ACPD Atmospheric Chemistry and Physics Discussions ACPD 1680-7375 Copernicus GmbH Göttingen, Germany 10.5194/acpd-8-18219-2008 The impact of traffic emissions on atmospheric ozone and OH: results from QUANTIFY Hoor P. 1 Borken-Kleefeld J. 2 Caro D. 3 Dessens O. 4 Endresen O. 5 Gauss M. 6 Grewe V. 7 Hauglustaine D. 3 Isaksen I. S. A. 6 Jöckel P. 1 Lelieveld J. 1 Meijer E. 8 Olivie D. 9 Prather M. 10 Schnadt Poberaj C. 11 Staehelin J. 11 Tang Q. 10 van Aardenne J. 12 van Velthoven P. 8 Sausen R. 7 Max Planck Institute for Chemistry, Department of Atmospheric Chemistry, 55020 Mainz, Germany Transportation Studies, German Aerospace Center (DLR), Berlin, Germany Laboratoire des Sciences du Climat et de l'Environment (LSCE), CEN de Saclay, Gif-sur-Yvette, France Centre for Atmospheric Science, Department of Chemistry, Cambridge, UK DNV, Det Norske Veritas (DNV), Oslo, Norway Department of Geosciences, University of Oslo, Norway Deutsches Zentrum für Luft- und Raumfahrt, Institut für Physik der Atmosphäre, Oberpaffenhofen, 82234 Wessling, Germany Royal Netherlands Meteorological Institute, KNMI, De Bilt, The Netherlands Meteo France, CNRS, Toulouse, France Department of Earth System Science, University of California, Irvine, USA Institute for Atmospheric and Climate Science, Swiss Federal Institute of Technology, Zürich, Switzerland Joint Research Center, JRC, Ispra, Italy 21 10 2008 8 5 18219 18266 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-discuss.net/8/18219/2008/acpd-8-18219-2008.html The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/8/18219/2008/acpd-8-18219-2008.pdf

To estimate the impact of emissions by road, aircraft and ship traffic on ozone and OH of the present-day atmosphere seven different atmospheric chemistry models simulated the atmospheric composition of the year 2003. Based on newly developed global emission inventories for road, maritime and aircraft emission data sets each model performed a series of five simulations: A base scenario using the full set of emissions, three sensitivity studies with each individual sector of transport reduced by 5% and one simulation with all traffic related emissions reduced by 5%. The approach minimizes non-linearities in atmospheric chemical effects and are later scaled to 100%. <br><br> The global annual mean impact of ship emissions on ozone in the boundary layer leads to an increase of ozone of 1.2%, followed by road (0.87%) and aircraft emissions (0.3%). In the upper troposphere between 200–300 hPa both road and ship traffic affect ozone by 1.1%, whereas aircraft emissions contribute 0.9%. However, the sensitivity of ozone formation per NO<sub>x</sub> molecule emitted is highest for aircraft exhausts. <br><br> The local maximum effect of the summed traffic emissions on the ozone column predicted by the models is 4.0 DU and occurs over the northern subtropical Atlantic. The impact of traffic emissions on total ozone in the Southern Hemisphere is approximately half of the northern hemispheric perturbation. <br><br> Below 800 hPa both ozone and OH respond most sensitively to ship emissions in the marine boundary layer over the Atlantic, where the effect can exceed 10% (zonal mean) which is 80% of the total traffic induced ozone perturbation. In the Southern Hemisphere ship emissions contribute relatively strongly to the total ozone perturbation by 60%–80% throughout the year (equivalent to 1–1.5 ppbv). <br><br> Road emissions have the strongest impact on ozone in the continental boundary layer and the free troposphere in summer. They also affect the upper troposphere particularly during northern summer associated with strong convection in mid latitudes. Ozone perturbations due to road traffic show the strongest seasonal cycle in the northern troposphere, and can even change sign in the continental boundary layer during winter. <br><br> The OH concentration in the boundary layer is most strongly affected by ship emissions, which has a significant influence on the lifetime of many trace gases including methane. Methane lifetime changes due to ship emissions amount to 4.1%, followed by road (1.6%) and air traffic (1.0%).

 References Andreae, M. and Merlet, P.: Emission of trace gases and aerosols from biomass burning, Global Biogeochem. Cy., 15, 955–966, 2001. Bian, H. and Prather, M.: Fast-J2: Accurate Simulation of stratospheric photolysis in global chemical models, J. Atmos. Sci., 41, 281–296, 2002. Borken, J. and Steller, H.: Report on the Draft Emission Inventories for Road Transport in the year 2000, Tech. rep., Deutsches Institut für Luft- und Raumfahrt (DLR), Institut für Verkehrsforschung, 2006. Borken, J., Steller, H., Meretei, T., and Vanhove, F.: Global and country inventory of road passenger and freight transportation - Their fuel consumption and their emissions of air pollutants in the year 2000, Transportation Research Records, Journal of the Transportation Research Board, 2011, \doi10.3141/2011-14, 127–136, 2007. Brasseur, G P., Müller, J., and Garnier, C.: Atmospheric impact of NO<sub>x</sub> emissions by subsonic aircraft: A three-dimensional model study, J. Geophys. Res., 101, 1423–1428, 1996. Carver, G. and Scott, P.: IMPACT: an implicit time integration scheme for chemical species and families, Ann. Geophys., 18, 337–346, 2000. Carver, G., Brown, P., and Wild, O.: The ASAD atmospheric chemistry integration package and chemical reaction database, Comp. Physics Communications, 105, 197–215, 1997. Corbett, J. and Koehler, H.: Updated emissions from ocean shipping, J. Geophys. Res., 108, 4650, doi:10.1029/2003JD003751, 2003. Dalsoren, S. and Isaksen, I.: CTM study of changes in tropospheric hydroxyl distribution 1990–2001 and its impact on methane, Geophys. Res. Lett., 33, L23811, \doi10.1029/2006GL027295, 2006. Dameris, M., Grewe, V., Ponater, M., Deckert, R., Eyring, V., Mager, F., Matthes, S., Schnadt, C., Stenke, A., Steil, B., Brühl, C., , and Giorgetta, M.: Long-term changes and variability in a transient simulation with a chemistry-climate model employing realistic forcing, Atmos. Chem. Phys., 5, 2121–2145, 2005. Endresen, O., Sorgand, E., Sundet, J., Dalsoren, S., Isaksen, I., Berglen, T., and Gravir, G.: Emission from international sea transportation and environmental impact, J. Geophys. Res., 108, 4560, \doi10.1029/2002JD002898, 2003. Endresen, O., Sorgard, E., Behrens, H., Brett, P., and Isaksen, I.: A historical reconstruction of ships' fuel consumption and emissions, J. Geophys. Res., 112, D12301, doi:10.1029/2006JD007630, 2007. Eyers, C., Norman, P., Middel, J., Plohr, M., Michot, S., Atkinson, K., and Christou, R.: AERO2K Global Aviation Emissions Inventories for 2002 and 2025, Tech. Rep. 04/01113, QinetiQ, prefixhttp://elib.dlr.de/1328, 2004. Eyring, V., Köhler, H., J., v., and Lauer, A.: Emissions from international shipping: 1. The last 50 years, J. Geophys. Res., 110, D17305, \doi10.1029/2004JD005619, 2005. Eyring, V., Stevenson, D. S., Lauer, A., Dentener, F. J., Butler, T., Collins, W. J., Ellingsen, K., Gauss, M., Hauglustaine, D. A., Isaksen, I. S. A., Lawrence, M. G., Richter, A., Rodriguez, J. M., Sanderson, M., Strahan, S. E., Sudo, K., Szopa, S., van Noije, T. P. C., and Wild, O.: Multi-model simulations of the impact of international shipping on Atmospheric Chemistry and Climate in 2000 and 2030, Atmos. Chem. Phys., 7, 757–780, 2007. Folberth, G., Hauglustaine, D., Ciais, P., and Lathiäre, J.: On the role of atmospheric chemistry in the global CO<sub>2</sub> budget, Geophys. Res. Lett., 32, L08801, \doi10.1029/2004GL021812, 2005. Ganzeveld, L., van Aardenne, J., Butler, T., Lawrence, M., Metzger, S., Stier, P., Zimmermann, P., and Lelieveld, J.: Technical Note: Anthropogenic and natural offline emissions and the online EMissions and dry DEPosition submodel EMDEP of the Modular Earth Submodel system (MESSy), Atmos. Chem. Phys. Discuss., 6, 5457–5483, 2006. Gauss, M., Isaksen, I., Wong, S., and Wang, W.-C.: Impact of H<sub>2</sub>O emissions from cryoplanes and kerosene aircraft on the atmosphere, J. Geophys. Res., 108, 4304, \doidoi:10.1029/2002JD002623, 2003. Gauss, M., Isaksen, I. S. A., Lee, D. S., and Søvde, O. A.: Impact of aircraft NO<sub>x</sub> emissions on the atmosphere - tradeoffs to reduce the impact, Atmos. Chem. Phys., 6, 1529–1548, 2006. Giannakopoulos, C., Chipperfield, M., Law, K., and Pyle, J.: Validation and intercomparison of wet and dry deposition schemes using 210Pb in a global three-dimensional off-line chemical transport model, J. Geophys. Res., 104, 23 761–23 784, 1999. Granier, C. and Brasseur, G.: The impact of road traffic on global tropospheric ozone, Geophys. Res. Lett., 30, 1086, \doi10.1029/2002GL015972, 2003. Grewe, V.: Technical note: A diagnostic for ozone contributions of various NO$_x$ emissions in multi-decadal chemistry-climate model simulations, Atmos. Chem. Phys., 4, 327–342, 2004. Grewe, V.: Impact of climate variability on tropospheric ozone, Sci. Tot. Env., 374, 167–181, 2007. Grewe, V., Brunner, D., Dameris, M., Grenfell, J., Hein, R., Shindell, D., and Staehelin, J.: Origin and variability of upper tropospheric nitrogen oxides and ozone at northern mid-latitudes, Atmos. Environ., 35, 3421–3433, 2001. Grewe, V., Dameris, M., Fichter, C., and Sausen, R.: Impact of aircraft NO$_X$ emissions. Part I: Interactively coupled climate-chemistry simulations and sensitivities to climate-chemistry feedback, lightning and model resolution, Meteor. Z., 177–186, 2002. Grewe, V., Stenke, A., Ponater, M., Sausen, R., Pitari, G., Iachetti, D., Rogers, H., Dessens, O., Pyle, J., Isaksen, I., Gulstad, L., Sovde, O., Marizy, C., and Pascuillo, E.: Climate impact of supersonic air traffic: an approach to optimize a potential future supersonic fleet - results from the EU-project SCENIC, Atmos. Chem. Phys., 7, 5129–5145, 2007. Hauglustaine, D., Hourdin, F., Walters, S., Jourdain, J., Filiberti, M.-A., Lamarque, J.-F., and Holland, E.: Interactive chemistry in the Laboratoire de Météorologie Dynamique general circulation model: Description and background tropospheric chemistry evaluation, J. Geophys. Res., 109, D04314, \doi10.1029/2003JD003957, 2004. Hedegaard, G., Brandt, J., Christensen, J H., Frohn, L. M.and~Geels, C., Hansen, K M., and Stendel, M.: Impacts of climate change on air pollution levels in the Northern Hemisphere with special focus on Europe and the Arctic, Atmos. Chem. Phys., 8, 3337–3367, 2008. Hidalgo, H. and Crutzen, P.: The tropospheric and stratospheric composition perturbed by NO$_x$ emissions of high-altitude aircraft, J. Geophys. Res., 82, 5833–5866, 1977. Holtslag, A. A M. and Boville, B.: Local vesus nonlocal boundary-layer diffusion in a global climate model, J. Climate, 6, 1825–1842, 1993. Houweling, S., Dentener, F., and Lelieveld, J.: The impact of nonmethane hydrocarbon compounds on tropospheric photochemistry, J. Geophys. Res., 103, 10 673–10 696, 1998. Hsu, J., Prather, M., and Wild, O.: Diagnosing the stratosphere-to-troposphere flux of ozone in a chemistry transport model, J. Geophys. Res., 110, D19305, doi:10.1029/2005JD006045, 2005. Hsu, J. e a.: Are the TRACE-P measurements representative of the western Pacific during March 2001?, J. Geophys. Res., 109, D02314, doi:10.1029/2003JD004002, 2004. Isaksen, I., Zerefos, C., Kourtidis, K., Meleti, C., Dalsoren, S., Sundet, J., Grini, A., Zanis, P., and Balis, D.: Tropospheric ozone changes at unpolluted and semipolluted regions induced by stratospheric ozone changes, J. Geophys. Res., 110, D02302, \doi10.1029/2004JD004618, 2005. Kahn Ribeiro, S., Kobayashi, S., Beuthe, M., Gasca, J., Greene, D., Lee, D., Muromachi, Y., Newton, P., Plotkin, S., Sperling, D., Wit, R., and Zhou, P.: Transport and its infrastructure, in: Climate Change 2007: Mitigation. Contribution of Working Group III to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, IPCC, edited by Metz, B., Davidson, O., Bosch, P., Dave, R., and Meyer, L., Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 2007. Kerkweg, A and, S R., Tost, H., and Jöckel, P.: Technical note: Implementation of prescribed (OFFLEM), calculated (ONLEM), and pseudo-emissions (TNUDGE) of chemical species in the Modular Earth Submodel System (MESSy), Atmos. Chem. Phys., 6, 3603–3609, 2006. Law, K. and Nisbet, E.: Sensitivity of the methane growth rate to changes in methane emissions from natural gas and coal, J. Geophys. Res., 101, 14 387–14 397, 1996. Law, K., Plantevin, P., Shallcross, D., Rogers, H., Pyle, J., Grouhel, C., Thouret, V., and Marenco, A.: Evaluation of modelled O<sub>3</sub> using MOZAIC data, J. Geophys. Res., 103, 25 721–25 737, 1998. Law, K., Plantevin, P., Thouret, V., Marenco, A., Asman, W., Lawrence, M., Crutzen, P., Muler, J., Hauglustaine, D., and Kanakidou, M.: Comparison between global chemistry transport model results and Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) data, J. Geophys. Res., 105, 1503–1525, 2000. Lawrence, M G. and Crutzen, P J.: Influence of NO$_x$ emission from ships on tropospheric photochemistry and climate, Nature, 402, 167–170, 1999. Lelieveld, J., Peters, W., Dentener, F., and Krol, M.: Stability of tropospheric hydroxyl chemistry, J. Geophys. Res., 107, 4715, \doi10.1029/2002JD002272, 2002. Lelieveld, J., Dentener, F., Peters, W., and Krol, M.: On the role of hydroxyl radicals in the self-cleansing capacity of the troposphere, Atmos. Chem. Phys., 4, 2337–2344, 2004. Lemke, P., Ren, J., Alley, R., Allison, I., Carrasco, J., Flato, G., Fujii, Y., Kaser, G., Mote, P., Thomas, R., and T., Z.: Observations: Changes in Snow, Ice and Frozen Ground, in: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, IPCC, edited by Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K., Tignor, M., and Miller, H., Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 2007. Matthes, S., Grewe, V., Sausen, R., and Roelofs, G.: Global impact of road traffic emissions on tropospheric ozone, Atmos. Chem. Phys., 7, 1707–1718, 2007. Meijer, E., van Velthoven, P., Brunner, D., Huntrieser, H., and Kelder, H.: Improvement and evaluation for the parametrisation of nitrogen oxide production by lightning, Phys. Chem. of the Earth, 26/8, 557–583, 2001. Niemeier, U., Granier, C., Kornblueh, L., Walters, S., and Brasseur, G.: Global impact of road traffic on atmospheric chemical composition and on ozone climate forcing, J. Geophys. Res., 111, D09301, \doi10.1029/2006JD006407, 2006. O'Connor, F., Carver, G., Savage, N., Pyle, J., Methven, J., Arnold, S., Dewey, K., and Kent, J.: Comparison and visualisation of high-resolution transport modelling with aircraft measurements, Atm. Sci. Lett., 6, 164–170, \doi10.1002/asl.111, 2005. Ohara, T., Akimoto, H., Kurokawa, J., Horii, N., Yamaji, K., Yan, X., and Hayasaka, T.: An Asian emission inventory of anthropogenic emission sources for the period 1980–2020, Atmos. Chem. Phys., 7, 4419–4444, 2007. Olivier, J., van Aardenne, J., Dentener, F., Ganzeveld, L., and Peters, J.: Recent trends in global greenhouse gas emissions: regional trends and spatial distribution of key sources, in: Non-CO<sub>2</sub> Greenhouse Gases (NCGG-4), pp. 325–330, Millpress, Rotterdam, 2005. Pickering, K E., Wang, Y., Tao, W., Price, C., and Muller, J.-F.: Vertical distribution of lightning NO$_x$ for use in regional and global chemical transport models, J. Geophys. Res., 109, 31 203–31 216, 1998. Prather, M.: Numerical advection by conservation of second-order moments, J. Geophys. Res., 91, 6671–6681, 1986. Price, C. and Rind, D.: A simple lightning parameterization for calculating global lightning distributions, J. Geophys. Res., 97, 9919–9933, 1992. Sausen, R., Isaksen, I., Grewe, V., Schumann, U., Hauglustaine, D., Lee, D., Myhre, G., Köhler, M., Pitari, G., Strordal, F., and Zerefos, C.: Aviation radiative forcing in 2000: An update on IPCC(1999), Meteor.Z., 555–561, 2005. Savage, N., Law, K., Pyle, J., Richter, A., Nüss, H., and Burrows, J.: Using GOME NO<sub>2</sub> satellite data to examine regional differences in TOMCAT model performance, Atmos. Chem. Phys., 4, 1895–1912, 2004. Schumann, U.: The impact of nitrogen oxides emissions from aircraft upon the atmosphere at flight altitudes – results from the AERONOX project, Atmos. Environ., 31, 1723–1733, 1997. Schumann, U. and Huntrieser, H.: The global lightning-induced nitrogen oxides source, Atmos. Chem. Phys., 7, 3823–3907, 2007. Schumann, U., Schlager, H., Arnold, F., Ovarlez, J., Kelder, H., Hov, O., Hayman, G., Isaksen, I., Staehelin, J., and Whitefield, P.: Pollution from aircraft emissions in the North Atlantic flight corridor: Overview on the POLINAT projects, J. Geophys. Res., 105, 3605–3632, \doi10.1029/1999JD900941, 2000. Sovde, O. A., Gauss, M., Isaksen, I. S. A., Pitari, G., and Marizy, C.: Aircraft pollution - a futuristic view, Atmos. Chem. Phys., 7, 3621–3632, 2007. Stevenson, D., Dentener, F., Schultz, M., Ellingsen, K., van Noije, T., Wild, O., Zeng, G., Amann, M., Atherton, C., Bell, N., Bergmann, D., Bey, I., Butler, T., Cofala, J., Collins, W., Derwent, R., Doherty, R., Drevet, J., Eskes, H., Fiore, A., Gauss, M., Hauglustaine, D., Horowitz, L., Isaksen, I., Krol, M., Lamarque, J.-F., Lawrence, M., Montanaro, V., Müller, J.-F., Pitari, G., Prather, M., Pyle, J., Rast, S., Rodriguez, J., Sanderson, M., Savage, N., Shindell, D., Strahan, S., Sudo, K., and Szopa, S.: Multimodel ensemble simulations of present-day and near-future tropospheric ozone, 111, D08301, \doi10.1029/2005JD006338, 2006. Tiedtke, M.: A Comprehensive Mass Flux Scheme for Cumulus Parameterisation on Large Scale Models, Mon. Weather Rev., 117, 1779–1800, 1989. van Aardenne, J., Dentener, F., Olivier, J., Peters, J., and Ganzeveld, L.: The EDGAR3.2 Fast Track 2000 data set (32FT2000), www.mnp.nl/edgar/model/v32ft2000edgar/docv32ft2000, Joint Research Center, Institute for Environment and Sustainability (JRC-IES), Climate Change Unit, TP280, 21020 Ispra, Italy, 2005. van Noije, T., Eskes, H., Dentener, F., Stevenson, D., Ellingsen, K., Schultz, M., and Wild, O.: Multi-model ensemble simulations of tropospheric NO<sub>2</sub> compared with GOME retrievals for the year 2000, Atmos. Chem. Phys., 6, 2943–2979, 2006a. van Noije, T., Segers, A., and van Velthoven, P.: Time series of the stratosphere-troposphere exchange of ozone simulated with reanalyzed and operational forecast data, J. Geophys. Res., 111, D03301, \doi10.1029/2005JD006081, 2006b. von Kuhlmann, R., Lawrence, M G., Crutzen, P., and Rasch, P.: A model for studies of tropospheric ozone and nonmethane hydrocarbons: Model description and ozone results, J. Geophys. Res., 108, 4294, \doi10.1029/2002JD002893, 2003a. von Kuhlmann, R., Lawrence, M G., Crutzen, P., and Rasch, P.: A model for studies of tropospheric ozone and nonmethane hydrocarbons: Model evaluation of ozone related species, J. Geophys. Res., 108, 4729, \doi10.1029/2002JD003348, 2003b. Wild, O., Sundet, J., Prather, M., Isaksen, I., Akimoto, H., Browell, E., and Oltmans, S.: Chemical transport model ozone simulations for spring 2001 over the western Pacific: Comparisons with TRACE-P lidar, ozonesondes, and Total Ozone Mapping Spectrometer columns, J. Geophys. Res., 8826, \doi10.1029/2002JD003283, 2003.