ACE Spectroscopic Issues for the Atmospheric Chemistry Experiment (ACE) Chris Boone, Kaley Walker, and Peter Bernath HITRAN meeting June, 2008.

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Presentation transcript:

ACE Spectroscopic Issues for the Atmospheric Chemistry Experiment (ACE) Chris Boone, Kaley Walker, and Peter Bernath HITRAN meeting June, 2008

ACE Atmospheric Chemistry Experiment n Satellite mission for remote sensing of the Earth’s atmosphere, with a primary focus on Arctic ozone n Developed by the Canadian Space Agency n Launched August 2003, science operations began February 2004 n Operating well, no major problems yet. n Currently funded through April 2009.

ACE Solar Occultation

ACE Instruments n Infrared Fourier Transform Spectrometer operating between 2 and 13 microns with a resolution of 0.02 cm -1 (  25 cm MPD) n 2-channel visible/near infrared Imagers, operating at and 1.02 microns n UV / Visible spectrometer (MAESTRO) to 1.03 microns, resolution ~1-2 nm n Suntracker n Startracker

ACE ACE-FTS (ABB-Bomem) Interferometer-sideInput optics-side

ACE SNR Courtesy of Ryan Hughes

ACE CO 2 microwindows Discarded 14 CO 2 microwindows.

ACE Scale CO 2 microwindows? HITRANScaled intensities Retrievals from a single microwindow, average of 95 occultations Sticking with HITRAN.

ACE HNO 3 Internal Consistency Reduce all HNO 3 line intensities in the 1700 cm -1 region by 8.5% for version 3.0 processing. From November 2007 June 2008, verifying that we used the updated HNO 3 parameters

ACE CF 4 residuals Large residuals from HNO 3. Similar issues with ClONO 2.

HNO 3 Spectroscopy Evaluation Geoffrey Toon Jet Propulsion Laboratory California Institute of Technology In July 2006, HITRAN released a complete replacement for HNO 3, based on the work of Flaud et al., [2006] “MIPAS database: Validation of HNO 3 line parameters using MIPAS satellite measurements”, ACP, 6, , 2006 How well does this new linelist describe the HNO 3 absorption?

HNO 3 ground-state bands nu nu nu nu nu nu nu7 + nu nu6 + nu nu nu8 + nu nu6 + nu nu nu nu nu5 + nu nu7 + nu nu6 + nu nu5 + nu nu2 + nu nu2 + nu nu nu3 + nu nu nu2 + nu nu2 + nu nu nu nu1 + nu nu1 + nu nu1 + nu nu1 + nu nu1 + nu nu1 + nu nu1 + nu nu1 + nu nu nu5 + nu nu nu5 + nu nu nu nu4 + nu nu3 + nu nu4 + nu nu3 + nu nu4 + nu nu3 + nu nu4 + nu nu3 + nu nu2 + nu nu4 + nu nu3 + nu nu2 + nu nu2 + nu6 Bold indicates present in July 2006 HITRAN update

Examples of missing HNO 3 bands Fits to MkIV balloon spectra acquired at km tangent altitude inside the polar winter vortex showing various missing HNO 3 bands. nu1+nu9 nu1 2nu3

HNO 3 Summary (Geoff Toon) July 2006 HNO 3 update is an improvement on HITRAN 2004: Reduced inconsistencies between 900 and 1700 cm -1 bands Improved fits to the 900 and 1200 cm -1 regions Introduced a J-dependent widths (900 cm -1 region only) But serious deficiencies remain: nu 3 band at 1300 cm -1 (the strongest) is still problematic Strength of 1205 cm -1 band is too small (20%) No lines above 1770 cm -1 (e.g. nu 1 fundamental at 3550 cm -1 ) Missing the vast majority of overtone and combination bands, Missing most hot bands and all heavy isotopologs HNO 3 widths are all constant, except for the 900 cm -1 region HNO 3 spectroscopic deficiencies are a major obstacle to further progress in the use of solar occultation spectra to measure or detect trace gases (e.g. SO 2, HDO, H 2 CO, HOCl, OH, HO 2 )

ACE Pseudolines COCl 2 COClF Eventually want real spectroscopic parameters (or cross sections) for these molecules. For now, pseudolines allow retrievals.

ACE H 2 O spectroscopic parameters n Below about 15 km, H 2 O lines in the ACE- FTS spectra exhibit bad w-shaped residuals. n At least partially deviations from the Voigt lineshape, but there could also be a contribution from poor spectroscopic parameters (very weak lines). n Very bad consistency between lines. n Determine parameters from the ACE-FTS spectra (not the ideal solution).

ACE H 2 O (continued) n Parameters of interest are the pressure broadening (including a temperature dependence), intensity, and pressure shift. n Using many different occultations, initially attempted to determine both broadening parameter and its temperature dependence, but that didn’t work out well (took a week to converge, sometimes didn’t converge). n Fix temperature dependence (HITRAN). n Choose a single line for “calibration.”

ACE HITRAN: pbhw = NEW: pbhw = All residuals shown are from sr10909 (a tropical occultation).

ACE Does changing broadening parameters affect VMR? Change intensity by ~3%? Still debating this one.

ACE HITRAN: pbhw = , strength = 6.21e-24, pshift = NEW: pbhw = , strength = 6.71e-24 (+8%), pshift = Use the line at cm -1 to calibrate those at lower altitudes. Note: minimal occultation set. Final values will be derived from a set of 95 tropical occultations before after Simultaneously fit with the line at cm -1 using multiple rays across the field of view.

ACE Internal consistency? The line at cm -1 would have been more consistent with the other two strong lines without the change in broadening parameter. Note: different # of data points averaged for the two lines for this altitude

ACE HITRAN: pbhw = , strength = 1.4e-24 NEW: pbhw = , strength = 2.83e-24 (+102%) before after H2OH2O

ACE HITRAN: pbhw = , strength = 2.98e-24 NEW: pbhw = , strength = 4.09e-24 (+37%)

ACE Big changes in the weakest H 2 O lines Line (cm-1) HITRAN pbhw NEW pbhw HITRAN strength NEW strength strength change HITRAN pshift NEW pshift e e-24+8% e e-24+37% e e % e e-24+46% e e-24+48% e e-25+75% e e-24+42% e e-24+8% e e-24+73% e e-24+89% e e-24+21%

ACE H 2 O summary n Huge changes in intensities for the lines used to retrieve H 2 O at lowest altitudes. n Generate parameters from 95 tropical occultations (instead of just 4). n H 2 O is an interference for a lot of other molecules in the troposphere. Try to improve the spectroscopic parameters for those H 2 O lines as well.

ACE CH 4 line mixing? Red curve is the contribution in the window from NO 2. Line mixing in weak CH 4 lines could yield problems with low altitude NO 2, HCl, and CH 4, plus weak absorbers H 2 CO, CH 3 Cl, acetone,….

ACE C2H6C2H6C2H6C2H6 Residuals in CH 3 Cl window (near 2967 cm -1 ) without C 2 H 6. Red curve is the C 2 H 6 contribution in this window, calculated from Geoff Toon’s pseudolines. No C 2 H 6 data near 2967 cm -1 for HITRAN (including C 2 H 6 update). Lack of C 2 H 6 in calculated spectrum yields overestimate of CH 3 Cl

ACE CFC-12 ? Near 922 cm -1 Near 1161 cm -1

ACE Lineshape problem in CO? CO lines

ACE HCl calibration? HITRAN HCl Residuals with HCl line  cm  cm  cm -1 HCl problem or other molecules?

ACE Summary n HNO 3 problems. Internal consistency. Bad residuals degrading results for other molecules, preventing SO 2 retrievals. n HNO 3 pseudolines to allow SO 2 retrieval? n H 2 O weak lines exhibit poor internal consistency, causes accuracy problems with ACE tropospheric H 2 O retrievals. n Fix C 2 H 6, especially missing data regions. n CH 4 line mixing parameters for weak lines.