<?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>9</volume_number>
		<issue_number>6</issue_number>
		<publication_year>2009</publication_year>
	</journal>
	<doi>10.5194/acpd-9-23073-2009</doi>
	<article_url>http://www.atmos-chem-phys-discuss.net/9/23073/2009/</article_url>
	<abstract_html>http://www.atmos-chem-phys-discuss.net/9/23073/2009/acpd-9-23073-2009.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys-discuss.net/9/23073/2009/acpd-9-23073-2009.pdf</fulltext_pdf>
	<start_page>23073</start_page>
	<end_page>23101</end_page>
	<publication_date>2009-11-02</publication_date>
	<article_title content_type="html">Tracing the fate of atmospheric nitrate deposited onto a forest ecosystem in eastern Asia using  &amp;Delta;&lt;sup&gt;17&lt;/sup&gt;O</article_title>
	<authors>
		<author numeration="1" affiliations="1">
			<name>U. Tsunogai</name>
			<email>urumu@mail.sci.hokudai.ac.jp</email>
		</author>
		<author numeration="2" affiliations="1">
			<name>D. D. Komatsu</name>
		</author>
		<author numeration="3" affiliations="1">
			<name>S. Daita</name>
		</author>
		<author numeration="4" affiliations="1,4">
			<name>G. Abbas Kazemi</name>
		</author>
		<author numeration="5" affiliations="1">
			<name>F. Nakagawa</name>
		</author>
		<author numeration="6" affiliations="2">
			<name>I. Noguchi</name>
		</author>
		<author numeration="7" affiliations="3">
			<name>J. Zhang</name>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">Earth and Planetary System Science, Faculty of Science, Hokkaido University,  Sapporo, Japan</affiliation>
		<affiliation numeration="2" content_type="html">Hokkaido Institute of Environmental Sciences, Sapporo, Japan</affiliation>
		<affiliation numeration="3" content_type="html">Graduate School of Science and Engineering, University of Toyama,  Toyama, Japan</affiliation>
		<affiliation numeration="4" content_type="html">now at: Faculty of Earth Sciences, Shahrood University of Technology, Shahrood, Iran</affiliation>
	</affiliations>
	<abstract content_type="html">The stable isotopic compositions of nitrate in precipitation (wet deposition) and
      groundwater (spring, lake, and stream water) were determined for the island of Rishiri,
      Japan, so as to use the &lt;sup&gt;17&lt;/sup&gt;O anomalies (&amp;Delta;&lt;sup&gt;17&lt;/sup&gt;O) to trace the fate
      of atmospheric nitrate that had deposited onto the island ecosystem, which is
      a representative background forest ecosystem for eastern Asia. The deposited nitrate had
      large &lt;sup&gt;17&lt;/sup&gt;O anomalies with &amp;Delta;&lt;sup&gt;17&lt;/sup&gt;O values ranging from
      +20.8&amp;permil; to +34.5&amp;permil (&lt;i&gt;n&lt;/i&gt;= 32) with +26.2&amp;permil; being the annual
      average. The maximum &amp;Delta;&lt;sup&gt;17&lt;/sup&gt;O value of +34.5&amp;permil;, obtained for
      precipitation on 23 to 24 February 2007, was an extraordinarily large value among values for
      all samples of precipitation. Most nitrate in the sample might have been produced through
      the heterogeneous reaction of NO&lt;sub&gt;3&lt;/sub&gt; radical with hydrocarbons in a highly polluted
      air mass that had been supplied from megacities on the eastern coast of the Asian
      continent. On the other hand, nitrate in groundwater had small &amp;Delta;&lt;sup&gt;17&lt;/sup&gt;O values
      ranging from +0.9&amp;permil; to 3.2&amp;permil; (&lt;i&gt;n&lt;/i&gt;=19), which corresponds to an average
      mixing ratio of atmospheric nitrate to total nitrate of 7%. Comparing the inflow and
      outflow of atmospheric nitrate in groundwater within the island, we estimated that the
      direct drainage accounts for 10.5&amp;plusmn;5.2% of atmospheric nitrate that has deposited on
      the island and that the residual portion has undergone biological processing before being
      exported from the forest ecosystem.</abstract>
	<references>
		<reference numeration="1" content_type="text"> Akimoto,~H.: Global air quality and pollution, Science, 302, 1716–1719, 2003. </reference>
		<reference numeration="2" content_type="text"> Alexander,~B., Hastings,~M G., Allman,~D J., Dachs,~J., Thornton,~J A., and Kunasek,~S A.: Quantifying atmospheric nitrate formation pathways based on a~global model of the oxygen isotopic composition ($\Delta \chem^17O$) of atmospheric nitrate, Atmos. Chem. Phys., 9, 5043–5056, 2009. </reference>
		<reference numeration="3" content_type="text"> Asai,~K., Zhang,~J., Asai,~K., Mandal,~A K., Mogi,~K., and Hasegawa,~K.: Residence time of submarine fresh groundwater discharge in Rishiri Island, north Japan: Application of groundwater age tracers of Tritium, CFCs and \chemSF_6, EOS, 89(53), AGU Fall Meeting Suppl Abstract (H53E-1134), 2008. </reference>
		<reference numeration="4" content_type="text"> Burns,~D A., and Kendall,~C.: Analysis of $\delta \chem^15N$ and $\delta \chem^18O$ to differentiate \chemNO_3^- sources in runoff at two watersheds in the Catskill Mountains of New York, Water Resour. Res., 38, 1051, doi:10.1029/2001WR000292, 2002. </reference>
		<reference numeration="5" content_type="text"> Campbell,~D H., Kendall,~C., Chang,~C C Y., Silva,~S R., and Tonnessen,~K A.: Pathways for nitrate release from an alpine watershed: Determination using $\delta \chem^15N$ and $\delta \chem^18O$, Water Resour. Res., 38, 1052, doi:10.1029/2001WR000294, 2002. </reference>
		<reference numeration="6" content_type="text"> Casciotti,~K L., Sigman,~D M., Galanter Hastings,~M., Böhlke,~J K., and Hilkert,~A.: Measurement of the oxygen isotopic composition of nitrate in seawater and freshwater using the denitrifier method, Anal. Chem., 74, 4905–4912, 2002. </reference>
		<reference numeration="7" content_type="text"> Duce,~R A., LaRoche,~J., Altieri,~K., Arrigo,~K R., Baker,~A R., Capone,~D G., Cornell,~S., Dentener,~F., Galloway,~J., Ganeshram,~R S., Geider,~R J., Jickells,~T., Kuypers,~M M., Langlois,~R., Liss,~P S., Liu,~S M., Middelburg,~J J., Moore,~C M., Nickovic,~S., Oschlies,~A., Pedersen,~T., Prospero,~J., Schlitzer,~R., Seitzinger,~S., Sorensen,~L L., Uematsu,~M., Ulloa,~O., Voss,~M., Ward,~B., and Zamora,~L.: Impacts of atmospheric anthropogenic nitrogen on the open ocean, Science, 320, 893–897, 2008. </reference>
		<reference numeration="8" content_type="text"> Durka,~W., Schulze,~E.-D., Gebauer,~G., and Voerkeliust,~S.: Effects of forest decline on uptake and leaching of deposited nitrate determined from \chem^15N and $\chem^18O$ measurements, Nature, 372, 765–767, 1994. </reference>
		<reference numeration="9" content_type="text"> EANET: Data Report 2007, Network center for EANET (Acid Deposition Monitoring Network in East Asia), Nigata, Japan, 229~pp., 2008. </reference>
		<reference numeration="10" content_type="text"> Fenn,~M E., Poth,~M A., Aber,~J D., Baron,~J S., Bormann,~B T., Johnson,~D W., Lemly,~A D., McNulty,~S G., Ryan,~D F., and Stottlemyer,~R.: Nitrogen excess in north American ecosystems: Predisposing factors, ecosystem responses, and management strategies, Ecol. Appl., 8, 706–733, 1998. </reference>
		<reference numeration="11" content_type="text"> Galloway,~J N., Townsend,~A R., Erisman,~J W., Bekunda,~M., Cai,~Z., Freney,~J R., Martinelli,~L A., Seitzinger,~S P., and Sutton,~M A.: Transformation of the nitrogen cycle: recent trends, questions, and potential solutions, Science, 320, 889–892, 2008. </reference>
		<reference numeration="12" content_type="text"> Grennfelt,~P. and Hultberg,~H.: Effects of nitrogen deposition on the acidification of terrestrial and aquatic ecosystems, Water Air Soil Poll., 30, 945–963, 1986. </reference>
		<reference numeration="13" content_type="text"> Guttikunda,~S K., Tang,~Y H., Carmichael,~G R., Kurata,~G., Pan,~L., Streets,~D G., Woo,~J H., Thongboonchoo,~N., and Fried,~A.: Impacts of Asian megacity emissions on regional air quality during spring 2001,~J. Geophys. Res., 110, D20301, doi:10.1029/2004jd004921, 2005. </reference>
		<reference numeration="14" content_type="text"> Haruki,~M., Fujiwara,~A., Matsuda,~K., Natsume,~S., Yajima,~T., Namikawa,~K., and Niiyama,~K.: Forest vegetation in Rishiri and Rebun Islands in Hokkaido, Japan, Rishiri Stud., 23, 27–91, 2004 (in Japanese with English abstract). </reference>
		<reference numeration="15" content_type="text"> Hayashi,~T., Marui,~A., and Yasuhara,~M.: Characteristics of water chemistry of inland water and submarine discharged groundwater in Rishiri island, northern Japan,~J. Jpn. Assoc. Hydrol. Sci., 29, 123–138, 1999 (in Japanese). </reference>
		<reference numeration="16" content_type="text"> Ijiri,~A., Tsunogai,~U., and Gamo,~T.: Simple method for oxygen-18 determination of milligram quantities of water using \chemNaHCO_3 reagent, Rapid Commun. Mass Sp., 17, 1472–1478, 2003. </reference>
		<reference numeration="17" content_type="text"> Kaiser,~J., Hastings,~M G., Houlton,~B Z., Röckmann,~T., and Sigman,~D M.: Triple oxygen isotope analysis of nitrate using the denitrifier method and thermal decomposition of \chemN_2O, Anal. Chem., 79, 599–607, 2007. </reference>
		<reference numeration="18" content_type="text"> Komatsu,~D D., Ishimura,~T., Nakagawa,~F., and Tsunogai,~U.: Determination of the \chem^15N/\chem^14N, \chem^17O/\chem^16O, and \chem^18O/\chem^16O ratios of nitrous oxide by using continuous-flow isotope-ratio mass spectrometry, Rapid Commun. Mass Sp., 22, 1587–1596, 2008. </reference>
		<reference numeration="19" content_type="text"> Kool,~D M., Wrage,~N., Oenema,~O., Dolfing,~J., and Van Groenigen,~J W.: Oxygen exchange between (de)nitrification intermediates and \chemH_2O and its implications for source determination of \chemNO_3^- and \chemN_2O: a~review, Rapid Commun. Mass Sp., 21, 3569–3578, doi:10.1002/rcm.3249, 2007. </reference>
		<reference numeration="20" content_type="text"> Marui,~A., Yasuhara,~M., and Hayashi,~T.: Visit to valuable water springs (46) Valuable water springs on Rishiri island in Hokkaido, Japan: Kanrozen spring and submarine groundwater discharge, J. Jpn. Assoc. Groundwater Hydrol., 41, 213–220, 1999 (in Japanese). </reference>
		<reference numeration="21" content_type="text"> Marui,~A.: Groundwater conditions along the seawater/freshwater interface on a~volcanic island and a~depositional area in Japan, Geolog. Quart., 47, 381–388, 2003. </reference>
		<reference numeration="22" content_type="text"> McIlvin,~M R. and Altabet,~M A.: Chemical Conversion of nitrate and nitrite to nitrous oxide for nitrogen and oxygen isotope analysis in freshwater and seawater, Anal. Chem., 77, 5589–5595, 2005. </reference>
		<reference numeration="23" content_type="text"> Michalski,~G., Scott,~Z., Kabiling,~M., and Thiemens,~M H.: First measurements and modeling of $\Delta \chem^17O$ in atmospheric nitrate, Geophys. Res. Lett., 30, 1870, doi:10.1029/2003GL017015, 2003. </reference>
		<reference numeration="24" content_type="text"> Michalski,~G., Meixner,~T., Fenn,~M., Hernandez,~L., Sirulnik,~A., Allen,~E., and Thiemens,~M.: Tracing atmospheric nitrate deposition in a~complex semiarid ecosystem using $\Delta \chem^17O$, Environ. Sci. Technol., 38, 2175–2181, 2004. </reference>
		<reference numeration="25" content_type="text"> Miller,~M F.: Isotopic fractionation and the quantification of \chem^17O anomalies in the oxygen three-isotope system: an appraisal and geochemical significance, Geochim. Cosmochim. Ac., 66, 1881–1889, 2002. </reference>
		<reference numeration="26" content_type="text"> Morin,~S., Savarino,~J., Frey,~M M., Yan,~N., Bekki,~S., Bottenheim,~J W., and Martins,~J M F.: Tracing the origin and fate of \chemNO_x in the Arctic Atmosphere using stable isotopes in nitrate, Science, 322, 730–732, doi:10.1126/science.1161910, 2008. </reference>
		<reference numeration="27" content_type="text"> Morin,~S., Savarino,~J., Frey,~M M., Domine,~F., Jacobi,~H W., Kaleschke,~L., and Martins,~J M F.: Comprehensive isotopic composition of atmospheric nitrate in the Atlantic Ocean boundary layer from 65 degrees S to 79 degrees N,~J. Geophys. Res., 114, D05303, doi:10.1029/2008jd010696, 2009. </reference>
		<reference numeration="28" content_type="text"> Murdoch,~P S. and Stoddard,~J L.: The Role of Nitrate in the Acidification of Streams in the Catskill Mountains of New York, Water Resour. Res., 28, 2707–2720, 1992. </reference>
		<reference numeration="29" content_type="text"> Noguchi,~I., Hayashi,~K., Aikawa,~M., Ohizumi,~T., Minami,~Y., Kitamura,~M., Takahashi,~A., Tanimoto,~H., Matsuda,~K., and Hara,~H.: Temporal trend of non-sea salt sulfate and nitrate in wet deposition in Japan, Water Air Soil Poll., 7, 67–75, 2007. </reference>
		<reference numeration="30" content_type="text"> Ohte,~N., Sebestyen,~S D., Shanley,~J B., Doctor,~D H., Kendall,~C., Wankel,~S D., and Boyer,~E W.: Tracing sources of nitrate in snowmelt runoff using a~high-resolution isotopic technique, Geophys. Res. Lett., 31, L21506, doi:10.1029/2004GL020908, 2004. </reference>
		<reference numeration="31" content_type="text"> Paerl,~H W.: Coastal eutrophication and harmful algal blooms: Importance of atmospheric deposition and groundwater as \qutnew nitrogen and other nutrient sources, Limnol. Oceanogr., 42, 1154–1165, 1997. </reference>
		<reference numeration="32" content_type="text"> Tanimoto,~H., Kajii,~Y., Hirokawa,~J., Akimoto,~H., and Minko,~N P.: The atmospheric impact of boreal forest fires in far eastern Siberia on the seasonal variation of carbon monoxide: Observations at Rishiri, a~northern remote island in Japan, Geophys. Res. Lett., 27, 4073–4076, 2000. </reference>
		<reference numeration="33" content_type="text"> Tietema,~A., Emmett,~B A., Gundersen,~P., Kjonaas,~O J., and Koopmans,~C J.: The fate of N-15-labelled nitrogen deposition in coniferous ecosystems, Forest Ecol. Manag., 101, 19–27, 1998. </reference>
		<reference numeration="34" content_type="text"> Tilman,~D., Wedin,~D., and Knops,~J.: Productivity and sustainability influenced by biodiversity in grassland ecosystems, Nature, 379, 718–720, 1996. </reference>
		<reference numeration="35" content_type="text"> Tsunogai,~U., and Wakita,~H.: Precursory chemical changes in ground water: Kobe earthquake, Japan, Science, 269, 61–63, 1995. </reference>
		<reference numeration="36" content_type="text"> Tsunogai,~U., Nakagawa,~F., Komatsu,~D D., and Gamo,~T.: Stable carbon and oxygen isotopic analysis of atmospheric carbon monoxide using continuous-flow isotope ratio MS by isotope monitoring of CO, Anal. Chem., 74, 5695–5700, 2002. </reference>
		<reference numeration="37" content_type="text"> Tsunogai,~U., Nakagawa,~F., Gamo,~T., and Ishibashi,~J.: Stable isotopic compositions of methane and carbon monoxide in the Suiyo hydrothermal plume, Izu-Bonin arc: tracers for microbial consumption/production, Earth Planet. Sc. Lett., 237, 326–340, 2005. </reference>
		<reference numeration="38" content_type="text"> Tsunogai,~U., Kido,~T., Hirota,~A., Ohkubo,~S B., Komatsu,~D D., and Nakagawa,~F.: Sensitive determinations of stable nitrogen isotopic composition of organic nitrogen through chemical conversion into \chemN_2O, Rapid Commun. Mass Sp., 22, 345–354, 2008. </reference>
		<reference numeration="39" content_type="text"> Uno,~I., Uematsu,~M., Hara,~Y., He,~Y J., Ohara,~T., Mori,~A., Kamaya,~T., Murano,~K., Sadanaga,~Y., and Bandow,~H.: Numerical study of the atmospheric input of anthropogenic total nitrate to the marginal seas in the western North Pacific region, Geophys. Res. Lett., 34, L17817, doi:10.1029/2007GL030338, 2007. </reference>
		<reference numeration="40" content_type="text"> Williams,~M W., Baron,~J S., Caine,~N., Sommerfeld,~R., and Sanford,~R.: Nitrogen Saturation in the Rocky Mountains, Environ. Sci. Technol., 30, 640–646, 1996. </reference>
		<reference numeration="41" content_type="text"> Williard,~K W J., DeWalle,~D R., Edwards,~P J., and Sharpe,~W E.: $\chem^18O$ isotopic separation of stream nitrate sources in mid-Appalachian forested watersheds,~J. Hydrol., 252, 174–188, 2001. </reference>
		<reference numeration="42" content_type="text"> Yamaguchi,~H., and Ohara,~T.: Groundwater in Rishiri Island, Hokkaido : No. 1, J. Jap. Soc. Eng. Geol., 12, 109–120, 1971 (in Japanese). </reference>
		<reference numeration="43" content_type="text"> Yamaguchi,~H.: Hydrologic balance in the Island of Rishiri, Rep. Geol. Survey Hokkaido, 47, 1–21, 1975 (in Japanese with English abstract). </reference>
		<reference numeration="44" content_type="text"> Zeng,~J., Tohjima,~Y., Fujinuma,~Y., Mukai,~H., and Katsumoto,~M.: A~study of trajectory quality using methane measurements from Hateruma Island, Atmos. Environ., 37, 1911–1919, 2003. </reference>
		<reference numeration="45" content_type="text"> Zhang,~X Y., Zhang,~P., Zhang,~Y., Li,~X J., and Qiu,~H.: The trend, seasonal cycle, and sources of tropospheric \chemNO_2 over China during 1997–2006 based on satellite measurement, Sci. China Ser. D, 50, 1877–1884, 2007. </reference>
	</references>
</article>

