Validation of ACE-FTS N 2 O measurements

The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar occultation technique. One of these instruments, the ACE Fourier Transform Spectrometer (ACE-FTS), is measuring volume mixing ratio (VMR) profiles of nitrous oxide (N 2 O) from the upper troposphere to the lower mesosphere at a vertical resolution of about 3–4 km. In this study, the quality of the ACE-FTS version 2.2 N 2 O data is assessed through comparisons with coincident measurements made by other satellite, balloon-borne, aircraft, and ground-based instruments. These consist of vertical profile comparisons with the SMR, MLS, and MIPAS satellite instruments, multiple aircraft flights of ASUR, and single balloon flights of SPIRALE and FIRS-2, and partial column comparisons with a network of ground-based Fourier Transform InfraRed spectrometers (FTIRs). Overall, the quality of the ACE-FTS version 2.2 N 2 O VMR profiles is good over the entire altitude range from 5 to 60 km. Between 6 and 30 km, the mean absolute differences for the satellite comparisons lie between -42 ppbv and +17 ppbv, with most within ±20 ppbv. This corresponds to relative deviations from the mean that are within ±15%, except for comparisons with MIPAS near 30 km, for which they are as large as 22.5%. Between 18 and 30 km, the mean absolute differences are generally within ±10 ppbv, again excluding the aircraft and balloon comparisons. From 30 to 60 km, the mean absolute differences are within ±4 ppbv, and are mostly between -2 and +1 ppbv. Given the small N 2 O VMR in this region, the relative deviations from the mean are therefore large at these altitudes, with most suggesting a negative bias in the ACE-FTS data between 30 and 50 km. In the comparisons with the FTIRs, the mean relative differences between the ACE-FTS and FTIR partial columns are within ±6.6% for eleven of the twelve contributing stations. This mean relative difference is negative at ten stations, suggesting a small negative bias in the ACE-FTS partial columns over the altitude regions compared. Excellent correlation ( R =0.964) is observed between the ACE-FTS and FTIR partial columns, with a slope of 1.01 and an intercept of -0.20 on the line fitted to the data.

[1]  T. Blumenstock,et al.  Comparison of ILAS-II and ground-based FTIR measurements of O3 , HNO3 , N2O, and CH4 over Kiruna, Sweden , 2006 .

[2]  P. Duchatelet,et al.  Comparisons between ground-based FTIR and MIPAS N 2 O and HNO 3 profiles before and after assimilation in BASCOE , 2006 .

[3]  Yuk L. Yung,et al.  The Atmospheric Trace Molecule Spectroscopy (ATMOS) Experiment: Deployment on the ATLAS Space Shuttle Missions , 1996 .

[4]  P. E. Morris,et al.  Optimized forward model and retrieval scheme for MIPAS near-real-time data processing. , 2000, Applied optics.

[5]  C. Rodgers,et al.  Retrieval of atmospheric temperature and composition from remote measurements of thermal radiation , 1976 .

[6]  R. A. Plumb A “tropical pipe” model of stratospheric transport , 1996 .

[7]  P. Duchatelet,et al.  Evolution of a dozen non-CO2 greenhouse gases above central Europe since the mid-1980s , 2005 .

[8]  J. H. Park,et al.  Measurements of methane and nitrous oxide distributions by the improved stratospheric and mesospheric sounder: Retrieval and validation , 1996 .

[9]  H. Levy,et al.  Three‐dimensional simulations of stratospheric N2O: Predictions for other trace constituents , 1986 .

[10]  E. Dlugokencky,et al.  Inverse modeling estimates of the global nitrous oxide surface flux from 1998–2001 , 2006 .

[11]  Arndt Meier,et al.  Measurements of trace gas emissions from Australian forest fires and correlations with coincident measurements of aerosol optical depth , 2005 .

[12]  Laurence S. Rothman,et al.  The HITRAN molecular spectroscopic database: edition of 2000 including updates through 2001 , 2003 .

[13]  D. Murtagh,et al.  An overview of the Odin atmospheric mission , 2002 .

[14]  S. Reimann,et al.  Our changing atmosphere: evidence based on long-term infrared solar observations at the Jungfraujoch since 1950. , 2008, The Science of the total environment.

[15]  L. E. Amraoui,et al.  The northern hemisphere stratospheric vortex during the 2002–03 winter: Subsidence, chlorine activation and ozone loss observed by the Odin Sub‐Millimetre Radiometer , 2004 .

[16]  J. Notholt,et al.  An uncertainty budget for ground‐based Fourier transform infrared column measurements of HCl, HF, N2O, and HNO3 deduced from results of side‐by‐side instrument intercomparisons , 1997 .

[17]  P. Crutzen,et al.  Chlorine activation and ozone depletion in the Arctic vortex: Observations by the Halogen Occultation Experiment on the Upper Atmosphere Research Satellite , 1996 .

[18]  M. Prather,et al.  Photochemical evolution of ozone in the lower tropical stratosphere , 1996 .

[19]  T. Clarmann,et al.  MIPAS: an instrument for atmospheric and climate research , 2007 .

[20]  J. Kuttippurath Study of stratospheric composition using airborne submillimeter radiometry and a chemical transport model , 2005 .

[21]  Clive D Rodgers,et al.  Inverse Methods for Atmospheric Sounding: Theory and Practice , 2000 .

[22]  D. Fahey,et al.  Reactive nitrogen and its correlation with ozone in the lower stratosphere and upper troposphere , 1993 .

[23]  M. Toohey,et al.  Estimating biases and error variances through the comparison of coincident satellite measurements , 2007 .

[24]  Justus Notholt,et al.  Seasonal variations of atmospheric trace gases in the high Arctic at 79°N , 1997 .

[25]  C. Piccolo,et al.  Odin/SMR Limb Observations of Trace Gases in the Polar Lower Stratosphere during 2004-2005 , 2006 .

[26]  K. Chance,et al.  Smithsonian stratospheric far‐infrared spectrometer and data reduction system , 1995 .

[27]  G. Manney,et al.  Correlations of stratospheric abundances of NO y , O3, N2O, and CH4 derived from ATMOS measurements , 1998 .

[28]  Aidan E. Roche,et al.  Bulk properties of isentropic mixing into the tropics in the lower stratosphere , 1996 .

[29]  Tatsuya Yokota,et al.  Characteristics and performance of the Improved Limb Atmospheric Spectrometer (ILAS) in orbit , 2002 .

[30]  Michael Buchwitz,et al.  First direct observation of the atmospheric CO 2 year-to-year increase from space , 2007 .

[31]  J. Gille,et al.  Stratospheric transport from the tropics to middle latitudes by planetary-wave mixing , 1993, Nature.

[32]  K. Shine,et al.  Intergovernmental panel on climate change , 1996, Environmental science and pollution research international.

[33]  M. Prather,et al.  Tracer-tracer correlations: Three-dimensional model simulations and comparisons to observations , 1997 .

[34]  D. Wardle,et al.  The ACE-MAESTRO instrument on SCISAT: description, performance, and preliminary results. , 2007, Applied optics.

[35]  R. Müller,et al.  Monthly averages of nitrous oxide and ozone for the Northern and Southern Hemisphere high latitudes: A “1‐year climatology” derived from ILAS/ILAS‐II observations , 2006 .

[36]  M. Buchwitz,et al.  Comparisons between SCIAMACHY and ground-based FTIR data for total columns of CO, CH 4 , CO 2 and N 2 O , 2005 .

[37]  F. Hase Inversion von Spurengasprofilen aus hochaufgelösten bodengebundenen FTIR-Messungen in Absorption , 2000 .

[38]  M. Chipperfield,et al.  Subtropical trace gas profiles determined by ground-based FTIR spectroscopy at Izaña (28° N, 16° W): Five-year record, error analysis, and comparison with 3-D CTMs , 2004 .

[39]  B. Connor,et al.  Northern and southern hemisphere ground-based infrared spectroscopic measurements of tropospheric , 1998 .

[40]  R. Müller,et al.  Monthly averaged ozone and nitrous oxide from the Improved Limb Atmospheric Spectrometer (ILAS) in the Northern and Southern Hemisphere polar regions , 2004 .

[41]  Forschungszentrum Karlsruhe,et al.  Inversion von Spurengasprofilen aus hochaufgelösten bodengebundenen FTIR-Messungen in Absorption * , 2000 .

[42]  E. J. Williamson,et al.  The stratospheric and mesospheric sounder on Nimbus 7 , 1980, Philosophical Transactions of the Royal Society of London. Series A, Mathematical and Physical Sciences.

[43]  L. W. Sterritt,et al.  The cryogenic limb array etalon spectrometer (CLAES) on UARS: Experiment description and performance , 1993 .

[44]  John C. Gille,et al.  Validation of CH4 and N2O measurements by the cryogenic limb array etalon spectrometer instrument on the Upper Atmosphere Research Satellite , 1996 .

[45]  D. Griffith,et al.  Intercomparison of NDSC Ground-Based Solar FTIR Measurements of Atmospheric Gases at Lauder, New Zealand , 2003 .

[46]  B. Heese,et al.  Quantification of the transport of chemical constituents from the polar vortex to midlatitudes in the lower stratosphere using the high-resolution advection model MIMOSA and effective diffusivity , 2002 .

[47]  P. Newman,et al.  An objective determination of the polar vortex using Ertel's potential vorticity , 1996 .

[48]  B. T. Marshall,et al.  Validation of ozone measurements from the Atmospheric Chemistry Experiment (ACE) , 2008 .

[49]  D. Fahey,et al.  Quantifying Transport Between the Tropical and Mid-Latitude Lower Stratosphere , 1996, Science.

[50]  M. Newchurch,et al.  On the Assessment and Uncertainty of Atmospheric Trace Gas Burden Measurements with High Resolution Infrared Solar Occultation Spectra from Space , 1996 .

[51]  Michael Olberg,et al.  Odin/SMR limb observations of stratospheric trace gases: Level 2 processing of ClO, N2O, HNO3, and O3 , 2005 .

[52]  Peter H. Siegel,et al.  The Earth observing system microwave limb sounder (EOS MLS) on the aura Satellite , 2006, IEEE Transactions on Geoscience and Remote Sensing.

[53]  B. Connor,et al.  Validation of version 5.20 ILAS HNO3, CH4, N2O, O3, and NO2 using ground-based measurements at Arrival Heights and Kiruna , 2002 .

[54]  Gang Li,et al.  The HITRAN 2008 molecular spectroscopic database , 2005 .

[55]  P. Bernath,et al.  N2O and O3 arctic column amounts from PARIS-IR observations: Retrievals, characterization and error analysis , 2007 .

[56]  M. H. Proffitt,et al.  High-latitude ozone loss outside the Antarctic ozone hole , 1989, Nature.

[57]  P. Bernath,et al.  Retrievals for the atmospheric chemistry experiment Fourier-transform spectrometer. , 2005, Applied optics.

[58]  William G. Read,et al.  Retrieval algorithms for the EOS Microwave limb sounder (MLS) , 2006, IEEE Transactions on Geoscience and Remote Sensing.

[59]  B. Dawson,et al.  INTERGOVERNMENTAL PANEL ON CLIMATE CHANGE (IPCC) , 2008 .

[60]  Guy Brasseur,et al.  Aeronomy of the Middle Atmosphere: Chemistry and Physics of the Stratosphere and Mesosphere , 1984 .

[61]  Martin Riese,et al.  CRyogenic Infrared Spectrometers and Telescopes for the Atmosphere - CRISTA , 1999, Optical Remote Sensing of the Atmosphere.

[62]  Bernd Funke,et al.  Mixing Processes during the Antarctic Vortex Split in September–October 2002 as Inferred from Source Gas and Ozone Distributions from ENVISAT–MIPAS , 2005 .

[63]  William Bell,et al.  Network for the detection of stratospheric change fourier transform infrared intercomparison at Table Mountain Facility, November 1996. , 1999 .

[64]  J. Pyle,et al.  The water vapour budget of the stratosphere studied using LIMS and SAMS satellite data , 1986 .

[65]  V. Catoire,et al.  SPIRALE: a multispecies in situ balloonborne instrument with six tunable diode laser spectrometers. , 2005, Applied optics.

[66]  John J. Barnett,et al.  Remote Sensing of Atmospheric Structure and Composition by Pressure Modulator Radiometry from Space: The ISAMS Experiment on UARS , 1993, Optical Remote Sensing of the Atmosphere.

[67]  G. Toon,et al.  Validation of the Improved Limb Atmospheric Spectrometer-II (ILAS-II) Version 1.4 nitrous oxide and methane profiles , 2006 .

[68]  C. Rinsland,et al.  Intercomparison of retrieval codes used for the analysis of high-resolution, ground-based FTIR measurements , 2004 .

[69]  R. P. Lowe,et al.  Atmospheric Chemistry Experiment (ACE): Mission overview. , 2005 .

[70]  D. R. Bates,et al.  Atmospheric nitrous oxide , 1967 .

[71]  E. Mahieu,et al.  Atmospheric Trace Molecule Spectroscopy (ATMOS) Experiment Version 3 data retrievals. , 2002, Applied optics.

[72]  S. Wofsy,et al.  Tracer‐tracer relationships and lower stratospheric dynamics: CO2 and N2O correlations during SPADE , 1994 .

[73]  Maximilian Reuter,et al.  Corrigendum to "First direct observation of the atmospheric CO 2 year-to-year increase from space" published in Atmos. Chem. Phys., 7, 4249-4256, 2007 , 2007 .

[74]  B. Lawrence,et al.  Measurements of N2O by the UARS improved Stratospheric and Mesospheric Sounder during the Early Northern Winter 1991/92 , 1994 .

[75]  E. Mahieu,et al.  Observed Trends in Total Vertical Column Abundances of Atmospheric Gases from IR Solar Spectra Recorded at the Jungfraujoch , 1997 .

[76]  T. Shepherd,et al.  Correlations of long-lived chemical species in a middle atmosphere general circulation model , 2003 .

[77]  J. Gille,et al.  Simulation of stratospheric N2O in the NCAR CCM2: Comparison with CLAES data and global budget analyses , 1994 .

[78]  C. Piccolo,et al.  Precision validation of MIPAS-Envisat products , 2007 .

[79]  K. Schäfer,et al.  Infrared spectroscopy of tropospheric trace gases: combined analysis of horizontal and vertical column abundances. , 1997, Applied optics.

[80]  Jean-Francois Lamarque,et al.  NITROGEN DEPOSITION ONTO THE UNITED STATES AND WESTERN EUROPE: SYNTHESIS OF OBSERVATIONS AND MODELS , 2005 .

[81]  K. Jucks,et al.  Validation and data characteristics of nitrous oxide and methane profiles observed by the Improved Limb Atmospheric Spectrometer (ILAS) and processed with the Version 5.20 algorithm , 2003 .

[82]  S. Solomon,et al.  Comparison of 2‐D model simulations of ozone and nitrous oxide at high latitudes with stratospheric measurements , 1992 .

[83]  Veerabhadran Ramanathan,et al.  Trace gas trends and their potential role in climate change , 1985 .

[84]  J. Holton A dynamically based transport parameterization for one-dimensional photochemical models , 1986 .

[85]  C. Piccolo,et al.  Odin/SMR limb observations of stratospheric trace gases: Validation of N2O , 2005 .

[86]  Stauffer,et al.  Variations in atmospheric N2O concentration during abrupt climatic changes , 1999, Science.

[87]  P. Bernath,et al.  Technical Note: New ground-based FTIR measurements at Ile de la Réunion: Observations, error analysis, and comparisons with independent data , 2008 .

[88]  Lance E. Christensen,et al.  Early validation analyses of atmospheric profiles from EOS MLS on the aura Satellite , 2006, IEEE Transactions on Geoscience and Remote Sensing.

[89]  K. Jucks,et al.  Stratospheric and mesospheric HOx: Results from Aura MLS and FIRS‐2 , 2006 .

[90]  Guy P. Brasseur,et al.  Aeronomy of the Middle Atmosphere , 2009 .

[91]  C. McLinden,et al.  Global modeling of the isotopic analogues of N2O: Stratospheric distributions, budgets, and the 17O–18O mass‐independent anomaly , 2003 .

[92]  B. Connor,et al.  Infrared measurements of the ozone vertical distribution above Kitt Peak , 1995 .

[93]  Kimberly Strong,et al.  Ground-Based Solar Absorption FTIR Spectroscopy: Characterization of Retrievals and First Results from a Novel Optical Design Instrument at a New NDACC Complementary Station , 2007 .

[94]  Peter F. Bernath,et al.  Atmospheric chemistry experiment (ACE): Analytical chemistry from orbit , 2006 .

[95]  M. McElroy,et al.  Nitrous Oxide: A Natural Source of Stratospheric NO , 1971 .

[96]  C. Rinsland,et al.  Spectroscopic study of the seasonal variation of carbon monoxide vertical distribution above Kitt Peak , 1995 .

[97]  John P. Burrows,et al.  Ozone depletion observed by the Airborne Submillimeter Radiometer (ASUR) during the Arctic winter 1999/2000 , 2002 .

[98]  B. Connor,et al.  Intercomparison of remote sounding instruments , 1999 .

[99]  J. Staehelin,et al.  Measurements of NO, NO y , N 2 O, and O 3 during SPURT: implications for transport and chemistry in the lowermost stratosphere , 2005 .

[100]  K. Chance,et al.  Validation of ILAS v5.2 data with FIRS‐2 balloon observations , 2002 .

[101]  W. V. Snyder,et al.  Validation of the Aura Microwave Limb Sounder middle atmosphere water vapor and nitrous oxide measurements , 2007 .

[102]  Curtis P. Rinsland,et al.  Secular trend and seasonal variability of the column abundance of N2O above the Jungfraujoch station determined from IR solar spectra , 1994 .

[103]  P. Crutzen The influence of nitrogen oxides on the atmospheric ozone content , 1970 .

[104]  A. Lacis,et al.  Greenhouse effect due to atmospheric nitrous oxide , 1976 .

[105]  F. Hasea,et al.  Intercomparison of retrieval codes used for the analysis of high-resolution , ground-based FTIR measurements , 2004 .

[106]  J. Pyle,et al.  Observations of CH4 and N2O by the NIMBUS 7 SAMS: A comparison with in situ data and two‐dimensional numerical model calculations , 1984 .

[107]  P. M. Lang,et al.  Atmospheric gas concentrations over the past century measured in air from firn at the South Pole , 1996, Nature.

[108]  Peter Barthol,et al.  CRyogenic Infrared Spectrometers and Telescopes for the Atmosphere - CRISTA , 1999, Optical Remote Sensing of the Atmosphere.

[109]  K. Kelly,et al.  Ozone loss in the Arctic polar vortex inferred from high-altitude aircraft measurements , 1990, Nature.

[110]  Malcolm K. W. Ko,et al.  Interrelationships between mixing ratios of long‐lived stratospheric constituents , 1992 .

[111]  T. Blumenstock,et al.  Observation of unusual chlorine activation by ground-based infrared and microwave spectroscopy in the late Arctic winter 2000/01 , 2005 .

[112]  Manuel López-Puertas,et al.  MIPAS level 2 operational analysis , 2006 .

[113]  J. Lelieveld,et al.  N2O and O3 relationship in the lowermost stratosphere: A diagnostic for mixing processes as represented by a three-dimensional chemistry-transport model , 2000 .