K. Chance

Harvard-Smithsonian Center for Astrophysics, Cambridge, Massachusetts, United States

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Publications (361)556.75 Total impact

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    ABSTRACT: The Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) airborne instrument is a testbed for upcoming air quality satellite instruments that will measure backscattered ultraviolet, visible and near-infrared light from geostationary orbit. GeoTASO flew on the NASA Falcon aircraft in its first intensive field measurement campaign during the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) Earth Venture Mission over Houston, Texas in September 2013. Measurements of backscattered solar radiation between 420–465 nm collected on four days during the campaign are used to determine slant column amounts of NO2 at 250 m × 250 m spatial resolution with a fitting precision of 2.2 × 1015 molecules cm−2. These slant columns are converted to tropospheric NO2 vertical columns using a radiative transfer model and trace gas profiles from the Community Multiscale Air Quality (CMAQ) model. Total column NO2 from GeoTASO is well correlated with ground-based Pandora observations (r = 0.90 on the most polluted and cloud-free day of measurements), with GeoTASO NO2 slightly higher for the most polluted observations. Surface NO2 mixing ratios inferred from GeoTASO using the CMAQ model show good correlation with NO2 measured in situ at the surface during the campaign (r = 0.91 for the most polluted day). NO2 slant columns from GeoTASO also agree well with preliminary retrievals from the GEO-CAPE Airborne Simulator (GCAS) which flew on the NASA King Air B200 (r = 0.84, slope = 0.94). Enhanced NO2 is resolvable over areas of traffic NOx emissions and near individual petrochemical facilities.
    Full-text · Article · Dec 2015
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    J. Bak · J. H. Kim · X. Liu · K. Chance · J. Kim

    Full-text · Dataset · Oct 2015
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    ABSTRACT: To improve the trace gas retrieval from Airborne Compact Atmospheric Mapper (ACAM) during the DSICOVER-AQ campaigns, we characterize the signal to noise ratio (SNR) of the ACAM measurement. From the standard deviations of the fitting residuals, the SNRs of ACAM nadir measurements are estimated to vary from ~300 at 310 nm to ~1000 in the blue spectral region; the zenith data are noisier due to reduced levels of illumination and lower system throughput and also show many more pixels with abrupt anomalous values; therefore, a new method is developed to derive a solar irradiance reference at the top of the atmosphere (TOA) from average nadir measurements, at instrument spectral resolution and including instrument calibration characteristics. Using this reference can significantly reduce fitting residuals and improve the retrievals. This approach derives an absolute reference for direct fitting algorithms involving radiative transfer calculations and thus can be applied to both aircraft and ground-based measurements. The comparison of ACAM radiance with simulations using coincident ozonesonde and OMI data shows large wavelength-dependent biases in ACAM data, varying from ~−19% at 310 nm to 5% at 360 nm. Correcting ACAM radiance in direct-fitting based ozone profile algorithm significantly improves the consistency with OMI total ozone.
    Preview · Article · Sep 2015 · Journal of Spectroscopy
  • J. Bak · X. Liu · J. H. Kim · M. T. Deland · K. Chance
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    ABSTRACT: The presence of polar mesospheric clouds (PMCs) at high latitudes could affect the retrieval of ozone profiles using backscattered ultraviolet (BUV) measurements. PMC-induced errors in ozone profile retrievals from Ozone Monitoring Instrument (OMI) BUV measurements are investigated through comparisons with Microwave Limb Sounder (MLS) ozone measurements. This comparison demonstrates that the presence of PMCs leads to systematic biases at altitudes above 6 hPa in summer high latitudes; the biases increase from ~ −2 % at 2 hPa to ~ −20 % at 0.5 hPa on average, and are significantly correlated with brightness of PMCs. Sensitivity studies show that the radiance sensitivity to PMCs strongly depends on wavelengths, increasing by a factor of ~ 4 from 300 to 265 nm. It also strongly depends on the PMC scattering, thus depending on viewing geometry. The optimal estimation-based retrieval sensitivity analysis shows that PMCs located at 80–85 km have the greatest effect on ozone retrievals at ~ 0.2 hPa (~ 60 km), where the retrieval errors range from −2.5 % with PMC optical depth (POD) of 10−4 to −20 % with 10−3 at back scattering angles, and the impacts increase by a factor of ~ 5 at forward scattering angles due to stronger PMC sensitivities. To reduce the interference of PMCs on ozone retrievals, we perform simultaneous retrievals of POD and ozone with a loose constraint of 10−3 for POD, which results in retrieval errors of 1–4 × 10−4. It is demonstrated that the negative bias of OMI ozone retrievals relative to MLS could be improved by including the PMC in the forward model calculation and retrieval.
    No preview · Article · Sep 2015 · Atmospheric Chemistry and Physics
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    ABSTRACT: This paper presents our new formaldehyde (H2CO) retrievals, obtained from spectra recorded by the nadir instrument of the Ozone Mapping and Profiler Suite (OMPS) flown on-board NASA's Suomi National Polar-orbiting Partnership (SUOMI-NPP) satellite. Our algorithm is similar to the one currently in place for the production of NASA's Ozone Monitoring Instrument (OMI) operational H2CO product. We are now able to produce a consistent set of long term data from two different instruments that share a similar concept. The ongoing overlap period between OMI and OMPS offers a perfect opportunity to study the consistency between both data sets. The different spatial and spectral resolution of the instruments is a source of discrepancy in the retrievals despite the similarity of the physic assumptions of the algorithm. We have concluded that the reduced spectral resolution of OMPS in comparison with OMI is not a significant obstacle in obtaining good quality retrievals. Indeed, the improved signal to noise ratio (SNR) of OMPS with respect to OMI helps to reduce the noise of the retrievals performed using OMPS spectra. However, the size of OMPS spatial pixels imposes a limitation in the capability to distinguish particular features of H2CO that are discernible with OMI. With root mean square (RMS) residuals ~ 5 × 10−4 for individual pixels we estimate the detection limit to be about 7.5 × 1015 molecules cm−2. Total vertical column densities (VCD) errors for individual pixels range between 40 % for pixels with high concentrations to 100 % or more for pixels with concentrations at or below the detection limit. We compare different OMI products with our OMPS product using one year of data, between September 2012 and September 2013. The seasonality of the retrieved slant columns is captured similarly by all products but there are discrepancies in the values of the VCDs. The mean biases among the two OMI products and our OMPS product are 21 % between OMI SAO and OMPS SAO and 38 % between OMI BIRA and OMPS SAO for eight selected regions.
    Full-text · Article · Sep 2015
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    ABSTRACT: An online version of the OMI (Ozone Monitoring Instrument) near-ultraviolet (UV) aerosol retrieval algorithm was developed to retrieve aerosol optical thickness (AOT) and single scattering albedo (SSA) based on the optimal estimation (OE) method. Instead of using the traditional look-up tables for radiative transfer calculations, it performs online radiative transfer calculations with the Vector Linearized Discrete Ordinate Radiative Transfer (VLIDORT) model to eliminate interpolation errors and improve stability. The OE-based algorithm has the merit of providing useful estimates of uncertainties simultaneously with the inversion products. 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 AOT and 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 estimated retrieval noise and smoothing error perform well in representing the envelope curve of actual biases of AOT at 388 nm between the retrieved AOT and AERONET measurements. The forward model parameter errors were analyzed separately for both AOT and SSA retrievals. The surface albedo 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 future studies.
    Full-text · Article · Jun 2015 · Atmospheric Chemistry and Physics
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    J. Bak · X. Liu · J. C. Wei · L. L. Pan · K. Chance · J. H. Kim
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    ABSTRACT: Motivated by the need of obtaining a more accurate global ozone distribution in the upper troposphere and lower stratosphere (UTLS), we have investigated the use of a tropopause-based (TB) ozone climatology in ozone profile retrieval from the Ozone Monitoring Instrument (OMI). Due to the limited vertical ozone information in the UTLS region from OMI backscattered ultraviolet radiances, better climatological a priori information is important for improving ozone profile retrievals. We present the new TB climatology and evaluate the result of retrievals against previous work. The TB climatology is created using ozonesonde profiles from 1983 through 2008 extended with climatological ozone data above sonde burst altitude (∼35 km) with the corresponding temperature profiles used to identify the thermal tropopause. The TB climatology consists of the mean states and 1σ standard deviations for every month for each 10 latitude band. Compared to the previous TB climatology by Wei et al. (2010), three additional processes are applied in deriving our climatology: (1) using a variable shifting offset to define the TB coordinate, (2) separating ozonesonde profiles into tropical and extratropical regimes based on a threshold of 14 km in the thermal tropopause height, and (3) merging with an existing climatology from 5-10 km above the tropopause. The first process changes the reference of profiles to a variable position between local and mean tropopause heights within ±5 km of the tropopause and to the mean tropopause elsewhere. The second helps to preserve characteristics of either tropical or extratropical ozone structures depending on tropopause height, especially in the subtropical region. The third improves the climatology above ozonesonde burst altitudes and in the stratosphere by using climatology derived from many more satellite observations of ozone profiles. With aid from the National Centers for Environmental Prediction (NCEP) Global Forecast System (GFS) tropopause height, the new climatology and retrieval can better represent the dynamical variability of ozone in the tropopause region. The new retrieval result demonstrates significant improvement of UTLS ozone, especially in the extratropical UTLS, when evaluated using ozonesonde measurements and the meteorological data. The use of TB climatology significantly enhances the spatial consistency and the statistical relationship between ozone and potential vorticity/tropopause height in the extratropical UTLS region. Comparisons with ozonesonde measurements show substantial improvements in both mean biases and their standard deviations over the extratropical lowermost stratosphere and upper troposphere. Overall, OMI retrievals with the TB climatology show improved ability in capturing ozone gradients across the tropopause found in tropical/extratropical ozonesonde measurements.
    Full-text · Dataset · May 2015
  • S. Hayashida · X. Liu · A. Ono · K. Yang · K. Chance
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    ABSTRACT: We report observations from space using ultraviolet (UV) radiance for significant enhancement of ozone in the lower troposphere over Central and Eastern China (CEC). The recent retrieval products of the Ozone Monitoring Instrument (OMI) onboard the Earth Observing System (EOS)/Aura satellite revealed the spatial and temporal variation of ozone distributions in multiple layers in the troposphere. We compared the OMI-derived ozone over Beijing with airborne measurements by the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program. The correlation between OMI and MOZAIC ozone in the lower troposphere was reasonable, which assured the reliability of OMI ozone retrievals in the lower troposphere under enhanced ozone conditions. The ozone enhancement was clearly observed over CEC, with Shandong Province as its center, and most notable in June in any given year. Similar seasonal variations were observed throughout the nine-year OMI measurement period of 2005 to 2013. The ozone enhancement in June was associated with the enhancement of carbon monoxide (CO) and hotspots, which is consistent with previous studies of in-situ measurements such those made by the MTX2006 campaign. A considerable part of this ozone enhancement could be attributed to the emissions of ozone precursors from open crop residue burning (OCRB) after the winter wheat harvest, in addition to emissions from industrial activities and automobiles. The ozone distribution presented in this study is also consistent with some model studies that apply emissions from OCRB. The lower tropospheric ozone distribution is first shown from OMI retrieval in this study, and the results will be useful in clarifying any unknown factors that influence ozone distribution by comparison with model simulations.
    No preview · Article · Jan 2015 · Atmospheric Chemistry and Physics
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    ABSTRACT: We present and discuss the Smithsonian Astrophysical Observatory (SAO) formaldehyde (H2CO) retrieval algorithm for the Ozone Monitoring Instrument (OMI) which is the operational retrieval for NASA OMI H2CO. The version of the algorithm described here includes relevant changes with respect to the operational one, including differences in the reference spectra for H2CO, the fit of O-2-O-2 collisional complex, updates in the high-resolution solar reference spectrum, the use of a model reference sector over the remote Pacific Ocean to normalize the retrievals, an updated air mass factor (AMF) calculation scheme, and the inclusion of scattering weights and vertical H2CO profile in the level 2 products. The setup of the retrieval is discussed in detail. We compare the results of the updated retrieval with the results from the previous SAO H2CO retrieval. The improvement in the slant column fit increases the temporal stability of the retrieval and slightly reduces the noise. The change in the AMF calculation has increased the AMFs by 20 %, mainly due to the consideration of the radiative cloud fraction. Typical values for retrieved vertical columns are between 4 x 10(15) and 4 x 10(16) moleculescm(-2), with typical fitting uncertainties ranging between 45 and 100 %. In high-concentration regions the errors are usually reduced to 30 %. The detection limit is estimated at 1 x 10(16) moleculescm(-2).
    Full-text · Article · Jan 2015 · Atmospheric Measurement Techniques
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    ABSTRACT: Formaldehyde (CH2O), a key atmospheric oxidation intermediate that is detectable from satellite-based UV/visible spectrometers, is primarily formed when hydroxyl radical (OH) reacts with volatile organic compounds (VOC) and is removed by photolysis, reaction with OH or deposition. We investigate the influence of OH and VOC variability on the CH2O column using a steady state model and the WRF-Chem regional chemical transport model over the southeast United States for the summer of 2012 (June-August). The steady state model indicates that the CH2O column primarily depends on OH production rates (POH) at low concentrations of OH (<3×106moleculescm-3), on both POH and VOC reactivity (VOCR: Σiki[VOC]i) at moderate concentrations of OH (3×106-7×106moleculescm-3) and on VOCR at high concentrations of OH (>7×106moleculescm-3). When constrained with WRF-Chem values of boundary layer average POH and VOCR, the steady state model of CH2O explains most of the daily (r2=0.93) and average June-August (r2=0.97) spatial variance of the fully simulated cloud-free CH2O column. These findings imply that measurements of the CH2O column offer the potential to better understand the processes affecting oxidation, particularly in remote regions, where OH concentrations are low. The findings also suggest that the inference of VOC emissions based on measurements of CH2O, or any other intermediate oxidation species with a photolytic lifetime that is short relative to removal by reaction with OH (e.g., glyoxal), should carefully account for the influence of OH on the observed pattern, especially where OH concentrations are below 5×106moleculescm-3, as occurs in remote forests, where OH strongly varies, as occurs downwind of large nitrogen oxide (NOx: NO+NO2) emission sources, or where OH sources are potentially biased.
    No preview · Article · Jan 2015 · Journal of Geophysical Research Atmospheres
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    ABSTRACT: Nigeria has a high population density and large fossil fuel resources but very poorly managed energy infrastructure. Satellite observations of formaldehyde (HCHO) and glyoxal (CHOCHO) reveal very large sources of anthropogenic nonmethane volatile organic compounds (NMVOCs) from the Lagos megacity and oil/gas operations in the Niger Delta. This is supported by aircraft observations over Lagos and satellite observations of methane in the Niger Delta. Satellite observations of carbon monoxide (CO) and nitrogen dioxide (NO2) show large seasonal emissions from open fires in December–February (DJF). Ventilation of central Nigeria is severely restricted at that time of year, leading to very poor ozone air quality as observed from aircraft (MOZAIC) and satellite (TES). Simulations with the GEOS-Chem chemical transport model (CTM) suggest that maximum daily 8-h average (MDA8) ozone exceeds 70 ppbv over the region on a seasonal mean basis, with significant contributions from both open fires (15–20 ppbv) and fuel/industrial emissions (7–9 ppbv). The already severe ozone pollution in Nigeria could worsen in the future as a result of demographic and economic growth, although this would be offset by a decrease in open fires.
    Preview · Article · Dec 2014 · Atmospheric Environment
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    ABSTRACT: We present an algorithm for the retrieval of glyoxal from backscattered solar radiation, and apply it to spectra measured by the Ozone Monitoring Instrument (OMI). The algorithm is based on direct spectrum fitting, and adopts a two-step fitting routine to account for liquid water absorption. Previous studies have shown that glyoxal retrieval algorithms are highly sensitive to the position of the spectral fit window. This dependence was systematically tested on real and simulated OMI spectra. We find that a combination of errors resulting from uncertainties in reference cross sections and spectral features associated with the Ring effect are consistent with the fit-window dependence observed in real spectra. This implies an optimal fitting window of 435-461 nm, consistent with previous satellite glyoxal retrievals. The results from the retrieval of simulated spectra also support previous findings that have suggested that glyoxal is sensitive to NO2 cross-section temperature. The retrieval window limits of the liquid water retrieval are also tested. A retrieval window 385-470 nm reduces interference with strong spectral features associated with sand. We show that cross-track dependent offsets (stripes) present in OMI can be corrected using offsets derived from retrieved slant columns over the Sahara, and apply the correction to OMI data. Average glyoxal columns are on average lower than those of previous studies likely owing to the choice of reference sector for offset correction. OMI VCDs (vertical column densities) are lower compared to other satellites over the tropics and Asia during the monsoon season, suggesting that the new retrieval is less sensitive to water vapour abundance. Consequently we do not see significant glyoxal enhancements over tropical oceans. OMI-derived glyoxal-to-formaldehyde ratios over biogenic and anthropogenic source regions are consistent with surface observations.
    No preview · Article · Nov 2014 · Atmospheric Measurement Techniques
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    ABSTRACT: The Airborne Compact Atmospheric Mapper (ACAM), an ultraviolet/visible/near-infrared spectrometer, has been flown on board the NASA UC-12 aircraft during the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaigns to provide remote sensing observations of tropospheric and boundary-layer pollutants from its radiance measurements. To assure the tracegas retrieval from ACAM measurements we perform detailed characterization and verification of ACAM slit functions. The wavelengths and slit functions of ACAM measurements are characterized for the air-quality channel (similar to 304-500 nm) through cross-correlation with a high-resolution solar irradiance reference spectrum after necessarily accounting for atmospheric gas absorption and the ring effect in the calibration process. The derived slit functions, assuming a hybrid combination of asymmetric Gaussian and top-hat slit functions, agree very well with the laboratory-measured slit functions. Comparisons of trace-gas retrievals between using derived and measured slit functions demonstrate that the cross-correlation technique can be reliably used to characterize slit functions for trace-gas retrievals.
    No preview · Article · Nov 2014 · Atmospheric Measurement Techniques
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    ABSTRACT: We present a numerical testbed for remote sensing of aerosols, together with a demonstration for evaluating retrieval synergy from a geostationary satellite constellation. The testbed combines inverse (optimal-estimation) software with a forward model containing linearized code for computing particle scattering (for both spherical and non-spherical particles), a kernel-based (land and ocean) surface bi-directional reflectance facility, and a linearized radiative transfer model for polarized radiance. Calculation of gas absorption spectra uses the HITRAN (High-resolution TRANsmission molecular absorption) database of spectroscopic line parameters and other trace species cross-sections. The outputs of the testbed include not only the Stokes 4-vector elements and their sensitivities (Jacobians) with respect to the aerosol single scattering and physical parameters (such as size and shape parameters, refractive index, and plume height), but also DFS (Degree of Freedom for Signal) values for retrieval of these parameters. This testbed can be used as a tool to provide an objective assessment of aerosol information content that can be retrieved for any constellation of (planned or real) satellite sensors and for any combination of algorithm design factors (in terms of wavelengths, viewing angles, radiance and/or polarization to be measured or used). We summarize the components of the testbed, including the derivation and validation of analytical formulae for Jacobian calculations. Benchmark calculations from the forward model are documented. In the context of NASA's Decadal Survey Mission GEO-CAPE (GEOstationary Coastal and Air Pollution Events), we demonstrate the use of the testbed to conduct a feasibility study of using polarization measurements in and around the O-2 A band for the retrieval of aerosol height information from space, as well as an to assess potential improvement in the retrieval of aerosol fine and coarse mode aerosol optical depth (AOD) through the synergic use of two future geostationary satellites, GOES-R (Geostationary Operational Environmental Satellite R-series) and TEMPO (Tropospheric Emissions: Monitoring of Pollution). Strong synergy between GEOS-R and TEMPO are found especially in their characterization of surface bi-directional reflectance, and thereby, can potentially improve the AOD retrieval to the accuracy required by GEO-CAPE.
    Full-text · Article · Oct 2014 · Journal of Quantitative Spectroscopy and Radiative Transfer
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    Full-text · Dataset · Sep 2014
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    ABSTRACT: OMI HCHO is validated over the continental US (CONUS), and used to analyze regional sources in Northeast Asia (NA) and Southeast Asia (SA). OMI HCHO Version 2.0 data show unrealistic trends, which prompted the production of a corrected OMI HCHO data set. EOF and SVD are utilized to compare the spatial and temporal variability between OMI HCHO against GOME and SCIAMACHY, and against GEOS-Chem. CONUS HCHO chemistry is well studied; its concentrations are greatest in the southeastern US with annual cycle maximums corresponding to the summer vegetation. The corrected OMI HCHO agrees with this understanding as well as with the other sensors measurements and has no unrealistic trends. In NA the annual cycle is super-posed by extremely large concentrations in polluted mega-cities. The other sensors generally agree with NA's OMI HCHO regional distribution, but megacity signal is not seen in GEOS-Chem. Our study supports the findings proposed by others that the emission inventory used in GEOS-Chem significantly underestimates anthropogenic influence on HCHO emission over megacities. The persistent mega-city signal is also present in SA. In SA the spatial and temporal patterns of OMI HCHO show a maximum in the dry season. The patterns are in remarkably good agreement with fire counts, which illustrates that the variability of HCHO over SA is strongly influenced by biomass burning. The corrected OMI HCHO data has realistic trends, conforms to well-known sources over CONUS, and has shown a stationary large concentration over polluted Asian mega-cities, and a widespread biomass burning in SA.
    Full-text · Article · May 2014 · Science of The Total Environment
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    ABSTRACT: We use a 2005-2009 record of isoprene emissions over Africa derived from OMI satellite observations of formaldehyde (HCHO) to better understand the factors controlling isoprene emission on the scale of the continent and evaluate the impact of isoprene emissions on atmospheric composition in Africa. OMI-derived isoprene emissions show large seasonality over savannas driven by temperature and leaf area index (LAI), and much weaker seasonality over equatorial forests driven by temperature. The commonly used MEGAN (version 2.1) global isoprene emission model reproduces this seasonality but is biased high, particularly for equatorial forests, when compared to OMI and relaxed-eddy accumulation measurements. Isoprene emissions in MEGAN are computed as the product of an emission factor Eo, LAI, and activity factors dependent on environmental variables. We use the OMI-derived emissions to provide improved estimates of Eo that are in good agreement with direct leaf measurements from field campaigns (r = 0.55, bias = -19%). The largest downward corrections to MEGAN Eo values are for equatorial forests and semi-arid environments, and this is consistent with latitudinal transects of isoprene over West Africa from the AMMA aircraft campaign. Total emission of isoprene in Africa is estimated to be 77 Tg C a-1, compared to 104 Tg C a-1 in MEGAN. Simulations with the GEOS-Chem oxidant-aerosol model suggest that isoprene emissions increase mean surface ozone in West Africa by up to 8 ppbv, and particulate matter by up to 1.5 μg m-3, due to coupling with anthropogenic influences.
    No preview · Article · Feb 2014 · Atmospheric Chemistry and Physics
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    ABSTRACT: Future geostationary satellite observations of tropospheric ozone aim to improve monitoring of surface ozone air quality. However, ozone retrievals from space have limited sensitivity in the lower troposphere (boundary layer). Data assimilation in a chemical transport model can propagate the information from the satellite observations to provide useful constraints on surface ozone. This may be aided by correlated satellite observations of carbon monoxide (CO), for which boundary layer sensitivity is easier to achieve. We examine the potential of concurrent geostationary observations of ozone and CO to improve constraints on surface ozone air quality through exploitation of ozone–CO model error correlations in a joint data assimilation framework. The hypothesis is that model transport errors diagnosed for CO provide information on corresponding errors in ozone. A paired-model analysis of ozone–CO error correlations in the boundary layer over North America in summer indicates positive error correlations in continental outflow but negative regional-scale error correlations over land, the latter reflecting opposite sensitivities of ozone and CO to boundary layer depth. Aircraft observations from the ICARTT campaign are consistent with this pattern but also indicate strong positive error correlations in fine-scale pollution plumes. We develop a joint ozone–CO data assimilation system and apply it to a regional-scale Observing System Simulation Experiment (OSSE) of the planned NASA GEO-CAPE geostationary mission over North America. We find substantial benefit from joint ozone–CO data assimilation in informing US ozone air quality if the instrument sensitivity for CO in the boundary layer is greater than that for ozone. A high-quality geostationary measurement of CO could potentially relax the requirements for boundary layer sensitivity of the ozone measurement. This is contingent on accurate characterization of ozone–CO error correlations. A finer-resolution data assimilation system resolving the urban scale would need to account for the change in sign of the ozone–CO error correlations between urban pollution plumes and the regional atmosphere.
    No preview · Article · Feb 2014 · Atmospheric Environment
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    J. Bak · X. Liu · J. H. Kim · K. Chance · D. P. Haffner
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    ABSTRACT: The accuracy of total ozone computed from the Smithsonian Astrophysical Observatory (SAO) optimal estimation (OE) ozone profile algorithm (SOE) applied to the Ozone Monitoring Instrument (OMI) is assessed through comparisons with ground-based Brewer spectrometer measurements from 2005 to 2008. We also make comparisons with the three OMI operational ozone products, derived from the NASA Total Ozone Mapping Spectrometer (TOMS), KNMI Differential Optical Absorption Spectroscopy (DOAS), and KNMI OE (KOE) algorithms. Excellent agreement is observed between SAO and Brewer, with a mean difference of less than ±1% at most individual stations. The KNMI OE algorithm systematically overestimates Brewer total ozone by 2% at low/mid latitudes and 5% at high latitudes while the TOMS and DOAS algorithms underestimate it by ~1.65% on average. Standard deviations of ~1.8% are found for both SOE and TOMS, but DOAS and KOE have scatters of 2.2% and 2.6%, respectively. The stability of the SOE algorithm is found to have insignificant dependence on viewing geometry, cloud parameters, total ozone column. In comparison, the KOE differences to Brewer values are significantly correlated with solar and viewing zenith angles, with a significant deviation depending on cloud parameters and total ozone amount. The TOMS algorithm exhibits similar stability to SOE with respect to viewing geometry and total column ozone, but stronger cloud parameter dependence. The dependence of DOAS on the algorithmic variables is marginal compared to KOE, but distinct compared to the SOE and TOMS algorithms. Comparisons of All four OMI products with Brewer show no apparent long-term drift but a seasonally affected feature, especially for KOE and TOMS. The substantial differences in the KOE vs. SOE algorithm performance cannot be sufficiently explained by the use of soft calibration (in SOE) and the use of different a priori error covariance matrix, but other algorithm details cause larger fitting residuals by a factor of 2-3 for KOE.
    Full-text · Article · Jan 2014 · Atmospheric Chemistry and Physics
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    ABSTRACT: Ozone is a tropospheric pollutant and plays a key role in determining the air quality that affects human wellbeing. In this study, we compare the capability of two hypothetical grating spectrometers onboard a geostationary (GEO) satellite to sense ozone in the lowermost troposphere (surface and the 0-1 km column). We consider one week during the Northern Hemisphere summer simulated by a chemical transport model, and use the two GEO instrument configurations to measure ozone concentration (1) in the thermal infrared (GEO TIR) and (2) in the thermal infrared and the visible (GEO TIR+VIS). These configurations are compared against each other, and also against an ozone reference state and a priori ozone information. In a first approximation, we assume clear sky conditions neglecting the influence of aerosols and clouds. A number of statistical tests are used to assess the performance of the two GEO configurations. We consider land and sea pixels and whether differences between the two in the performance are significant. Results show that the GEO TIR+VIS configuration provides a better representation of the ozone field both for surface ozone and the 0-1 km ozone column during the daytime especially over land.
    Full-text · Article · Jan 2014

Publication Stats

13k Citations
556.75 Total Impact Points

Institutions

  • 1970-2015
    • Harvard-Smithsonian Center for Astrophysics
      • • Division of Atomic and Molecular Physics
      • • Division of Optical and Infrared Astronomy
      Cambridge, Massachusetts, United States
  • 2006
    • Dalhousie University
      • Department of Physics and Atmospheric Science
      Halifax, Nova Scotia, Canada
  • 2005
    • Harvard University
      • Department of Earth and Planetary Sciences
      Cambridge, Massachusetts, United States
  • 1999
    • Universität Bremen
      • Institute of Environmental Physics
      Bremen, Bremen, Germany
  • 1991
    • University of Oregon
      • Department of Physics
      Eugene, Oregon, United States
  • 1990
    • United States Naval Observatory
      Вашингтон, Maine, United States
  • 1415
    • The University of Edinburgh
      • School of GeoSciences
      Edinburgh, SCT, United Kingdom