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Atmospheric Isotopologues Observed by ACE-FTS and Modeled with WACCM

This talk discusses the observation and modeling of atmospheric isotopologues using ACE-FTS and WACCM. It explores the reactions, kinetic isotope effect, and isotopic composition of various gases. The talk also highlights the agreement between ACE-FTS and WACCM in most areas.

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Atmospheric Isotopologues Observed by ACE-FTS and Modeled with WACCM

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  1. Atmospheric Isotopologues Observed by ACE-FTS and Modeled with WACCM Mahdi Yousefi Peter Bernath Eric Buzan Chris Beale Chris Boone ISMS Talk, June 19, 2017

  2. Greenhouse Gases – IPCC 2013

  3. Atmospheric Chemistry Experiment (ACE)

  4. ACE-FTS Spectra

  5. ACE N2O, 15.5 km, 2ν3mode P(27) P(25) P(24) P(26) Forward Model

  6. ACE Version 3.5 VMR Products

  7. Isotopologues react at different rates @ 25oC Lighter isotopes consumed faster Remaining gas enriched in heavy isotopes Kinetic Isotope Effect

  8. Atmospheric Circulation

  9. Isotope ratios usually reported as delta values, e.g. δ13C, δD , Delta Notation

  10. Component of Community Earth System Model (CESM) • 3D model, surface to ~150 km • Simulates chemistry and dynamics of atmosphere • Isotopologues treated as separate species • Reactions • Photolysis • Lower boundary conditions Whole Atmosphere Community Climate Model (WACCM) Marsh, D. R., Mills, M. J., Kinnison, D. E., Lamarque, J.-F., Calvo, N. and Polvani, L. M.: Climate Change from 1850 to 2005 Simulated in CESM1(WACCM), J. Clim., 26(19), 7372–7391, doi:10.1175/JCLI-D-12-00558.1, 2013.

  11. ACE N2O N15NO

  12. ACE vs WACCM N2O ACE N15NO WACCM

  13. ACE CH4 CH3D • 13CH4 Buzan, E. M., Beale, C. A., Boone, C. D., & Bernath, P. F. (2016). Global stratospheric measurements of the isotopologues of methane from the Atmospheric Chemistry Experiment Fourier transform spectrometer. Atmospheric Measurement Techniques, 9(3), 1095–1111.

  14. WACCM CH4 Time Series δ13C δD

  15. CH4 Balloon Comparison WACCM (Model) ACE-FTS (Satellite) Röckmann et al. (in situ balloon) Röckmann, T., Brass, M., Borchers, R. & Engel, A. The isotopic composition of methane in the stratosphere: high-altitude balloon sample measurements. Atmos. Chem. Phys.11, 13287–13304 (2011).

  16. ACE 13CO CH4 + oxidants → CO CO2+ hν → CO + O CO + OH → CO2 + H Beale, C. A., Buzan, E. M., Boone, C. D., & Bernath, P. F. (2015). Near-global distribution of CO isotopic fractionation in the Earth’s atmosphere. Journal of Molecular Spectroscopy, 1–8.

  17. ACE vs WACCM CO ACE WACCM Beale, C. A., Buzan, E. M., Boone, C. D., & Bernath, P. F. (2015). Near-global distribution of CO isotopic fractionation in the Earth’s atmosphere. Journal of Molecular Spectroscopy, 1–8.

  18. ACE CO2 OC18O OC17O

  19. First global measurements of isotopologues of N2O, CH4, CO, CO2 • Isotopic data is a useful tracer of upper atmospheric processes • CH4 and N2O show influence of Brewer-Dobson circulation • 13CO and CO2 shows seasonal variation in mesosphere • Good agreement between ACE-FTS and WACCM in most areas Summary

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