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<front>
<journal-meta>
<journal-id journal-id-type="publisher">ACPD</journal-id>
<journal-title-group>
<journal-title>Atmospheric Chemistry and Physics Discussions</journal-title>
<abbrev-journal-title abbrev-type="publisher">ACPD</abbrev-journal-title>
<abbrev-journal-title abbrev-type="nlm-ta">Atmos. Chem. Phys. Discuss.</abbrev-journal-title>
</journal-title-group>
<issn pub-type="epub">1680-7375</issn>
<publisher><publisher-name></publisher-name>
<publisher-loc>Göttingen, Germany</publisher-loc>
</publisher>
</journal-meta>
<article-meta>
<article-id pub-id-type="doi">10.5194/acp-2017-382</article-id>
<title-group>
<article-title>Inconsistent decadal variations between surface and free tropospheric nitrogen oxides over United States</article-title>
</title-group>
<contrib-group><contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Jiang</surname>
<given-names>Zhe</given-names>
<ext-link>https://orcid.org/0000-0002-0086-7486</ext-link>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Worden</surname>
<given-names>Helen</given-names>
<ext-link>https://orcid.org/0000-0002-5949-9307</ext-link>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Worden</surname>
<given-names>John R.</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>Henze</surname>
<given-names>Daven K.</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>Jones</surname>
<given-names>Dylan B. A.</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>Arellano</surname>
<given-names>Avelino F.</given-names>
<ext-link>https://orcid.org/0000-0002-2615-5831</ext-link>
</name>
<xref ref-type="aff" rid="aff5">
<sup>5</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Fischer</surname>
<given-names>Emily V.</given-names>
</name>
<xref ref-type="aff" rid="aff6">
<sup>6</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Zhu</surname>
<given-names>Liye</given-names>
</name>
<xref ref-type="aff" rid="aff6">
<sup>6</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Miyazaki</surname>
<given-names>Kazuyuki</given-names>
<ext-link>https://orcid.org/0000-0002-1466-4655</ext-link>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
<xref ref-type="aff" rid="aff7">
<sup>7</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Boersma</surname>
<given-names>K. Folkert</given-names>
<ext-link>https://orcid.org/0000-0002-4591-7635</ext-link>
</name>
<xref ref-type="aff" rid="aff8">
<sup>8</sup>
</xref>
<xref ref-type="aff" rid="aff9">
<sup>9</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Payne</surname>
<given-names>Vivienne H.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
</contrib-group><aff id="aff1">
<label>1</label>
<addr-line>National Center for Atmospheric Research, Boulder, CO, USA</addr-line>
</aff>
<aff id="aff2">
<label>2</label>
<addr-line>Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA, USA</addr-line>
</aff>
<aff id="aff3">
<label>3</label>
<addr-line>Department of Mechanical Engineering, University of Colorado, Boulder, CO, USA</addr-line>
</aff>
<aff id="aff4">
<label>4</label>
<addr-line>Department of Physics, University of Toronto, Toronto, ON, Canada</addr-line>
</aff>
<aff id="aff5">
<label>5</label>
<addr-line>Department of Hydrology and Atmospheric Sciences, University of Arizona, Tucson, AZ, USA</addr-line>
</aff>
<aff id="aff6">
<label>6</label>
<addr-line>Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA</addr-line>
</aff>
<aff id="aff7">
<label>7</label>
<addr-line>Japan Agency for Marine-Earth Science and Technology, Yokohama, Japan</addr-line>
</aff>
<aff id="aff8">
<label>8</label>
<addr-line>Wageningen University, Meteorological and Air Quality department, Wageningen, the Netherlands</addr-line>
</aff>
<aff id="aff9">
<label>9</label>
<addr-line>Royal Netherlands Meteorological Institute, De Bilt, The Netherlands</addr-line>
</aff>
<pub-date pub-type="epub">
<day>06</day>
<month>06</month>
<year>2017</year>
</pub-date>
<volume>2017</volume>
<fpage>1</fpage>
<lpage>27</lpage>
<permissions>
<copyright-statement>Copyright: &#x000a9; 2017 Zhe Jiang et al.</copyright-statement>
<copyright-year>2017</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/preprints/acp-2017-382/">This article is available from https://acp.copernicus.org/preprints/acp-2017-382/</self-uri>
<self-uri xlink:href="https://acp.copernicus.org/preprints/acp-2017-382/acp-2017-382.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/preprints/acp-2017-382/acp-2017-382.pdf</self-uri>
<abstract>
<p>Decreases in surface emissions of nitrogen oxides (NO&lt;sub&gt;x&lt;/sub&gt;&amp;thinsp;=&amp;thinsp;NO&amp;thinsp;+&amp;thinsp;NO&lt;sub&gt;2&lt;/sub&gt;) in North America have led to substantial improvements in air-quality over the last several decades. Here we show that satellite observations of tropospheric nitrogen dioxide (NO&lt;sub&gt;2&lt;/sub&gt;) columns over the contiguous United States (US) do not decrease after about 2009, while surface NO&lt;sub&gt;2&lt;/sub&gt; concentrations continue to decline through to the present. This divergence, if it continues, could have a substantial impact on surface air quality due to mixing of free-tropospheric air into the boundary layer. Our results show only limited contributions from local effects such as fossil fuel emissions, lightning, or instrument artifacts, but we do find a possible relationship of NO&lt;sub&gt;2&lt;/sub&gt; changes to decadal climate variability. Our analysis demonstrates that the intensity of transpacific transport is stronger in El Niño years and weaker in La Niña years, and consequently, that decadal-scale climate variability impacts the contribution of Asian emissions on North American atmospheric composition. Because of the short lifetime, it is usually believed that the direct contribution of long-range transport to tropospheric NO&lt;sub&gt;x&lt;/sub&gt; distribution is limited. If our hypothesis about transported Asian emissions is correct, then this observed divergence between satellite and surface NO&lt;sub&gt;x&lt;/sub&gt; could indicate mechanisms that allow for either NO&lt;sub&gt;x&lt;/sub&gt; or its reservoir species to have a larger than expected effect on North American tropospheric composition. These results therefore suggest more aircraft and satellite studies to determine the possible missing processes in our understanding of the long-range transport of tropospheric NO&lt;sub&gt;x&lt;/sub&gt;.</p>
</abstract>
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