References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-10-12295-2010

Ozone, carbon monoxide and nitrogen oxides time series at four alpine GAW mountain stations in central Europe

Gilge

¹ Plass-Duelmer

¹ Fricke

¹ Kaiser

² Ries

³ Buchmann

⁴ Steinbacher

⁴

Hohenpeissenberg Meteorological Observatory, German Meteorological Service (DWD), Hohenpeissenberg, Germany

Central Institute for Meteorology and Geodynamics (ZAMG), Vienna, Austria

Federal Environment Agency (UBA), Zugspitze, Germany

Swiss Federal Laboratories for Materials Science and Technology (EMPA), Duebendorf, Switzerland

23 12 2010

10 24 12295 12316

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

This article is available from http://www.atmos-chem-phys.net/10/12295/2010/acp-10-12295-2010.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/12295/2010/acp-10-12295-2010.pdf

Long-term, ground based in-situ observations of ozone (O3) and its precursor gases nitrogen dioxide (NO2) and carbon monoxide (CO) from the four sites Hohenpeissenberg and Zugspitze (D), Sonnblick (A) and Jungfraujoch (CH) are presented for the period 1995–2007. These Central European alpine mountain observatories cover an altitude range of roughly 1000 to 3500 m. Comparable analytical methods and common quality assurance (QA) procedures are used at all sites. For O3 and CO, calibration is linked to primary calibrations (O3) or CO standards provided by the Central Calibration Laboratory (CCL) at NOAA/ESRL. All stations have been audited by the World Calibration Centre (WCC) for CO and O3 (WCC-Empa; CH). Data from long-term measurements of NO2 and CO are only available from Hohenpeissenberg and Jungfraujoch. Both sites show slightly decreasing mixing ratios of the primarily emitted NO2 and the partly anthropogenically emitted CO between 1995 and 2007. The findings are generally consistent with shorter observation periods at Zugspitze and Sonnblick and thus are considered to represent regional changes in Central European atmospheric composition at this altitude range. Over the same period, 1995–2007, the O3 mixing ratios have slightly increased at three of the four sites independent of wind sector. Trends are often more pronounced in winter and less in summer; highest declines of NO2 and CO are observed in winter and the lowest in summer, whereas the strongest O3 increase was detected in winter and lowest or even decline in summer, respectively. Weekly cycles demonstrate anthropogenic impact at all elevations with enhanced NO2 on working days compared to weekends. Enhanced O3 values on working days indicating photochemical production from anthropogenic precursors are only observed in summer, whereas in all other seasons anti-correlation with NO2 was found due to reduced O3 values on working days. Trends are discussed with respect to anthropogenic impacts and vertical mixing. The observed trends for NO2 at the alpine mountain sites are less pronounced than trends estimated based on emission inventories.

References 1

Balzani-Lööv, J. M., Henne, S., Legreid, G., Staehelin, J., Reimann, S., Prevot, A. S. H., Steinbacher, M., and Vollmer, M. K.: Estimation of background concentrations of trace gases at the Swiss Alpine site Jungfraujoch (3580 m a.s.l.), JGR, 113, D22305, doi:10.1029/2007JD009751, 2008.

Brönnimann, S., Schuepbach, E., Zanis, P., Buchmann, B., and Wanner, H.: A climatology of regional background ozone at different elevations in Switzerland (1992–1998), Atmos. Environ., 34(29–30), 5191–5198, 2000.

Brönnimann, S., Buchmann, B., and Wanner, H.: Trends in near surface ozone concentrations in Switzerland: the 1990s, Atmos. Environ., 36(17), 2841–2852, 2002.

Buchmann, B., Klausen, J. and Zellweger, C.: Traceability of Long-Term Atmospheric Composition Observations across Global Monitoring Networks, Chimia, 63(2009), doi:10.2533/chimia, 2009.

Carslaw, D. C.: On the changing seasonal cycles and trends of ozone at Mace Head, Ireland, Atmos. Chem. Phys., 5, 3441–3450, doi:10.5194/acp-5-3441-2005, 2005.

Chevalier, A., Gheusi, F., Delmas, R., Ordóñez, C., Sarrat, C., Zbinden, R., Thouret, V., Athier, G., and Cousin, J.-M.: Influence of altitude on ozone levels and variability in the lower troposphere: a ground-based study for western Europe over the period 20012004, Atmos. Chem. Phys., 7, 4311–4326, doi:10.5194/acp-7-4311-2007, 2007.

Chevalier, A., Gheusi, F., Attié, J.-L., Delmas, R., Zbinden, R., Athier, G., and Cousin, J.-M.: Carbon monoxide observations from ground stations in France and Europe and long trends in the free troposphere, Atmos. Chem. Phys. Discuss., 8, 3313–3356, doi:10.5194/acpd-8-3313-2008, 2008.

Colette, A. and Ancellet, G.: Impact of vertical transport processes on the vertical layering of tropospheric ozone above Europe. Part II: Climatological analysis of the last 30 years, Atmos. Environ., 39, 5423–5435, 2005.

Colette, A., Ancellet, G., and Borchi, F.: Impact of vertical transport processes on the vertical layering of tropospheric ozone above Europe. Part I: Study of air mass origin using multi-variate analysis and clustering, Atmos. Environ., 39, 5409–5422, 2005.

Derwent, R. G., Jenkin, M. E., Saunders, S. M., Pilling, M. J., Simmonds, P. G., Passant, N. R., Dollard, G. J., Dumitrean, P., and Kent, A.: Photochemical ozone formation in north west Europe and its control, Atmos. Environ., 37, 1983–1991, 2003.

Derwent, R. G., Simmonds, P. G., O'Doherty, S., Stevenson, D. S., Collins, W. J., Sanderson, M. G., Johnson, C. E., Dentener, F., Cofala, J., Mechler, R., and Amann, M.: External influences on Europe's air quality: baseline methane, carbon monoxide and ozone from 1990 and 2030 at Mace Head, Ireland, Atmos. Environ., 40, 844–855, 2006.

Derwent, R. G., Simmonds, P. G., Manning, A. J., and Spain, T. G.: Trends over a 20-year period from 1987 to 2007 in surface ozone at the atmospheric research station, Mace Head, Ireland, Atmos. Environ., 41, 9091–9098, 2007.

Derwent, R., Stevenson, D., Collins, W., and Johnson, C.: Intercontinental transport and the origins of the ozone observed at surface sites in Europe, Atmos. Environ., 38(13), 1891–1901, 2004.

Dils, B., Demoulin, P., Mahieu, E., Steinbacher, M., Buchmann, B. and De Mazière, M.: Ground-based CO observations at the Jungfraujoch from 1997 till 2007: Comparison between FTIR and NDIR measurements, Geomon annual meeting, Genève, 26–29 January 2009, http://hdl.handle.net/2268/16041, 2009.

Duncan, B. N., Logan, J. A., Bey, I., Megretskaia, I. A., Yantosca, R. M., Novelli, P. C., Jones, N. B., and Rinsland, C. P.: Global budget of CO, 1988–1997: Source estimates and validation with a global model, J. Geophys. Res. Atmos., 112, D22301, doi:10.1029/2007JD008459, 2007.

EEA: Assessment of ground-level ozone in EEA member countries, with a focus on long-term trends, Technical Report No 7/2009, EEA (European Environment Agency), ISBN 978-92-9213-003-9, 2009. (1)

EEA: European Community emission inventory report 1990–2007 under the UNECE Convention on Long-range Transboundary Air Pollution (LRTAP), Technical Report No 8/2009, EEA (European Environment Agency), ISBN 978-92-9213-005-3, 2009. (2)

Fischer, H., Lawrence, M., Gurk, Ch., Hoor, P., Lelieveld, J., Hegglin, M. I., Brunner, D., and Schiller, C.: Model simulations and aircraft measurements of vertical, seasonal and latitudinal O3 and CO distributions over Europe, Atmos. Chem. Phys., 6, 339–348, doi:10.5194/acp-6-339-2006, 2006.

Forrer, J., Rüttimann, R., Schneiter, D., Fischer, A., Buchmann, B., and Hofer, P.: Variability of trace gases at the high-Alpine site Jungfraujoch caused by meteorological transport processes, J. Geophys. Res., 105(D10), 12241–12251, 2000.

GAWSIS: GAW Station Information System: http://gaw.empa.ch/ gawsis, 2009.

Gerbig, C., Schmitgen, S., Kley, D., Volz-Thomas, A., Dewey, K., and Haaks, D.: An improved fast-response vacuum-UV resonance fluorescence CO instrument, J. Geophys. Res.-Atmos., 104, 1699–1704, 1999.

Gilge, S.: Quality Assurance of long-term CO Measurements, Poster at Joint WMO/GAW-Accent Workshop, EMPA Duebendorf, Switzerland, (http://www.empa.ch/plugin/template/empa/*/43919), 2005.

Gomiscek, B., Ciglar, R., Scheel, H. E., and Veber, M.: Analysis of the Ozone Spring Maximum at the Krvavec Elevated TOR Site, in: Eurotrac Vol 1, Transaction: Ecology and the Environment, Volume 35, Online ISSN: 1743–3541, Print ISBN: 1-85312-678-0, edited by: Borrell, P. M., EUROTRAC-2 International Scientific Secretariat, Germany, Pages: 856, Published: 1999.

Gros, V., Bonsang, B., Martin, D., Novelli, C. P., and Kazan, V.: Carbon monoxide short term measurements at Amsterdam island: estimations of biomass burning emission rates, Chemosphere – Global Change Science, 1(1-3), 163–172, 1999.

Henne, S., Furger, M., Nyeki, S., Steinbacher, M., Neininger, B., de Wekker, S. F. J., Dommen, J., Spichtinger, N., Stohl, A., and Prévôt, A. S. H.: Quantification of topographic venting of boundary layer air to the free troposphere, Atmos. Chem. Phys., 4, 497–509, doi:10.5194/acp-4-497-2004, 2004.

Honrath, R. E., Owen, R. C., Val Martin, M., Reid, J. S., Lapina, K., Fiahlo, P., Dziobak, M. P., Kleissel, J., and Westphal, D. L.: Regional and hemispheric impacts of anthropogenic and biomass burning emissions on summertime CO and O3 in the North Atlantic lower free troposphere. J. Geophys. Res.-Atmos., 109, D24310, doi:10.1029/2004JD005147, 2004.

Jenkin, M. E., Davies, T. J., and Stedman, J. R.: The origin and day-of-week dependence of photochemical ozone episodes in the UK, Atmos. Environ., 36, 999–1012, 2002.

Jenkin, M. E.: Analysis of the sources and partitioning of oxidant in the UK. Part 1: The NOx-dependence of annual mean concentrations of nitrogen dioxide and ozone, Atmos. Environ., 38, 5117–5129, 2004.

Jenkin, M. E.: Trends in ozone concentration distributions in the UK since 1990: Local, regional and global influences, Atmos. Environ., 42, 5434–5445, 2008.

Jonson, J. E., Simpson, D., Fagerli, H., and Solberg, S.: Can we explain the trends in European ozone levels?, Atmos. Chem. Phys., 6, 51–66, doi:10.5194/acp-6-51-2006, 2006.

Kaiser, A., Scheifinger, H., Weiss, A., Gilge, S., Ries, L., Cemas, D., and Jesenovec, B.: Transport of nitrogen oxides, carbon monoxide and ozone to the Alpine Global Atmosphere Watch stations Jungfraujoch (Switzerland), Zugspitze and Hohenpeissenberg (Germany), Sonnblick (Austria) and Mt Krvavec (Slovenia), Atmos. Environ., 41, 9273–9287, doi:10.1016/j.atmosenv.2007.09.027, 2007.

Meszaros, T., Haszpra, L., and Gelencser, A.: Tracking changes in carbon monoxide budget over Europe between 1995 and 2000, Atmos. Environ., 39, 7297–7306, 2005.

Monks, P. S.: A review of the observations and origins of the spring ozone maximum, Atmos. Environ., 34, 3545–3561, 2000.

Naja, M., Akimoto, H., and Staehelin, J.: Ozone in background and photochemically aged air over central Europe: Anlysis of longterm ozonesonde data from Hohenpeissenberg and Payerne, J. Geophys. Res., 108(D2), 4063–4073, 2003.

Novelli, P. C., Masarie, K. A., Lang, P. M., Hall, B. D., Myers, R. C., and Elkins, J. W.: Re-analysis of tropospheric CO trends: Effects of the 1997–1998 wild fires, J. Geophys. Res.-Atmos., 108, 4464, doi:4410.1029/2002JD003031, 2003.

Oltmans, S., Lefohn, A., Harris, J., Galbally, I., Scheel, H., Bodeker, G., Brunke, E., Claude, H., Tarasick, D., Johnson, B., Simmonds, P., Shadwick, D., Anlauf, K., Schmidlin, F., Fujimoto, T., Akagi, K., Meyer, C., Nichol, S., Davies, J., Redondas, A., and Cuevas, E.: Long-term changes in tropospheric ozone, Atmos. Environ., 40, 3156–3173, 2006.

Ordónez, C., Mathis, H., Furger, M., Henne, S., Hüglin, C., Staehelin, J., and Prévôt, A. S. H.: Changes of daily surface ozone maxima in Switzerland in all seasons from 1992 to 2002 and discussion of summer 2003, Atmos. Chem. Phys., 5, 1187–1203, doi:10.5194/acp-5-1187-2005, 2005.

Pfister, G., Petron, G., Emmons, L. K., Gille, J. C., Edwards, D. P., Lamarque, J. F., Attie, J. L., Granier, C., and Novelli, P. C.: Evaluation of CO simulations and the analysis of the CO budget for Europe, J. Geophys. Res.-Atmos., 109, doi:10.1029/2004JD004691, 2004.

Reimann, S., Vollmer, M. K., Folini, D., Steinbacher, M., Hill, M., Buchmann, B., Zander, R., and Mahieu, E.: Observations of Anthropogenic Halocarbons at the High-Alpine site of Jungfraujoch for assessment of trends and European sources, Sci. Total Environ., 391, 224–231, 2008.

Ribas, A. and Penuelas, J.: Temporal patterns of surface ozone levels in different habitats of the North Western Mediterranean basin, Atmos. Environ., 38, 985–992, 2004.

Sachs, L., Angewandte Statistik: Anwendung statistischer Methoden, 7 Aufl., Springer Verlag berlin Heidelberg, 1992, ISBN 3-540-52085-6.

Schaub, D., Weiss, A. K., Kaiser, J. W., Petritoli, A., Richter, A., Buchmann, B., and Burrows, J. P.: A transboundary transport episode of nitrogen dioxide as observed from GOME and its impact in the Alpine region, Atmos. Chem. Phys., 5, 23–37, doi:10.5194/acp-5-23-2005, 2005.

Scheel, H., Areskoug, H., Geiss, H., Gomiscek, B., Granby, K., Haszpra, L., Klasinc, L., Kley, D., Laurila, T., Lindskog, A., Roemer, M., Schmitt, R., Simmonds, P., Solberg, S., and Toupance, G.: On the Spatial Distribution and Seasonal Variation of Lower-Troposphere Ozone over Europe, J. Atmos. Chem., 28, 11–28, 1997.

Simmonds, P. G., Manning, A. J., Derwent, R. G., Ciais, P., Ramonet, M., Kazan, V., and Ryall, D.: A burning question: Can recent growth rate anomalies in greenhouse gases be attributed to large-scale biomass burning events?, Atmos. Environ., 39, 2513–2517, 2005.

Vautard, R., Honoré, C., Beekmann, M., and Rouil, L.: Simulation of ozone during the August 2003 heat wave and emission control scenarios, Atmos. Environ., 39, 3291–3303, 2005.

Vestreng, V., Adams, M., and Goodwin, J.: Inventory review 2004: Emission data reported to CLRTAP and under the NEC directive, EMEP/MSC-W status report 1/04, The Norwegian Meteorological Institute, Oslo, Norway, 2004.

Vingarzan, R.: A review of surface ozone background levels and trends, Atmos. Environ., 38, 3431–3442, 2004.

WMO, WMO Global Atmosphere Watch (GAW) Strategic Plan (2008–2015), GAW Report No. 172 (WMO TD NO. 1384), World Meteorological Organization, Geneva, Switzerland, http://gaw.empa.ch/gawsis, 2007.

Yurganov, L. N., Blumenstock, T., Grechko, E. I., Hase, F., Hyer, E. J., Kasischke, E. S., Koike, M., Kondo, Y., Kramer, I., Leung, F. Y., Mahieu, E., Mellqvist, J., Notholt, J., Novelli, P. C., Rinsland, C. P., Scheel, H. E., Schulz, A., Strandberg, A., Sussmann, R., Tanimoto, H., Velazco, V., Zander, R., and Zhao, Y.: A quantitative assessment of the 1998 carbon monoxide emission anomaly in the Northern Hemisphere based on total column and surface concentration measurements, J. Geophys. Res.-Atmos., 109, doi:10.1029/2004JD004559, 2004.

Yurganov, L. N., Duchatelet, P., Dzhola, A. V., Edwards, D. P., Hase, F., Kramer, I., Mahieu, E., Mellqvist, J., Notholt, J., Novelli, P. C., Rockmann, A., Scheel, H. E., Schneider, M., Schulz, A., Strandberg, A., Sussmann, R., Tanimoto, H., Velazco, V., Drummond, J. R., and Gille, J. C.: Increased Northern Hemispheric carbon monoxide burden in the troposphere in 2002 and 2003 detected from the ground and from space, Atmos. Chem. Phys., 5, 563–573, doi:10.5194/acp-5-563-2005, 2005.

Zanis, P., Ganser, A., Zellweger, C., Henne, S., Steinbacher, M., and Staehelin, J.: Seasonal variability of measured ozone production efficiencies in the lower free troposphere of Central Europe, Atmos. Chem. Phys., 7, 223–236, doi:10.5194/acp-7-223-2007, 2007.

Zbinden, R. M., Cammas, J.-P., Thouret, V., Nédélec, P., Karcher, F., and Simon, P.: Mid-latitude tropospheric ozone columns from the MOZAIC program: climatology and interannual variability, Atmos. Chem. Phys., 6, 1053–1073, doi:10.5194/acp-6-1053-2006, 2006.

Zellweger, C., Forrer, J., Hofer, P., Nyeki, S., Schwarzenbach, B., Weingartner, E., Ammann, M., and Baltensperger, U.: Partitioning of reactive nitrogen (NOy) and dependence on meteorological conditions in the lower free troposphere, Atmos. Chem. Phys., 3, 779–796, doi:10.5194/acp-3-779-2003, 2003.

Zellweger, C., Ammann, M., Buchmann, B., Hofer, P., Lugauer, M., Rüttimann, R., Streit, N., Weingartner, E. and Baltensperger U.: Summertime NOy speciation at the Jungfraujoch, 3580 m above sea level, Switzerland, J. Geophys. Res., 105(D5), 6655–6667, 2000.

Zellweger, C., Hüglin, C., Klausen, J., Steinbacher, M., Vollmer, M., and Buchmann, B.: Inter-comparison of four different carbon monoxide measurement techniques and evaluation of the long-term carbon monoxide time series of Jungfraujoch, Atmos. Chem. Phys., 9, 3491–3503, doi:10.5194/acp-9-3491-2009, 2009.