Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 9 19 2009 10.5194/acp-9-7419-2009 http://www.atmos-chem-phys.net/9/7419/2009/ http://www.atmos-chem-phys.net/9/7419/2009/acp-9-7419-2009.html http://www.atmos-chem-phys.net/9/7419/2009/acp-9-7419-2009.pdf 7419 7429 2009-10-05 Lightning-produced NO_x during the Northern Australian monsoon; results from the ACTIVE campaign L. Labrador lorenzo.labrador@manchester.ac.uk G. Vaughan W. Heyes D. Waddicor A. Volz-Thomas H.-W. Pätz H. Höller School of Earth Atmospheric and Environmental Sciences, University of Manchester, UK Iinstitut für Chemie und Dynamik der Geosphäre 2, Forschungszentrum Jülich GmbH, Germany Deutsches Zentrum für Luft- und Raumfahrt, Institut für Physik der Atmosphäre, Oberpfaffenhofen, Germany Measurements of nitrogen oxides onboard a high altitude aircraft were carried out for the first time during the Northern Australian monsoon in the framework of the Aerosol and Chemical Transport in Tropical Convection (ACTIVE) campaign, in the area around Darwin, Australia. During one flight on 22 January 2006, average NO_x volume mixing ratios (vmr) of 984 and 723 parts per trillion (ppt) were recorded for both in and out of cloud conditions, respectively. The in-cloud measurements were made in the convective outflow region of a storm 56 km south-west of Darwin, whereas those out of cloud were made due south of Darwin and upwind from the storm sampled. This storm produced a total of only 8 lightning strokes, as detected by an in-situ lightning detection network, ruling out significant lightning-NO_x production. 5-day backward trajectories suggest that the sampled airmasses had travelled over convectively-active land in Northern Australia during that period. The low stroke count of the sampled storm, along with the high out-of-cloud NO_x concentration, suggest that, in the absence of other major NO_x sources during the monsoon season, a combination of processes including regional transport patterns, convective vertical transport and entrainment may lead to accumulation of lightning-produced NO_x, a situation that contrasts with the pre-monsoon period in Northern Australia, where the high NO_x values occur mainly in or in the vicinity of storms. These high NO_x concentrations may help start ozone photochemistry and OH radical production in an otherwise NO_x-limited environment. Baehr, J., Schlager H., Ziereis, H., Stock, P., van Velthoven, P., Busen R., Ström, J., and Schumann, U.: Aircraft observations of NO, NO_y, CO and O₃ in the upper troposphere from 60° N to 60° S – Interhemispheric differences at midlatitudes, Geophys. Res. Lett., 30(11), 1598, doi:10.1029/2003gl1016935, 2003. Baumgardner, D., Jonsson, H., Dawson, W., Connor, D., and Newton R.: The cloud aerosol and precipitation spectrometer (CAPS); a new instrument for cloud investigations, Atmos. Res., 59–60, 251–264. 2002. Betz, H.-D., Schmidt, K., Oettinger, W. P., and Wirz, M.:. Lightning Detection with 3D-Discrimination of Intracloud and Cloud-to-Ground Discharges. J. Geophys. Res. Lett., 31, L11108, doi:10.1029/2004GL019821, 2004. Bond, D. W., Steiger, S., Zhang, R., Tie, X., and Orville, R. E.: The importance of NO_x production by lightning in the tropics, Atmos. Env. 36, 1509–1519, 2002. Crutzen, P. J.: The role of NO and NO₂ in the chemistry of the stratosphere and troposphere. Ann. Rev. Earth Planet. Sci., 7, 443–472, 1979. Chameides, W. L. and Walker, J. C. G.: A photochemical theory of ozone. J. Geophys. Res., 78, 8751–8760, 1973. Gerbing, C., Schmitgen, S., Kley, D., and Volz-Thomas, A.: An improved fast-response Vacuum-UV resonance fluorescence CO instrument., J. Geophys. Res., 104(D1) 1699–1704, 1999. Heyes W., J., Vaughan, G., Allen, G., Volz-Thomas, A., Pätz, H.-W., and Bussen, R.: Composition of the TTL over Darwin: local mixing or long-range transport? Atmos. Chem Phys. Dis,. 9, 7299-7322, 2009 Huntrieser, H., Feigl, C., Schlager, H., Schroeder F., Gerbig, C., van Velthoven, P., Flatoy, F., Thery, C., Petzold, A., Holler, H., and Schumann, U.: Airborne measurements of NO_x, trace species and small particles during the European lightning nitrogen oxides experiment. J. Geophys. Res. 107, Article Number: 4113, 2002. Huntrieser, H., Schlager, H., Roiger, A., Lichtenstern, M., Schumann, U., Kurz, C., Brunner, D., Schweirz, C., Richter, A., and Stohl, A.: Lightning-produced NO_x over Brazil during TROCCINOX: airborne measurements in tropical and subtropical and the importance of mesoscale convective systems, Atmos. Chem. Phys., 7, 2987–3013, 2007. Höller, H., Betz, H.-D., Schmidt, K., Calheiros, R., V., May, P., Houngninou, E., and Scialom, G.: Lightning detection network (LINET) in Brazil, Australia, Africa and Germany, Atmos. Chem. Phys. Discuss., 9, 6061–6146, 2009 Jaeglé, L., Jacob D. J., Wang, Y., Weinheimer, A. J., Ridley, B. A, Campos, T. L., Sachse, G. W., and Hagen, D. E.: Sources and chemistry of NO_x in the upper troposphere over the United States, Geophys. Res. Lett., 25(10), 1705–1708, 1998. Keenan, T. D. and Carbone, R. E.: Propagation and diurnal evolution of warm season cloudiness in the Australian and maritime continent region, Mon. Weather Rev., 136, 973–994, 2008. Kondo, Y., Koike, M., Kita, K., Ikeda, H., Tagekawa, N., Kawakami, S., Blake, D., Liu, S. C., Ko, M., Myazaky, Y., Irie H., Higashi Y., Liley, B., Nishi, N., Zhao, Y., and Ogawa, T.: Effects of biomass burning, lightning, and convection on O³, CO, and NO_y over the tropical Pacific and Australia in August-October 1998 and 1999, J. Geophys. Res., 108(D3), 8402, doi:10.1029/2001JD000820, 2003. Labrador, L. J., von Kuhlmann, R., and Lawrence, M. G.: Strong sensitivity of the global OH mean concentration and the tropospheric oxidizing efficiency to the source of NO_x from lightning, Geophys. Res. Lett. 31, L06102, doi:10.1029/2003GL019229, 2004. May, P. T., Mather, J. H., Vaughan, G., Jakob, C., McFarquhar, G. M., Bower, K. N., and Mace, G. G..: The Tropical Warm Pool International Experiment (TWPICE), B. Am. Meteor. Soc., 89, 632–645, 2008. Murphy, D. M., Fahey, D. W., Proffitt, M. H., Liu, S. C., Chan, K. R., Eubank, C. S., Kawa, S. R., and Kelly, K. K.: Reactive nitrogen and its correlation with ozone in the lower stratosphere and upper stratosphere, J. Geophys. Res., 98(D5), 8751–8773, 1993. Pickering,~K. E., Thompson, A. M., Tao, W.-K. and Kucsera, T. L.: Upper Tropospheric Ozone Production Following Mesoscale Convection during STEP/EMEX, J. Geophys. Res., 98(D5), 8737–8749, 1993. Pickering,~K. E., Thomson,~A. M., Wang,~Y., Tao,~W.-K., McNamara,~D. P., Kirchhoff,~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., 101, 23993–24102, doi:10.1029/96JD00346, 1996. Ridley, B., Ott, L., Pickering, K., Emmons, L., Monztka, D., Wenhiemer, A., Knapp, D., Li, L., Heymsfield, G., McGill, M., Kucera, P., Mahoney, M. J., Baumgardner, D., Schultz, M., and Brasseur, G.: Florida thunderstorms: A faucet of reactive nitrogen to the upper troposphere, J. Geophys. Res. 109, D17305, doi:10.1029/2004JD004769, 2004. Russell, P. B., Pfister, L., and Selkirk, H. B.: The tropical experiment of the Stratosphere-Troposphere Exchange project (STEP): science objectives, operations, and summary findings, J. Geophys. Res., 98(D5), 8563–8589, 1993. Schumann, U. and Huntrieser H.: The Global lightning-induced nitrogen oxides source, Atmos. Chem. Phys. 8, 3823–3907, 2007. Stockwell, D. Z., Giannakopoulos, C., Plantevin, P.-H., Carver, G. D., Chipperfield, M. P., Law, K. S., Pyle, J. A., Shallcross, D. E., and Wang, K.-Y.: Modelling NO_x from lightning and its impact on global chemical fields, Atmos. Environ., 33, 4477–4493, 1999. Tie, X., Zhang, R., Brasseur, G., Emmons, L., and Wengfan, L.: Effects of lightning on reactive nitrogen and nitrogen reservoir species in the troposphere, J. Geophys. Res., 16(D3), 3167–3718, 2002. Torres, A. L., Buchan, H., and Tuck, A. F.: Tropospheric nitric oxide measurements over the Amazon basin, J. Geophys. Res., 93, 1396–1406, 1988. Vaughan, G., Schiller, C., MacKenzie, A. R., Bower, K., Peter, T., Schläger, H., Harris, N. R. P., and May, P. T.: SCOUT-03/ACTIVE High-altitude aircraft measurements around deep tropical convection, B. Am. Meteor. Soc. 89, 647–662, 2008. Volz-Thomas, A., Berg, M., Heil, T., Houben, N., Lerner, A., Petrick, W., Raak, D., and Pätz, H.-W.: Measurements of total odd nitrogen (NO_y) aboard MOZAIC in-service aircraft: instrument design, operation and performance, Atmos. Chem. Phys., 5, 583–595, 2005. Volz-Thomas, A., Berg, M., Heil, T., Houben, N., Lerner, A., Petrick, W., Raak, D., and Pätz, H.-W: Measurements of total odd nitrogen (NO_y) aboard MOZAIC in-service aircraft: instrument design, operation and performance, Atmos. Chem. Phys., 5, 583–595, 2005.