<?xml version="1.0" encoding="UTF-8"?>
<!DOCTYPE article PUBLIC "-//NLM//DTD Journal Publishing DTD v3.0 20080202//EN" "http://dtd.nlm.nih.gov/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>
</journal-title-group>
<issn pub-type="epub">1680-7324</issn>
<publisher><publisher-name>Copernicus GmbH</publisher-name>
<publisher-loc>Göttingen, Germany</publisher-loc>
</publisher>
</journal-meta>
<article-meta>
<article-id pub-id-type="doi">10.5194/acp-12-4885-2012</article-id>
<title-group>
<article-title>Renewed methane increase for five years (2007–2011) observed by solar FTIR spectrometry</article-title>
</title-group>
<contrib-group><contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Sussmann</surname>
<given-names>R.</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>Forster</surname>
<given-names>F.</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>Rettinger</surname>
<given-names>M.</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>Bousquet</surname>
<given-names>P.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
<xref ref-type="aff" rid="aff3">
<sup>3</sup>
</xref>
</contrib>
</contrib-group><aff id="aff1">
<label>1</label>
<addr-line>Karlsruhe Institute of Technology, IMK-IFU, Garmisch-Partenkirchen, Germany</addr-line>
</aff>
<aff id="aff2">
<label>2</label>
<addr-line>Laboratoire des Sciences du Climat et de l&apos;Environnement, IPSL-LSCE, CEA-CNRS-UVSQ, UMR8212 91191, France</addr-line>
</aff>
<aff id="aff3">
<label>3</label>
<addr-line>Université de Versailles Saint Quentin en Yvelines, France</addr-line>
</aff>
<pub-date pub-type="epub">
<day>04</day>
<month>06</month>
<year>2012</year>
</pub-date>
<volume>12</volume>
<issue>11</issue>
<fpage>4885</fpage>
<lpage>4891</lpage>
<permissions>
<license xlink:type="simple">
<license-p>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.</license-p>
</license>
</permissions>
<self-uri xlink:href="http://www.atmos-chem-phys.net/12/4885/2012/acp-12-4885-2012.html">This article is available from http://www.atmos-chem-phys.net/12/4885/2012/acp-12-4885-2012.html</self-uri>
<self-uri xlink:href="http://www.atmos-chem-phys.net/12/4885/2012/acp-12-4885-2012.pdf">The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/4885/2012/acp-12-4885-2012.pdf</self-uri>
<abstract>
<p>Trends of column-averaged methane for the time period (1996, Sep 2011) are
derived from the mid-infrared (mid-IR) solar FTIR time series at the
Zugspitze (47.42° N, 10.98° E, 2964 m a.s.l.) and Garmisch (47.48° N, 11.06° E, 743 m a.s.l.). Trend analysis comprises a fit to the
de-seasonalized time series along with bootstrap resampling for quantifying
trend uncertainties. We find a positive trend during [1996, 1998] of 9.0
[3.2, 14.7] ppb yr&lt;sup&gt;−1&lt;/sup&gt; for Zugspitze (95% confidence interval), an
insignificant growth during [1999, mid 2006] of 0.8 [−0.1, 1.7] ppb yr&lt;sup&gt;−1&lt;/sup&gt;
(Zugspitze), and a significant renewed increase during [mid 2006, Sep 2011]
of 5.1 [4.2, 6.0] ppb yr&lt;sup&gt;−1&lt;/sup&gt; for Garmisch, which is in agreement with 4.8 [3.8,
5.9] ppb yr&lt;sup&gt;−1&lt;/sup&gt; for Zugspitze.
&lt;br&gt;&lt;/br&gt;
The agreement of methane trends at the two closely neighboring FTIR sites
Zugspitze and Garmisch within the uncertainties indicates a good
station-to-station consistency as a basis for future trend analyses by the
ground-based mid-IR FTIR network on the global scale. Furthermore, the
Zugspitze FTIR trend for the time interval [Jul 2006, Jun 2009] is found to
agree with the trend derived from SCIAMACHY (WFM-DOAS v2.0.2) data within
the 95% confidence intervals. In case a 1000-km pixel selection radius
around the Zugspitze is used, the confidence interval is narrower for the
FTIR trend (6.9 [4.2, 9.5]  ppb yr&lt;sup&gt;−1&lt;/sup&gt;) compared to SCIAMACHY (7.1 [5.1,
8.6] ppb yr&lt;sup&gt;−1&lt;/sup&gt;). If, however, a loosened pixel selection is used (&amp;approx;1000-km
half-width latitudinal band), the SCIAMACHY trend significance interval is
narrower (6.8 [5.1, 8.6] ppb yr&lt;sup&gt;−1&lt;/sup&gt;) compared to Zugspitze FTIR (5.7 [3.0,
8.3] ppb yr&lt;sup&gt;−1&lt;/sup&gt;).
&lt;br&gt;&lt;/br&gt;
While earlier studies using surface network data revealed changes of
8.0 ± 0.6 ppb in 2007, 6.4 ± 0.6 ppb in 2008, and 4.7 ± 0.6 ppb in 2009
(Dlugokencky et al., 2011), our updated result proves that the renewed
methane increase meanwhile has been persisting for &gt;5 years [mid 2006, Sep 2011]. 
This is either the longest and largest positive trend anomaly since
the beginning of systematic observations more than 25 years ago or the onset
of a new period of strongly increasing CH&lt;sub&gt;4&lt;/sub&gt; levels in the atmosphere.
Several scenarios have been developed to explain the persistent increase
observed, mainly invoking an increase in emissions from natural wetlands, an
increase in fossil fuel-related emissions or a decrease in OH
concentrations. However, more work is needed to fully attribute this
increase to a particular source or sink.</p>
</abstract>
<counts><page-count count="7"/></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"> Angelbratt, J., Mellqvist, J., Blumenstock, T., Borsdorff, T., Brohede, S., Duchatelet, P., Forster, F., Hase, F., Mahieu, E., Murtagh, D., Petersen, A. K., Schneider, M., Sussmann, R., and Urban, J.: A new method to detect long term trends of methane (CH&lt;sub&gt;4&lt;/sub&gt;) and nitrous oxide (N&lt;sub&gt;2&lt;/sub&gt;O) total columns measured within the NDACC ground-based high resolution solar FTIR network, Atmos. Chem. Phys., 11, 6167–6183, http://dx.doi.org/10.5194/acp-11-6167-2011doi:10.5194/acp-11-6167-2011, 2011. </mixed-citation>
</ref>
<ref id="ref2">
<label>2</label><mixed-citation publication-type="other" xlink:type="simple"> Aydin, M., Verhulst, K. R., Saltzman, E. S., Battle, M. O., Montzka, S. A., Blake, D. R., Tang, Q., and Prather, M. J.: Recent decreases in fossil-fuel emissions of ethane and methane derived from firn air, Nature, 476, 198–201, 2011. </mixed-citation>
</ref>
<ref id="ref3">
<label>3</label><mixed-citation publication-type="other" xlink:type="simple"> Bergamaschi, P, Frankenberg, C., Meirink, J.F., Krol, M, Villani, M. G., Houweling, S., Dentener, F., Dlugokencky, E.J., Miller, J.B., Gatti, L.V., Engel, A., and Levin, I.: Inverse modeling of global and regional CH4 emissions using SCIAMACHY satellite retrievals, J. Geophys. Res., 114, D22301, http://dx.doi.org/10.1029/2009JD012287doi:10.1029/2009JD012287, 2009. </mixed-citation>
</ref>
<ref id="ref4">
<label>4</label><mixed-citation publication-type="other" xlink:type="simple"> Bloom, A. A., Palmer, P. I., Fraser, A., Reay, D. S., and Frankenberg, C.: Large-Scale Controls of Methanogenesis Inferred from Methane and Gravity Spaceborne Data, Science, 327, 322–325, http://dx.doi.org/10.1126/science.1175176doi:10.1126/science.1175176, 2010. </mixed-citation>
</ref>
<ref id="ref5">
<label>5</label><mixed-citation publication-type="other" xlink:type="simple"> Bousquet, P., Ciais, P., Miller, J. B., Dlugokencky, E. J., Hauglustaine, D. A., Prigent, C., Van der Werf, G. R., Peylin, P., Brunke, E. G., Carouge, C., Langenfels, R. L., Lathiere, J., Papa, F., Ramonet, M., Schmidt, M., Steele, L. P., Tyler, S. C., and White, J.: Contribution of anthropogenic and natural sources to atmospheric methane variability, Nature, 443, 439–443, 2006. </mixed-citation>
</ref>
<ref id="ref6">
<label>6</label><mixed-citation publication-type="other" xlink:type="simple"> Bousquet, P., Ringeval, B., Pison, I., Dlugokencky, E. J., Brunke, E.-G., Carouge, C., Chevallier, F., Fortems-Cheiney, A., Frankenberg, C., Hauglustaine, D. A., Krummel, P. B., Langenfelds, R. L., Ramonet, M., Schmidt, M., Steele, L. P., Szopa, S., Yver, C., Viovy, N., and Ciais, P.: Source attribution of the changes in atmospheric methane for 2006–2008, Atmos. Chem. Phys., 11, 3689-3700, http://dx.doi.org/10.5194/acp-11-3689-2011doi:10.5194/acp-11-3689-2011, 2011. </mixed-citation>
</ref>
<ref id="ref7">
<label>7</label><mixed-citation publication-type="other" xlink:type="simple"> Crevoisier, C., Nobileau, D., Fiore, A. M., Armante, R., Ch$\acute\textrme$din, A., and Scott, N. A.: Tropospheric methane in the tropics – first year from IASI hyperspectral infrared observations, Atmos. Chem. Phys., 9, 6337–6350, http://dx.doi.org/10.5194/acp-9-6337-2009doi:10.5194/acp-9-6337-2009, 2009. </mixed-citation>
</ref>
<ref id="ref8">
<label>8</label><mixed-citation publication-type="other" xlink:type="simple"> Dentener, F., Peters, W., Krol, M., van Weele, M., Bergamaschi, P., and Lelieveld, J.: Inter-annual variability and trend of CH&lt;sub&gt;4&lt;/sub&gt; lifetime as a measure for OH changes in the 1979–1993 time period, J. Geophys. Res.-A, 108, 4442, http://dx.doi.org/10.1029/2002JD002916doi:10.1029/2002JD002916, 2003. </mixed-citation>
</ref>
<ref id="ref9">
<label>9</label><mixed-citation publication-type="other" xlink:type="simple"> Dlugokencky, E. J., Houweling, S., Bruhwiler, L., Masarie, K. A., Lang, P. M., Miller, J. B., and Tans, P. P.: Atmospheric methane levels off: Temporary pause or a new steady-state?, Geophys. Res. Lett., 30, 1992, http://dx.doi.org/10.1029/2003GL018126doi:10.1029/2003GL018126, 2003. </mixed-citation>
</ref>
<ref id="ref10">
<label>10</label><mixed-citation publication-type="other" xlink:type="simple"> Dlugokencky, E. J., Bruhwiler, L., White, J. W. C., Emmons, L. K., Novelli, P. C., Montzka, S. A., Masarie, K. A., Lang, P. M., Crotwell, A. M., Miller, J. B., and Gatti, L. V.: Observational constraints on recent increases in the atmospheric CH&lt;sub&gt;4&lt;/sub&gt; burden, Geophys. Res. Lett., 36, L18803, http://dx.doi.org/10.1029/2009GL039780doi:10.1029/2009GL039780, 2009. </mixed-citation>
</ref>
<ref id="ref11">
<label>11</label><mixed-citation publication-type="other" xlink:type="simple"> Dlugokencky, E. J., Nisbet, E. G., Fisher, R., and Lowry, D.: Global atmospheric methane: budget, changes and dangers, Phil. Trans. R. Soc. A, 369, 2058–2072, http://dx.doi.org/10.1098/rsta.2010.0341doi:10.1098/rsta.2010.0341, 2011. </mixed-citation>
</ref>
<ref id="ref12">
<label>12</label><mixed-citation publication-type="other" xlink:type="simple"> EDGAR4 database: Emission Database for Global Atmospheric Research (EDGAR), release version 4.2, http://edgar.jrc.ec.europa.eu, European Commission, Joint Research Centre (JRC)/Netherlands Environmental Assessment Agency (PBL), 2012. </mixed-citation>
</ref>
<ref id="ref13">
<label>13</label><mixed-citation publication-type="other" xlink:type="simple"> Forster, P., Ramaswamy, V., Artaxo, P., Berntsen, T., Betts, R., Fahey, D., Haywood, J., Lean, J., Lowe, D., Myhre, G., Nganga, J., R. Prinn, G. Raga, M. S., and Dorland, R. V.: Changes in Atmospheric Constituents and in Radiative Forcing, Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change~(IPCC), 2007. </mixed-citation>
</ref>
<ref id="ref14">
<label>14</label><mixed-citation publication-type="other" xlink:type="simple"> Frankenberg, C, Bergamaschi, P., Butz, A., Houweling, S., Meirink, J.F., Notholt, J., Petersen, A.K., Schrijver, H., Warneke, T., and Aben, I.: Tropical methane emissions: A revised view from SCIAMACHY onboard ENVISAT, Geophys. Res. Lett., 35, L15811, http://dx.doi.org/10.1029/2008GL034300doi:10.1029/2008GL034300, 2008. </mixed-citation>
</ref>
<ref id="ref15">
<label>15</label><mixed-citation publication-type="other" xlink:type="simple"> Frankenberg, C., Aben, I., Bergamaschi, P., Dlugokencky, E.J., van Hees, R., Houweling, S., van der Meer, P., Snel, R., and Tol, P.: Global column-averaged methane mixing ratios from 2003 to 2009 as derived from SCIAMACHY: Trends and variability, J. Geophys. Res., 116, D04302, http://dx.doi.org/10.1029/2010JD014849doi:10.1029/2010JD014849, 2011. </mixed-citation>
</ref>
<ref id="ref16">
<label>16</label><mixed-citation publication-type="other" xlink:type="simple"> Gardiner, T., Forbes, A., de Mazi$\grave\textrme$re, M., Vigouroux, C., Mahieu, E., Demoulin, P., Velazco, V., Notholt, J., Blumenstock, T., Hase, F., Kramer, I., Sussmann, R., Stremme, W., Mellqvist, J., Strandberg, A., Ellingsen, K., and Gauss, M.: Trend analysis of greenhouse gases over Europe measured by a network of ground-based remote FTIR instruments, Atmos. Chem. Phys., 8, 6719–6727, http://dx.doi.org/10.5194/acp-8-6719-2008doi:10.5194/acp-8-6719-2008, 2008. </mixed-citation>
</ref>
<ref id="ref17">
<label>17</label><mixed-citation publication-type="other" xlink:type="simple"> Montzka, S. A., Krol, M., Dlugokencky, E., Hall, B., Jockel, P., and Lelieveld, J.: Small Interannual Variability of Global Atmospheric Hydroxyl, Science, 331, 67–69, http://dx.doi.org/10.1126/science.1197640doi:10.1126/science.1197640, 2011. </mixed-citation>
</ref>
<ref id="ref18">
<label>18</label><mixed-citation publication-type="other" xlink:type="simple"> Olsen, S. C. and Randerson, J. T.: Differences between surface and column atmospheric CO&lt;sub&gt;2&lt;/sub&gt; and implications for carbon cycle research, J. Geophys. Res., 109, D02301, 2004, doi:10.1029/2003JD003968. </mixed-citation>
</ref>
<ref id="ref19">
<label>19</label><mixed-citation publication-type="other" xlink:type="simple"> Rigby, M., Prinn, R. G., Fraser, P. J. Simmonds, P. G., Langenfelds, R. L., Huang, J., Cunnold, D. M., Steele, L. P., Krummel, P. B., Weiss, R. F., O&apos;Doherty, S., Salameh, P. K., Wang, H. J., Harth, C. M., Mühle, J., and Porter, L. W.: Renewed growth of atmospheric methane, Geophys. Res. Lett., 35, L22805, http://dx.doi.org/10.1029/2008GL036037doi:10.1029/2008GL036037, 2008. </mixed-citation>
</ref>
<ref id="ref20">
<label>20</label><mixed-citation publication-type="other" xlink:type="simple"> Ringeval, B., de Noblet-Ducoudre, N., Ciais, P., Bousquet, P., Prigent, C., Papa, F., and Rossow, W. B.: An attempt to quantify the impact of changes in wetland extent on methane emissions on the seasonal and interannual time scales, Global Biogeochem. Cy., 24, Gb2003, doi:10.1029/2008GB003354, 2010. </mixed-citation>
</ref>
<ref id="ref21">
<label>21</label><mixed-citation publication-type="other" xlink:type="simple"> Schneider, U., Fuchs, T., Meyer-Christoffer, A., and Rudolf, B.: Global precipitation analysis products of the GPCC, Global Precip. Climatol. Cent., Dtsch. Wetterdienst, Offenbach am Main, Germany, 2008. </mixed-citation>
</ref>
<ref id="ref22">
<label>22</label><mixed-citation publication-type="other" xlink:type="simple"> Schneising, O., Buchwitz, M., Reuter, M., Heymann, J., Bovensmann, H., and Burrows, J. P.: Long-term analysis of carbon dioxide and methane column-averaged mole fractions retrieved from SCIAMACHY, Atmos. Chem. Phys., 11, 2863–2880, http://dx.doi.org/10.5194/acp-11-2863-2011doi:10.5194/acp-11-2863-2011, 2011. </mixed-citation>
</ref>
<ref id="ref23">
<label>23</label><mixed-citation publication-type="other" xlink:type="simple"> Schneising, O., Bergamaschi, P., Bovensmann, H., Buchwitz, M., Burrows, J. P., Deutscher, N. M., Griffith, D. W. T., Heymann, J., Macatangay, R., Messerschmidt, J., Notholt, J., Rettinger, M., Reuter, M., Sussmann, R., Velazco, V. A., Warneke, T., Wennberg, P. O., and Wunch, D.: Atmospheric greenhouse gases retrieved from SCIAMACHY: comparison to ground-based FTS measurements and model results, Atmos. Chem. Phys., 12, 1527–1540, http://dx.doi.org/10.5194/acp-12-1527-2012doi:10.5194/acp-12-1527-2012, 2012. </mixed-citation>
</ref>
<ref id="ref24">
<label>24</label><mixed-citation publication-type="other" xlink:type="simple"> Spahni, R., Wania, R., Neef, L., van Weele, M., Pison, I., Bousquet, P., Frankenberg, C., Foster, P.N., Joos, F., Prentice, I.C., and van Velthoven, P.: Constraining global methane emissions and uptake by ecosystems, Biogeosciences, 8., 643–1665, 2011. </mixed-citation>
</ref>
<ref id="ref25">
<label>25</label><mixed-citation publication-type="other" xlink:type="simple"> Sussmann, R. and Borsdorff, T.: Technical Note: Interference errors in infrared remote sounding of the atmosphere, Atmos. Chem. Phys., 7, 3537–3557, http://dx.doi.org/10.5194/acp-7-3537-2007doi:10.5194/acp-7-3537-2007, 2007. </mixed-citation>
</ref>
<ref id="ref26">
<label>26</label><mixed-citation publication-type="other" xlink:type="simple"> Sussmann, R. and Schäfer, K.: Infrared spectroscopy of tropospheric trace gases: combined analysis of horizontal and vertical column abundances, Appl. Opt., 36, 735–741, 1997. </mixed-citation>
</ref>
<ref id="ref27">
<label>27</label><mixed-citation publication-type="other" xlink:type="simple"> Sussmann, R., Stremme, W., Buchwitz, M., and de Beek, R.: Validation of ENVISAT/SCIAMACHY columnar methane by solar FTIR spectrometry at the Ground-Truthing Station Zugspitze, Atmos. Chem. Phys., 5, 2419–2429, http://dx.doi.org/10.5194/acp-5-2419-2005doi:10.5194/acp-5-2419-2005, 2005. </mixed-citation>
</ref>
<ref id="ref28">
<label>28</label><mixed-citation publication-type="other" xlink:type="simple"> Sussmann, R., Borsdorff, T., Rettinger, M., Camy-Peyret, C., Demoulin, P., Duchatelet, P., Mahieu, E., and Servais, C.: Technical Note: Harmonized retrieval of column-integrated atmospheric water vapor from the FTIR network – first examples for long-term records and station trends, Atmos. Chem. Phys., 9, 8987–8999, http://dx.doi.org/10.5194/acp-9-8987-2009doi:10.5194/acp-9-8987-2009, 2009. </mixed-citation>
</ref>
<ref id="ref29">
<label>29</label><mixed-citation publication-type="other" xlink:type="simple"> Sussmann, R., Forster, F., Rettinger, M., and Jones, N.: Strategy for high-accuracy-and-precision retrieval of atmospheric methane from the mid-infrared FTIR network, Atmos. Meas. Tech., 4, 1943–1964, http://dx.doi.org/10.5194/amt-4-1943-2011doi:10.5194/amt-4-1943-2011, 2011. </mixed-citation>
</ref>
<ref id="ref30">
<label>30</label><mixed-citation publication-type="other" xlink:type="simple"> van der Werf, G. R., Randerson, J. T., Giglio, L., Collatz, G. J., Mu, M., Kasibhatla, P. S., Morton, D. C., DeFries, R. S., Jin, Y., and van Leeuwen, T. T.: Global fire emissions and the contribution of deforestation, savanna, forest, agricultural, and peat fires (1997–2009), Atmos. Chem. Phys., 10, 11707–11735, http://dx.doi.org/10.5194/acp-10-11707-2010doi:10.5194/acp-10-11707-2010, 2010. </mixed-citation>
</ref>
<ref id="ref31">
<label>31</label><mixed-citation publication-type="other" xlink:type="simple"> Walter, B. P., Heimann, M., and Matthews, E.: Modeling modern methane emissions from natural wetlands: 2. Interannual variations 1982–1993, J. Geophys. Res., 106, 34207–34219, http://dx.doi.org/10.1029/2001JD900164doi:10.1029/2001JD900164, 2001. </mixed-citation>
</ref>
<ref id="ref32">
<label>32</label><mixed-citation publication-type="other" xlink:type="simple"> WMO World Data Centre for Greenhouse Gases: http://ds.data.jma.go.jp/gmd/wdcgg/introduction.html, last access: 31 March 2012, 2012. </mixed-citation>
</ref>
<ref id="ref33">
<label>33</label><mixed-citation publication-type="other" xlink:type="simple"> Zander, R., Demoulin, Ph., Ehhalt, D. H., and Schmidt, U.: Secular Increase of the Vertical Column Abundance of Methane Derived from IR Solar Spectra Recorded at the Jungfraujoch Station, J. Geophys. Res., 94, 11029–11039, 1989. </mixed-citation>
</ref>
</ref-list>
</back>
</article>