Global Free-tropospheric NO2 Abundances Derived Using a Cloud Slicing Technique from AURA OMI

We derive free-tropospheric NO2 volume mixing ratios (VMRs) by applying a cloud-slicing technique to data from the Ozone Monitoring Instrument (OMI) on the Aura satellite. In the cloud-slicing approach, the slope of the above-cloud NO2 column versus the cloud scene pressure is proportional to the NO2 VMR. In this work, we use a sample of nearby OMI pixel data from a single orbit for the linear fit. The OMI data include cloud scene pressures from the rotational-Raman algorithm and above-cloud NO2 vertical column density (VCD) (defined as the NO2 column from the cloud scene pressure to the top of the atmosphere) from a differential optical absorption spectroscopy (DOAS) algorithm. We compare OMI-derived NO2 VMRs with in situ aircraft profiles measured during the NASA Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in 2006. The agreement is generally within the estimated uncertainties when appropriate data screening is applied. We then derive a global seasonal climatology of free-tropospheric NO2 VMR in cloudy conditions. Enhanced NO2 in the free troposphere commonly appears near polluted urban locations where NO2 produced in the boundary layer may be transported vertically out of the boundary layer and then horizontally away from the source. Signatures of lightning NO2 are also shown throughout low and middle latitude regions in summer months. A profile analysis of our cloud-slicing data indicates signatures of lightning-generated NO2 in the upper troposphere. Comparison of the climatology with simulations from the global modeling initiative (GMI) for cloudy conditions (cloud optical depth less than10) shows similarities in the spatial patterns of continental pollution outflow. However, there are also some differences in the seasonal variation of free-tropospheric NO2 VMRs near highly populated regions and in areas affected by lightning-generated NOx

Validation of OMI Tropospheric NO2 Observations During INTEX-B and Application to Constrain NOx Emissions Over the Eastern United States and Mexico

We compare tropospheric NO2 column measurements from the Ozone Monitoring Instrument (OMI) aboard the EOS Aura satellite with coincident in situ aircraft measurements on vertical spirals over the southern United States, Mexico, and the Gulf of Mexico during the INTEX-B campaign in March 2006. Good correlation with no significant bias (r2=0.67, slope=0.99±0.17, n=12) is found for the ensemble of comparisons when the aircraft could spiral sufficiently low to sample most of the NO2 column. Urban spirals where large extrapolations were needed below the aircraft floor (1000 ft) showed poorer agreement. We use the OMI observations together with a global chemical transport model (GEOS-Chem) to estimate emissions of nitrogen oxides over the eastern United States and Mexico in March 2006. Comparison to EPA's National Emissions Inventory 1999 (NEI99) calls for a decrease in power plant emissions and an increase in on-road vehicle emissions relative to that inventory. The rise in vehicular emissions is offsetting the reduction in power plant and industry emissions. These findings are consistent with independent assessments. Our OMI-derived emission estimates for Mexico are higher by a factor of 2.0±0.5 than bottom-up emissions, similar to a comparison between the recently released Mexican NEI99 inventory and the bottom-up showing that the Mexican NEI99 inventory is 1.6–1.8× higher.Earth and Planetary SciencesEngineering and Applied Science

NO2 Total and Tropospheric Vertical Column Densities from OMI on EOS Aura: Update

The Ozone Monitoring Instrument (OMI), which is on the EOS AURA satellite, retrieves vertical column densities (VCDs) of NO2, along with those of several other trace gases. The relatively high spatial resolution and daily global coverage of the instrument make it particularly well-suited to monitoring tropospheric pollution at scales on the order of 20 km. The OMI NO2 algorithm distinguishes polluted regions from background stratospheric NO2 using a separation algorithm that relies on the smoothly varying stratospheric NO2 and estimations of both stratospheric and tropospheric air mass factors (AMFs). Version 1 of OMI NO2 data has been released for public use. An overview of OMI NO2 data, some recent results and a description of the improvements for version 2 of the algorithm will be presented

Observation of slant column NO2 using the super-zoom mode of AURA-OMI

We retrieve slant column NO2 from the superzoom mode of the Ozone Monitoring Instrument (OMI) to explore its utility for understanding NOx emissions and variability. Slant column NO2 is operationally retrieved from OMI (Boersma et al., 2007; Bucsela et al., 2006) with a nadir footprint of 13×24 km2, the result of averaging eight detector elements on board the instrument. For 85 orbits in late 2004, OMI reported observations from individual “superzoom” detector elements (spaced at 13×3 km2 at nadir). We assess the spatial response of these individual detector elements in-flight and determine an upper-bound on spatial resolution of 9 km, in good agreement with on-ground calibration (7 km FWHM). We determine the precision of the super-zoom mode to be 2.1×10^15 molecules cm?2, approximately a factor of ?8 lower than an identical retrieval at operational scale as expected if random noise dominates the uncertainty. We retrieve slant column NO2 over the Satpura power plant in India; Seoul, South Korea; Dubai, United Arab Emirates; and a set of large point sources on the Rihand Reservoir in India using differential optical absorption spectroscopy (DOAS). Over these sources, the super-zoom mode of OMI observes variation in slant column NO2 of up to 30 × the instrumental precision within one operational footprint.Delft University of Technolog

Indirect validation of tropospheric nitrogen dioxide retrieved from the OMI satellite instrument : insight into the seasonal variation of nitrogen oxides at northern midlatitudes

We examine the seasonal variation in lower tropospheric nitrogen oxides (NOx = NO + NO2) at northern midlatitudes by evaluating tropospheric NO2 columns observed from the Ozone Monitoring Instrument (OMI) satellite instrument with surface NO2 measurements (SouthEastern Aerosol Research and Characterization and Air Quality System) and current bottom-up NOx emission inventories, using a global model of tropospheric chemistry (GEOS-Chem). The standard (SP) and DOMINO (DP) tropospheric NO2 column products from OMI exhibit broadly similar spatial and seasonal variation, but differ substantially over continental source regions. A comparison of the two OMI tropospheric NO2 products with in situ surface NO2 concentrations and bottom-up NOx emissions over the southeast United States indicates that annual mean NO2 columns from the DP are biased high by 21%–33% and those from the SP are biased high by 27%–43%. The bias in SP columns is highly seasonal, 67%–74% in summer compared with -6% to -1% in winter. Similar seasonal differences exist between top-down and bottom-up NOx emission inventories over North America, Europe, and East Asia. The air mass factor largely explains the observed seasonal difference between the DP and SP, and in turn the seasonal SP bias. We develop a third product (DP_GC) using averaging kernel information from the DP and NO2 vertical profiles from GEOS-Chem. This product reduces to 5%–21% the annual mean bias over the southeast United States. We use the seasonal variation in the DP_GC to estimate the seasonal variation in the lifetime of lower tropospheric NOx against oxidation to HNO3 over the eastern United States. The effective NOx lifetime at OMI overpass time (early afternoon) ranges from 7.6 h in summer to 17.8 h in winter, consistent within 3 h of the simulated lifetime. GEOS-Chem calculations reveal that the seasonal variation in OMI NO2 columns largely reflects gas-phase oxidation of NO2 in summer with an increasing role for heterogenous chemistry in winter

Indirect validation of tropospheric nitrogen dioxide retrieved from the OMI satellite instrument : insight into the seasonal variation of nitrogen oxides at northern midlatitudes

We examine the seasonal variation in lower tropospheric nitrogen oxides (NOx = NO + NO2) at northern midlatitudes by evaluating tropospheric NO2 columns observed from the Ozone Monitoring Instrument (OMI) satellite instrument with surface NO2 measurements (SouthEastern Aerosol Research and Characterization and Air Quality System) and current bottom-up NOx emission inventories, using a global model of tropospheric chemistry (GEOS-Chem). The standard (SP) and DOMINO (DP) tropospheric NO2 column products from OMI exhibit broadly similar spatial and seasonal variation, but differ substantially over continental source regions. A comparison of the two OMI tropospheric NO2 products with in situ surface NO2 concentrations and bottom-up NOx emissions over the southeast United States indicates that annual mean NO2 columns from the DP are biased high by 21%–33% and those from the SP are biased high by 27%–43%. The bias in SP columns is highly seasonal, 67%–74% in summer compared with -6% to -1% in winter. Similar seasonal differences exist between top-down and bottom-up NOx emission inventories over North America, Europe, and East Asia. The air mass factor largely explains the observed seasonal difference between the DP and SP, and in turn the seasonal SP bias. We develop a third product (DP_GC) using averaging kernel information from the DP and NO2 vertical profiles from GEOS-Chem. This product reduces to 5%–21% the annual mean bias over the southeast United States. We use the seasonal variation in the DP_GC to estimate the seasonal variation in the lifetime of lower tropospheric NOx against oxidation to HNO3 over the eastern United States. The effective NOx lifetime at OMI overpass time (early afternoon) ranges from 7.6 h in summer to 17.8 h in winter, consistent within 3 h of the simulated lifetime. GEOS-Chem calculations reveal that the seasonal variation in OMI NO2 columns largely reflects gas-phase oxidation of NO2 in summer with an increasing role for heterogenous chemistry in winter

Near-real time retrieval of tropospheric NO₂ from OMI

We present a new algorithm for the near-real time retrieval – within 3 h of the actual satellite measurement – of tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI). The retrieval is based on the combined retrieval-assimilation-modelling approach developed at KNMI for off-line tropospheric NO2 from the GOME and SCIAMACHY satellite instruments. We have adapted the off-line system such that the required a priori information – profile shapes and stratospheric background NO2 – is now immediately available upon arrival (within 80 min of observation) of the OMI NO2 slant columns and cloud data at KNMI. Slant columns for NO2 are retrieved using differential optical absorption spectroscopy (DOAS) in the 405–465 nm range. Cloud fraction and cloud pressure are provided by a new cloud retrieval algorithm that uses the absorption of the O2-O2 collision complex near 477 nm. On-line availability of stratospheric slant columns and NO2 profiles is achieved by running the TM4 chemistry transport model (CTM) forward in time based on forecast ECMWF meteo and assimilated NO2 information from all previously observed orbits. OMI NO2 slant columns, after correction for spurious across-track variability, show a random error for individual pixels of approximately 0.7×10¹5 molec cm¿². Cloud parameters from OMI's O2-O2 algorithm have similar frequency distributions as retrieved from SCIAMACHY's Fast Retrieval Scheme for Cloud Observables (FRESCO) for August 2006. On average, OMI cloud fractions are higher by 0.011, and OMI cloud pressures exceed FRESCO cloud pressures by 60 hPa. A sequence of OMI observations over Europe in October 2005 shows OMI's capability to track changeable NOx air pollution from day to day in cloud-free situations

A new stratospheric and tropospheric NO2 retrieval algorithm for nadir-viewing satellite instruments : applications to OMI

We describe a new algorithm for the retrieval of nitrogen dioxide (NO2) vertical columns from nadir-viewing satellite instruments. This algorithm (SP2) is the basis for the Version 2.1 OMI This algorithm (SP2) is the basis for the Version 2.1 Ozone Monitoring Instrument (OMI) NO2 Standard Product and features a novel method for separating the stratospheric and tropospheric columns. NO2 Standard Product and features a novel method for separating the stratospheric and tropospheric columns. The approach estimates the stratospheric NO2 directly from satellite data without using stratospheric chemical transport models or assuming any global zonal wave pattern. Tropospheric NO2 columns are retrieved using air mass factors derived from high-resolution radiative transfer calculations and a monthly climatology of NO2 profile shapes. We also present details of how uncertainties in the retrieved columns are estimated. The sensitivity of the retrieval to assumptions made in the stratosphere-troposphere separation is discussed and shown to be small, in an absolute sense, for most regions. We compare daily and monthly mean global OMI NO2 retrievals using the SP2 algorithm with those of the original Version 1 Standard Product (SP1) and the Dutch DOMINO product. The SP2 retrievals yield significantly smaller summertime tropospheric columns than SP1, particularly in polluted regions, and are more consistent with validation studies. SP2 retrievals are also relatively free of modeling artifacts and negative tropospheric NO2 values. In a reanalysis of an INTEX-B validation study, we show that SP2 largely eliminates an similar to 20% discrepancy that existed between OMI and independent in situ springtime NO2 SP1 measurements

Ground-based validation of EOS-Aura OMI NO2 vertical column data in the midlatitude mountain ranges of Tien Shan (Kyrgyzstan) and Alps (France)

Ground-based UV-visible instruments for NO2 vertical column measurements have been operating at Issyk-Kul station, in Kyrgyzstan, and Observatoire de Haute-Provence (OHP), in France, since 1983 and 1992, respectively. These measurements have already been used for validation of ERS-2 Global Ozone Monitoring Experiment (GOME) and Envisat Scanning Imaging Absorption Spectrometer for Atmospheric Cartography (SCIAMACHY) NO2 column data. Building upon the successful missions of GOME and SCIAMACHY, the Ozone Monitoring Experiment (OMI) was launched by NASA onboard the EOS Aura satellite in July 2004. Here we present the results of recent comparisons between OMI NO2 operational data (standard product) and correlative ground-based twilight measurements in midlatitudes, at Issyk-Kul and OHP, in 2004–2006. The stratospheric NO2 columns, observed by OMI and our ground-based instruments, have been corrected for NO2 diurnal change and normalized to local noon values using a photochemical box model. According to our comparison, OMI stratospheric NO2 columns underestimate ground-based measurements by (0.3 ± 0.3) × 1015 molecules/cm2 and (0.7 ± 0.6) × 1015 molecules/cm2 at Issyk-Kul and OHP, respectively. The effect of tropospheric pollution on the NO2 measurements in both regions of observations has been identified and discussed