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<article language="en">
	<journal>
		<journal_title>Atmospheric Chemistry and Physics</journal_title>
		<journal_url>www.atmos-chem-phys.net</journal_url>
		<issn>1680-7316</issn>
		<eissn>1680-7324</eissn>
		<volume_number>6</volume_number>
		<issue_number>12</issue_number>
		<publication_year>2006</publication_year>
	</journal>
	<doi>10.5194/acp-6-5381-2006</doi>
	<article_url>http://www.atmos-chem-phys.net/6/5381/2006/</article_url>
	<abstract_html>http://www.atmos-chem-phys.net/6/5381/2006/acp-6-5381-2006.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys.net/6/5381/2006/acp-6-5381-2006.pdf</fulltext_pdf>
	<start_page>5381</start_page>
	<end_page>5390</end_page>
	<publication_date>2006-11-29</publication_date>
	<article_title content_type="html">Radiocarbon analysis in an Alpine ice core: record of anthropogenic and biogenic contributions to carbonaceous aerosols in the past (1650&amp;ndash;1940)</article_title>
	<authors>
		<author numeration="1" affiliations="1,2">
			<name>T. M. Jenk</name>
		</author>
		<author numeration="2" affiliations="1,2">
			<name>S. Szidat</name>
		</author>
		<author numeration="3" affiliations="2">
			<name>M. Schwikowski</name>
			<email>margit.schwikowski@psi.ch</email>
		</author>
		<author numeration="4" affiliations="1,2">
			<name>H. W. Gäggeler</name>
		</author>
		<author numeration="5" affiliations="2">
			<name>S. Brütsch</name>
		</author>
		<author numeration="6" affiliations="3">
			<name>L. Wacker</name>
		</author>
		<author numeration="7" affiliations="4">
			<name>H.-A. Synal</name>
		</author>
		<author numeration="8" affiliations="2">
			<name>M. Saurer</name>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">Department of Chemistry and Biochemistry, University of Bern, Bern, Switzerland</affiliation>
		<affiliation numeration="2" content_type="html">Paul Scherrer Institut, Villigen PSI, Switzerland</affiliation>
		<affiliation numeration="3" content_type="html">Institute for Particle Physics, ETH Hönggerberg, Zürich, Switzerland</affiliation>
		<affiliation numeration="4" content_type="html">Paul Scherrer Institut, c/o Institute for Particle Physics, ETH Hönggerberg, Zürich, Switzerland</affiliation>
	</affiliations>
	<abstract content_type="html">Long-term concentration records of carbonaceous particles (CP) are of
increasing interest in climate research due to their not yet completely
understood effects on climate. Nevertheless, only poor data on their
concentrations and sources before the 20th century are available. We
present a first long-term record of organic carbon (OC) and elemental carbon
(EC) concentrations &amp;ndash; the two main fractions of CP &amp;ndash; along with the
corresponding fraction of modern carbon (f&lt;sub&gt;M&lt;/sub&gt;) derived from radiocarbon
(&lt;sup&gt;14&lt;/sup&gt;C) analysis in ice. This allows a distinction and quantification of
natural (biogenic) and anthropogenic (fossil) sources in the past. CP were
extracted from an ice archive, with resulting carbon quantities in the
microgram range. Analysis of &lt;sup&gt;14&lt;/sup&gt;C by accelerator mass spectrometry (AMS)
was therefore highly demanding. We analysed 33 samples of 0.4 to 1 kg ice
from a 150.5 m long ice core retrieved at Fiescherhorn glacier in December
2002 (46&amp;deg;33&apos;3.2&quot; N, 08&amp;deg;04&apos;0.4&quot; E; 3900 m a.s.l.). Samples were taken
from bedrock up to the firn/ice transition, covering the time period
1650&amp;ndash;1940 and thus the transition from the pre-industrial to the industrial
era. Before ~1850, OC was approaching a purely biogenic origin with a
mean concentration of 24 μg kg&lt;sup&gt;&amp;minus;1&lt;/sup&gt; and a standard deviation of 7 μg kg&lt;sup&gt;&amp;minus;1&lt;/sup&gt;.
In 1940, OC concentration was about a factor of 3 higher
than this biogenic background, almost half of it originating from
anthropogenic sources, i.e. from combustion of fossil fuels. The biogenic EC
concentration was nearly constant over the examined time period with 6 μg kg&lt;sup&gt;&amp;minus;1&lt;/sup&gt;
and a standard deviation of 1 μg kg&lt;sup&gt;&amp;minus;1&lt;/sup&gt;. In 1940, the
additional anthropogenic input of atmospheric EC was about 50 μg kg&lt;sup&gt;&amp;minus;1&lt;/sup&gt;.</abstract>
	<references>
		<reference numeration="1" content_type="text"> Baltensperger, U., Schwikowski, M., Jost, D. T., Gäggeler, H. W., and Poulida, O.: Scavenging of atmospheric constituents in mixed phase clouds at the high-alpine site Jungfraujoch; Part I: Basic concept and cloud scavenging, Atmos. Environ., 32, 3975&amp;ndash;3983, 1998. </reference>
		<reference numeration="2" content_type="text"> Bazhev, A. M., Rototaeva, O., Heintzenberg, J., Stenberg, M., and Pinglot, J. F.: Phyiscal and chemical studies in the region of the southern slope of Mount Elbrus, Caucasus, J. Glaciol., 44, 214&amp;ndash;222, 1998. </reference>
		<reference numeration="3" content_type="text"> Boutton, T. W.: Stable carbon isotope ratios of natural materials: II. Atmospheric, terrestrial, marine and freshwater environments, in: Carbon Isotope Techniques, edited by: Coleman, D. C. and Fry, B., San Diego, Academic Press, 173&amp;ndash;185, 1991. </reference>
		<reference numeration="4" content_type="text"> Brimblecombe, P.: The Big Smoke, Methunen, London, 1987. </reference>
		<reference numeration="5" content_type="text"> Cachier, H. and Pertuisot, M. H.: Particulate carbon in Arctic ice, Analysis Magazine, 22, 34&amp;ndash;37, 1994. </reference>
		<reference numeration="6" content_type="text"> Chylek, P. and Coakley Jr., A.: Aerosols and climate, Science, 183, 75&amp;ndash;77, 1974. </reference>
		<reference numeration="7" content_type="text"> Chylek, P., Johnson, B., and Wu, H.: Black carbon concentration in a Greenland DYE-3 ice core, Geophys. Res. Lett., 19, 1951&amp;ndash;1953, 1992. </reference>
		<reference numeration="8" content_type="text"> Chylek, P., Johnson, B., Damiano, P. A., Taylor, K. C., and Clement, P.: Biomass burning record and black carbon in the GISP2 ice core, Geophys. Res. Lett., 22, 89&amp;ndash;92, 1995. </reference>
		<reference numeration="9" content_type="text"> Clarke, A. D. and Noone, K. J.: Soot in the arctic snowpack: A cause for perturbations in radiative transfer, Atmos. Environ., 19, 2045&amp;ndash;2053, 1985. </reference>
		<reference numeration="10" content_type="text"> Crutzen, P. J. and Ramanathan, V.: The parasol effect on climate, Science, 302, 1679&amp;ndash;1680, 2003. </reference>
		<reference numeration="11" content_type="text"> Currie, L. A.: Evolution and multidisciplinary frontiers of $^14$C aerosol science, Radiocarbon, 42, 115&amp;ndash;126, 2000. </reference>
		<reference numeration="12" content_type="text"> Davidson, I. C., Phalen, R. F., and Solomon, P. A.: Airborne particulate Matter and Human Health: A Review, Aerosol. Sci. Technol., 39, 737&amp;ndash;749, 2005. </reference>
		<reference numeration="13" content_type="text"> Eglinton, T. I., Eglinton, G., Dupont, L., Sholkovitz, E. R., Montlucon, D., and Reddy, C. M.: Composition, age and provenance of organic matter in NW African dust over the Atlantic Ocean, Geochem. Geophys Geosyst., 3(8), 1050, doi:10.1029/2001GC000269, 2002. </reference>
		<reference numeration="14" content_type="text"> Eichler, A., Schwikowski, M., Gäggeler, H.W., Furrer, V., Synal, H.-A., Beer, J., Sauer, M., and Funk, M.: Glaciochemical dating of an ice core from the upper Grenzgletscher (4200 m~a.s.l.), J. Glaciol., 46, 507&amp;ndash;515, 2000. </reference>
		<reference numeration="15" content_type="text"> Groisman, P. Y., Karl, T. R., and Knight, R. W.: Observed impact of snow cover on the heat balance and the rise of continental spring temperatures, Science, 263, 198&amp;ndash;200, 1993. </reference>
		<reference numeration="16" content_type="text"> Hansen, J. E. and Sato, M.: Trends of measured climate forcing agents, PNAS, 98, 14 778&amp;ndash;14 783, 2001. </reference>
		<reference numeration="17" content_type="text"> Hansen, J. and Nazarenko, L.: Soot climate forcing via snow and ice albedos, Proceedings of the National Academy of Sciences, 101(2), 423&amp;ndash;428, 2004. </reference>
		<reference numeration="18" content_type="text"> Haywood, J. M., Roberts, D. L., Slingo, A., Edwards, J. M., and Shine, K. P.: General circulation model calculations of the direct radiative forcing by anthropogenic sulfate and fossil-fuel soot aerosol, J. Climate, 10, 1562&amp;ndash;1577, 1997. </reference>
		<reference numeration="19" content_type="text"> Holdsworth, G., Higuchi, K., Zielinski, G. A., Mayewski, P. A., Wahlen, M., Deck, B., Chylek, P., Johnson, B., and Damiano, P.: Historical biomass burning: Late 19$^th$ century pioneer agriculture revolution in northern hemispheric ice core data and its atmospheric interpretation, J. Geophys. Res., 101, 23 317&amp;ndash;23 334, 1996. </reference>
		<reference numeration="20" content_type="text"> Hua, Q., Zoppi, U., Williams, A., and Smith, A.: Small-mass AMS radiocarbon analysis at ANTARES, Nucl. Instr. Meth. Phys. Res. B, 223, 284&amp;ndash;292, doi:10.1016/j.nimb.2004.04.057, 2003. </reference>
		<reference numeration="21" content_type="text"> Huber, T.: Bestimmung historischer Spurenstoffverläufe in alpinem Firn mittels kontinuierlicher Ionenchromatographischer Analyse, PhD Thesis, University of Bern, 2001. </reference>
		<reference numeration="22" content_type="text"> Intergovernmental Panel on Climate Change (IPCC): Third Assessment Report, Climate Change 2001: The Scientific Basis, edited by: Houghton, J. T., Ding, Y., Griggs, D. J., et al., Cambridge Univ. Press, New York, 2001. </reference>
		<reference numeration="23" content_type="text"> Jacobsen, M. C., Hansson, H.-C., Noone, K. J., and Charlson, R. J.: Organic atmospheric aerosols: review and state of the science, Rev. Geophys., 38(2), 267&amp;ndash;294, 2000. </reference>
		<reference numeration="24" content_type="text"> Jacobson, M. Z.: Control of fossil-fuel particulate carbon and organic matter. Possibly the most effective method of slowing global warming, J. Geophys. Res., 107(D19), 4410&amp;ndash;4431, doi:10.1029/2001JD001376, 2002. </reference>
		<reference numeration="25" content_type="text"> Jacobson, M. Z.: Climate response of fossil fuel and biofuel soot, accounting for soot&apos;s feedback to snow and sea ice albedo and emissivity, J. Geophys. Res., 109, D21201, doi:10.1029/2004JD004945, 2004. </reference>
		<reference numeration="26" content_type="text"> Jenk, T. M., Szidat, S., Schwikowski, M., Gäggeler, H. W., Bolius, D., Wacker, L., Synal, H.-A., and Saurer, M.: Microgram level radiocarbon ($^14$C) determination on carbonaceous particles in ice, Nucl. Instr. Meth. Phys. Res. B, in press, 2006. </reference>
		<reference numeration="27" content_type="text"> Junker, C. and Liousse, C.: A global emission inventory of carbonaceous aerosol from historic records of fossil fuel and biofuel consumption for the period 1860&amp;ndash;1997, Atmos. Chem. Phys. Discuss., 6, 4897&amp;ndash;4927, 2006. </reference>
		<reference numeration="28" content_type="text"> Lavanchy, V. M. H., Gäggeler, H. W., Schotterer, U., Schwikowski, M., and Baltensperger, U.: Historical record of carbonaceous particle concentrations from a European high-alpine glacier (Colle Gnifetti, Switzerland), J. Geophys. Res., 104(D), 21 227&amp;ndash;21 236, 1999a. </reference>
		<reference numeration="29" content_type="text"> Lavanchy, V. M. H., Gäggeler, H. W., Nyeki, S., and Baltensperger, U.: Elemental carbon (EC) and black carbon (BC) measurements with a thermal method and an aethalometer at the high alpine research station Jungfraujoch, Atmos. Environ., 33, 2759&amp;ndash;2769, 1999b. </reference>
		<reference numeration="30" content_type="text"> Lemire, K. R., Allen, D. T., Klouda, G. A., and Lewis, C. W.: Fine particulate matter source attribution for Southeast Texas using $^14$C/$^13$C ratios, J. Geophys. Res., 107, 4613&amp;ndash;4619, 2002. </reference>
		<reference numeration="31" content_type="text"> Levine, J. S., Cofer III, W. S., Sebacher, D. I., Rhinehart, R. P., Winstead, E. L., Sebacher, S., Hinkle, C. R., Schmaltzer, P. A., and Koller Jr, A. M.: The effects of fire on biogenic emissions of methane and nitric oxide from wetlands, J. Geophys. Res., 95, 1853&amp;ndash;1864 1992. </reference>
		<reference numeration="32" content_type="text"> Loh, A. I., Bauer J. E., and Druffel, R. M.: Variable ageing and storage of dissolved organic components in the open ocean, Nature, 430, 877&amp;ndash;881, doi:10.1038/nature02780, 2004. </reference>
		<reference numeration="33" content_type="text"> Novakov, T. and Penner, J. E.: Large contribution of organic aerosols to cloud-condensation-nuclei concentrations, Nature, 365, 823&amp;ndash;826, 1993. </reference>
		<reference numeration="34" content_type="text"> Pataki, D. E., Bowling, D. R., and Ehleringer, J. R.: Seasonal cycle of carbon dioxide and its isotopic composition in an urban atmosphere: Anthropogenic and biogenic effects, J. Geophys. Res., 108(D23), 473&amp;ndash;4742, doi:10.1029/2003JD003865, 2003. </reference>
		<reference numeration="35" content_type="text"> Penner, J. E., Eddlemann, H., and Novakov, T.: Towards the Devlopement of a global Inventory for Black Carbon Emissions, Atmos. Environ., 27A, 1277&amp;ndash;1297, 1993. </reference>
		<reference numeration="36" content_type="text"> Penner, J. E., Charlson, R. J., Hales, J. M., Laulainen, N. S., Leifer, R., Novakov, T., Ogren, J., Radke, L. F., Schwartz, S. E., and Travis, L.: Quantifying and minimizing uncertainty of climate forcing by anthropogenic aerosols, Bull. Am. Meteorol. Soc., 75, 375&amp;ndash;400, 1994. </reference>
		<reference numeration="37" content_type="text"> Petzold, A. and Niessner, R.: Method comparison study on soot-selective techniques, Mikrochim. Acta, 117, 215&amp;ndash;237, 1995. </reference>
		<reference numeration="38" content_type="text"> Pfister, C.: Geschichte des Kantons Bern seit 1798, Bd. IV, Im Strom der Modernisierung. Bevölkerung, Wirtschaft und Umwelt 1700&amp;ndash;1914, Historischer Verein, Bern, 1995. </reference>
		<reference numeration="39" content_type="text"> Reddy, C. M., Pearson, A., Xu, L., McNichol, A. P., Benner Jr., B. A., Wise, S. A., Klouda, G. A., Currie, L. A., and Eglinton, T. I.: Radiocarbon as a tool to apportion the sources of polycyclic aromatic hydrocarbons and black carbon in environmental samples, Environ. Sci. Technol., 36, 1774&amp;ndash;1782, 2002. </reference>
		<reference numeration="40" content_type="text"> Reimer, P. J., Baillie, M. G. L., Bard, E., Bayliss, A., Beck, J. W., Bertrand, C., Blackwell, P. G., Buck, C. E., Burr, G., Cutler, K. B., Damon, P. E., Edwards, R. L., Fairbanks, R. G., Friedrich, M., Guilderson, T. P., Hughen, K. A., Kromer, B., McCormac, F. G., Manning, S., Bronk-Ramsey, C., van der Plicht, J., and Weyhenmeyer, C. E.: IntCal04 terrestrial radiocarbon age calibraion, 0&amp;ndash;26 cal kyr BP, Radiocarbon, 46, 1029&amp;ndash;1058, 2004. </reference>
		<reference numeration="41" content_type="text"> Schotterer, U., Stichler, W., Graf, W., Gourcy, L., Huber, T., and Ginot, P.: Stable Isotopes in alpine ice cores: do they record climate variability?, Proc. Intern. Conf. on Isotope Techniques in the Study of Environmental Change, IAEA Vienna, 1998. </reference>
		<reference numeration="42" content_type="text"> Schwerzmann, A., Funk, M., Blatter, H., Lüthi, M., Schwikowski, M., and Palmer, A.: A method to reconstruct past accumulation rates in alpine firn regions: A study on Fiescherhorn, Swiss Alps, J. Geophys. Res., 111, F01014, doi:10.1029/2005JF000283, 2006. </reference>
		<reference numeration="43" content_type="text"> Schwikowski, M., Brütsch, S., Gäggeler, H. W., and Schotterer, U.: A high-resolution air chemistry record from an Alpine ice core: Fiescherhorn glacier, Swiss Alps, J. Geophys. Res., 104, 13 709&amp;ndash;13 719, 1999a. </reference>
		<reference numeration="44" content_type="text"> Schwikowski, M., Döscher, A., Gäggeler, H. W., and Schotterer, U.: Anthropogenic versus natural sources of atmospheric sulphate from an Alpine ice core, Tellus B , 51, 938&amp;ndash;951, 1999b. </reference>
		<reference numeration="45" content_type="text"> Sharma, S., Lavoué, D., Cachier, H., Barrie, L. A., and Gong, S. L.: Long-term trends of the black carbon concentrations in the Canadian Arctic, J. Geophys. Res.-Atmos., 109, D15203, doi:10.1029/2003JD004331, 2004. </reference>
		<reference numeration="46" content_type="text"> Slater, J. F., Currie, L. A., Dibb, J. E., and Benner Jr., B. A.: Distinguishing the relative contribution of fossil fuel and biomass combustion to aerosols deposited at Summit, Grenland through isotopic and molecular characterization of insoluble carbon, Atmos. Environ., 36, 4463&amp;ndash;4477, 2002. </reference>
		<reference numeration="47" content_type="text"> Stuiver, M. and Polach, H. A.: Discussion: Reporting of $^14$C Data Radiocarbon, 19, 355&amp;ndash;363, 1977. </reference>
		<reference numeration="48" content_type="text"> Synal, H.-A., Jacob, S., and Suter, M.: The PSI/ETH small radiocarbon dating system, Nucl. Instr. Meth. Phys. Res. B, 172, 1&amp;ndash;7, 2000. </reference>
		<reference numeration="49" content_type="text"> Szidat, S., Jenk, T. M., Gäggeler, H. W., Synal, H.-A., Fisseha, R., Baltensperger, U., Kalberer, M., Samburova, V., Wacker, L., Saurer, M., Schwikowski, M., and Hajdas, I.: Source apportionment of Aerosols by $^14$C measurements in different carbonaceous particle fractions, Radiocarbon, 46, 475&amp;ndash;484, 2004a. </reference>
		<reference numeration="50" content_type="text"> Szidat, S., Jenk, T. M., Gäggeler, H. W., Synal, H.-A., Fisseha, R., Baltensperger, U., Kalberer, M., Samburova, V., Reimann, S., Kasper-Giebl, A., and Hajdas, I.: Radiocarbon ($^14$C)-deduced biogenic and anthropogenic contributions to organic carbon (OC) of urban aerosols from Zürich, Switzerland, Atmos. Environ., 38, 4035&amp;ndash;4044, 2004b. </reference>
		<reference numeration="51" content_type="text"> Szidat, S., Jenk, T. M., Gäggeler, H. W., Synal, H.-A., Hajdas, I., Bonani, G., and Saurer, M.: THEODORE, a two-step heating system for the EC/OC determination of radiocarbon ($^14$C) in the environment, Nucl. Instr. Meth. Phys. Res. B, 223&amp;ndash;224, 829&amp;ndash;836, 2004c. </reference>
		<reference numeration="52" content_type="text"> Szidat, S., Jenk, T. M., Synal, H.-A., Kalberer, M., Wacker, L., Hajdas, I., Kasper-Giebl, A., and Baltensperger, U.: Contributions of fossil fuel, biomass burning, and biogenic emissions to carbonaceous aerosols in Zürich as traced by $^14$C, J. Geophys. Res., 111, D07206, doi:10.1029/2005JD0065902006, 2006. </reference>
		<reference numeration="53" content_type="text"> Thompson, L. G., Davis, M. E., Mosley-Thompson, E., Sowers, T. A., Henderson, K. A., Zagorodnov, V. S., Lin, P.-N., Mikhalenko, V. N., Campen, R. K., Bolzan, J. F., Cole-Dai, J., Francou, B.: A 25 000-Year Tropical Climate History from Bolivian Ice Cores, Science, 282, 1858&amp;ndash;1864, doi:10.1126/science.282.5395.1858, 1998. </reference>
		<reference numeration="54" content_type="text"> Widory, D., Roy, S., LeMoullec, Y., Goupil, G., Cocherie, A., and Guerrot, C.: The origin of atmospheric particles in Paris: a view through carbon and lead isotopes, Atmos. Environ., 38, 953&amp;ndash;961, 2004. </reference>
	</references>
</article>

