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<article xmlns:xlink="http://www.w3.org/1999/xlink" xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:oasis="http://docs.oasis-open.org/ns/oasis-exchange/table" xml:lang="en" dtd-version="3.0" article-type="review-article"><?xmltex \bartext{Opinion}?>
  <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-23-15445-2023</article-id><title-group><article-title>Paul J. Crutzen – a pioneer in Earth system <?xmltex \hack{\break}?> science and a founding member of the journal <italic>Atmospheric Chemistry and Physics</italic></article-title><alt-title>Paul J. Crutzen – a pioneer in Earth system science</alt-title>
      </title-group><?xmltex \runningtitle{Paul~J.~Crutzen -- a pioneer in Earth system science}?><?xmltex \runningauthor{R.~M\"{u}ller et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Müller</surname><given-names>Rolf</given-names></name>
          <email>ro.mueller@fz.juelich.de</email>
        <ext-link>https://orcid.org/0000-0002-5024-9977</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Pöschl</surname><given-names>Ulrich</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-1412-3557</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Koop</surname><given-names>Thomas</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-7571-3684</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4">
          <name><surname>Peter</surname><given-names>Thomas</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5">
          <name><surname>Carslaw</surname><given-names>Ken</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-6800-154X</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Institute of Energy and Climate Research (IEK-7), Forschungszentrum Jülich, Jülich, Germany</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Multiphase Chemistry Department, Max-Planck-Institut (MPI) für Chemie, Mainz, Germany</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Faculty of Chemistry, Bielefeld University, Bielefeld, Germany </institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>Institute for Atmospheric and Climate Science, ETH Zurich, Zurich, Switzerland</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>Institute for Climate and Atmospheric Science, University of Leeds, Leeds, UK</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Rolf Müller (ro.mueller@fz.juelich.de)</corresp></author-notes><pub-date><day>18</day><month>December</month><year>2023</year></pub-date>
      
      <volume>23</volume>
      <issue>24</issue>
      <fpage>15445</fpage><lpage>15453</lpage>
      <history>
        <date date-type="received"><day>30</day><month>June</month><year>2023</year></date>
           <date date-type="rev-request"><day>5</day><month>July</month><year>2023</year></date>
           <date date-type="rev-recd"><day>27</day><month>October</month><year>2023</year></date>
           <date date-type="accepted"><day>7</day><month>November</month><year>2023</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2023 Rolf Müller et al.</copyright-statement>
        <copyright-year>2023</copyright-year>
      <license license-type="open-access"><license-p>This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><self-uri xlink:href="https://acp.copernicus.org/articles/23/15445/2023/acp-23-15445-2023.html">This article is available from https://acp.copernicus.org/articles/23/15445/2023/acp-23-15445-2023.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/23/15445/2023/acp-23-15445-2023.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/23/15445/2023/acp-23-15445-2023.pdf</self-uri>
      <abstract><title>Abstract</title>

      <p id="d1e149">Paul Jozef Crutzen was a pioneer in the atmospheric sciences, a kind-hearted and humorous person with empathy for the private lives of his colleagues and students, and a man who upheld the highest scientific standards for himself and for others. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere, from the mesosphere to the stratosphere and from the stratosphere to the troposphere. In particular, he was the first to describe the <inline-formula><mml:math id="M1" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-driven ozone depletion cycle in the stratosphere, he was among the first to develop the idea of chemical formation of ozone in the troposphere, he provided key concepts to explain the “ozone hole”, and he made fundamental discoveries about the effects of biomass burning on the troposphere. Understanding and addressing the causes of anthropogenic air pollution and climate change were the driving motivations for his scientific work. In his work, he did not shy away from challenge and provocation. His work on smoke from fires  after a potential nuclear war inspired new research on a concept now known as “nuclear winter”. He also initiated the reopening of the debate on “geoengineering” – a concept now referred to as “climate intervention”. He also brought the term “Anthropocene” to the popular debate. Moreover, he had a strong influence on atmospheric science through his educational role; there is a very large number of outstanding scientists who started their career with scientific work with Paul. In 2000, Paul was among the founders of the journal <italic>Atmospheric Chemistry and Physics</italic>, which was unique at the time in providing public discussion of published preprints as well as what we now call “open access” to published articles. Paul's work on human impacts on atmosphere and climate has had a profound impact on the environmental policies of  many countries for decades. In the future, his work will continue to be a guide for generations of scientists and environmental policymakers to come.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e175">Paul Crutzen was always full of scientific ideas that he pursued and also shared generously with colleagues and students. He was also a very hard-working individual; when he focused on a particular scientific problem, he could forget the world around him. Despite all of his concentration on science, he always had time for his family and never forgot how important the private lives of his colleagues and students were. You could always discuss the events of the day with him, from political issues to the weather and sports.</p>
      <p id="d1e178">Particularly impressive about Paul's scientific achievements is the range of different topics in atmospheric science to which he made fundamental contributions <xref ref-type="bibr" rid="bib1.bibx53 bib1.bibx36" id="paren.1"/>; a short overview is given below in Sect. <xref ref-type="sec" rid="Ch1.S2.SS2"/>. Paul's research interests included topics in<?pagebreak page15446?> the mesosphere, the stratosphere, and the troposphere, with a particular emphasis on the issues of climate change and air quality <xref ref-type="bibr" rid="bib1.bibx33 bib1.bibx34 bib1.bibx35" id="paren.2"><named-content content-type="pre">e.g.</named-content></xref>; in this context, the role of aerosol particles – <?xmltex \hack{\mbox\bgroup}?>including<?xmltex \hack{\egroup}?> black carbon – became a focus of his work <xref ref-type="bibr" rid="bib1.bibx43 bib1.bibx58" id="paren.3"><named-content content-type="pre">e.g.</named-content></xref>. Moreover, he was involved in the first studies on the global effects of a thick smoke layer in the atmosphere produced by fires caused by a possible nuclear war <xref ref-type="bibr" rid="bib1.bibx22 bib1.bibx4" id="paren.4"/>. This work inspired research on “nuclear winter” starting in the mid-1980s <xref ref-type="bibr" rid="bib1.bibx67 bib1.bibx2 bib1.bibx59 bib1.bibx9" id="paren.5"><named-content content-type="pre">e.g.</named-content></xref>. Paul also sparked a new debate by breaking the taboo regarding a possible cooling of the climate by increasing the Earth's albedo through stratospheric sulfur injections <xref ref-type="bibr" rid="bib1.bibx19" id="paren.6"/>. Finally, he popularised the term “Anthropocene” as the epoch dating from the commencement of geologically significant human impact on the Earth's system (<xref ref-type="bibr" rid="bib1.bibx18" id="altparen.7"/>; <xref ref-type="bibr" rid="bib1.bibx24" id="altparen.8"/>; <xref ref-type="bibr" rid="bib1.bibx23" id="altparen.9"/>; <xref ref-type="bibr" rid="bib1.bibx3" id="altparen.10"/>; see also Sect. <xref ref-type="sec" rid="Ch1.S4"/>).</p>
      <p id="d1e227">Paul was  a key figure in establishing the journal <italic>Atmospheric Chemistry and Physics</italic> (ACP). ACP  has been a pioneer in transparent peer review since it was founded in the year 2000 <xref ref-type="bibr" rid="bib1.bibx56 bib1.bibx57 bib1.bibx31" id="paren.11"/>. The special issue “20 years of Atmospheric Chemistry and Physics”, of which this paper is a part and which celebrates more than 20 years of ACP, contains two papers that are directly related to topics that Paul brought up. These two papers are on  the global consequences of a possible nuclear exchange <xref ref-type="bibr" rid="bib1.bibx60" id="paren.12"><named-content content-type="pre">nuclear winter;</named-content></xref> and on climate intervention <xref ref-type="bibr" rid="bib1.bibx68" id="paren.13"/>.</p>
      <p id="d1e244">Paul Crutzen himself provided a very good description of his life and of his scientific work in his published Nobel lecture <xref ref-type="bibr" rid="bib1.bibx17" id="paren.14"/> on the occasion of the 1995 Nobel Prize in Chemistry, which he shared with Mario J. Molina and Frank Sherwood Rowland. Shorter biographical texts are also available <xref ref-type="bibr" rid="bib1.bibx50 bib1.bibx42 bib1.bibx51 bib1.bibx61 bib1.bibx63 bib1.bibx71 bib1.bibx72" id="paren.15"/>. Moreover, there are two more recent and detailed memoirs describing Paul's life and his scientific achievements (<xref ref-type="bibr" rid="bib1.bibx53" id="altparen.16"/>; <xref ref-type="bibr" rid="bib1.bibx36" id="altparen.17"/>; see also <uri>https://www.mpic.de/3864489/paul-crutzen</uri>, last access: 14 December 2023). Finally, there is a book <xref ref-type="bibr" rid="bib1.bibx41" id="paren.18"/> on the recent history (1959–2000) of the Max Planck Institute (MPI) for Chemistry (“Otto-Hahn-Institut”) in Mainz, where Paul worked from 1980; this book also contains a wide range of information on Paul's research during this period.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Paul Crutzen: the person and the scientist</title>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>The person</title>
      <p id="d1e281">Paul Jozef Crutzen was born in Amsterdam on 3 December 1933 and passed away in Mainz on 28 January 2021. He was the son of Anna Gurk and Jozef Crutzen. In Amsterdam, on 14 February 1958, he married Terttu Soininen; Paul and Terttu have two daughters, Ilona and Sylvia, and three grandchildren <xref ref-type="bibr" rid="bib1.bibx53" id="paren.19"/>. There is no doubt that Paul was a very hard-working man. He once said “see, this is the life of a scientist, always working”. He was very dedicated and demanded the same of his collaborators and students. If the only opportunity to talk science with him was on a Saturday afternoon, you had no choice but to accept his invitation and come to the office. However, this intensity also meant that he was always very interested in the work of colleagues and students; you could count on a well-elaborated reply from Paul in a very short time frame to any scientific text you sent him, be it a paper draft, parts of a doctoral thesis, or any other kind of text.</p>
      <p id="d1e287">Nevertheless, no matter how much Paul concentrated on his scientific work, he always had time for his family (Fig. <xref ref-type="fig" rid="Ch1.F1"/>). He himself mentioned that weekends were reserved for family, especially during the time when his daughters were young. The entire Crutzen family has fond memories of family gatherings, weekends, holidays, and vacations with Paul. For his colleagues, Paul was a very pleasant person to be with, and science was not necessarily the main subject of conversation. One could chat with Paul over a coffee or an evening meal on many other topics that he was interested in, such as sports. For example, he was always well-informed about the performance of the Dutch ice-skating team and was interested in football,<fn id="Ch1.Footn1"><p id="d1e292">Football is the game referred to in American English as soccer.</p></fn> particularly with respect to the performance of the top team of his hometown (Ajax Amsterdam). Moreover, he followed the football team of the town that he moved to in 1980 (1. FSV Mainz 05) and watched matches live in the Mainz stadium.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><?xmltex \currentcnt{1}?><?xmltex \def\figurename{Figure}?><label>Figure 1</label><caption><p id="d1e298">Paul Crutzen with his daughter Ilona in 1961 (picture courtesy of Ilona Crutzen).</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/15445/2023/acp-23-15445-2023-f01.jpg"/>

        </fig>

</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>The scientist</title>
      <?pagebreak page15447?><p id="d1e315">Paul's scientific achievements are too numerous and their scope too broad to be covered in detail in this brief note <xref ref-type="bibr" rid="bib1.bibx17 bib1.bibx53 bib1.bibx36" id="paren.20"><named-content content-type="pre">for more information, see e.g.</named-content></xref>. However, stratospheric ozone chemistry, in general, and <inline-formula><mml:math id="M2" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> chemistry, in particular, were what started his scientific work, even before his doctoral research <xref ref-type="bibr" rid="bib1.bibx53" id="paren.21"/>. He proposed the ground-breaking idea that reactions catalysed by NO and <inline-formula><mml:math id="M3" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> control the ozone concentration in the middle stratosphere <xref ref-type="bibr" rid="bib1.bibx11" id="paren.22"/>, according to the following catalytic cycle:

                <disp-formula specific-use="align" content-type="numbered"><mml:math id="M4" display="block"><mml:mtable displaystyle="true"><mml:mlabeledtr id="Ch1.E1"><mml:mtd><mml:mtext>1</mml:mtext></mml:mtd><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow><mml:mo>→</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="Ch1.E2"><mml:mtd><mml:mtext>2</mml:mtext></mml:mtd><mml:mtd><mml:mstyle class="stylechange" displaystyle="true"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">O</mml:mi></mml:mrow><mml:mo>→</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow><mml:mo>.</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula>

            Here, the sum of NO and <inline-formula><mml:math id="M5" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is defined as <inline-formula><mml:math id="M6" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow><mml:mo>=</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:mrow></mml:math></inline-formula> and O indicates that an oxygen atom in its ground state (O(<inline-formula><mml:math id="M7" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:math></inline-formula>P)).</p>
      <p id="d1e476">The discovery of this mechanism in 1970 was a crucial step towards facilitating a quantitative description of the chemistry of the stratospheric ozone layer; prior to Paul's discovery, the dominant catalytic loss cycle of stratospheric ozone (D<inline-formula><mml:math id="M8" display="inline"><mml:msub><mml:mi/><mml:mi mathvariant="normal">N</mml:mi></mml:msub></mml:math></inline-formula>, through Reactions <xref ref-type="disp-formula" rid="Ch1.E1"/> and <xref ref-type="disp-formula" rid="Ch1.E2"/>) was not known (Fig. <xref ref-type="fig" rid="Ch1.F2"/>). It is now known that D<inline-formula><mml:math id="M9" display="inline"><mml:msub><mml:mi/><mml:mrow class="chem"><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:msub></mml:math></inline-formula>, the reaction <inline-formula><mml:math id="M10" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">O</mml:mi></mml:mrow><mml:mo>→</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:mrow></mml:math></inline-formula>, originally proposed by <xref ref-type="bibr" rid="bib1.bibx8" id="text.23"/>, is only a minor sink of stratospheric ozone and that <inline-formula><mml:math id="M11" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">HO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-induced catalysis  is important only close to the tropopause and above about 45 <inline-formula><mml:math id="M12" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula> (e.g. <xref ref-type="bibr" rid="bib1.bibx55" id="altparen.24"/>; see also Fig. <xref ref-type="fig" rid="Ch1.F2"/>). The recognition that chlorine (D<inline-formula><mml:math id="M13" display="inline"><mml:msub><mml:mi/><mml:mi mathvariant="normal">Cl</mml:mi></mml:msub></mml:math></inline-formula>) also catalytically contributes to stratospheric ozone loss came a few years after the discovery of the <inline-formula><mml:math id="M14" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>-induced cycle <xref ref-type="bibr" rid="bib1.bibx49" id="paren.25"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2" specific-use="star"><?xmltex \currentcnt{2}?><?xmltex \def\figurename{Figure}?><label>Figure 2</label><caption><p id="d1e585">Dependence of various production and destruction reactions on altitude: the left-hand panel presents the mean reaction rates; the right hand-panel shows the relative importance of the individual contributions to ozone loss in the gas phase. D<inline-formula><mml:math id="M15" display="inline"><mml:msub><mml:mi/><mml:mrow class="chem"><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:msub></mml:math></inline-formula> represents the Chapman reaction (the reaction <inline-formula><mml:math id="M16" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>), D<inline-formula><mml:math id="M17" display="inline"><mml:msub><mml:mi/><mml:mrow class="chem"><mml:mi mathvariant="normal">N</mml:mi></mml:mrow></mml:msub></mml:math></inline-formula> represents <inline-formula><mml:math id="M18" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> catalysis (Reactions <xref ref-type="disp-formula" rid="Ch1.E1"/> and <xref ref-type="disp-formula" rid="Ch1.E2"/>), D<inline-formula><mml:math id="M19" display="inline"><mml:msub><mml:mi/><mml:mrow class="chem"><mml:mi mathvariant="normal">H</mml:mi></mml:mrow></mml:msub></mml:math></inline-formula> represents <inline-formula><mml:math id="M20" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">HO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> catalysis (by H, OH, and <inline-formula><mml:math id="M21" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">HO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>), and D<inline-formula><mml:math id="M22" display="inline"><mml:msub><mml:mi/><mml:mrow class="chem"><mml:mi mathvariant="normal">Cl</mml:mi></mml:mrow></mml:msub></mml:math></inline-formula> represents <inline-formula><mml:math id="M23" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">ClO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>  catalysis <xref ref-type="bibr" rid="bib1.bibx49" id="paren.26"/>. Moreover, P denotes production of odd oxygen (by the reaction <inline-formula><mml:math id="M24" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow><mml:mo>+</mml:mo><mml:mi>h</mml:mi><mml:mi mathvariant="italic">ν</mml:mi></mml:mrow></mml:math></inline-formula>) and D denotes total ozone destruction. The dominant ozone loss cycle in the stratosphere (D<inline-formula><mml:math id="M25" display="inline"><mml:msub><mml:mi/><mml:mrow class="chem"><mml:mi mathvariant="normal">N</mml:mi></mml:mrow></mml:msub></mml:math></inline-formula>) was not known prior to Paul's work <xref ref-type="bibr" rid="bib1.bibx11" id="paren.27"/>. (Figure adapted from <xref ref-type="bibr" rid="bib1.bibx27" id="altparen.28"/>, and <xref ref-type="bibr" rid="bib1.bibx37" id="altparen.29"/>; figure courtesy of Jens-Uwe Grooß.)</p></caption>
          <?xmltex \igopts{width=455.244094pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/15445/2023/acp-23-15445-2023-f02.png"/>

        </fig>

      <p id="d1e742">The recognition of the strong effect of <inline-formula><mml:math id="M26" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> on stratospheric ozone had a major impact, as emissions of <inline-formula><mml:math id="M27" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> caused by a possible fleet of supersonic planes was the first stratospheric ozone depletion issue that was studied <xref ref-type="bibr" rid="bib1.bibx38 bib1.bibx12" id="paren.30"/>. Paul also investigated how tropospheric nitrogen-containing compounds (like <inline-formula><mml:math id="M28" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula>) can enter the stratosphere and cause the formation of stratospheric <inline-formula><mml:math id="M29" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx10 bib1.bibx52" id="paren.31"/>. He initiated the first studies on the budget of <inline-formula><mml:math id="M30" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula> in the atmosphere and how it is influenced by human activity <xref ref-type="bibr" rid="bib1.bibx10" id="paren.32"/>.</p>
      <p id="d1e814">Tropospheric chemistry, in particular the chemical production of ozone in the troposphere, was of great importance to Paul <xref ref-type="bibr" rid="bib1.bibx17 bib1.bibx36" id="paren.33"/>. The OH radical <xref ref-type="bibr" rid="bib1.bibx44 bib1.bibx25 bib1.bibx17" id="paren.34"/> is responsible for the oxidation of <inline-formula><mml:math id="M31" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> (and many other compounds emitted into the atmosphere). It was found that, in environments containing sufficient NO, the methane oxidation chain could produce ozone in large quantities – compared with the downward flux of ozone from the stratosphere to the troposphere <xref ref-type="bibr" rid="bib1.bibx13 bib1.bibx7" id="paren.35"/>. At that time, very little was known about the homogeneous and heterogeneous reactions affecting the methane oxidation chain in the troposphere; therefore, initial conclusions remained uncertain <xref ref-type="bibr" rid="bib1.bibx15" id="paren.36"/>. However, some years later, along with Jack Fishman and Susan Solomon, Paul presented observational evidence of strong in situ tropospheric ozone production <xref ref-type="bibr" rid="bib1.bibx33 bib1.bibx35" id="paren.37"/>. Later, Paul's work on tropospheric ozone led him to realise the importance of biomass burning for the chemistry of the atmosphere <xref ref-type="bibr" rid="bib1.bibx26 bib1.bibx20" id="paren.38"/>.</p>
      <p id="d1e847">Paul's work on smoke from fires after a possible nuclear war and the absorption of sunlight by the smoke <xref ref-type="bibr" rid="bib1.bibx22 bib1.bibx4" id="paren.39"/> introduced the concept that the use of nuclear weapons would have global impacts that go far beyond the more obvious direct effects. This work inspired substantial research activity: <xref ref-type="bibr" rid="bib1.bibx67" id="text.40"/> and <xref ref-type="bibr" rid="bib1.bibx2" id="text.41"/>, soon followed by <xref ref-type="bibr" rid="bib1.bibx59" id="text.42"/> and <xref ref-type="bibr" rid="bib1.bibx9" id="text.43"/>, calculated the surface temperature response to fires after a nuclear war and introduced the term nuclear winter <xref ref-type="bibr" rid="bib1.bibx60" id="paren.44"><named-content content-type="pre">see also</named-content></xref>. Paul's original intention, however, at the outset of these studies <xref ref-type="bibr" rid="bib1.bibx36" id="paren.45"/> was to explore the impact of nitrogen oxides, which might form as a result of a possible nuclear war, on stratospheric ozone, a concept that had been discussed earlier <xref ref-type="bibr" rid="bib1.bibx69" id="paren.46"><named-content content-type="pre">e.g.</named-content></xref>. Paul counted his contribution to this field as important from a political point of view. Indeed, along with John Birks, Jeannie Peterson, Alan Robock, Carl Sagan, Georgiy Stenchikov, Brian Toon, and Richard Turco, he was presented with the 2022 Future of Life Award (<uri>https://futureoflife.org/project/future-of-life-award/</uri>, last access: 14 December 2023) by the Future of Life Institute.  The award was presented to this team for reducing the risk of nuclear war by developing and popularising the science of nuclear winter.</p>
      <p id="d1e882">After the impact of chlorofluorocarbons (CFCs) on stratospheric ozone was identified <xref ref-type="bibr" rid="bib1.bibx49" id="paren.47"/>, Paul published a modelling study on this topic in the same year <xref ref-type="bibr" rid="bib1.bibx14" id="paren.48"/>. In 1985, the ozone hole was discovered by <xref ref-type="bibr" rid="bib1.bibx32" id="text.49"/>. A year later, Paul – along with Frank Arnold – showed that the formation of stratospheric particles (well above the temperature threshold for ice formation) and the nitric acid uptake into these particles are crucial aspects of ozone hole chemistry <xref ref-type="bibr" rid="bib1.bibx21" id="paren.50"/>. Heterogeneous chemistry <xref ref-type="bibr" rid="bib1.bibx64" id="paren.51"/> and an ozone loss cycle specific for ozone hole conditions <xref ref-type="bibr" rid="bib1.bibx48" id="paren.52"/> turned out to be further key processes explaining the chemical processes responsible for the formation of the ozone hole. Furthermore, Paul suggested that carbonyl sulfide (COS) constitutes the major non-volcanic source of aqueous sulfuric acid aerosol particles in the stratosphere <xref ref-type="bibr" rid="bib1.bibx16" id="paren.53"/>.</p>
      <?pagebreak page15448?><p id="d1e907">In recognition of the importance of the multi-phase chemistry on atmospheric aerosol particles <xref ref-type="bibr" rid="bib1.bibx1" id="paren.54"/> and the many unknown processes regarding their microphysics, Paul initiated a junior research group in Mainz in the early 1990s. The name of the group was “Heterogene Chemie und Mikrophysik atmosphärischer Aerosolteilchen” (“Heterogeneous chemistry and  microphysics of atmospheric aerosol particles” in English). An important starting point of this research was the paper by <xref ref-type="bibr" rid="bib1.bibx46" id="text.55"/>, who reported on the homogeneous and heterogeneous freezing rates of sulfuric acid droplets under stratospheric conditions, which has implications for the theory of the formation of nitric acid trihydrate particles in the polar stratosphere. The three authors of that paper are shown in Fig. <xref ref-type="fig" rid="Ch1.F3"/>. This photograph was taken by Thomas Koop.  At the same time, the scene was photographed by A. R. Ravishankara, who also wanted to take a picture of the authors of the <xref ref-type="bibr" rid="bib1.bibx46" id="text.56"/> paper.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><?xmltex \currentcnt{3}?><?xmltex \def\figurename{Figure}?><label>Figure 3</label><caption><p id="d1e924">Paul Crutzen (right) during a summer school in 1993 with Thomas Peter (left) and Beiping Luo (middle) at Paestum, Italy (picture by Thomas Koop).</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/15445/2023/acp-23-15445-2023-f03.jpg"/>

        </fig>

      <p id="d1e933">Further work of the junior research group showed the occurrence and importance of a new type of polar stratospheric cloud (Type Ib) that consisted of liquid rather than crystalline particles <xref ref-type="bibr" rid="bib1.bibx5 bib1.bibx6 bib1.bibx40" id="paren.57"/>; other groups also investigated liquid polar stratospheric clouds <xref ref-type="bibr" rid="bib1.bibx66" id="paren.58"/>. It later became clear that these liquid clouds, and not the frozen nitric acid hydrate or ice particles, are the main hosts of heterogeneous chemical reactions responsible for chlorine activation and, thus, polar ozone depletion <xref ref-type="bibr" rid="bib1.bibx62 bib1.bibx39" id="paren.59"><named-content content-type="pre">e.g.</named-content></xref>. In another study <xref ref-type="bibr" rid="bib1.bibx47" id="paren.60"/>, the junior research group showed that the composition and freezing behaviour of the liquid particles depends on small-scale temperature fluctuations in the atmosphere. As it turned out, the smallest droplets reached higher <inline-formula><mml:math id="M32" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">HNO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> concentrations than larger ones, thus counterintuitively increasing the smaller droplets' likelihood to crystallise. When Paul, who was himself rather short in stature, first learnt about this result during a discussion, he commented on it with a pinch of self-irony and a big smile: “Never neglect the small ones!”.</p>
      <p id="d1e961">A discussion about Paul as a scientist is not complete without talking about his role in the scientific community. Throughout his career, Paul interacted and collaborated with many important, influential scientists. These collaborations are easily noticeable upon investigation of his list of publications. However, perhaps even more impressive is the educational impact that he had. There is a very large number of outstanding scientists who had – and have – an extraordinary career that started with a PhD, a postdoc, or an early scientific interaction with Paul. The inspiration for these careers clearly came from Paul, and they started at the various institutions at which he was active.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Paul Crutzen and the birth of a new journal</title>
      <?pagebreak page15449?><p id="d1e973">For many years <xref ref-type="bibr" rid="bib1.bibx29" id="paren.61"/>, Paul Crutzen has been an editor of classical journals (<italic>Tellus</italic> and the <italic>Journal of Atmospheric Chemistry</italic>). In 2000, however, Paul was also key in the pioneering work of establishing a new, unique concept of scientific  publishing: public discussion of preprints and open-access publishing. Along with Ulrich Pöschl and Arne Richter, Paul helped found the journal <italic>Atmospheric Chemistry and Physics</italic> (ACP)”, published by the European Geophysical Society (EGS, which is now the European Geosciences Union – EGU). The first paper was submitted to ACP in 2001.</p>
      <p id="d1e988">Scientific discussions have been documented before the invention of ACP; for example, in the <italic>Electronic Transactions in Artificial Intelligence</italic> (ETAI) and the <italic>Journal of Interactive Media in Education</italic> (JIME) <xref ref-type="bibr" rid="bib1.bibx57" id="paren.62"><named-content content-type="post">section “Comparison to earlier initiatives with two- or multi-stage open peer review”</named-content></xref>. Further, the review process in <italic>Journal of the Chemical Society, Faraday Transactions</italic> and in the <italic>Proceedings of the Combustion Institute</italic> is “open”, in the sense that these journals have a long history of meetings and their subsequent publication of the discussion. <italic>Faraday Discussions</italic> collects questions and answers through delegate discussion during meetings (rather than online or through a text forum): a discussion which is then edited and published alongside the articles in each volume. A similar procedure is followed by the Combustion Institute <xref ref-type="bibr" rid="bib1.bibx54" id="paren.63"><named-content content-type="pre">see</named-content><named-content content-type="post">for an example</named-content></xref>. The interactive open-access process (as we call it today) with a multi-stage public peer review as practised in ACP, however, had not been introduced in scientific publishing prior to the launch of ACP <xref ref-type="bibr" rid="bib1.bibx57" id="paren.64"/>.</p>
      <p id="d1e1022">Initially, when the concept of public peer review and a public discussion of submitted manuscripts was introduced, there was some confusion in the community about the status of discussion papers. Since then, however, it has become clear that discussion papers are preprints similar to the manuscripts posted on other preprint servers like <uri>https://arxiv.org/</uri> (last access: 14 December 2023) but with the additional feature of undergoing public peer review and discussion. This is also reflected on the web pages of ACP and other interactive open-access journals of the EGU. The ACP concept is now well-established among EGU journals and, over the years, many newly established journals have followed this example (and future journals will continue to do so; <xref ref-type="bibr" rid="bib1.bibx31" id="altparen.65"/>).</p>
      <p id="d1e1031">In an e-mail on 18 September 2000, Arne Richter wrote that a “meeting of the `younger and wilder' atmospheric scientists under the lead of Ulrich Pöschl and Paul Crutzen regarding the launch of a new EGS journal on atmospheric chemistry took place on 15 September in Mainz”; this meeting was the birthplace of the new journal ACP <xref ref-type="bibr" rid="bib1.bibx28" id="paren.66"/>. ACP was founded in 2000 with Paul as a member of the advisory board. At that time, the development and success of ACP could hardly have been foreseen.</p>
      <p id="d1e1038">Today, ACP is a very well-established and highly ranked scientific journal.  Starting with only 7 published papers in 2001 (34 in 2002 and 158 in 2003) the number of papers published by ACP increased steadily until 2010, when more than 800 papers were published. In recent years, more than 800 papers per year regularly appear in ACP <xref ref-type="bibr" rid="bib1.bibx57 bib1.bibx31" id="paren.67"/>. In Paul's words,<disp-quote>
  <p id="d1e1045">It has been an amazing journey: over a short period of merely a decade, a novel idea originating from Uli Pöschl and developed by an enthusiastic group of hundreds of scientists, created a new way of scientific publishing and communication, initially covering the fields of atmospheric chemistry and physics. The example has since been followed by many successors in other disciplines, with more to come <xref ref-type="bibr" rid="bib1.bibx28" id="paren.68"/>.</p>
</disp-quote></p>
</sec>
<sec id="Ch1.S4">
  <label>4</label><title>Anthropocene</title>
      <p id="d1e1060">With the Anthropocene concept <xref ref-type="bibr" rid="bib1.bibx18 bib1.bibx24 bib1.bibx23 bib1.bibx3" id="paren.69"/>, Paul expressed his insight that humanity is indeed changing the planet as a whole and should take responsibility for its development. He actively advocated this concept until recently (Fig. <xref ref-type="fig" rid="Ch1.F4"/>). The Anthropocene concept also led to the development of the iconic “great acceleration” figures <xref ref-type="bibr" rid="bib1.bibx36" id="paren.70"><named-content content-type="pre">see e.g. Fig. 2 in</named-content></xref> that show increases in population, in greenhouse gases, in fertiliser consumption, and many other signatures of human impact on the Earth system since the industrial revolution <xref ref-type="bibr" rid="bib1.bibx65" id="paren.71"/>.</p>
      <p id="d1e1076">In 2009, the Anthropocene Working Group (AWG; Fig. <xref ref-type="fig" rid="Ch1.F4"/>) was established within the Subcommission on Quaternary Stratigraphy as an interdisciplinary research group dedicated to formalising the Anthropocene as the current geologic time epoch and, more generally, to studying the Anthropocene as a geological time unit. The term Anthropocene became popular after Paul Crutzen proposed it spontaneously at a conference in 2000 to refer to the current epoch <xref ref-type="bibr" rid="bib1.bibx3 bib1.bibx53 bib1.bibx36" id="paren.72"/>.  Today, the evaluation of the Anthropocene as a formal unit in the geological timescale continues <xref ref-type="bibr" rid="bib1.bibx30 bib1.bibx70 bib1.bibx45 bib1.bibx36" id="paren.73"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4"><?xmltex \currentcnt{4}?><?xmltex \def\figurename{Figure}?><label>Figure 4</label><caption><p id="d1e1089">Meeting of the Anthropocene Working Group (AWG) at the Max Planck Institute for Chemistry (MPI für Chemie) in March 2017. The people on the picture, clockwise from bottom left to bottom right, are as follows: Franz Mauelshagen, Institut für transformative Nachhaltigkeitsforschung (IASS), Potsdam; Colin Waters, University of Leicester, Leicester, and AWG; Jürgen Renn, MPI für Wissenschaftsgeschichte, Berlin; Bernd Scherer, Haus der Kulturen der Welt (HKW), Berlin; Jos Lelieveld, MPI für Chemie, Mainz; Reinhold Leinfelder, Freie Universität Berlin, Berlin, and AWG; Davor Vidas, Fridtjof Nansen Institut, Oslo, and AWG; Mark Williams, University of Leicester, Leicester, and AWG; Christoph Rosol, HKW und MPI für Wissenschaftsgeschichte, Berlin; Mark Lawrence, IASS, Potsdam; Susanne Benner, MPI für Chemie, Mainz; Jan Zalasiewicz, University of Leicester, Leicester, and AWG; Astrid Kaltenbach, MPI für Chemie, Mainz; Ulrich Pöschl, MPI für Chemie, Mainz; and Paul J. Crutzen, MPI für Chemie, Mainz, and AWG (picture by Simone Schweller, MPI für Chemie).</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/23/15445/2023/acp-23-15445-2023-f04.jpg"/>

      </fig>

</sec>
<sec id="Ch1.S5" sec-type="conclusions">
  <label>5</label><title>The impact of Paul Crutzen on atmospheric chemistry and physics</title>
      <p id="d1e1107">Paul Crutzen had very broad scientific interests and an enormous influence on science; his interests covered practically the entire atmosphere, from the ground to the mesosphere. The body of Paul's scientific work is too extensive and broad to be covered here, but some examples have been given above. At the same time, the appreciation of Paul's personality would be incomplete without acknowledging his interest and care for the private lives of the people around him, especially his family.</p>
      <?pagebreak page15450?><p id="d1e1110">On top of his contribution to science, he was also a key figure in the development of an entirely  new approach to scientific publishing that began with the journal <italic>Atmospheric Chemistry and Physics</italic> (ACP). When ACP was founded in 2000, it was unique in that it featured public discussion of published preprints and, furthermore, open access to finally accepted and published papers. The 20st anniversary of this journal is celebrated in this special issue. Paul's legacy is honoured in ACP in the form of the ACP Paul Crutzen Publication Award, which was created to recognise an outstanding publication in ACP in a particular year. The first prize was awarded in 2021.</p>
      <?pagebreak page15451?><p id="d1e1116"><?xmltex \hack{\newpage}?>Paul's work not only had a profound impact on the scientific world but also influenced the environmental politics of many countries. His scientific work will continue to provide guidance for the evolution of science. Likewise, his ideas will continue to have a strong influence on future global policies needed to halt the warming of Earth's climate and the destruction of our planet as we know it.</p>
</sec>

      
      </body>
    <back><notes notes-type="dataavailability"><title>Data availability</title>

      <p id="d1e1124">No data sets were used in this article.</p>
  </notes><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e1130">UP, TK, TP, KC, and RM all contributed to putting together the material for this paper and to writing the manuscript.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e1136">At least one of the (co-)authors is a member of the editorial board of <italic>Atmospheric Chemistry and Physics</italic>. The peer-review process was guided by an independent editor, and the authors also have no other competing interests to declare.</p>
  </notes><notes notes-type="disclaimer"><title>Disclaimer</title>

      <p id="d1e1145">Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims made in the text, published maps, institutional affiliations, or any other geographical representation in this paper. While Copernicus Publications makes every effort to include appropriate place names, the final responsibility lies with the authors.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e1151">First of all, we thank Terttu Crutzen for reading and commenting on the manuscript. Further, we thank Susanne Benner, John W. Birks, Guy Brasseur, Sylvia Crutzen, Barbara Ervens, Astrid Kaltenbach, A. R. Ravishankara, and Alan Robock for comments on this paper. We thank Paul's daughter, Ilona, and his grandson, Jamie Paul, for providing pictures from the family archives. Figure <xref ref-type="fig" rid="Ch1.F2"/> is courtesy of Jens-Uwe Grooß.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e1158">The article processing charges for this open-access publication were covered by the Forschungszentrum Jülich.</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e1164">This paper was edited by Barbara Ervens and Gabriele Stiller and reviewed by Alan Robock, Guy Brasseur, and one anonymous referee.</p>
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