable for relevant studies. Detailed advantages of using the OE method were described and discussed in this paper.

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