References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-8-1751-2008

Evaluation of model-simulated source contributions to tropospheric ozone with aircraft observations in the factor-projected space

Shim

¹ ³ Wang

¹ Yoshida

² ⁴

Department of Earth and Atmospheric Sciences, Georgia Institute of Technology, 311 Ferst Drive, Atlanta, GA 30332, USA

Goddard Earth Science & Technology Center, University of Maryland, Baltimore County, Baltimore, MD 21228, USA

now at: Jet Propulsion Laboratory, California Institute of Technology, 4800 Oak Grove Drive Pasadena, CA 91109, USA

now at: Atmospheric Chemistry and Dynamics Branch, NASA Goddard Space Flight Center, Greenbelt, MD 20771, USA

26 03 2008

8 6 1751 1761

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.

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The full text article is available as a PDF file from http://www.atmos-chem-phys.net/8/1751/2008/acp-8-1751-2008.pdf

Trace gas measurements of TOPSE and TRACE-P experiments and corresponding global GEOS-Chem model simulations are analyzed with the Positive Matrix Factorization (PMF) method for model evaluation purposes. Specially, we evaluate the model simulated contributions to O3 variability from stratospheric transport, intercontinental transport, and production from urban/industry and biomass burning/biogenic sources. We select a suite of relatively long-lived tracers, including 7 chemicals (O3, NOy, PAN, CO, C3H8, CH3Cl, and 7Be) and 1 dynamic tracer (potential temperature). The largest discrepancy is found in the stratospheric contribution to 7Be. The model underestimates this contribution by a factor of 2–3, corresponding well to a reduction of 7Be source by the same magnitude in the default setup of the standard GEOS-Chem model. In contrast, we find that the simulated O3 contributions from stratospheric transport are in reasonable agreement with those derived from the measurements. However, the springtime increasing trend over North America derived from the measurements are largely underestimated in the model, indicating that the magnitude of simulated stratospheric O3 source is reasonable but the temporal distribution needs improvement. The simulated O3 contributions from long-range transport and production from urban/industry and biomass burning/biogenic emissions are also in reasonable agreement with those derived from the measurements, although significant discrepancies are found for some regions.

References 1

Atlas, E. L., Ridley, B. A., and Cantrell, C.: Tropospheric Ozone Production about the Spring Equinox (TOPSE) Experiment: Introduction, J. Geophys. Res. 108(D4), 8353, doi:10.1029/2002JD003172, 2003.

Benkovitz, C. M., Schwartz C. E., Jensen, M. P., et al.: Global gridded inventories of anthropogenic emissions for sulfur and nitrogen, J. Geophys. Res., 101(D22), 29 239–29 253, 1996.

Berntsen, T. K., Karlsdottir S., and Jaffe D. A.: Influence of Asian emissions on the composition of air reaching the northwestern United States, Geophys. Res. Lett., 26, 2171–2174, 1999.

Bey, I., Jacob, D. J., Yantosca, R. M., et al.: Global modeling of troposheric chemistry with assimilated meteorology: Model description and evaluation, J. Geophys. Res, 106, 23 073–23 096, 2001.

Chameides, W. L., Davis, D. D., Rodgers, M. O., et al.: Net ozone photochemical production over the eastern and central north Pacific as inferred from CTE/CITE 1 observations during fall 1983, J. Geophys. Res., 92, 2131–2152, 1987.

Chen, P.: Isentropic cross-tropopause mass exchange in the extratropics, J. Geophys. Res., 100, 16 661–16 673, 1995.

Chin, M., Jacob, D. J., and Munger, J. W., et al.: Relationship of ozone and carbon monoxide over North America, J. Geophys. Res., 99, 14 565–14 573, 1994.

Dibb, J. E., Meeker, L. D., Finkel, R. C. J., et al.: Estimation of stratospheric input to the Arctic troposphere: $^7$Be and $^10$Be in aerosols at Alert, Canada, J. Geophys. Res, 99, 12 855–12 864, 1994.

Dibb, J. E., Talbot, R. W., Scheuer, E., et al.: Stratospheric influence on the northern North American free troposphere during TOPSE: $^7$Be as a stratospheric tracer, J. Geophys. Res., 108(D4), 8363, doi:10.1029/2001JD001347, 2003.

Duncan, B. N., Martin, R. V., Staudt, A. C., et al.: Interannual and seasonal variability of biomass burning emissions constrained by satellite observations, J. Geophys. Res., 108(D2), 4100, doi:10.1029/2002JD002378, 2003.

Fishman, J. and Seiler, W.: Correlative nature of ozone and carbon monoxide in the troposphere: Implications for the tropospheric ozone budget, J. Geophys. Res., 88, 3662–3670, 1983.

Holton, J. R., Haynes P. H., McInyre, E. M., et al.: Stratosphere-troposphere exchange, Rev. Geophys, 33, 403–439, 1995.

Jacob, D. J., Logan J. A., and Murti P. P.: Effect of rising Asian emissions on surface ozone in the United States, Geophys. Res. Lett., 26, 2175–2178, 1999.

Jacob, D. J., Crawford, J. H., Kleb, M. M., et al.: Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission: Design, execution, and first results, J. Geophys. Res., 108(D20), 1–19, 2003.

Jaffe, D., Anderson, T., Covert, D., et al.: Transport of Asian air pollution to North America, Geophys. Res. Lett., 26, 711–714, 1999.

Lee, E., Chan, C. K., and Paatero, P.: Application of positive matrix factorization in source apportionment of particulate pollutants in Hong Kong, Atmos. Envron., 33, 3201–3212, 1999.

Liu, H., Jacob, D. J., Bey, I., and Yantosca, R. M.: Constraints from $^210$Pb and $^7$Be on wet deposition and transport in a global three-dimensional chemical tracer model driven by assimilated meteorological fields, J. Geophys. Res., 106, 12 109–12 128, 2001.

Liu, H., Jacob, D. J., Chan, L. Y., et al.: Sources of tropospheric ozone along the Asian Pacific Rim: An analysis of ozonesonde observations, J. Geophys. Res., 107(D21), 4573, doi:10.1029/2001JD002005, 2002.

Liu, H., Jacob, D. J., Dibb, J. E., Fiore, A. M., et al.: Constraints on the sources of tropospheric ozone from $^210$Pb-$^7$Be-O3 correlations, J. Geophys. Res., 109, D07306, doi:10.1029/2003JD003988, 2004.

Liu, S. C., Trainer, M., Fehsenfeld, F. C., et al.: Ozone production in the rural troposphere and the implications for regional and global ozone distributions, J. Geophys. Res., 92, 4191–4207, 1987.

Liu, W., Wang, Y., Russell, A., et al.: Atmospheric aerosols over two urban-rural pairs in southeastern United States: Chemical composition and sources, Atmos. Environ., 39, 4453–4470, 2005.

Logan, J. A.: Tropospheric ozone: Seasonal behavior, trends, and anthropogenic influence, J. Geophys. Res., 90, 10 463–10 482, 1985.

Mauzerall, D. L., Narita, D., Akimoto, H., et al.: Seasonal characteristics of tropospheric ozone production and mixing ratios over East Asia: A global three dimensional chemical transport model analysis, J. Geophys. Res., 105, 17 895–17 910, 2000.

McLinden, C. A., Olsen, S. C., and Hannegan, B., et al.: Stratospheric ozone in 3- D models: A simple chemistry and the cross-tropopause flux, J. Geophys. Res., 105, 14 653–14 665, 2000.

Olivier, J. G. J. and Berdowski, J. J. M.: Global emissions sources and sinks, in: The Climate System, edited by: Berdowski, J., Guicherit, R., and Heij, B. J., A A Balkema Publishers/Swets & Zeitlinger Publishers, Lisse, The Netherlands, ISBN 90-5809-255-0, 33–78, 2001.

Oltmans, S. J. and Levy II, H.: Seasonal cycle of surface ozone over the western North Atlantic, Nature, 358, 392–394, 1992.

Paatero, P. and Tapper, U.: Positive Matrix Factorization: a non-negative factor model with optimal utilization of error estimates of data values, Environmetrics, 5, 111–126, 1994.

Paatero, P.: Least squares formulation of robust non-negative factor analysis, Chemomet. Intell. Lab. Sys., 37, 23–35, 1997.

Paatero, P., Hopke, P. K., Song, X.-H., et al.: Understanding and controlling rotations in factor analytic models, Chemomet. Intell. Lab. Sys., 60, 253–264, 2002.

Parrish, D. D., Holloway, J. S., Trainer, M., et al.: Export of North American ozone pollutions to the North Atlantic Ocean, Science, 259, 1436–1439, 1993.

Penkett, S. A. and Brice K. A.: The spring maximum in photo-oxidants in the Northern Hemisphere troposphere, Nature, 319, 655–657, 1986.

Shim, C., Wang, Y., Singh, H. B., et al.: Source characteristics of oxygenated volatile organic compounds and hydrogen cyanide, J. Geophys. Res., 112, D10305, doi:10.1029/2006JD007543, 2007.

Tanimoto, H., Wild, O., Kato, S., et al.: Seasonal cycles of ozone and oxidized nitrogen species in northeast Asia: 2. A model analysis of the roles of chemistry and transport, J. Geophys. Res., 107(D23), 4706, doi:10.1029/2001JD001497, 2002.

Wang, Y., Jacob, D. J., and Logan, J. A.: Global simulation of tropospheric O3-NOx-hydrocarbon chemistry, 3. origin of troposheric ozone and effects of non-methane hydrocarbons, J. Geophys. Res., 103, 10 757–10 767, 1998b.

Wang, Y., Liu, S. C., Wine, P. H., et al.: Factors Controlling Tropospheric O3, OH, NOx, and SO2 over the Tropical Pacific during PEM-Tropics B, J. Geophys. Res., 106, 32 733–32 748, 2001.

Wang, Y., Ridley, B., Fried, A., et al.: Springtime photochemistry at northern mid and high latitudes, J. Geophys. Res., 108(D4), 8358, doi:10.1029/2002JD002227, 2003a.

Wang, Y., Shim, C., Blake, N., et al.: Intercontinental transport of pollution manifested in the variability and seasonal trend of springtime O3 at northern middle and high latitudes, J. Geophys. Res., 108(D21), 4683, doi:10.1029/2003JD003592, 2003b.

Wang, Y. and T. Zeng; On tracer correlations in the troposphere: The case of ethane and propane, J. Geophys. Res., 109, D24306, doi:10.1029/2004JD005023, 2004.

Wang, Y., Choi, Y. S., Zeng, T., et al.: Late-spring increase of trans-Pacific pollution transport in the upper troposphere, Geosphys. Res. Lett., 33, L01811, doi:10.1029/2005GL024975, 2006.

Wild, O. and Akimoto, H.: Intercontinental transport of ozone and its precursors in a three-dimensional global CTM, J. Geophys. Res., 106, 27 729–27 744, 2001.

Yoshida, Y., Wang, Y. H., Zeng, T., et al.: A three-dimensional global model study of atmospheric methyl chloride budget and distributions, J. Geophys. Res., 109, D24309, doi:24310.21029/2004JD004951, 2004.