<?xml version="1.0" encoding="utf-8" standalone="no"?>
<!DOCTYPE article SYSTEM "http://www.atmos-chem-phys-discuss.net/inc/acpd/copernicus.dtd">
<article language="en">
	<journal>
		<journal_title>Atmospheric Chemistry and Physics Discussions</journal_title>
		<journal_url>www.atmos-chem-phys-discuss.net</journal_url>
		<issn>1680-7367</issn>
		<eissn>1680-7375</eissn>
		<volume_number>8</volume_number>
		<issue_number>5</issue_number>
		<publication_year>2008</publication_year>
	</journal>
	<doi>10.5194/acpd-8-18651-2008</doi>
	<article_url>http://www.atmos-chem-phys-discuss.net/8/18651/2008/</article_url>
	<abstract_html>http://www.atmos-chem-phys-discuss.net/8/18651/2008/acpd-8-18651-2008.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys-discuss.net/8/18651/2008/acpd-8-18651-2008.pdf</fulltext_pdf>
	<start_page>18651</start_page>
	<end_page>18688</end_page>
	<publication_date>2008-10-29</publication_date>
	<article_title content_type="html">Gaseous mercury distribution in the upper troposphere and lower stratosphere observed onboard the CARIBIC passenger aircraft</article_title>
	<authors>
		<author numeration="1" affiliations="1">
			<name>F. Slemr</name>
			<email>slemr@mpch-mainz.mpg.de</email>
		</author>
		<author numeration="2" affiliations="2">
			<name>R. Ebinghaus</name>
		</author>
		<author numeration="3" affiliations="1">
			<name>C. A. M. Brenninkmeijer</name>
		</author>
		<author numeration="4" affiliations="3">
			<name>M. Hermann</name>
		</author>
		<author numeration="5" affiliations="2">
			<name>H. H. Kock</name>
		</author>
		<author numeration="6" affiliations="4">
			<name>B. G. Martinsson</name>
		</author>
		<author numeration="7" affiliations="1">
			<name>T. Schuck</name>
		</author>
		<author numeration="8" affiliations="5">
			<name>D. Sprung</name>
		</author>
		<author numeration="9" affiliations="6">
			<name>P. van Velthoven</name>
		</author>
		<author numeration="10" affiliations="5">
			<name>A. Zahn</name>
		</author>
		<author numeration="11" affiliations="7">
			<name>H. Ziereis</name>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">Max-Planck-Institut fÃ¼r Chemie (MPI), Air Chemistry Division, Joh.-J.-Becherweg 27, 55128 Mainz, Germany</affiliation>
		<affiliation numeration="2" content_type="html">GKSS-Research Centre, Institute for Coastal Research (GKSS), Max-Planck-Str. 1, 21502 Geesthacht, Germany</affiliation>
		<affiliation numeration="3" content_type="html">Leibniz-Institut fÃ¼r TroposphÃ¤renforschung (IFT), Permoserstr. 15, 04318 Leipzig, Germany</affiliation>
		<affiliation numeration="4" content_type="html">University of Lund, Division of Nuclear Physics, P.O. Box 118, 22100 Lund, Sweden</affiliation>
		<affiliation numeration="5" content_type="html">Institute for Meteorology and Climate Research (IMK), Forschungszentrum Karlsruhe, Weberstr. 5, 76133 Karlsruhe, Germany</affiliation>
		<affiliation numeration="6" content_type="html">Royal Netherlands Meteorological Institute (KNMI), P.O.Box 201, 3730 AE, de Bilt, The Netherlands</affiliation>
		<affiliation numeration="7" content_type="html">Deutsches Zentrum fÃ¼r Luft- und Raumfahrt (DLR), Institut fÃ¼r Physik der AtmosphÃ¤re, 82230 Wessling, Germany</affiliation>
	</affiliations>
	<abstract content_type="html">Total gaseous mercury (TGM) was measured onboard a passenger aircraft during
monthly CARIBIC flights (&lt;b&gt;C&lt;/b&gt;ivil &lt;b&gt;A&lt;/b&gt;ircraft for &lt;b&gt;R&lt;/b&gt;egular &lt;b&gt;I&lt;/b&gt;nvestigation of the
Atmosphere &lt;b&gt;B&lt;/b&gt;ased on an &lt;b&gt;I&lt;/b&gt;nstrumented &lt;b&gt;C&lt;/b&gt;ontainer) made between May 2005 and March
2007 on the routes Frankfurt-SÃ£o Paulo-Santiago de Chile and back
(seven times four flights) and Frankfurt-Guangzhou-Manila and back
(twelve times four flights). The data provide for the first time an insight
into the seasonal distributions of TGM in the upper troposphere and lower
stratosphere (UT/LS) of both hemispheres and demonstrate the importance of
mercury emissions from biomass burning in the Southern Hemisphere. Numerous
plumes were observed in the upper troposphere, the larger of which could be
characterized in terms of Hg/CO emission ratios and their probable origins.
During the flights to China TGM correlated with CO in the upper troposphere
with a seasonally dependent slope reflecting the longer lifetime of
elemental mercury when compared to that of CO. A pronounced depletion of TGM
was always observed in the extratropical lowermost stratosphere. TGM
concentrations there were found to decrease with the increasing
concentrations of particles. Combined with the large concentrations of
particle bond mercury in the stratosphere observed by others, this finding
suggests either a direct conversion of TGM to particle bound mercury or an
indirect conversion via a semivolatile bivalent mercury compound. Based on
concurrent measurements of SF&lt;sub&gt;6&lt;/sub&gt; during two flights, the rate of this
conversion is estimated to 0.4 ng m&lt;sup&gt;&amp;minus;3&lt;/sup&gt; yr&lt;sup&gt;&amp;minus;1&lt;/sup&gt;. A zero TGM
concentration was not observed during some 200 flight hours in the lowermost
stratosphere suggesting an equilibrium between the gaseous and particulate
mercury.</abstract>
	<references>
		<reference numeration="1" content_type="text"> Banic, C M., Beauchamp, S T., Tordon, R J., Schroeder, W H., Steffen, A., Anlauf, K A., and Wong, K H T.: Vertical distribution of gaseous elemental mercury in Canada, J. Geophys. Res., 108(D9), 4264, doi:10.1029/2002JD002116, 2003. </reference>
		<reference numeration="2" content_type="text"> Baron, P A. and Willeke K.: Aerosol Measurements: Principles Techniques and Applications, John Wiley and Sons, New York, 1131 pp., 2001. </reference>
		<reference numeration="3" content_type="text"> Brenninkmeijer, C A M., Crutzen, P., Boumard, F., Dauer, T., Dix, B., Ebinghaus, R., Filippi, D., Fischer, H., Franke, H., FrieÃŸ, U., Heintzenberg, J., Helleis, F., Hermann, M., Kock, H H., Koeppel, C., Lelieveld, J., Leuenberger, M., Martinsson, B G., Miemczyk, S., Moret, H P., Nguyen, H N., Nyfeler, P., Oram, D., O&apos;Sullivan, D., Penkett, S., Platt, U., Pupek, M., Ramonet, M., Randa, B., Reichelt, M., Rhee, T S., Rohwer, J., Rosenfeld, K., Scharffe, D., Schlager, H., Schumann, U., Slemr, F., Sprung, D., Stock, P., Thaler, R., Valentino, F., van~Velthoven, P., Waibel, A., Wandel, A., Waschitschek, K., Wiedensohler, A., Xueref-Remy, I., Zahn, A., Zech, U., and Ziereis, H.: Civil Aircraft for the regular investigation of the atmosphere based on an instrumented container: The new CARIBIC system, Atmos. Chem. Phys., 7, 4953â€“4976, 2007. </reference>
		<reference numeration="4" content_type="text"> Cantrell, C A.: Technical Note: Review of methods for linear least-squares fitting of data and application to atmospheric chemistry problems, Atmos. Chem. Phys., 8, 5477â€“5487, 2008. </reference>
		<reference numeration="5" content_type="text"> Ebinghaus, R. and Slemr, F.: Aircraft measurements of atmospheric mercury over southern and eastern Germany, Atmos. Environ., 34, 895â€“903, 2000. </reference>
		<reference numeration="6" content_type="text"> Ebinghaus, R., Kock, H H., Coggins, A M., Spain, T G., Jennings, S G., and Temme, C.: Long-term measurements of atmospheric mercury at Mace Head, Irish west coast, between 1995 and 2001, Atmos. Environ. 36, 5267â€“5276, 2002. </reference>
		<reference numeration="7" content_type="text"> Ebinghaus, R., Slemr, F., Brenninkmeijer, C A M., van~Velthoven, P., Zahn, A., Hermann, M., O&apos;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. </reference>
		<reference numeration="8" content_type="text"> 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, 253â€“267, 2003a. </reference>
		<reference numeration="9" content_type="text"> 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. Cy., 17, 1039, doi:10.1029/2002GB001972, 2003b. </reference>
		<reference numeration="10" content_type="text"> Friedli, H R., Radke, L F., Prescott, R., Li, P., Wo, 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. </reference>
		<reference numeration="11" content_type="text"> Gloor, M., Dlugokencky, E., Brenninkmeijer, C., Horowitz, L., Hurst, D F., Dutton, G., Crevoisier, C., Machida, T., and Tans, P.: Three-dimensional SF$_6$ data and tropospheric transport simulations: Signals, modeling accuracy, and implications for inverse modeling, J. Geophys. Res., 112, D15112, doi:10.1029/2006JD007973, 2007. </reference>
		<reference numeration="12" content_type="text"> Holmes, C D., Jacob, D J., and Yang, X.: Global lifetime of elemental mercury against oxidation by atomic bromine in the free troposphere, Geophys. Res. Lett., 33, L20808, doi:10.1029/2006GL027176, 2006. </reference>
		<reference numeration="13" content_type="text"> 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, 3029â€“3038, 2005. </reference>
		<reference numeration="14" content_type="text"> Kellerhals, M., Beauchamp, S., Balzer, W., Blanchard, P., Froude, F., Harvey, B., McDonald, K., Pilote, M., Poissant, L., Puckett, K., Schroeder, B., Steffen, A., and Tordon, R.: Temporal and spatial variability of total gaseous mercury in Canada: results from the Canadian Atmospheric Mercury Measurement Network (CAMNet), Atmos. Environ. 37, 1003â€“1011, 2003. </reference>
		<reference numeration="15" content_type="text"> Landis, M S., Stevens, R K., Schaedlich, F., and Prestbo, E M.: Development and chracterization of an annular denuder methodology for the measurement of divalent inorganic reactive gaseous mercury in ambient air, Environ. Sci. Technol., 36, 3000â€“3009, 2002. </reference>
		<reference numeration="16" content_type="text"> Lin, C.-J., Pongprueksa, P., Lindberg, S E., Pehkonen, S O., Byun, D., and Jang, C.: Scientific uncertainties in atmospheric mercury models. I. Model science evaluation, Atmos. Environ, 40, 2911â€“2928, 2006. </reference>
		<reference numeration="17" content_type="text"> Lindberg, S E., Turner, R R., Meyers, T P., Taylor Jr., G E., and Schroeder, W H.: Atmospheric concentrations and deposition of Hg to a deciduous forest at Walker Branch watershed, Tennessee, USA, Water Air Soil Poll. 56, 577â€“594, 1991. </reference>
		<reference numeration="18" content_type="text"> Lindberg, S., Bullock, R., Ebinghaus, R., Engstrom, D., Feng, X., Fitzgerald, W., Pirrone, N., Prestbo, E., and Seigneur, C.: A synthesis of progress and uncertainties in attributiin the sources of mercury in deposition, Ambio, 36, 19â€“32, 2007. </reference>
		<reference numeration="19" content_type="text"> Maiss, M., Steele, L P., Francey, R J., Fraser, P J., Langenfelds, R L., Trivett, N B A., and Levin, I.: Sulfur hexafluoride â€“ a powerful new atmospheric tracer, Atmos. Environ. 30, 1621â€“1629, 1996. </reference>
		<reference numeration="20" content_type="text"> Martinsson, B G.: An external beam PIXE/PESA setup for characterization of fine aerosols, Nucl. Instrum. Methods, B22, 356â€“363, 1987. </reference>
		<reference numeration="21" content_type="text"> Mergler, D., Anderson, H A., Chan, L H M., Mahaffey, K R., Murray, M., Sakamoto, M., and Stern, A H.: Methyl mercury exposure and Health effects in humans: A worldwide concern, Ambio, 36, 3â€“11, 2007. </reference>
		<reference numeration="22" content_type="text"> Munthe, J., WÃ¤ngberg, I., Pirrone, N., Iverfeldt, A., Ferrara, R., Ebinghaus, R., Feng, X., Gardfeldt, K., Keeler, G., Lanzillotta, E., Lindberg, S E., Lu, J., Mamane, Y., Prestbo, E., Schmolke, S., Schroeder, W H., Sommar, J., Sprovieri, F., Szevens, R K., Stratton, W., Tuncel, G., and Urba, A.: Intercomparison of methods for sampling and analysis of atmospheric mercury species, Atmos. Environ, 35, 3007â€“3017, 2001. </reference>
		<reference numeration="23" content_type="text"> Murphy, D M., Thomson, D S., and Mahoney, M J.: In situ measurements of organics, meteoritic material, mercury, and other elements in aerosols at 5 to 19 kilometers, Science, 282, 1664â€“1669, 1998. </reference>
		<reference numeration="24" content_type="text"> Murphy, D M., Hudson, P K., Thomson, D S., Sheridan, P J., and Wilson, J C.: Observations of mercury-containing aerosols, Environ. Sci. Technol., 40, 3163â€“3167, 2006. </reference>
		<reference numeration="25" content_type="text"> Pan, L L., Randel, W J., Gary, B L., Mahoney, M J., and Hintsa, E J.: Definitions and sharpness of the extratropical tropopause: A trace gas perspective, J. Geophys. Res., 109, D23103, doi:10.1029/2004JD004982, 2004. </reference>
		<reference numeration="26" content_type="text"> Prestbo, E M. and Bloom, N S.: Mercury speciation absorption (MESA) method for combustion flue gas: methodology, artifacts, intercomparisons, and atmospheric implications, Water Air Soil Poll., 80, 145â€“158, 1995. </reference>
		<reference numeration="27" content_type="text"> Radke, L F., Friedli, H R., and Heikes, B G.: Atmospheric mercury over the NE Pacific during spring 2002: Gradients, residence time, upper troposphere lower stratosphere loss, and long-range transport, J. Geophys. Res., 112, D19305, doi:10.1029/2005JD005828, 2007. </reference>
		<reference numeration="28" content_type="text"> Scheele, M., Siegmund, P., and Van Velthoven, P.: Sensitivity of trajectories to data resolution and its dependence on the starting point: In or outside a tropopause fold, Meteorol. Appl., 3, 267â€“273, 1996. </reference>
		<reference numeration="29" content_type="text"> Scheuhammer; A M., Meyer, M W., Sandheinrich, M B., and Murray, M W.: Effects of environmental methylmercury on the health of wild bird, mammals, and fish, Ambio, 36, 12â€“18, 2007. </reference>
		<reference numeration="30" content_type="text"> Schroeder, W H. and Munthe, J.: Atmospheric mercury â€“ an overview, Atmos. Environ., 32, 809â€“822, 1998. </reference>
		<reference numeration="31" content_type="text"> Selin, N E., Jacob, D J., Park, R J., Yantosca, R M., Strode, S., JaeglÃ©, 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. </reference>
		<reference numeration="32" content_type="text"> Slemr, F., Schuster, G., and Seiler, W.: Distribution, speciation, and budget of atmospheric mercury, J. Atmos. Chem., 3, 407â€“434, 1985. </reference>
		<reference numeration="33" content_type="text"> Slemr, F. and Scheel, H E.: Trends in atmospheric concentrations at the summit of the Wank Mountain, Southern Germany, Atmos. Environ. 32, 845â€“853, 1998. </reference>
		<reference numeration="34" content_type="text"> Slemr, F., Ebinghaus, R., Simmonds, P G., and Jennings S G.: European emissions of mercury derived from long-term observations at Mace Head, on the western Irish coast, Atmos. Environ., 40, 6966â€“6974, 2006. Slemr, F., Brunke, E.-G., Labuschagne, C., and Ebinghaus, R.: Total gaseous mecrury concentrations at the Cape Point GAW station and their seasonality, Geophys. Res. Lett., 35, L11807, doi:10.1029/2008GL033741, 2008. </reference>
		<reference numeration="35" content_type="text"> Stiller, G P., von~Clarmann, T., HÃ¶pfner, M., Glatthor, N., Grabowski, U., Kellmann, S., Kleinert, A., Linden, A., Milz, M., Reddmann, T., Steck, T., Fischer, H., Funke, B., López-Puertas, M., and Engel, A.: Global distribution of mean age of stratospheric air from MIPAS SF$_6$ measurements, Atmos. Chem. Phys., 8, 677â€“695, 2008. </reference>
		<reference numeration="36" content_type="text"> Strobel, H A.: Chemical Instrumentation, Addison-Wesley Publ. Co., London, pp. 427, 1973. </reference>
		<reference numeration="37" content_type="text"> Strode, S A., JaeglÃ©, L., Jaffe, D A., Swartzendruber, P C., Selin, N E., Holmes, C., and Yantosca, R M.: Trans-Pacific transport of mercury, J. Geophys. Res., 113, D15305, doi:10.1029/JD009428, 2008. </reference>
		<reference numeration="38" content_type="text"> Swartzendruber, P C., Jaffe, D A., Prestbo, E M., Weiss-Penzias, P., Selin, N E., Park, R., Jacob, D J., Strode, S., and JaeglÃ©, L.: Observations of resctive gaseous mercury in the free troposphere at the Mount Bachelor Observatory, J. Geophys. Res., 111, D24301, doi:10.1029/2006JD007415, 2006. </reference>
		<reference numeration="39" content_type="text"> Swartzendruber, P C., Chand, D., Jaffe, D A., Smith, J., Reidmiller, D., Gratz, L., Keeler, J., Strode, S., JaeglÃ©, L., and Talbot, R.: Vertical distribution of mercury, CO, ozone, and aerosol scattering coefficient in the Pacific Northwest during the spring 2006 INTEX-B campaign, J. Geophys. Res., 113, D10305, doi:10.1029/2007JD009579, 2008. </reference>
		<reference numeration="40" content_type="text"> Talbot, R., Mao, H., Scheuer, E., Dibb, J., and Avery, M.: Total depletion of Hg$^0$ in the upper troposphere â€“ lower stratosphere, Geophys. Res. Lett., 34, L23804, doi:10.1029/2007GL031366, 2007a. </reference>
		<reference numeration="41" content_type="text"> Talbot, R., Mao, H., Scheuer, E., Dibb, J., Avery, M., Browell, E., Sachse, G., Vay, S., Blake, D., Huey, G., and Fuelberg, H.: Factors influencing the large-scale distribution of Hg&amp;deg; in the Mexico City area and over the North Pacific, Atmos. Chem. Phys., 8, 2103â€“2114, 2008. </reference>
		<reference numeration="42" content_type="text"> Temme, C., Einax, J W., Ebinghaus, R., and Schroeder, W H.: Measurements of atmospheric mercury species at a coastal site in the Antarctic and over the South Atlantic Ocean during polar summer, Environ. Sci. Technol., 37, 22â€“31, 2003a. </reference>
		<reference numeration="43" content_type="text"> Temme, C., Slemr, F., Ebinghaus, R., and Einax, J W.: Distribution of mercury over the Atlantic Ocean in 1996 and 1999â€“2001, Atmos. Environ., 37, 1889â€“1897, 2003b. </reference>
		<reference numeration="44" content_type="text"> Weiss-Penzias, P., Jaffe, D., Swartzendruber, P., Hafner, W., and Chand, D.: 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, 4366â€“4379, 2007. </reference>
		<reference numeration="45" content_type="text"> York, D.: Least-square fitting of a straight line, Can. J. Phys., 44, 1079â€“1086, 1966. </reference>
		<reference numeration="46" content_type="text"> Zahn, A., Brenninkmeijer, C A M., Asman, W A H., Crutzen, P J., Heinrich, G., Fischer, H., Cuijpers, J W M., and van Velthoven, P F J.: Budgets of O&lt;sub&gt;3&lt;/sub&gt; and CO in the upper troposphere: CARIBIC passenger aircraft results 1997â€“2001, J. Geophys. Res., 107(D17), 4337, doi:10.1029/2001JD001529, 2002. </reference>
	</references>
</article>

