<?xml version="1.0" encoding="UTF-8"?>
<!DOCTYPE article PUBLIC "-//NLM//DTD Journal Publishing DTD v3.0 20080202//EN" "https://jats.nlm.nih.gov/nlm-dtd/publishing/3.0/journalpublishing3.dtd">
<article xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink" article-type="research-article" dtd-version="3.0" xml:lang="en">
<front>
<journal-meta>
<journal-id journal-id-type="publisher">ACP</journal-id>
<journal-title-group>
<journal-title>Atmospheric Chemistry and Physics</journal-title>
<abbrev-journal-title abbrev-type="publisher">ACP</abbrev-journal-title>
<abbrev-journal-title abbrev-type="nlm-ta">Atmos. Chem. Phys.</abbrev-journal-title>
</journal-title-group>
<issn pub-type="epub">1680-7324</issn>
<publisher><publisher-name>Copernicus Publications</publisher-name>
<publisher-loc>Göttingen, Germany</publisher-loc>
</publisher>
</journal-meta>
<article-meta>
<article-id pub-id-type="doi">10.5194/acp-13-8787-2013</article-id>
<title-group>
<article-title>Gravitational separation in the stratosphere – a new indicator of atmospheric circulation</article-title>
</title-group>
<contrib-group><contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Ishidoya</surname>
<given-names>S.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Sugawara</surname>
<given-names>S.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Morimoto</surname>
<given-names>S.</given-names>
</name>
<xref ref-type="aff" rid="aff3">
<sup>3</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Aoki</surname>
<given-names>S.</given-names>
</name>
<xref ref-type="aff" rid="aff4">
<sup>4</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Nakazawa</surname>
<given-names>T.</given-names>
</name>
<xref ref-type="aff" rid="aff4">
<sup>4</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Honda</surname>
<given-names>H.</given-names>
</name>
<xref ref-type="aff" rid="aff5">
<sup>5</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Murayama</surname>
<given-names>S.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
</contrib-group><aff id="aff1">
<label>1</label>
<addr-line>National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba 305-8569, Japan</addr-line>
</aff>
<aff id="aff2">
<label>2</label>
<addr-line>Miyagi University of Education, Sendai 980-0845, Japan</addr-line>
</aff>
<aff id="aff3">
<label>3</label>
<addr-line>National Institute of Polar Research, Tokyo 190-8518, Japan</addr-line>
</aff>
<aff id="aff4">
<label>4</label>
<addr-line>Center for Atmospheric and Oceanic Studies, Tohoku University, Sendai 980-8578, Japan</addr-line>
</aff>
<aff id="aff5">
<label>5</label>
<addr-line>Institute of Space and Astronautical Science (ISAS), Japan Aerospace Exploration Agency (JAXA), Sagamihara 252-5210, Japan</addr-line>
</aff>
<pub-date pub-type="epub">
<day>03</day>
<month>09</month>
<year>2013</year>
</pub-date>
<volume>13</volume>
<issue>17</issue>
<fpage>8787</fpage>
<lpage>8796</lpage>
<permissions>
<copyright-statement>Copyright: &#x000a9; 2013 S. Ishidoya et al.</copyright-statement>
<copyright-year>2013</copyright-year>
<license license-type="open-access">
<license-p>This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit <ext-link ext-link-type="uri"  xlink:href="https://creativecommons.org/licenses/by/3.0/">https://creativecommons.org/licenses/by/3.0/</ext-link></license-p>
</license>
</permissions>
<self-uri xlink:href="https://acp.copernicus.org/articles/13/8787/2013/acp-13-8787-2013.html">This article is available from https://acp.copernicus.org/articles/13/8787/2013/acp-13-8787-2013.html</self-uri>
<self-uri xlink:href="https://acp.copernicus.org/articles/13/8787/2013/acp-13-8787-2013.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/13/8787/2013/acp-13-8787-2013.pdf</self-uri>
<abstract>
<p>As a basic understanding of the dynamics of the atmospheric circulation, it
has been believed that gravitational separation of atmospheric components is
observable only in the atmosphere above the turbopause. However, we found,
from our high-precision measurements of not only the isotopic ratios of
N&lt;sub&gt;2&lt;/sub&gt;, O&lt;sub&gt;2&lt;/sub&gt; and Ar but also the mole fraction of Ar, that gravitational
separation occurs even in the stratosphere below the turbopause; their
observed vertical profiles are in good agreement with those expected
theoretically from molecular mass differences. The O&lt;sub&gt;2&lt;/sub&gt;/N&lt;sub&gt;2&lt;/sub&gt; ratio
observed in the middle stratosphere, corrected for gravitational separation,
showed the same mean air age as estimated from the CO&lt;sub&gt;2&lt;/sub&gt; mole fraction.
Simulations with a 2-dimensional model of the middle atmosphere indicated
that a relationship between gravitational separation and the age of air in
the stratosphere would be significantly affected if the Brewer–Dobson
circulation was enhanced due to global warming. Therefore, gravitational
separation is usable as a new indicator of changes in the atmospheric
circulation in the stratosphere.</p>
</abstract>
<counts><page-count count="10"/></counts>
</article-meta>
</front>
<body/>
<back>
<ref-list>
<title>References</title>
<ref id="ref1">
<label>1</label><mixed-citation publication-type="other" xlink:type="simple">Adachi, Y., Kawamura, K., Armi, L., and Keeling, R. F.: Diffusive separation of the lower atmosphere, Science, 311, 1429, 2006.</mixed-citation>
</ref>
<ref id="ref2">
<label>2</label><mixed-citation publication-type="other" xlink:type="simple">Aoki, S., Nakazawa, T., Machida, T., Sugawara, S., Morimoto, S., Hashida, G., Yamanouchi, T., Kawamura, K., and Honda, H.: Carbon dioxide variations in the stratosphere over Japan, Scandinavia and Antarctica, Tellus, 55B, 178–186, 2003.</mixed-citation>
</ref>
<ref id="ref3">
<label>3</label><mixed-citation publication-type="other" xlink:type="simple">Austin, J. and Li, F.: On the relationship between the strength of the Brewer–Dobson circulation and the age of stratospheric air, Geophys. Res. Lett., 33, L17807, &lt;a href=&quot;http://dx.doi.org/10.1029/2006GL026867&quot;&gt;https://doi.org/10.1029/2006GL026867&lt;/a&gt;, 2006.</mixed-citation>
</ref>
<ref id="ref4">
<label>4</label><mixed-citation publication-type="other" xlink:type="simple">Banks, P. M. and Kockarts, G.: Aeronomy, Parts A and B, Academic Press, Inc. New York, USA, 32–63, 1973.</mixed-citation>
</ref>
<ref id="ref5">
<label>5</label><mixed-citation publication-type="other" xlink:type="simple">Bender, M. L., Tans, P. P., Ellis, J. T., Orchard, J., and Habfast, K.: High precision isotope ratio mass spectrometry method for measuring the O&lt;sub&gt;2&lt;/sub&gt;/N&lt;sub&gt;2&lt;/sub&gt; ratio of air, Geochim. Cosmochim. Acta, 58, 4751–4758, 1994.</mixed-citation>
</ref>
<ref id="ref6">
<label>6</label><mixed-citation publication-type="other" xlink:type="simple">Blaine, T. W., Keeling, R. F., and Paplawsky, W. J.: An improved inlet for precisely measuring the atmospheric Ar/N&lt;sub&gt;2&lt;/sub&gt; ratio, Atmos. Chem. Phys., 6, 1181–1184, &lt;a href=&quot;http://dx.doi.org/10.5194/acp-6-1181-2006&quot;&gt;https://doi.org/10.5194/acp-6-1181-2006&lt;/a&gt;, 2006.</mixed-citation>
</ref>
<ref id="ref7">
<label>7</label><mixed-citation publication-type="other" xlink:type="simple">Brewer, A.: Evidence for a world circulation provided by the measurement of helium and water vapor in the stratosphere, Q. J. Roy. Meteorol. Soc., 75, 351–363, 1949.</mixed-citation>
</ref>
<ref id="ref8">
<label>8</label><mixed-citation publication-type="other" xlink:type="simple">Engel, A., Möbius, T., Bönisch, H., Schmidt, U., Heinz, R., Levin, I., Atlas, E., Aoki, S., Nakazawa, T., Sugawara, S., Moore, F., Hurst, D., Elkins, J., Schauffler, S., Andrews, A., and Boering, K.: Age of stratospheric air unchanged within uncertainties over the past 30 years,  Nature Geosci., 2, 28–31, &lt;a href=&quot;http://dx.doi.org/10.1038/Ngeo388&quot;&gt;https://doi.org/10.1038/Ngeo388&lt;/a&gt;, 2009.</mixed-citation>
</ref>
<ref id="ref9">
<label>9</label><mixed-citation publication-type="other" xlink:type="simple">Etheridge, D. M., Steele, L. P., Langenfelds, R. L., Francey, R. J., Barnola, J.-M., and Morgan, V. I.: Natural and anthropogenic changes in atmospheric CO&lt;sub&gt;2&lt;/sub&gt; over the last 1000 years from air in Antarctic ice and firn, J. Geophys. Res., 101, 4115–4128, 1996.</mixed-citation>
</ref>
<ref id="ref10">
<label>10</label><mixed-citation publication-type="other" xlink:type="simple">Grew, K. E. and Ibbs, L. T.: Thermal Diffusion in Gases, Cambridge Univ. Press, New York, USA, 151 pp., 1952.</mixed-citation>
</ref>
<ref id="ref11">
<label>11</label><mixed-citation publication-type="other" xlink:type="simple">Honda, H.: Balloon-borne cryogenic whole air sampling system, ISAS Research Note 433, The Institute of Space and Astronautical Science, Sagamihara, Japan, 1990.</mixed-citation>
</ref>
<ref id="ref12">
<label>12</label><mixed-citation publication-type="other" xlink:type="simple">Honda, H., Aoki, S., Nakazawa, T., Morimoto, S., and Yajima, N.: Cryogenic air sampling system for measurements of the concentrations of stratospheric trace gases and their isotopic ratios over Antarctica, J. Geomagn. Geoelectr., 48, 1145–1155, 1996.</mixed-citation>
</ref>
<ref id="ref13">
<label>13</label><mixed-citation publication-type="other" xlink:type="simple">Huang, T. Walters, S., Brasseur, G., Hauglustaine, D., and Wu, W.:  Description of SOCRATES – A chemical dynamical radiative two-dimensional model, NCAR/TN-440}+{EDD NCAR TECHNICAL NOTE, 1998.</mixed-citation>
</ref>
<ref id="ref14">
<label>14</label><mixed-citation publication-type="other" xlink:type="simple">Ishidoya, S., Aoki, S., and Nakazawa, T.: High precision measurements of the atmospheric O&lt;sub&gt;2&lt;/sub&gt;/N&lt;sub&gt;2&lt;/sub&gt; ratio on a mass spectrometer, J. Meteorol. Soc. Japan, 81, 127–140, 2003.</mixed-citation>
</ref>
<ref id="ref15">
<label>15</label><mixed-citation publication-type="other" xlink:type="simple">Ishidoya, S., Sugawara, S., Hashida, G., Morimoto, S., Aoki, S., Nakazawa, T., and Yamanouchi, T.: Vertical profiles of the O&lt;sub&gt;2&lt;/sub&gt;/N&lt;sub&gt;2&lt;/sub&gt; ratio in the stratosphere over Japan and Antarctica, Geophys. Res. Lett., 33, L13701, &lt;a href=&quot;http://dx.doi.org/10.1029/2006GL025886&quot;&gt;https://doi.org/10.1029/2006GL025886&lt;/a&gt;, 2006.</mixed-citation>
</ref>
<ref id="ref16">
<label>16</label><mixed-citation publication-type="other" xlink:type="simple">Ishidoya, S., Sugawara, S., Morimoto, S., Aoki, S., and Nakazawa, T.: Gravitational separation of major atmospheric components of nitrogen and oxygen in the stratosphere, Geophys. Res. Lett., 35, L03811, &lt;a href=&quot;http://dx.doi.org/10.1029/2007GL030456&quot;&gt;https://doi.org/10.1029/2007GL030456&lt;/a&gt;, 2008a.</mixed-citation>
</ref>
<ref id="ref17">
<label>17</label><mixed-citation publication-type="other" xlink:type="simple">Ishidoya, S., Morimoto, S., Sugawara, S., Watai, T., Machida, T. Aoki, S., Nakazawa, T., and Yamanouchi, T.: Gravitational separation suggested by O&lt;sub&gt;2&lt;/sub&gt;/N&lt;sub&gt;2&lt;/sub&gt;, δ&lt;sup&gt;15&lt;/sup&gt;N of N&lt;sub&gt;2&lt;/sub&gt;, δ&lt;sup&gt;18&lt;/sup&gt;O of O&lt;sub&gt;2&lt;/sub&gt;, Ar/N&lt;sub&gt;2&lt;/sub&gt; observed in the lowermost part of the stratosphere at northern middle and high latitudes in the early spring of 2002, Geophys. Res. Lett., 35, L03812, &lt;a href=&quot;http://dx.doi.org/10.1029/2007GL031526&quot;&gt;https://doi.org/10.1029/2007GL031526&lt;/a&gt;, 2008b.</mixed-citation>
</ref>
<ref id="ref18">
<label>18</label><mixed-citation publication-type="other" xlink:type="simple">Ishidoya, S., Aoki, S. Goto, D., Nakazawa, T., Taguchi, S., and Patra, P. K.: Time and space variations of the O&lt;sub&gt;2&lt;/sub&gt;/N&lt;sub&gt;2&lt;/sub&gt; ratio in the troposphere over Japan and estimation of global CO&lt;sub&gt;2&lt;/sub&gt; budget, Tellus B, }{ 64, 18964, 10.3402/tellusb.v64i0.18964, 2012.</mixed-citation>
</ref>
<ref id="ref19">
<label>19</label><mixed-citation publication-type="other" xlink:type="simple">Jacob, D. J.: Introduction to Atmospheric Chemistry, Princeton University Press, Princeton, 267 pp., 1999.</mixed-citation>
</ref>
<ref id="ref20">
<label>20</label><mixed-citation publication-type="other" xlink:type="simple">Khosravi, R., Brasseur, G., Smith, A., Rusch, D., Walters, S., Chabrillat, and Kockarts, G.: Response of the mesosphere to human-induced perturbations and solar variability calculated by a 2-D model, J. Geophys. Res.,  107, 4358, &lt;a href=&quot;http://dx.doi.org/10.1029/2001JD001235&quot;&gt;https://doi.org/10.1029/2001JD001235&lt;/a&gt;, 2002.</mixed-citation>
</ref>
<ref id="ref21">
<label>21</label><mixed-citation publication-type="other" xlink:type="simple">Lettau, H.: Diffusion in the upper atmosphere, Compendium of Meteorology, American Meteorological Society, Boston, 1951.</mixed-citation>
</ref>
<ref id="ref22">
<label>22</label><mixed-citation publication-type="other" xlink:type="simple">Lewis, J. S. and Prinn R. G.: Planets and Their Atmosphere: origin and evolution, International Geophysics Series, 33, Academic Press Inc., 33, 470 pp., 1984.</mixed-citation>
</ref>
<ref id="ref23">
<label>23</label><mixed-citation publication-type="other" xlink:type="simple">Li, F., Austin, J., and Wilson, J.: The Strength of the Brewer-Dobson Circulation in a changing climate: Coupled chemistry-climate model simulations, J. Climate, 21, 40–57, &lt;a href=&quot;http://dx.doi.org/10.1175/2007JCLI1663.1&quot;&gt;https://doi.org/10.1175/2007JCLI1663.1&lt;/a&gt;, 2008.</mixed-citation>
</ref>
<ref id="ref24">
<label>24</label><mixed-citation publication-type="other" xlink:type="simple">Massie, S. T. and Hunten, D. M.: Stratospheric eddy diffusion coefficients from tracer data, J. Geophys. Res., }{86, 9859–9868, 1981.</mixed-citation>
</ref>
<ref id="ref25">
<label>25</label><mixed-citation publication-type="other" xlink:type="simple">Nakazawa, T., Machida, T., Sugawara, S., Murayama, S., Morimoto, S., Hashida, G., Honda, H., and Itoh, T.: Measurements of the stratospheric carbon dioxide concentration over Japan using a Balloon-borne cryogenic sampler,  Geophys. Res. Lett., 22, p. 1229, &lt;a href=&quot;http://dx.doi.org/10.1029/95GL01188&quot;&gt;https://doi.org/10.1029/95GL01188&lt;/a&gt;, 1995.</mixed-citation>
</ref>
<ref id="ref26">
<label>26</label><mixed-citation publication-type="other" xlink:type="simple">Nakazawa, T., Morimoto, S., Aoki, S., and Tanaka, M.: Temporal and spatial variations of the carbon isotopic ratio of atmospheric carbon dioxide in the western Pacific region, J. Geophys. Res., 102, 1271–1285, 1997.</mixed-citation>
</ref>
<ref id="ref27">
<label>27</label><mixed-citation publication-type="other" xlink:type="simple">Park, J. H., Ko, M. K. W., Jackman, C. H., Plumb, R. A., Kaye, J. A., Sage, K. H.: Models and Measurements Intercomparison II, NASA/TM-1999-209554, &lt;a href=&quot;http://www.cs.odu.edu/ mln/ltrs-pdfs/NASA-99-tm209554.pdf&quot;&gt;http://www.cs.odu.edu/ mln/ltrs-pdfs/NASA-99-tm209554.pdf&lt;/a&gt;, 1999.</mixed-citation>
</ref>
<ref id="ref28">
<label>28</label><mixed-citation publication-type="other" xlink:type="simple">Ray, E. A., Moore, F. L., Rosenlof, K. H., Davis, S. M., Boenisch, H., Morgenstern, O., Smale, D., Rozanov, E., Hegglin, M., Pitari, G., Mancini, E., Braesicke, P., Butchart, N., Hardiman, S., Li, F., Shibata, K., and Plummer, D. A.: Evidence for changes in stratospheric transport and mixing over the past three decades based on multiple data sets and tropical leaky pipe analysis, J. Geophys. Res., 115, D21304, &lt;a href=&quot;http://dx.doi.org/10.1029/2010JD014206&quot;&gt;https://doi.org/10.1029/2010JD014206&lt;/a&gt;, 2010.</mixed-citation>
</ref>
<ref id="ref29">
<label>29</label><mixed-citation publication-type="other" xlink:type="simple">Severinghaus, J. P. and Battle, M. O.: Fractionation of gases in polar ice during bubble close-off: New constrains from firn air Ne, Kr and Xe observations, Earth Planet. Sci. Lett., }{244, 474–500, 2006.</mixed-citation>
</ref>
<ref id="ref30">
<label>30</label><mixed-citation publication-type="other" xlink:type="simple">Severinghaus, J. P., Grachev, A., and Battle, M.: Thermal fractionation of air in polar firn by seasonal temperature gradients, Geochem. Geophys. Geosys., 2, 1048, &lt;a href=&quot;http://dx.doi.org/10.1029/2000GC000146&quot;&gt;https://doi.org/10.1029/2000GC000146&lt;/a&gt;, 2001.</mixed-citation>
</ref>
<ref id="ref31">
<label>31</label><mixed-citation publication-type="other" xlink:type="simple">Stiller, G. P., Von Clarmann, T., Haenel, F., Funke, B., Glatthor, N., Grabowski, U., Kellmann, S., Kiefer, M., Linden, A., Lossow, S., and López-Puertas, M.: Observed temporal evolution of global mean age of stratospheric air for the 2002 to 2010 period, Atmos. Chem. Phys.,  12, 3311–3331, &lt;a href=&quot;http://dx.doi.org/10.5194/acp-12-3311-2012&quot;&gt;https://doi.org/10.5194/acp-12-3311-2012&lt;/a&gt;, 2012.</mixed-citation>
</ref>
<ref id="ref32">
<label>32</label><mixed-citation publication-type="other" xlink:type="simple">Waugh, D. W. and Hall, T. M.: Age of stratospheric air: Theory, observations, and models. Rev. Geophys., 40, 1010, &lt;a href=&quot;http://dx.doi.org/10.1029/2000RG000101&quot;&gt;https://doi.org/10.1029/2000RG000101&lt;/a&gt;, 2002.</mixed-citation>
</ref>
</ref-list>
</back>
</article>