Eric John Bucsela

An improved retrieval of tropospheric nitrogen dioxide from GOME

[1] We present a retrieval of tropospheric nitrogen dioxide (NO2) columns from the Global Ozone Monitoring Experiment (GOME) satellite instrument that improves in several ways over previous retrievals, especially in the accounting of Rayleigh and cloud scattering. Slant columns, which are directly fitted without low-pass filtering or spectral smoothing, are corrected for an artificial offset likely induced by spectral structure on the diffuser plate of the GOME instrument. The stratospheric column is determined from NO2 columns over the remote Pacific Ocean to minimize contamination from tropospheric NO2. The air mass factor (AMF) used to convert slant columns to vertical columns is calculated from the integral of the relative vertical NO2 distribution from a global 3-D model of tropospheric chemistry driven by assimilated meteorological data (Global Earth Observing System (GEOS)-CHEM), weighted by altitude-dependent scattering weights computed with a radiative transfer model (Linearized Discrete Ordinate Radiative Transfer), using local surface albedos determined from GOME observations at NO2 wavelengths. The AMF calculation accounts for cloud scattering using cloud fraction, cloud top pressure, and cloud optical thickness from a cloud retrieval algorithm (GOME Cloud Retrieval Algorithm). Over continental regions with high surface emissions, clouds decrease the AMF by 20– 30% relative to clear sky. GOME is almost twice as sensitive to tropospheric NO2 columns over ocean than over land. Comparison of the retrieved tropospheric NO2 columns for July 1996 with GEOS-CHEM values tests both the retrieval and the nitrogen oxide radical

Algorithm for NO/sub 2/ vertical column retrieval from the ozone monitoring instrument

We describe the operational algorithm for the retrieval of stratospheric, tropospheric, and total column densities of nitrogen dioxide (NO/sub 2/) from earthshine radiances measured by the Ozone Monitoring Instrument (OMI), aboard the EOS-Aura satellite. The algorithm uses the DOAS method for the retrieval of slant column NO/sub 2/ densities. Air mass factors (AMFs) calculated from a stratospheric NO/sub 2/ profile are used to make initial estimates of the vertical column density. Using data collected over a 24-h period, a smooth estimate of the global stratospheric field is constructed. Where the initial vertical column densities exceed the estimated stratospheric field, we infer the presence of tropospheric NO/sub 2/, and recalculate the vertical column density (VCD) using an AMF calculated from an assumed tropospheric NO/sub 2/ profile. The parameters that control the operational algorithm were selected with the aid of a set of data assembled from stratospheric and tropospheric chemical transport models. We apply the optimized algorithm to OMI data and present global maps of NO/sub 2/ VCDs for the first time.

Space-based Constraints on Spatial and Temporal Patterns of NOx Emissions in California, 2005−2008

We describe ground and space-based measurements of spatial and temporal variation of NO(2) in four California metropolitan regions. The measurements of weekly cycles and trends over the years 2005-2008 observed both from the surface and from space are nearly identical to each other. Observed decreases in Los Angeles and the surrounding cities are 46% on weekends and 9%/year from 2005-2008. Similar decreases are observed in the San Francisco Bay area and in Sacramento. In the San Joaquin Valley cities of Fresno and Bakersfield weekend decreases are much smaller, only 27%, and the decreasing trend is only 4%/year. We describe evidence that the satellite observations provide a uniquely complete view of changes in spatial patterns over time. For example, we observe variations in the spatial pattern of weekday-weekend concentrations in the Los Angeles basin with much steeper weekend decreases at the eastern edge of the basin. We also observe that the spatial extent of high NO(2) in the San Joaquin Valley has not receded as much as it has for other regions in the state. Analysis of these measurements is used to describe observational constraints on temporal trends in emission sources in the different regions.

Testing and improving OMI DOMINO tropospheric NO2 using observations from the DANDELIONS and INTEX‐B validation campaigns

We present a sensitivity analysis of the tropospheric NO2 retrieval from the Ozone Monitoring Instrument (OMI) using measurements from the Dutch Aerosol and Nitrogen Dioxide Experiments for Validation of OMI and SCIAMACHY (DANDELIONS) and Intercontinental Chemical Transport Experiment-B (INTEX-B) campaigns held in 2006. These unique campaigns covered a wide range of pollution conditions and provided detailed information on the vertical distribution of NO2. During the DANDELIONS campaign, tropospheric NO2 profiles were measured with a lidar in a highly polluted region of the Netherlands. During the INTEX-B campaign, NO2 profiles were measured using laser-induced fluorescence onboard an aircraft in a range of meteorological and polluted conditions over the Gulf of Mexico and the east Pacific. We present a comparison of measured profiles with a priori profiles used in the OMI tropospheric NO2 retrieval algorithm. We examine how improvements in surface albedo estimates improve the OMI NO2 retrieval. From these comparisons we find that the absolute average change in tropospheric columns retrieved with measured profiles and improved surface albedos is 23% with a standard deviation of 27% and no trend in the improved being larger or smaller than the original. We show that these changes occur in case studies related to pollution in the southeastern United States and pollution outflow in the Gulf of Mexico. We also examine the effects of using improved Mexico City terrain heights on the OMI NO2 product.

Revising the slant column density retrieval of nitrogen dioxide observed by the Ozone Monitoring Instrument

Abstract Nitrogen dioxide retrievals from the Aura/Ozone Monitoring Instrument (OMI) have been used extensively over the past decade, particularly in the study of tropospheric air quality. Recent comparisons of OMI NO2 with independent data sets and models suggested that the OMI values of slant column density (SCD) and stratospheric vertical column density (VCD) in both the NASA OMNO2 and Royal Netherlands Meteorological Institute DOMINO products are too large, by around 10–40%. We describe a substantially revised spectral fitting algorithm, optimized for the OMI visible light spectrometer channel. The most important changes comprise a flexible adjustment of the instrumental wavelength shifts combined with iterative removal of the ring spectral features; the multistep removal of instrumental noise; iterative, sequential estimates of SCDs of the trace gases in the 402–465 nm range. These changes reduce OMI SCD(NO2) by 10–35%, bringing them much closer to SCDs retrieved from independent measurements and models. The revised SCDs, submitted to the stratosphere‐troposphere separation algorithm, give tropospheric VCDs ∼10–15% smaller in polluted regions, and up to ∼30% smaller in unpolluted areas. Although the revised algorithm has been optimized specifically for the OMI NO2 retrieval, our approach could be more broadly applicable.

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.

Near-ultraviolet and blue spectral observations of sprites in the 320–460 nm region: N2 (2PG) emissions

Abstract : A near-ultraviolet (NUV) spectrograph (320-460 nm) was flown on the EXL98 aircraft sprite observation campaign during July 1998. In this wavelength range video rate (60 fields/sec) spectrographic observations found the NUV/blue emissions to be predominantly N2(2PG). The negligible level of N+2 (1NG) present in the spectrum is confirmed by observations of a co-aligned, narrowly filtered 427.8 nm imager and is in agreement with previous ground-based filtered photometer observations. The synthetic spectral fit to the observations indicates a characteristic energy of 1.8 eV, in agreement with our other NUV observations.

Atmospheric correction for NO 2 absorption in retrieving water-leaving reflectances from the SeaWiFS and MODIS measurements

The absorption by atmospheric nitrogen dioxide (NO2) gas in the visible has been traditionally neglected in the retrieval of oceanic parameters from satellite measurements. Recent measurements of NO2 from spaceborne sensors show that over the Eastern United States the NO2 column amount often exceeds 1 Dobson Unit (approximately 2.69x10(16) molecules/cm2). Our radiative transfer sensitivity calculations show that under high NO2 conditions (approximately 1x10(16) molecules/cm2) the error in top-of-atmosphere (TOA) reflectance in the blue channels of the sea-viewing wide field-of-view sensor (SeaWiFS) and moderate-resolution imaging spectroradiometer (MODIS) sensors is approximately 1%. This translates into approximately 10% error in water-leaving radiance for clear waters and to higher values (>20%) in the coastal areas. We have developed an atmospheric-correction algorithm that allows an accurate retrieval of normalized water-leaving radiances (nLws) in the presence of NO2 in the atmosphere. The application of the algorithm to 52 MODIS scenes over the Chesapeake Bay area show a decrease in the frequency of negative nLw estimates in the 412 nm band and an increase in the value of nLws in the same band. For the particular scene reported in this paper, the mean value of nLws in the 412 nm band increased by 17%, which is significant, because for the MODIS sensor the error in nLws attributable to the digitization error in the observed TOA reflectance over case 2 waters is approximately 2.5%.

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.

N I 8680‐ and 8629‐Å multiplets in the dayglow

The N I 8680- and 8629-A multiplets have been observed in the midlatitude dayglow during moderate-to-high solar activity. A rocket-borne near-infrared spectrometer of 13.4-A resolution recorded spectra between 120 and 219 km. Analysis yielded altitude profiles of emissions including the N2 first positive (1 PG) (2,1) band, the O2 atmospheric (0,1) and (1,2) bands, and the N I 8680- and 8629-A multiplets. Photoelectron impact models adequately described the measured 1 PG profile but significantly underestimated the N I multiplet emission rates. It is suggested that the primary source of the multiplets is photodissociation of N2. The contribution of this process was estimated from a model based on the shape of the N I 1200-A lines photoexcitation cross section. If the proposed excitation mechanism is correct, peak cross-section values for the 8680- and 8629-A multiplets would have to be 7.2 ± 5.2 × 10−20 and 5.7 ± 3.2 × 10−20 cm2, respectively.