Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 8 5 2008 10.5194/acpd-8-17581-2008 http://www.atmos-chem-phys-discuss.net/8/17581/2008/ http://www.atmos-chem-phys-discuss.net/8/17581/2008/acpd-8-17581-2008.html http://www.atmos-chem-phys-discuss.net/8/17581/2008/acpd-8-17581-2008.pdf 17581 17629 2008-09-26 A global stratospheric bromine monoxide climatology based on the BASCOE chemical transport model N. Theys theys@aeronomie.be M. Van Roozendael Q. Errera F. Hendrick F. Daerden S. Chabrillat M. Dorf K. Pfeilsticker A. Rozanov W. Lotz J. P. Burrows J.-C. Lambert F. Goutail H. K. Roscoe M. De Mazière Belgium Institute for Space Aeronomy (IASB-BIRA), Brussels, Belgium Institute for Environmental Physics, University of Heidelberg, Heidelberg, Germany Institute for Environmental Physics, University of Bremen, Bremen, Germany Service d'Aéronomie, Verrières-le-Buisson, France British Antarctic Survey, Cambridge, UK A new climatology of stratospheric BrO profiles based on dynamical and chemical indicators has been developed, with the aim to apply it to the retrieval of tropospheric BrO columns from space nadir measurements. The suitability of the adopted parameterization is evaluated based on three years of output data from the 3-D chemistry transport model BASCOE. The impact of the atmospheric dynamics on the stratospheric BrO distribution is treated by means of Br_y/ozone correlations build from 3-D-CTM model results, while photochemical effects are taken into account using stratospheric NO₂ columns as an indicator of the BrO/Br_y ratio. The model simulations have been optimized for bromine chemistry and budget, and validated through comparisons using an extensive data set of ground-based, balloon-borne and satellite limb (SCIAMACHY) stratospheric BrO observations. Aliwell, S. R., Van Roozendael, M., Johnston, P. V., Richter, A., Wagner, T., et al.: Analysis for BrO in zenith-sky spectra: An intercomparison exercise for analysis improvement, J. Geophys. Res., 107, D140, doi:10.1029/2001JD000329, 2002. Bingen, C., Fussen, D., and Vanhellemont, F.: A global climatology of stratospheric aerosol size distribution parameters derived from SAGE II data over the period 1984–2000: 1. Methodology and climatological observations, J. Geophys. Res., 109, D06201, doi:10.1029/2003JD003518, 2004. Bobrowski, N., Höninger, G., Galle, B., and Platt, U.: Detection of bromine monoxide in a volcanic plume, Nature, 423, 273–276, 2003. Boersma, K. F., Eskes, H. J., and Brinksma, E. J.: Error analysis for tropospheric NO₂ retrieval from space, J. Geophys. Res., 109, D04311, doi:10.1029/2003JD003962, 2004. Bovensmann, H., Burrows, J. P., Buchwitz, M., Frerick, J., No\"el, S., Rozanov, V. V., Chance, K. V., Goede, A. P. H.: SCIAMACHY: mission objectives and measurement modes, J. Atmos. Sci., 56, 127–150, 1999. Bracher, A., Amekudzi, L., Bramstedt, K., Eichmann, K.-U., Rozanov, A., von Savigny, C., and Burrows, J. P.: Global and Validation of SCIAMACHY O3 and NO₂ profiles from OL3.0 and IUP/IFE retrieval with collocated measurements from ACE-FTS, GOMOS, HALOE, MIPAS, POAM III and SAGE II, in: Proceedings of the ENVISAT Symposium 2007, Montreux, Switzerland, 23–27 April 2007, SP-636, 63472br.pdf, 2007. Butler, J. H., King, D. B., Lobert, J. M., Montzka, S. A., Yvon-Lewis, S. A., Hall, B. D., Warwick, N. J., Mondeel, D. J., Aydin, M., and Elkins, J. W.: Oceanic distributions and emissions of short-lived halocarbons, Global Biogeochem. Cy., 21, GB1023, doi:10.1029/2006GB002732, 2007. Butz, A., Bösch, H., Camy-Peyret, C., Chipperfield, M., Dorf, M., Dufour, G., Grunow, K., Jeseck, P., Kühl, S., Payan, S., Pepin, I., Pukite, J., Rozanov, A., von Savigny, C., Sioris, C., Wagner, T., Weidner, F., and Pfeilsticker, K.: Inter-comparison of stratospheric O₃ and NO₂ abundances retrieved from balloon borne direct sun observations and Envisat/SCIAMACHY limb measurements, Atmos. Chem. Phys., 6, 1293–1314, 2006. Carpenter, L. J. and Liss, P. S.: On temperature sources of bromoform and other reactive organic bromine gases, J. Geophys. Res. D., 105(D16), 20 539–20 547, 2000. Chance, K.: Analysis of BrO measurements from the Global Ozone Monitoring Experiment, Geophys. Res. Lett., 25, 3335–3338, 1998. Daerden, F., Larsen, N., Chabrillat, S., Errera, Q., Bonjean, S., Fonteyn, D., Hoppel, K., and Fromm, M.: A 3-D-CTM with detailed online PSC-microphysics: analysis of the Antarctic winter 2003 by comparison with satellite observations, Atmos. Chem. Phys., 7, 1755–1772, 2007. Dorf, M., Bösch, H., Butz, A., Camy-Peyret, C., Chipperfield, M. P., Engel, A., Goutail, F., Grunow, K., Hendrick, F., Hrechanyy, S., Naujokat, B., Pommereau, J.-P., Van Roozendael, M., Sioris, C., Stroh, F., Weidner, F., and Pfeilsticker, K.: Balloon-borne stratospheric BrO measurements: comparison with Envisat/SCIAMACHY BrO limb profiles, Atmos. Chem. Phys., 6, 2483–2501, 2006. Dorf, M., Butler, J. H. , Butz, A. , Camy-Peyret, C., Chipperfield, M. P., Kritten, L., Montzka, S. A., Simmes, B., Weidner, F., and Pfeilsticker, K.: Long-term observations of stratospheric bromine reveal slow down in growth, Geophys. Res. Lett., 33, L24803, doi:10.1029/2006GL027714, 2006b. Dorf, M., Butz, A., Camy-Peyret, C., Chipperfield, M. P., Kritten, L., and Pfeilsticker, K.: Bromine in the tropical troposphere and stratosphere as derived from balloon-borne BrO observations, Atmos. Chem. Phys. Discuss., 8, 12 999–13 015, 2008. Errera, Q. and Fonteyn, D.: Four-dimensional variational chemical assimilation of CRISTA stratospheric measurements, J. Geophys. Res., 106, 12 253–12 265, 2001. Errera, Q., Daerden, F., Chabrillat, S., Lambert, J. C., Lahoz, W. A., Viscardy, S., Bonjean, S., and Fonteyn, D.: 4D-Var Assimilation of MIPAS chemical observations: ozone and nitrogen dioxide analyses, Atmos. Chem. Phys. Discuss., 8, 8009–8057, 2008. Feng, W., Chipperfield, M. P., Dorf, M., Pfeilsticker, K., and Ricaud, P.: Mid-latitude ozone changes: studies with a 3-D CTM forced by ERA-40 analyses, Atmos. Chem. Phys., 7, 2357–2369, 2007. Fitzenberger, R., Bösch, R., Camy-Peyret, C., Chipperfiel, M. P., Harder, H., Platt, U., Sinnhuber, B.-M., Wagner, T., and Pfeilsticker, K.: First profile measurements of tropospheric BrO, Geophys. Res. Lett., 27, 2921–2924, 2000. Frieß, U., Hollwedel, J., König-Langlo, G., Wagner, T., and Platt, U.: Dynamics and chemistry of tropospheric bromine explosion events in the Antarctic coastal region, J. Geophys. Res., 109, D06305, doi:10.1029/2003JD004133, 2004. Fromm, M., Alfred, J., and Pitts, M.: A unified, long-term, highlatitude stratospheric aerosol and cloud database using SAM II, SAGE II, and POAM II/III data: Algorithm description, database definition, and climatology, J. Geophys. Res., 108(D12), 4366, doi:10.1029/2002JD002772, 2003. Geer, A. J., Lahoz, W. A., Bekki, S., Bormann, N., Errera, Q., Eskes, H. J., Fonteyn, D., Jackson, D. R., Juckes, M. N., Massart, S., Peuch, V.-H., Rharmili, S., and Segers, A.: The ASSET intercomparison of ozone analyses: method and first results, Atmos. Chem. Phys., 6, 5445–5474, 2006. Harder, H., Camy-Peyret, C., Ferlemann, F., Fitzenberger, R., Hawat, T., Osterkamp, H., Perner, D., Platt, U., Schneider, M., Vradelis, P., and Pfeilsticker, K.: Stratospheric BrO Profiles Measured at Different Latitudes and Seasons: Atmospheric Observations, Geophys. Res. Lett., 25, 3843–3846, 1998. Harder, H., Bösch, H., Camy-Peyret, C., Chipperfield, M., Fitzenberger, R., Payan, S., Perner, D., Platt, U., Sinnhuber,B., and Pfeilsticker, K.: Comparison of measured and modeled stratospheric BrO: Implications for the total amount of stratospheric bromine, Geophys. Res. Lett., 27 , 3695–3698, 2000. Hausmann, M. and Platt, U.: Spectroscopic measurement of bromine oxide and ozone in the high Arctic during Polar Sunrise Experiment 1992, J. Geophys. Res., 99, 25 399–25 414, 1994. Hebestreit, K., Stutz, J., Rosen, D., Matveiv, V., Peleg, M., Luria, M., and Platt, U.: DOAS measurements of tropospheric bromine oxide in mid-latitudes, Science, 283, 55–57, 1999. Hendrick, F., Van Roozendael, M., Chipperfield, M. P., Dorf, M., Goutail, F., Yang, X., Fayt, C., Hermans, C., Pfeilsticker, K., Pommereau, J.-P., Pyle, J. A., Theys, N., and De Mazière, M.: Retrieval of stratospheric and tropospheric BrO profiles and columns using ground-based zenith-sky DOAS observations at Harestua, 60° N, Atmos. Chem. Phys., 7, 4869–4885, 2007. Hendrick, F., Johnston, P. V., De Mazière, M., Fayt, C., Hermans, C., Kreher, K., Theys, N., and Van Roozendael, M.: One-decade trend analysis of stratospheric BrO over Harestua (60° N) and Lauder (45° S) reveals a decline, Geophys. Res. Lett., 35, L14801, doi:10.1029/2008GL034154, 2008a. Hendrick, F., Rozanov, A., Johnston, P. V., Bovensmann, H., De Mazière, M., Fayt, C., Hermans, C., Kreher, K., Lotz, W., Theys, N., Burrows, J. P., and Van Roozendael, M.: Multi-year comparison of stratospheric BrO vertical profiles retrieved from SCIAMACHY limb and ground-based UV-visible measurements, Atmos. Chem. Phys. Discuss., in preparation, 2008b. Holton, J. R., Haynes, P. H., McIntyre, M. E., Douglass, A. R., Rood, R. B., and Pfister, L.: Stratosphere-Troposphere Exchange, Rev. Geophys., 33(4), 403–439, 1995. Hönninger, G. and Platt, U.: Observations of BrO and its vertical distribution during surface ozone depletion at Alert, Atmos. Environ., 36, 2481–2489, 2002. Koike, M., Kondo, Y., Matthews, W. A., Johnston, P. V., et al.: Assessment of the uncertainties in the NO₂ and O₃ measurements by visible spectrometers, J. Atmos. Chem., 32, 121–145, 1999. Kovalenko, L. J., Livesey, N. L., Salawitch, R. J., Camy-Peyret, C., Chipperlfield, M. P., Cofield, R. E., Dorf, M., Drouin, B. J., Froidevaux, L., Fuller, R. A., Goutail, F., Jarnot, R. F., Jucks, K., Knosp, B. W., Lambert, A., MacKenzie, I. A., Pfeilsticker, K., Pommereau, J.-P., Read, W. G., Santee, M. L., Schwartz, M. J., Snyder, W. V., Stachnik, R., Stek, P. C., Wagner, P. A., and Waters, J. W.: Validation of Aura Microwave Limb Sounder BrO observations in the stratosphere, J. Geophys. Res., 112, D24S41, doi:10.1029/2007JD008817, 2007. Kreher, K., Johnston, P. V., Wood, S. W., Nardi, B., and Platt, U.: Ground-based measurements of tropospheric and stratospheric BrO at Arrival Heights, Antartica, Geophys. Res. Lett., 24, 3021–3024, 1997. Lambert, J.-C., Van Roozendael, M., De Mazière, M., Simon, P. C., Pommereau, J.-P., Goutail, F., Sarkissian, A., and Gleason, J. F.: Investigation of pole-to-pole performances of spaceborne atmospheric chemistry sensors with the NDSC, J. Atmos. Sci., 56, 176–193, 1999. Lary, D. J.: Gas phase atmospheric bromine photochemistry, J. Geophys. Res., 101, 1505–1516, 1996. Lary, D. J., Chipperfield, M. P., Toumi, R., and Lenton, T.: Heterogeneous atmospheric bromine photochemistry, J. Geophys. Res., 101, 1489–1504, 1996. Lary, D. J.: Halogens and the chemistry of the free troposphere, Atmos. Chem. Phys., 5, 227–237, 2005. Leser, H., Höninger, G., and Platt, U.: Max-DOAS measurements of BrO and NO₂ in the marine boundary layer, Geophys. Res. Lett., 30, 1537, doi:10.1029/2002GL015811, 2003. Logan, J. A.: An analysis of ozonesonde data for the troposphere: Recommendation for testing 3-D models and development of a gridded climatology for tropospheric ozone, J. Geophys. Res., 104, 16 115–16 149, 1999. McElroy, M. B., Salawitch, R. J., Wofsy, S. C., and Logan, J. A.: Reductions of Antarctic ozone due to synergistic interactions of chlorine and bromine, Nature, 321, 759–762, 1986. Montzka, S. A., Butler, J. H., Hall, B. D., Mondeel, D. J., and Elkins, J. W.: A decline in tropospheric organic bromine, Geophys. Res. Lett., 30(15), 1826, doi:10.1029/2003GL017745, 2003. Pfeilsticker, K., Sturges, W. T., Bösch, H., Camy-Peyret, C., Chipperfield, M. P., Engel, A., Fitzenberger, R., Müller, M., Payan, S., and Sinnhuber, B.-M.: Lower stratospheric organic and inorganic bromine budget for the arctic winter 1998/99, Geophys. Res. Lett., 27, 3305–3308, 2000. Platt, U. and Stutz, J.: Differential Optical Absorption Spectroscopy (DOAS), Principle and Applications, Springer Verlag, Heidelberg, Germany, 2006. Pundt, I., Pommereau, J.-P., Chipperfield, M. P., Van Roozendael, M., and Goutail, F.: Climatology of the stratospheric BrO vertical distribution by balloon-borne UV-visible spectrometry, J. Geophys. Res., 107(D24), 4806, doi:10.1029/2002JD002230, 2002. Quack, B., Atlas, E., Petrick, G., Stroud, V., Schauffler, S., and Wallace, D. W. R.: Oceanic bromoform sources for the tropical atmosphere, Geophys. Res. Lett., 31, L23S05, doi:10.1029/2004GL020597, 2004. Richter, A., Wittrock, F., Ladstätter-Weissenmayer, A., and Burrows, J. P.: GOME measurements of stratospheric and tropospheric BrO, Adv. Space Res., 29, 1667–1672, 2002. Rodgers, C. D.: Inverse Methods for Atmospheric Sounding, Theory and Practice, World Scientific Publishing, Singapore, 2000. Roscoe, H. K., Johnston, P. V., Van Roozendael, M., Richter, A., et al.: Slant column measurements of O₃ and NO₂ during the NDSC intercomparison of zenith-sky UV-visible spectrometers in June 1996, J. Atmos. Chem., 32, 281–314, 1999. Roscoe, H. K., Hill, J. G. T., Jones, A. E., and Sarkissian, A.: Improvements of the accuracy of zenith-sky measurements of total ozone by visible spectrometers II: use of daily air-mass factors, J. Quant. Spectrosc. Radiat. Trans., 68, 327–336, 2001. Rozanov, A., Bovensmann, H., Bracher, A., Hrechanyy, S., Rozanov, V., Sinnhuber, M., Stroh, F., and Burrows, J. P.: NO₂ and BrO vertical profile retrieval from SCIAMACHY limb measurements: Sensitivity studies, Adv. Space Res., 36(5), 846–854, 2005. Salawitch, R. J., Weisenstein, D. K., Kovalenko, L. J., Sioris, C. E., Wennberg, P. O., Chance, K., Ko, M. K. W., and McLinden, C. A.: Sensitivity of ozone to bromine in the lower stratosphere, Geophys. Res. Lett., 32, L05811, doi:10.1029/2004GL021504, 2005. Salawitch, R. J.: Atmospheric chemistry: biogenic bromine, Nature, 439, 275–277, 2006. Sander, S. P., Friedl, R. R., Golden, D. M., Kurylo, M. J., Huie, R. E., Orkin, V. L., Moortgaat, G. K., Ravishankara, A. R., Kolb, C. E., and Molina, M. J.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies. Evaluation Number 14: update of key reactions, Tech. rep., Jet Propulsion Laboratory, California Institute of Technology, Pasadena, California, 2003. Sander, S. P., Friedl, R. R., Ravishankara, A. R., et al.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies, Evaluation Number 15: update of key reactions, Tech. rep., Jet Propulsion Laboratory, California Institute of Technology, Pasadena, California, 2006. Schofield, R., Kreher, K., Connor, B. J., Johnston, P. V., Thomas, A., Shooter, D., Chipperfield, M. P., Rodgers, C. D., and Mount, G. H.: Retrieved tropospheric and stratospheric BrO columns over Lauder, New Zealand., J. Geophys. Res., 109, D14304, doi:10.1029/2003JD004463, 2004. Schofield, R., Johnston, P. V., Thomas, A., Kreher, K., Connor, B. J., Wood, S., Shooter, D., Chipperfield, M. P., Richter, A., von Glasow, R., and Rodgers, C. D.: Tropospheric and stratospheric BrO columns over Arrival Heights, Antartica, 2002, J. Geophys. Res., 111, D22310, doi:10.1029/2005JD007022, 2006. Sheode, N., Sinnhuber, B.-M., Rozanov, A., and Burrows, J. P.: Towards a climatology of stratospheric bromine monoxide from SCIAMACHY limb observations, Atmos. Chem. Phys. Discuss., 6, 6431–6466, 2006. Simpson, W. R., von Glasow, R., Riedel, K., Anderson, P., Ariya, P., Bottenheim, J., Burrows, J., Carpenter, L., Frieß, U., Goodsite, M. E., Heard, D., Hutterli, M., Jacobi, H.-W., Kaleschke, L., Neff, B., Plane, J., Platt, U., Richter, A., Roscoe, H., Sander, R., Shepson, P., Sodeau, J., Steffen, A., Wagner, T., and Wolff, E.: Halogens and their role in polar boundary-layer ozone depletion, Atmos. Chem. Phys., 7, 4375–4418, 2007. Sinnhuber, B.-M. and Folkins, I.: Estimating the contribution of bromoform to stratospheric bromine and its relation to dehydration in the tropical tropopause layer, Atmos. Chem. Phys., 6, 4755–4761, 2006. Sinnhuber, B.-M., Arlander, D. W., Bovensmann, H., et al.: Comparison of measurements and model calculations of stratospheric bromine monoxide, J. Geophys. Res., 107(D19), 4398, doi:10.1029//2001JD000940, 2002. Sinnhuber, B.-M., Rozanov, A., Sheode, N., Afe, O. T., Richter, A., Sinnhuber, M., Wittrock, F., Stiller, G. P., von Clarmann, T., Linden, A., and Burrows, J. P.: Global observations of stratospheric bromine monoxide from SCIAMACHY, Geophys. Res. Lett., 32, L20810, doi:10.1029/2005GL023839, 2005. Sioris, C. E., Kovalenko, L. J., McLinden, C. A., Salawitch, R. J., Van Roozendael, M., Goutail, F., Dorf, M., Pfeilsticker, K., Chance, K., von Savigny, C., Liu, X., Kurosu, T. P., Pommereau, J.-P., Bösch, H., and Frerick, J.: Latitudinal and vertical distribution of bromine monoxide in the lower stratosphere from Scanning Imaging Absorption Spectrometer for Atomspheric Chartography limb scattering measurements, J. Geophys. Res., 111, D14301, doi:10.1029/2005JD006479, 2006. Soller, R., Nicovich, J. M., and Wine, P. H.: Temperature-dependent rate coefficients for the reactions of Br(²P$_3/2)$, Cl(²P$_3/2)$, and O(³PJ) with BrONO₂, J. Phys. Chem. A, 105, 1416–1422, 2001. Solomon, S.: Stratospheric ozone depletion, A review of concepts and history, Rev. Geophys., 37(3), 275–316, 1999. Theys, N., Van Roozendael, M., Hendrick, F., Fayt, C., Hermans, C., Baray, J.-L., Goutail, F., Pommereau, J.-P., and De Mazière, M.: Retrieval of stratospheric and tropospheric BrO columns from multi-axis DOAS measurements at Reunion Island (21° S, 56° E), Atmos. Chem. Phys., 7, 4733–4749, 2007. Vandaele, A.-C., Fayt, C., Hendrick, F., Hermans, C., Humbled, F., et al.: An intercomparison campaign of ground-based UV-visible measurements of NO₂, BrO and OClO slant columns: Methods of analysis and results for NO₂, J. Geophys. Res., 110, D08305, doi:10.1029/2004JD005423, 2005. Van Roozendael, M., Wagner, T., Richter, A., Pundt, I., Arlander, D., Burrows, J. P., Chipperfield, M., Fayt, C., Johnston, P. V., Lambert, J.-C., Kreher, K., Pfeilsticker, K., Platt, U., Pommereau, J.-P., Sinnhuber, B.-M., Tornkvist, K. K., and Wittrock, F.: Intercomparison of BrO measurements from ERS-2 GOME, ground-based and balloon platforms, Adv. Space Res., 29, 1661–1666, 2002. Vigouroux, C., De Mazière, M., Errera, Q., Chabrillat, S., Mahieu, E., Duchatelet, P., Wood, S., Smale, D., Mikuteit, S., Blumenstock, T., Hase, F., and Jones, N.: Comparisons between ground-based FTIR and MIPAS N₂O and HNO₃ profiles before and after assimilation in BASCOE, Atmos. Chem. Phys., 7, 377–396, 2007. von Glasow, R., von Kuhlmann, R., Lawrence, M. G., Platt, U., and Crutzen, P. J.: Impact of reactive bromine chemistry in the troposphere, Atmos. Chem. Phys., 4, 2481–2497, 2004. Wagner, T. and Platt, U.: Satellite mapping of enhanced BrO concentrations in the troposphere, Nature, 395, 486–490, 1998. Wilmouth, D. M., Hanisco, T. F., Donahue, N. M., and Anderson, J. G.: Fourier transform ultraviolet spectroscopy of the A$^2\Pi_3/2\leftarrow$ X$^2\Pi_3/2$ transition of BrO, J. Phys. Chem. A., 103, 8935–8945, 1999. World Meteorological Organization (WMO): Scientific Assessment of Ozone Depletion: 2006, Global ozone research and monitoring project, Chapter 2: Halogenated Very Short-Lived Substances, Rep. 50, Geneva, Switzerland, 2007. Yang, X., Cox, R. A., Warwick, N. J., Pyle, J. A., Carver, G. D., O'Connor, F. M., and Savage, N. H.: Tropospheric bromine chemistry and its impact on ozone: a model study, J., Geophys. Res., 110, D23311, doi:10.1029/2005JD006244, 2005.