Retrieval of vertical columns of sulfur dioxide from SCIAMACHY and OMI: Air mass factor algorithm development, validation, and error analysis

[1] We develop an improved retrieval of sulfur dioxide (SO2) vertical columns from two satellite instruments (SCIAMACHY and OMI) that measure ultraviolet solar backscatter. For each SCIAMACHY and OMI observation, a local air mass factor (AMF) algorithm converts line-of-sight “slant” columns to vertical columns using altitude-dependent scattering weights computed with a radiative transfer model (LIDORT), weighted by relative vertical SO2 profile (shape factor) determined locally with a global atmospheric chemistry model (GEOS-Chem). The scattering weights account for viewing geometry, surface albedo, cloud scattering, absorption by ozone, and scattering and absorption by aerosols. Absorption of radiation by mineral dust can reduce seasonal mean instrument sensitivity by 50%. Mean SO2 shape factors simulated with GEOS-Chem and used in the AMF calculation are highly consistent with airborne in situ measurements (INTEX-A and INTEX-B); differences would affect the retrieved SO2 columns by 10%. The retrieved vertical columns are validated with coincident airborne in situ measurements (INTEX-A, INTEX-B, and a campaign over east China). The annual mean AMF errors are estimated to be 35–70% in polluted regions (e.g., East Asia and the eastern United States) and less than 10% over clear ocean regions. The overall SO2 error assessment is 45–80% for yearly averages over polluted regions. Seasonal mean SO2 columns retrieved from SCIAMACHY and OMI for 2006 are significantly spatially correlated with those from GEOS-Chem, in particular over the United States (r = 0.85 for SCIAMACHY and 0.82 for OMI). A sensitivity study confirms the sensitivity of SCIAMACHY and OMI to anthropogenic SO2 emissions.

[1]  John P. Burrows,et al.  Impact of transport of sulfur dioxide from the Asian continent on the air quality over Korea during May 2005 , 2008 .

[2]  D. Jacob,et al.  Impact of new laboratory studies of N2O5 hydrolysis on global model budgets of tropospheric nitrogen oxides, ozone, and OH , 2005, Geophysical Research Letters.

[3]  John P. Burrows,et al.  RING EFFECT: IMPACT OF ROTATIONAL RAMAN SCATTERING ON RADIATIVE TRANSFER IN EARTH’S ATMOSPHERE , 1998 .

[4]  S. Self,et al.  The volcanic explosivity index (VEI) an estimate of explosive magnitude for historical volcanism , 1982 .

[5]  Alan Fried,et al.  Surface and Lightning Sources of Nitrogen Oxides over the United States: Magnitudes, Chemical Evolution, and Outflow , 2007 .

[6]  T. Bertram,et al.  Measurement of HO2NO2 in the free troposphere during the Intercontinental Chemical Transport Experiment–North America 2004 , 2007 .

[7]  Robert J. D. Spurr,et al.  Air-mass factor formulation for spectroscopic measurements from satellites: application to formaldeh , 2001 .

[8]  Thomas P. Kurosu,et al.  A linearized discrete ordinate radiative transfer model for atmospheric remote-sensing retrieval , 2001 .

[9]  Daniel J. Jacob,et al.  The impact of transpacific transport of mineral dust in the United States , 2007 .

[10]  Robert J. D. Spurr,et al.  Evaluation of the OMI cloud pressures derived from rotational Raman scattering by comparisons with other satellite data and radiative transfer simulations , 2008 .

[11]  A. Krueger,et al.  Sighting of El Chich�n Sulfur Dioxide Clouds with the Nimbus 7 Total Ozone Mapping Spectrometer , 1983, Science.

[12]  Vincent R. Gray.  Climate Change 2007: The Physical Science Basis Summary for Policymakers , 2007 .

[13]  R. Hirsch,et al.  METHODS OF FITTING A STRAIGHT LINE TO DATA: EXAMPLES IN WATER RESOURCES , 1984 .

[14]  James F. Gleason,et al.  An improved retrieval of tropospheric nitrogen dioxide from GOME , 2002 .

[15]  Henk Eskes,et al.  Error analysis for tropospheric NO2 retrieval from space , 2004 .

[16]  Oleg Dubovik,et al.  Combined use of satellite and surface observations to infer the imaginary part of refractive index of Saharan dust , 2002 .

[17]  D. Jacob.  Heterogeneous chemistry and tropospheric ozone , 2000 .

[18]  D. Jacob,et al.  Transpacific Transport of Asian Anthropogenic Aerosols and its Impact on Surface Air Quality in the United States , 2006 .

[19]  Simon A. Carn,et al.  Long range transport and fate of a stratospheric volcanic cloud from Soufriere Hills volcano, Montserrat , 2007 .

[20]  E. M. Patterson,et al.  Complex Index of Refraction Between 300 and 700 nm for Saharan Aerosols , 1977 .

[21]  Christos Zerefos,et al.  On the Retrieval of Volcanic Sulfur Dioxide Emissions from GOME Backscatter Measurements , 2005 .

[22]  Jay R. Herman,et al.  Earth surface reflectivity climatology at 340–380 nm from TOMS data , 1997 .

[23]  Tom Simkin,et al.  Volcanoes of the World , 2011 .

[24]  Michael I. Mishchenko,et al.  Bidirectional Reflectance of Flat, Optically Thick Particulate Layers: An Efficient Radiative Transfer Solution and Applications to Snow and Soil Surfaces , 1999 .

[25]  Jeffrey M. Vukovich,et al.  Development of a United States–Mexico Emissions Inventory for the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study , 2005, Journal of the Air & Waste Management Association.

[26]  John P. Burrows,et al.  TROPOSPHERIC NO2 FROM GOME MEASUREMENTS , 2002 .

[27]  Xiong Liu,et al.  Remote sensed and in situ constraints on processes affecting tropical tropospheric ozone , 2006 .

[28]  M. Chin,et al.  Natural and transboundary pollution influences on sulfate‐nitrate‐ammonium aerosols in the United States: Implications for policy , 2004 .

[29]  John P. Burrows,et al.  SO 2 Retrieval from SCIAMACHY using the Weighting Function DOAS (WFDOAS) technique: comparison with Standard DOAS retrieval , 2008 .

[30]  W. D. Rooij,et al.  Expansion of Mie scattering matrices in generalized spherical functions , 1984 .

[31]  William H. Brune,et al.  Chemistry and transport of pollution over the Gulf of Mexico and the Pacific: spring 2006 INTEX-B campaign overview and first results , 2009 .

[32]  Thomas P. Kurosu,et al.  Global inventory of nitrogen oxide emissions constrained by space‐based observations of NO2 columns , 2003 .

[33]  A. Vandaele,et al.  SO2 Absorption Cross-section Measurement in the UV using a Fourier Transform Spectrometer , 1994 .

[34]  Axel Lauer,et al.  Satellite measurements of NO2 from international shipping emissions , 2004 .

[35]  B. Jobson,et al.  Emissions lifetimes and ozone formation in power plant plumes , 1998 .

[36]  P. Bhartia,et al.  Impact of tropospheric aerosol absorption on ozone retrieval from backscattered ultraviolet measurements , 1999 .

[37]  Mian Chin,et al.  Atmospheric Aerosol Properties and Climate Impacts , 2009 .

[38]  G. Carmichael,et al.  Asian emissions in 2006 for the NASA INTEX-B mission , 2009 .

[39]  E. Kassianov,et al.  Estimation of the mass absorption cross section of the organic carbon component of aerosols in the Mexico City Metropolitan Area , 2008 .

[40]  J. Burrows,et al.  Tropospheric sulfur dioxide observed by the ERS‐2 GOME instrument , 1998 .

[41]  Jeremy Firestone,et al.  Improving spatial representation of global ship emissions inventories. , 2008, Environmental science & technology.

[42]  Kai Yang,et al.  Band residual difference algorithm for retrieval of SO/sub 2/ from the aura ozone monitoring instrument (OMI) , 2006, IEEE Transactions on Geoscience and Remote Sensing.

[43]  D. Jacob,et al.  Sulfate Formation in Sea-Salt Aerosols: Constraints from Oxygen Isotopes , 2005 .

[44]  Joanna Joiner,et al.  First results from the OMI rotational Raman scattering cloud pressure algorithm , 2006, IEEE Transactions on Geoscience and Remote Sensing.

[45]  P. Levelt,et al.  Aerosols and surface UV products from Ozone Monitoring Instrument observations: An overview , 2007 .

[46]  Arlin J. Krueger,et al.  Volcanic sulfur dioxide measurements from the total ozone mapping spectrometer instruments , 1995 .

[47]  Mian Chin,et al.  Sources of carbonaceous aerosols over the United States and implications for natural visibility , 2003 .

[48]  Arlin J. Krueger,et al.  Sulfur dioxide emissions from Peruvian copper smelters detected by the Ozone Monitoring Instrument , 2007 .

[49]  Mian Chin,et al.  Anthropogenic and natural contributions to tropospheric sulfate: A global model analysis , 1996 .

[50]  R. Andres,et al.  A time‐averaged inventory of subaerial volcanic sulfur emissions , 1998 .

[51]  D. Jacob,et al.  Global modeling of tropospheric chemistry with assimilated meteorology : Model description and evaluation , 2001 .

[52]  D. Jacob,et al.  Formaldehyde Distribution over North America: Implications for Satellite Retrievals of Formaldehyde Columns and Isoprene Emission , 2006 .

[53]  Anne M. Thompson,et al.  Aircraft vertical profiles of trace gas and aerosol pollution over the mid‐Atlantic United States: Statistics and meteorological cluster analysis , 2006 .

[54]  Jassim A. Al-Saadi,et al.  REMOTE SENSING OF TROPOSPHERIC POLLUTION FROM SPACE , 2008 .

[55]  S. Madronich,et al.  Retrieval of aerosol single scattering albedo at ultraviolet wavelengths at the T1 site during MILAGRO , 2009 .

[56]  Brittany McClure,et al.  Validation of SO2 Retrievals from the Ozone Monitoring Instrument over NE China , 2008 .

[57]  Philip J. Rasch,et al.  Determining the UV imaginary index of refraction of Saharan dust particles from Total Ozone Mapping Spectrometer data using a three-dimensional model of dust transport , 2002 .

[58]  M. V. Roozendael,et al.  FRESCO+: an improved O 2 A-band cloud retrieval algorithm for tropospheric trace gas retrievals , 2008 .

[59]  Arlin J. Krueger,et al.  Retrieval of large volcanic SO2 columns from the Aura Ozone Monitoring Instrument: Comparison and limitations , 2007 .

[60]  J. Vedder,et al.  Measurement of stratospheric sulfur constituents , 1981 .

[61]  Philip B. Russell,et al.  Overview of the Summer 2004 Intercontinental Chemical Transport Experiment–North America (INTEX-A) , 2006 .

[62]  Johannes Orphal,et al.  Measurements of molecular absorption spectra with the SCIAMACHY pre-flight model: instrument characterization and reference data for atmospheric remote-sensing in the 230–2380 nm region , 2003 .

[63]  Oleg Dubovik,et al.  Aerosol ultraviolet absorption experiment (2002 to 2004), part 2: absorption optical thickness, refractive index, and single scattering albedo , 2005 .

[64]  Steffen Beirle,et al.  Satellite observations of atmospheric SO2 from volcanic eruptions during the time-period of 1996–2002 , 2004 .

[65]  James F. Gleason,et al.  Validation of OMI tropospheric NO2 column densities using direct‐Sun mode Brewer measurements at NASA Goddard Space Flight Center , 2008 .

[66]  Kelly Chance,et al.  Ultraviolet and visible spectroscopy and spaceborne remote sensing of the Earth's atmosphere , 2005 .

[67]  O. Edenhofer,et al.  Mitigation from a cross-sectoral perspective , 2007 .

[68]  John P. Burrows,et al.  BrO emission from volcanoes: A survey using GOME and SCIAMACHY measurements , 2004 .

[69]  Robert Spurr,et al.  Simultaneous derivation of intensities and weighting functions in a general pseudo-spherical discrete ordinate radiative transfer treatment , 2002 .

[70]  Steffen Beirle,et al.  Estimate of nitrogen oxide emissions from shipping by satellite remote sensing , 2004 .

[71]  N. A. Krotkov,et al.  Fire at Iraqi sulfur plant emits SO2 clouds detected by Earth Probe TOMS , 2004 .

[72]  N. Krotkov,et al.  Aircraft observations of dust and pollutants over northeast China: Insight into the meteorological mechanisms of transport , 2007 .

[73]  D. Pyle,et al.  Sulphur emissions to the stratosphere from explosive volcanic eruptions , 1996 .

[74]  David G. Streets,et al.  Analysis of aircraft and satellite measurements from the Intercontinental Chemical Transport Experiment (INTEX-B) to quantify long-range transport of East Asian sulfur to Canada , 2008 .

[75]  R. Martin,et al.  Global and regional decreases in tropospheric oxidants from photochemical effects of aerosols , 2003 .

[76]  J. Burrows,et al.  IMPROVED SCIAMACHY WFDOAS TOTAL OZONE RETRIEVAL: STEPS TOWARDS HOMOGENISING LONG-TERM TOTAL OZONE DATASETS FROM GOME, SCIAMACHY, AND GOME2 , 2007 .

[77]  John P. Burrows,et al.  SO 2 Measurements with Sciamachy , 2006 .

[78]  David G. Streets,et al.  Present and future emissions of air pollutants in China:: SO2, NOx, and CO , 2000 .

[79]  J. Hains.  A chemical climatology of lower tropospheric trace gases and aerosols over the Mid-Atlantic region , 2007 .