[en] Vertical mixing ratio profiles of four relatively long-lives gases, HCN, C2H2, CO, and C2H6, have been retrieved from 0.01 cm(-1) resolution infrared solar occultation spectra recorded between latitudes of 5.3 degrees N and 31.4 degrees N. The observations were obtained by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the Atmospheric Laboratory for Applications and Science (ATLAS) 3 shuttle flight, 3-12 November 1994. Elevated mixing ratios below the tropopause were measured for these gases during several of the occultations. The positive correlations obtained between the simultaneously measured mixing ratios suggest that the enhancements are likely the result of surface emissions, most likely biomass burning and/or urban industrial activities, followed by common injection via deep convective transport of the gases to the upper troposphere. The elevated levels of HCN may account for at least part of the "missing NOy" in the upper troposphere. Comparisons of the observations with values measured during a recent aircraft campaign are presented. Published by Elsevier Science Ltd.
Disciplines :
Earth sciences & physical geography
Author, co-author :
Rinsland, C. P.
Gunson, M. R.
Wang, P.-H.
Arduini, R. F.
Baum, B. A.
Minnis, P.
Goldman, A.
Abrams, M. C.
Zander, Rodolphe ; Université de Liège - ULiège > Services généraux (Faculté des sciences) > Relations académiques et scientifiques (Sciences)
Mahieu, Emmanuel ; Université de Liège - ULiège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
1. Danielsen, E. F., In situ evidence of rapid, vertical, irreversible transport of lower tropospheric air into the lower tropical stratosphere by convective cloud turrets and by large-scale upwelling in tropical cyclones, J. Geophys. Res., 1993, 98, 8665-8681.
2. Chatfield, R. B. and Crutzen, P. J., Sulfur dioxide in remote oceanic air: Cloud transport of reactive precursors, J. Geophys. Res., 1984, 89, 7111-7132.
3. Wang, C., Crutzen, P. J., Ramanathan, V. and Williams, S. F., The role of a deep convective storm over the tropical pacific ocean in the redistribution of atmospheric chemical species, J. Geophys. Res., 1995, 100, 11509-11516.
4. Pickering, K. E., Thompson, A. M., Wang, Y., Tao, W.-K., McNamara, D. P., Kirchoff, V. W. J. H., Heikes, B. G., Sachse, G. W., Bradshaw, J. D., Gregory, G. L. and Blake, D. R., Convective transport of biomass burning emissions over Brazil during TRACE A, J. Geophys. Res., 1996, 101, 23993-24012.
5. Smyth, S. B., Sandholm, S. T., Bradshaw, J. D., Talbot, R. W., Blake, D. R., Blake, N. J., Rowland, F. S., Singh, H. B., Gregory, G. L., Anderson, B. E., Sachse, G. W., Collins, J. E. and Bachmeier, A. S., Factors influencing the upper free tropospheric distribution of reactive nitrogen over the south atlantic during the TRACE A experiment, J. Geophys. Res., 1996, 101, 24165-24186.
6. Singh, H. B., Herlth, D., Koyler, R., Chatfield, R., Viezee, W., Salas, L. J., Chen, J., Bradshaw, J. D., Sandholm, S. T., Talbot, R., Gregory, G. L., Anderson, B., Sachse, G. W., Browell, E., Bachmeier, A. S., Blake, D. R., Heikes, B., Jacob, D. and Fuelberg, H. E., Impact of biomass burning emissions on the composition of the south atlantic troposphere: Reactive nitrogen and ozone, J. Geophys. Res., 1996, 101, 24203-24219.
7. Blake, N. J., Blake, D. R., Sive, B. C., Chen, T.-Y., Rowland, F. S., Collins Jr. J. E., Sachse, G. W. and Anderson, B. E., Biomass burning emissions and vertical distribution of atmospheric methyl halides and other reduced carbon gases in the south atlantic region, J. Geophys. Res., 1996, 101, 24151-24164.
8. Talbot, R. W., Bradshaw, R. D., Sandholm, S. T., Smyth, S., Blake, D. R., Blake, N. R., Sachse, G. W., Collins, J. E., Heikes, B. G., Anderson, B. E., Gregory, G. L., Singh, H. B., Lefer, B. L. and Bachmeier, A. S., Chemical characteristics of continental outflow over the tropical south atlantic ocean from Brazil and Africa, J. Geophys. Res., 1996, 101, 24187-24202.
9. Pickering, K. E., Thompson, A. M., Scala, J. R., Tao, W.-K., and Simpson, J., Ozone production potential following convective redistribution of biomass burning emissions, J. Atmos. Chem., 1992, 14, 297-313.
10. Browell, E. V., Fenn, M. A., Butler, C. F., Grant, W. B., Clayton, M. B., Fishman, J., Bachmeier, A. S., Anderson, B. E., Gregory, G. L., Fuelberg, H. E., Bradshaw, J. D., Sandholm, S. T., Blake, D. R., Heikes, B. G., Sachse, G. W., Singh, H. B. and Talbot, R. W., Ozone and aerosol distributions and air mass characteristics over the south atlantic basin during the burning season, J. Geophys. Res., 1996, 101, 24043-24068.
11. McKeen, S. A., Liu, S. C., Hsie, E.-Y., Lin, X., Bradshaw, J. D., Smyth, S., Gregory, G. L. and Blake, D. R., Hydrocarbon ratios during PEM-WEST A: A model perspective, J. Geophys. Res., 1996, 101, 2087-2109.
12. Rinsland, C. P., Gunson, M. R., Wang, P.-H., Arduini, R. F., Baum, B. A., Minnis, P., Goldman, A., Abrams, M. C., Zander, R., Mahieu, E., Salawitch, R. J., Michelsen, H. A., Irion, F. W. and Newchurch, M. J., ATMOS/ATLAS 3 infrared profile measurements of clouds in the tropical and subtropical upper troposphere, JQSRT, 1998, this issue.
13. Farmer, C. B., High resolution infrared spectroscopy of the sun and earth's atmosphere from space, Mikrochim. Acta [Wien], 1987, III, 189-214.
14. Farmer, C. B., Raper, O. F. and O'Callaghan, F. G., Final report on the first flight of the ATMOS instrument during the Spacelab 3 mission, April 29-May 6, 1985, JPL Publ. 87-32, 45pp., Jet Propulsion Laboratory, Pasadena, California, 1 October 1987.
15. Kaye, J. A. and Miller, T. L., The ATLAS series of shuttle missions, Geophys. Res. Lett., 1996, 23, 2285-2288.
16. Gunson, M. R., Abbas, M. M., Abrams, M. C., Allen, M., Brown, L. R., Brown, T. L., Chang, A. J., Goldman, A., Irion, F. W., Lowes, L. L., Mahieu, E., Manney, G. L., Michelsen, H. A., Newchurch, M. J., Rinsland, C. P., Salawitch, R. J., Stiller, G. P., Toon, G. C., Yung, Y. L. and Zander, R., The atmospheric trace molecule spectroscopy (ATMOS) experiment: Deploymnet on the ATLAS space shuttle missions, Geophys. Res. Lett., 1996, 23, 2333-2336.
17. Norton, R. H. and Rinsland, C. P., ATMOS data processing and science analysis methods, Appl. Opt., 1991, 30, 389-400.
18. Abrams, M. C., Chang, A. Y., Gunson, M. R., Abbas, M. M., Goldman, A., Irion, F. W., Michelsen, H. A., Newchurch, M. J., Rinsland, C. P., Stiller, G. P. and Zander, R., On the assessment and uncertainty of atmospheric trace gas burden measurements with high resolution infrared solar occultation spectra from space by the ATMOS experiment, Geophys. Res. Lett., 1996, 23, 2337-2340.
19. Carlotti, M., Global-fit approach to the analysis of limb-scanning atmospheric measurements, Appl. Opt., 1988, 27, 3250-3254.
20. Rinsland, C. P., Gunson, M. R., Foster, J. C., Toth, R. A., Farmer, C. B. and Zander, R., Stratospheric profiles of heavy water vapor isotopes and CH3D from analysis of the ATMOS spacelab 3 infrared solar spectra, J. Geophys. Res., 1991, 96, 1057-1068.
21. Brown, L. R., Gunson, M. R., Toth, R. A., Irion, F. W., Rinsland, C. P., and Goldman, A., 1995 atmospheric trace molecule spectroscopy (ATMOS) linelist, Appl. Opt., 1996, 35, 2828-2848.
22. Stiller, G. P., Gunson, M. R., Lowes, L. L., Abrams, M. C., Raper, O. F., Farmer, C. B., Zander, R. and Rinsland, C. P., Stratospheric and mesospheric pressure-temperature profiles from the rotational analysis of CO2 lines in ATMOS/ATLAS-1 infrared solar occultation spectra, J. Geophys. Res., 1995, 100, 3107-3117.
23. Abrams, M. C., Gunson, M. R., Lowes, L. L., Rinsland, C. P. and Zander, R., Pressure sounding of the middle atmosphere from ATMOS solar occultation measurements of atmospheric CO2 absorption lines, Appl. Opt., 1996, 35, 2810-2820.
24. Gelman, M., National Meteorological Center, private communication, 1994.
25. Warneck, P., Chemistry of the Natural Atmosphere, Chap. 9, Academic, San Diego, 1988.
26. Hofmann, D. J. and Peterson, J. T. eds., Climate Monitoring and Diagnostics Laboratory No. 23 Summary Report 1994-1995, U. S. Department of Commerce, National Oceanic and Atmospheric Administration, Environmental Research Laboratories, Chap. 5, National Technical Information Service, 5285 Port Royal Road, Springfield, VA, 1996.
27. Rothman, L. S., Rinsland, C. P., Goldman, A., Massie, S. T., Edwards, D. P., Flaud, J.-M., Perrin, A., Dana, V., Mandin, J.-Y., Schroeder, J., McCann, A., Gamache, R. R., Wattson, R. B., Yoshino, K., Chance, K., Jucks, K., Brown, L. R., Nemtchinov, V. and Varanasi, P., The HITRAN molecular spectroscopic database and HAWKS (HITRAN atmospheric workstation): 1996 edn, JQSRT, 1998, this issue.
28. Pine, A. S. and Stone, S. C., Torsional tunneling and A1-A2 splittings and air broadening of the rQo and pQ3 subbranches of the v7 band of ethane, J. Mol. Spectrosc., 1996, 175, 21-30.
29. Pine, A. S., private communication, 1997.
30. Rinsland, C. P., Mahieu, E., Zander, R., Gunson, M. R., Salawitch, R. J., Chang, A. Y., Goldman, A., Abrams, M. C., Abbas, M. M., Newchurch, M. J. and Irion, F. W., Trends of OCS, HCN, SF6, CHClF2 (HCFC-22) in the lower stratosphere from 1985 and 1994 atmospheric trace molecule spectroscopy experiment measurements near 30°N latitude, Geophys. Res. Lett., 1996, 23, 2349-2352.
31. Zander, R., Rinsland, C. P., Farmer, C. B., Namkung, J., Norton, R. H. and Russell III, J. M., Concentrations of carbonyl sulfide and hydrogen cyanide in the free upper troposphere and lower stratosphere deduced from ATMOS/Spacelab 3 infrared solar occultation spectra, J. Geophys. Res., 1988, 93, 1669-1678.
32. Mahieu, E., Rinsland, C. P., Zander, R., Demoulin, P., Delbouille, L. and Roland, G., Vertical column abundances of HCN deduced from ground-based infrared solar spectra, J. Atmos. Chem., 1995, 20, 299-310.
33. Jacob, D. J., Heikes, B. G., Fan, S.-M., Logan, J. A., Mauzerall, D. L., Bradshaw, J. D., Singh, H. B., Gregory, G. L., Talbot, R. W., Blake, D. R. and Sachse, G. W., Origin of ozone and NOx in the tropical troposphere: A photochemical analysis of aircraft observations over the south atlantic basin, J. Geophys. Res., 1996, 101, 24235-24250.
34. Lobert, J. M., Scharffe, D. H., Hao, W. M. and Crutzen, P. J., Importance of biomass burning in the atmospheric budgets of nitrogen-containing gases, Nature, 1990, 346, 552-554.
35. Yokelson, R. J., Susott, R., Ward, D. E., Reardon, J. and Griffith, D. W. T., Emissions from smoldering combustion of biomass measured by open-path FTIR, J. Geophys. Res., 1998, 102, 18865-18878.
36. Hurst, D. F., Griffith, D. W. T., Carras, J. N., Williams, D. J. and Fraser, P. J., Measurements of trace gases emitted by australian savanna fires during the 1990 dry season, J. Atmos. Chem., 1994, 18, 33-56.
37. Hurst, D. F., Griffith, D. W. T. and Cook, G. D., Trace gas emissions from biomass burning in tropical australian savannas, J. Geophys. Res., 1994, 99, 16441-16456.
38. Yokelson, R. J., Griffith, D. W. T. and Ward, D. E., Open-path Fourier transform infrared studies of large-scale laboratory biomass fires, J. Geophys. Res., 1996, 101, 21067-21080.
