References

ACPD

Atmospheric Chemistry and Physics Discussions

ACPD

1680-7375

Copernicus GmbH

Göttingen, Germany

10.5194/acpd-7-15533-2007

Factors influencing the large-scale distribution of Hg° in the Mexico City area and over the North Pacific

Talbot

¹ Mao

¹ Scheuer

¹ Dibb

¹ Avery

² Browell

² Sachse

² Vay

² Blake

³ Huey

⁴ Fuelberg

⁵

Institute for the Study of Earth, Oceans, and Space, Climate Change Research Center, University of New Hampshire, Durham, NH 03824, USA

NASA Langley Research Center, Chemistry and Dynamics Branch, Hampton, VA 23681, USA

University of California – Irvine, Department of Chemistry, Irvine, CA 92697, USA

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

Department of Meteorology, Florida State University, Tallahassee, FL 32306, USA

02 11 2007

7 6 15533 15563

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/7/15533/2007/acpd-7-15533-2007.html

The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/7/15533/2007/acpd-7-15533-2007.pdf

Gas-phase elemental mercury (Hg°) was measured aboard the NASA DC-8 aircraft during the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in spring 2006. Flights were conducted around Mexico City and on two subsequent deployments over the North Pacific based out of Honolulu, Hawaii and Anchorage, Alaska. Data obtained from 0.15–12 km altitude showed that Hg° exhibited a relatively constant vertical profile centered around 100 ppqv. Highly concentrated pollution plumes emanating from the Mexico City urban agglomeration revealed that mixing ratios of Hg° as large as 500 ppqv were related to combustion tracers such as CO, but not SO2 which is presumably released locally from coal burning, refineries, and volcanoes. Our analysis of Mexico City plumes indicated that widespread multi-source urban/industrial emissions may have a more important influence on Hg° than specific point sources. Over the Pacific, correlations with CO, CO2, CH4, and C2Cl4 were diffuse overall, but recognizable on flights out of Anchorage and Honolulu. In distinct plumes originating from the Asian continent the Hg°- CO relationship yielded an average value of ~0.56 ppqv/ppbv, in good agreement with previous findings. A prominent feature of the INTEX-B dataset was frequent total depletion of Hg° in the upper troposphere when stratospherically influenced air was encountered. Ozone data obtained with the differential absorption lidar (DIAL) showed that the stratospheric impact on the tropospheric column was a common and pervasive feature on all flights out of Honolulu and Anchorage. We propose that this is likely a major factor driving large-scale seasonality in Hg° mixing ratios, especially at mid-latitudes, and an important process that should be incorporated into global chemical transport models.

References 1

Bartlett, K. B., Sachse, G. W., Slate, T., Harward, C., and Blake, D. R.: Large-scale distribution of CH4 in the western North Pacific: Sources and transport from the Asian continent, J. Geophys. Res., 108(D20), 8807, doi:10.1029/2002JD003076, 2003.

Blake, D. R. and Rowland, F. S.: Urban leakage of liquefied petroleum gas and its impact on Mexico City air quality, Science, 269, 953–956, 1995.

Blake, N. J., Blake, D. R., Simpson, I. J., Meinardi, S., Swanson, A. L., Lopez, J. P., Katzenstein, A. S., Barletta, B., Shirai, T., Atlas, E., Sachse, G., Avery, M., Vay, S., Fuelberg, H. E., Kiley, C. M., Kita, K., and Rowland, F. S.: NMHCs and halocarbons in Asian continental outflow during the Transport and Chemical Evolution over the Pacific (TRACE-P) Field Campaign: Comparison with PEM-West B, J. Geophys. Res., 108(D20), 8806, doi:10.1029/2002JD003367, 2003.

Browell, E. V., Fenn, M. A., Butler, C. F., Grant, W. B., Merrill, J., Newell, R. E., Bradshaw, J. D., Sandholm, S., Anderson, B., Bandy, A. R., Bachmeier, A. S., Blake, D. R., Davis, D. D., Gregory, G. L. , Heikes, B., Kondo, Y., Liu, S., Rowland, F. S., Sachse, G. W., Singh, H., Talbot, R. W., and Thornton, D. C.: Large-scale air mass characteristics observed over Western Pacific during summertime, J. Geophys. Res., 101(D1), 1691–1712, 1996.

Browell, E. V., Fenn, M. A., Butler, C. F., Grant, W. B., Ismail, S., Ferrare, R. A., Kooi, S. A., Brackett, V. G., Clayton, M. B., Avery, M. A., Barrick, J. D. W., Fuelberg, H. E., Maloney, J. C., Newell, R. E., Zhu, Y., Mahoney, M. J., Anderson, B. E., Blake, D. R., Brune, W. H., Heikes, B. G., Sachse, G. W., Singh, H. B., and Talbot, R. W.: Large-scale air mass characteristics observed over the remote tropical Pacific Ocean during March-April 1999: Results from PEM-Tropics B field experiment, J. Geophys. Res., 106(D23), 32 481–32 501, 2001.

Browell, E. V., Fenn, M. A., Butler, C. F., Grant, W. B., Brackett, V. G., Hair, J. W., Avery, M. A., Newell, R. E., Hu, Y., Fuelberg, H. E., Jacob, D. J., Anderson, B. E., Atlas, E. L., Blake, D. R., Brune, W. H., Dibb, J. E., Fried, A., Heikes, B. G., Sachse, G. W., Sandholm, S. T., Singh, H. B., Talbot, R. W., Vay, S. A., and Weber, R. J.: Large-scale ozone and aerosol distributions, air mass characteristics, and ozone fluxes over the western Pacific Ocean in late winter/early spring, J. Geophys. Res., 108(D20), 8805, doi:10.1029/2002JD003290, 2003a.

Browell, E. V., Hair, J. W., Butler, C. F., Grant, W. B., DeYoung, R. J., Fenn, M. A., Brackett, V. G., Clayton, M. B., Brasseur, L. A., Harper, D. B., Ridley, B. A., Klonecki, A. A., Hess, P. G., Emmons, L. K., Tie, X., Atlas, E. L., Cantrell, C. A., Wimmers, A. J., Blake, D. R., Coffey, M. T., Hannigan, J. W., Dibb, J. E., Talbot, R. W., Flocke, F., Weinheimer, A. J., Fried, A., Wert, B., Snow, J. A., and Lefer, B. L.: Ozone, aerosol, potential vorticity, and trace gas trends observed at high-latitudes over North America from February to May 2000, J. Geophys. Res., 108(D4), 8369, doi:10.1029/2001JD001390, 2003b.

Brunke, E. G., Labyschagne, C., and Slemr, F.: Gaseous mercury emissions from a fire in the Cape Peninsula, South Africa, during January 2000, Geophys. Res. Lett., 28, 1483–1496, 2001.

Calvert, J. G. and Lindberg, S. E.: Mechanisms of mercury removal by O3 and OH in the atmosphere, Atmos. Environ., 39, 3355–3367, 2005.

Ebinghaus, R., Kock, H. H., Coggins, A. M., Spain, T. G., Jennings, S. G., and Temme C. H.: Long-term measurements of atmospheric mercury at Mace Head, Irish west coast, between 1995 and 2001, Atmos. Environ., 36, 5267–5276, 2002.

Ebinghaus, R., Slemr, F., Brenninkmeijer, C. A. M., van Velthoven, P., Zahn, A., Hermann, M., O'Sullivan, D. A., and Oram, D. E.: Emissions of gaseous mercury from biomass burning in South America in 2005 observed during CARIBIC flights, Geophys. Res. Lett., 34, L08813, doi:10.1029/2006GL028866, 2007.

Friedli, H. R., Radke, L. F., and Lu, J. Y.: Mercury in smoke from biomass fires, Geophys. Res. Lett., 28(17), 3223–3226, 2001.

Friedli, H. R., Radke, L. F., Lu, J. Y., Banic, C. M., Leaitch, W. R., and MacPherson, J. I.: Mercury emissions from burning of biomass from temperate North American forests: laboratory and airborne measurements, Atmos. Environ., 37, 253–267, 2003a.

Friedli, H. R., Radke, L. F., Prescott, R., Hobbs, P. V., and Sinha, P.: Mercury emissions from the August 2001 wildfires in Washington State and an agricultural waste fire in Oregon and atmospheric mercury budget estimates, Global Biogeochem. Cycles, 17(2), 1039, doi:10.1029/2002GB001972, 2003b.

Friedli, H. R., Radke, L. F., Prescott, R., Li, P., Woo, J.-H., and Carmichael, G. R.: Mercury in the atmosphere around Japan, Korea, and China as observed during the 2001 ACE-Asia field campaign: Measurements, distributions, sources, and implications, J. Geophys. Res., 109, D19S25, doi:10.1029/2003JD004244, 2004.

Hoell, J. M., Davis, D. D., Liu, S. C., Newell, R., Shipham, M., Akimoto, H., McNeal, R. J., Bendura, R. J., and Drewry, J. W.: Pacific Exploratory Mission-West (PEM-West A): September-October 1991, J. Geophys. Res., 101(D1), 1641–1654, 1996.

Hoell, J. M., Davis, D. D., Liu, S. C., Newell, R. E., Akimoto, H., McNeal, R. J., and Bendura, R. J.: The Pacific Exploratory Mission-West Phase B: February-March, 1994, J. Geophys. Res., 102(D23), 28 223–28 240, 1997.

Holton, J. R., Haynes, P. H., McIntyre, M. E., Douglass, A. R., Rood, R. B., and Pfister, L.: Stratosphere-troposphere exchange, Rev. Geophys., 33, 403–439, 1995.

Jacob, D. J., Crawford, J. H., Kleb, M. M., Connors, V. S., Bendura, R. J., Raper, J. L., Sachse, G. W., Gille, J. C., Emmons, L., and Heald, C. L.: Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission: Design, execution, and first results, J. Geophys. Res., 108(D20), 9000, doi:10.1029/2002JD003276, 2003.

Jaffe, D., Prestbo, E., Swartzendruber, P., Weiss-Penzias, P., Kato, S., Takami, A., Hatakeyama, S. and Kajii, Y.: Export of atmospheric mercury from Asia, Atmos. Environ., 39, 3029–3038, 2005.

Kim, K.-H., Ebinghaus, R., Schroeder, W. H., Blanchard, P., Kock, H. H., Steffen, A., Froude, F. A., Kim, M.-Y., Hong, S., and Kim, J.-H.: Atmospheric mercury concentrations from several observatory sites in the northern hemisphere, J. Atmos. Chem., 50, 1–24, 2005.

Knipping, E. M., Lakin, M. J., Foster, K. L., Jungwirth, P., Tobias, D. J., Gerber, R. B., Dabdub, D., and Finlayson-Pitts, B. J.: Experiments and simulations of ion-enhanced interfacial chemistry on aqueous NaCl aerosols, Science, 288, 301–306, 2000.

Lamborg, C. H., Fitzgerald, W. F., Damman, A. W. H., Benoit, J. M., Balcom, P. H., and Engstrom, D. R.: Modern and historic atmospheric mercury fluxes in both hemispheres: Global and regional mercury cycling implications, Global Biogeochem. Cycles, 16(4), 1104, doi:10.1029/2001GB001847, 2002.

Laurier, F. J. G., Mason, R. P., Whalin, L., and Kato, S.: Reactive gaseous mercury formation in the North Pacific Ocean's marine boundary layer: A potential role of halogen chemistry, J. Geophys. Res., 108(D17), 4529, doi:10.1029/2003JD003625, 2003.

Mao, H. and Talbot, R.: Role of meteorological processes in two New England ozone episodes during summer 2001, J. Geophys. Res., 109, D20305, doi:10.1029/2004JD004850, 2004.

Mao, H., Talbot, R., Sigler, J., Sive, B., and Hegarty, J.: Seasonal and diurnal variations of Hg° over New England, Atmos. Chem. Phys. Discuss., in press, 2007.

Mason, R. P. and Sheu, G.-R.: Role of the ocean in the global mercury cycle, Global Bio. Cycles, 16(4), 1093, doi:10.1029/2001GB001440, 2002.

McNeal, R. J., Jacob, D. J., Davis, D. D., and Liu, S. C.: NASA Global Tropospheric Experiment, IGACtivities Newsletter, No. 13, NOAA Pacific Marine Environmental Laboratory, Seattle, Washington, available at: http://www.igac.noaa.gov/newsletter/highlights/1998/gte.php, 1998.

Oum, K. W., Lakin, M. J., DeHaan, D. O., Brauers, T., and Finlayson-Pitts, B. J.: Formation of molecular chlorine from the photolysis of ozone and aqueous sea-salt particles, Science, 279, 74–77, 1998.

Pacyna, E. G. and Pacyna, J. M.: Global emission of mercury from anthropogenic sources in 1995, Water, Air, and Soil Pollution, 137, 149–165, 2002.

Radke, L. F., Friedli, H. R., and Heikes, B. G.: Atmospheric mercury over the NE Pacific during ITCT2K2: Gradients, residence time, stratosphere-troposphere exchange, and long-range transport, J. Geophys. Res., 112, D19305, doi:10.1029/2005JD005828, 2007.

Russo, R. S., Talbot, R. W., Dibb, J. E., Scheuer, E., Seid, G., Jordan, C. E., Fuelberg, H. E., Sachse, G. W., Avery, M. A., Vay, S. A., Blake, D. R., Blake, N. J., Atlas, E., Fried, A., Sandholm, S. T., Tan, D., Singh, H. B., Snow, J., and Heikes, B. G.: Chemical composition of Asian continental outflow over the western Pacific: Results from Transport and Chemical Evolution over the Pacific (TRACE-P), J. Geophys. Res., 108(D20), 8804, doi:10.1029/2002JD003184, 2003.

Schroeder, W. H. and Munthe, J.: Atmospheric mercury - an overview, Atmos. Environ., 5, 809–822, 1998.

Seigneur, C., Vijayaraghavan, K., Lohman, K., Karamchandani, P., and Scott, C.: Global source attribution for mercury deposition in the United States, Environ. Sci. Technol. 38, 555–569, 2004.

Seigneur, C., Vijayaraghavan, K., and Lohman, K.,: Atmospheric mercury chemistry: Sensitivity of global model simulations to chemical reactions, J. Geophys. Res., 111, D22306, doi:10.1029/2005JD006780, 2006.

Selin, N. E., Jacob, D. J., Park, R. J., Yantosca, R. M., Strode, S., Jaeglé, L., and Jaffe, D.: Chemical cycling and deposition of atmospheric mercury: Global constraints from observations, J. Geophys. Res., 112, D02308, doi:10.1029/2006JD007450, 2007.

Seo, K.-H. and Bowman, K. P.: A climatology of isentropic cross-tropopause exchange, J. Geophys. Res., 106, 28 159–28 172, 2001.

Sigler, J. M. and Lee, X.: Gaseous mercury in background forest soil in the northeastern United States, J. Geophys. Res., 111, G02007, doi:10.1029/2005JG000106, 2006.

Sigler, J. M., Lee, X., and Munger, W.: Emission and long-range transport of gaseous mercury from a large-scale Canadian boreal forest fire, Environ. Sci. Technol., 37, 4343–4347, 2003.

Slemr, F., Brunke, E.-G., Ebinghaus, R., Temme, C., Munthe, J., Wängberg, I., Schroeder, W., Steffen, A., and Berg, T.: Worldwide trend of atmospheric mercury since 1977, Geophys. Res. Lett., 30(10), 1516, doi:10.1029/2003GL016954, 2003.

Slemr, F. and Scheel, H. E.: Trends in atmospheric mercury concentrations at the summit of the Wank Mountain, Southern Germany, Atmos. Environ., 32(5), 845–853, 1998.

Streets, D. G., Hao, J., Wu, Y., Jiang, J., Chan, M., Tian, H., and Feng, X.: Anthropogenic mercury emissions in China, Atmos. Environ., 39, 7789–7806, 2005.

Streets, D. G., Tsai, N. Y., Akimoto, H., and Oka, K.: Trends in emissions of acidifying species in Asia, 1985–1997, Water, Air, Soil Pollut., 130, 187–192, doi:10.1023/A:1013883628877, 2001.

Strode, S. A., Jaegle, L. , Selin, N. E., Jacob, D. J., Park, R. J., Yantosca, R. M., Mason, R. P., and Slemr, F.: Air-sea exchange in the global mercury cycle, Global Biogeochem. Cycles, 21, GB1017, doi:10.1029/2006GB002766, 2007.

Talbot, R. W., Dibb, J. E., Lefer, B. L., Scheuer, E., Bradshaw, J. D., Sandholm, S. T., Smyth, S., Blake, D. R., Blake, N. J., Sachse, G. W., Collins, Jr., J. E., and Gregory, G. L.: Large scale distributions of tropospheric nitric, formic, and acetic acids over the western Pacific basin during wintertime, J. Geophys. Res., 102, 28 303–28 313, 1997a.

Talbot, R. W., et al.: Chemical characteristics of continental outflow from Asia to the troposphere over the western Pacific Ocean during February-March 1994: Results from PEM-West B, J. Geophys. Res., 102, 28 255–28 274, 1997b.

Talbot, R. W., Dibb, J. E., Scheuer, E. M., Kondo, Y., Koike, M., Singh, H. B., Salas, L. B., Fukui, Y., Ballentine, J. O., Meads, R. F., Miller, T. M., Hunton, D. E., Viggiano, A. A., Blake, D. R., Blake, N. J., Atlas, E., Flocke, F., Jacob, D. J., and Jaegle, L.: Reactive nitrogen budget during the NASA SONEX mission, Geophys. Res. Lett., 26, 3057–3060, 1999.

Talbot, R., Mao, H., Scheuer, E., Dibb, J., and Avery, M.: Total depletion of Hg° in the upper troposphere-lower stratosphere, Geophys. Res. Lett., in press, 2007.

Weiss-Penzias, P., Jaffe, D. A., Swartzendruber, P., Dennison, J. B., Chand, D., Hafner, W., and Prestbo, E.: Observations of Asian air pollution in the free troposphere at Mount Bachelor Observatory during the spring of 2004, J. Geophys. Res., 111, D10304, doi:10.1029/2005JD006522, 2006.

Weiss-Penzias, P., Jaffe, D., Swartzendruber, P., Hafner, W., Chand, D., and Prestbo, E.: Quantifying Asian and biomass burning sources of mercury using the Hg/CO ratio in pollution plumes observed at the Mount Bachelor observatory, Atmos. Environ., 41, 4366–4379, 2007.