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  <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-22-10901-2022</article-id><title-group><article-title>Numerical simulation of the impact of COVID-19 lockdown on tropospheric composition and<?xmltex \hack{\break}?> aerosol radiative forcing in Europe</article-title><alt-title>Aerosol effects in BLUESKY simulations</alt-title>
      </title-group><?xmltex \runningtitle{Aerosol effects in BLUESKY simulations}?><?xmltex \runningauthor{S.~F.~Reifenberg et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff12">
          <name><surname>Reifenberg</surname><given-names>Simon F.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-9113-9101</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Martin</surname><given-names>Anna</given-names></name>
          
        <ext-link>https://orcid.org/0009-0009-1822-142X</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Kohl</surname><given-names>Matthias</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-1829-4276</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Bacer</surname><given-names>Sara</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-0052-1968</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Hamryszczak</surname><given-names>Zaneta</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Tadic</surname><given-names>Ivan</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-4419-2502</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Röder</surname><given-names>Lenard</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-1551-009X</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Crowley</surname><given-names>Daniel J.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Fischer</surname><given-names>Horst</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Kaiser</surname><given-names>Katharina</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-3162-2502</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Schneider</surname><given-names>Johannes</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-7169-3973</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Dörich</surname><given-names>Raphael</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Crowley</surname><given-names>John N.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-8669-0230</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3 aff4">
          <name><surname>Tomsche</surname><given-names>Laura</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Marsing</surname><given-names>Andreas</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-5006-2133</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3 aff4">
          <name><surname>Voigt</surname><given-names>Christiane</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-8925-7731</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5">
          <name><surname>Zahn</surname><given-names>Andreas</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff6">
          <name><surname>Pöhlker</surname><given-names>Christopher</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-6958-425X</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff6">
          <name><surname>Holanda</surname><given-names>Bruna A.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff6">
          <name><surname>Krüger</surname><given-names>Ovid</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-3321-6655</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff6">
          <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="aff6 aff7 aff8">
          <name><surname>Pöhlker</surname><given-names>Mira</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Jöckel</surname><given-names>Patrick</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-8964-1394</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Dorf</surname><given-names>Marcel</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Schumann</surname><given-names>Ulrich</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-5255-6869</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Williams</surname><given-names>Jonathan</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-9421-1703</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff9">
          <name><surname>Bohn</surname><given-names>Birger</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-4177-3934</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff10">
          <name><surname>Curtius</surname><given-names>Joachim</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-3153-4630</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Harder</surname><given-names>Hardwig</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-6868-714X</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Schlager</surname><given-names>Hans</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff11">
          <name><surname>Lelieveld</surname><given-names>Jos</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-6307-3846</ext-link></contrib>
        <contrib contrib-type="author" corresp="yes" rid="aff1 aff11">
          <name><surname>Pozzer</surname><given-names>Andrea</given-names></name>
          <email>andrea.pozzer@mpic.de</email>
        <ext-link>https://orcid.org/0000-0003-2440-6104</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Atmospheric Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Particle Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Institute of Atmospheric Physics, Deutsches Zentrum für Luft- und Raumfahrt (DLR),<?xmltex \hack{\break}?> Oberpfaffenhofen, Germany</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>Institute for Physics of the Atmosphere, Johannes Gutenberg University Mainz, Mainz, Germany</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany</institution>
        </aff>
        <aff id="aff6"><label>6</label><institution>Multiphase Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany</institution>
        </aff>
        <aff id="aff7"><label>7</label><institution>Faculty of Physics and Earth Sciences, Leipzig Institute for Meteorology, University of Leipzig,<?xmltex \hack{\break}?> Leipzig, Germany</institution>
        </aff>
        <aff id="aff8"><label>8</label><institution>Experimental Aerosol and Cloud Microphysics Department, Leibniz Institute for Tropospheric Research, Leipzig, Germany</institution>
        </aff>
        <aff id="aff9"><label>9</label><institution>Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH,<?xmltex \hack{\break}?> Jülich, Germany</institution>
        </aff>
        <aff id="aff10"><label>10</label><institution>Institute for Atmospheric and Environmental Sciences, Goethe University of Frankfurt,<?xmltex \hack{\break}?> Frankfurt am Main, Germany</institution>
        </aff>
        <aff id="aff11"><label>11</label><institution>Climate and Atmosphere Research Center, The Cyprus Institute, Nicosia, Cyprus</institution>
        </aff>
        <aff id="aff12"><label>a</label><institution>now at: MARUM – Center for Marine Environmental Science, University of Bremen, Bremen, Germany</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Andrea Pozzer (andrea.pozzer@mpic.de)</corresp></author-notes><pub-date><day>26</day><month>August</month><year>2022</year></pub-date>
      
      <volume>22</volume>
      <issue>16</issue>
      <fpage>10901</fpage><lpage>10917</lpage>
      <history>
        <date date-type="received"><day>2</day><month>December</month><year>2021</year></date>
           <date date-type="accepted"><day>7</day><month>July</month><year>2022</year></date>
           <date date-type="rev-recd"><day>27</day><month>June</month><year>2022</year></date>
           <date date-type="rev-request"><day>10</day><month>December</month><year>2021</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2022 </copyright-statement>
        <copyright-year>2022</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/.html">This article is available from https://acp.copernicus.org/articles/.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/.pdf</self-uri>
      <abstract><title>Abstract</title>

      <p id="d1e453">Aerosols influence the Earth's energy balance directly by modifying the radiation transfer and
indirectly by altering the cloud microphysics.
Anthropogenic aerosol emissions dropped considerably  when the global COVID-19 pandemic
resulted in severe restraints on mobility, production, and public life in spring 2020.
We assess the effects of these reduced emissions
on direct and indirect aerosol radiative forcing over Europe, excluding contributions from contrails.
We simulate the atmospheric composition with the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model
in a baseline (business-as-usual) and a reduced emission scenario.
The model results are compared to aircraft observations
from the BLUESKY aircraft campaign performed in May–June 2020 over Europe.
The model agrees well with most of the observations, except for sulfur dioxide, particulate sulfate,
and nitrate in the upper troposphere, likely due to a biased representation of stratospheric aerosol chemistry
and missing information about volcanic eruptions.
The comparison with a baseline scenario shows that the largest relative differences for tracers
and aerosols are  found in the upper troposphere, around the aircraft cruise altitude, due to the
reduced aircraft emissions, while the largest absolute changes are present at the surface.
We also find an increase in all-sky shortwave radiation of 0.21 <inline-formula><mml:math id="M1" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05 <inline-formula><mml:math id="M2" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> at the surface in Europe for May 2020,
solely attributable to the direct aerosol effect, which is dominated by decreased aerosol scattering of sunlight,
followed by reduced aerosol absorption caused by lower concentrations of inorganic and black carbon aerosols in the troposphere.
A further increase in shortwave radiation from aerosol indirect effects was found to be much
smaller than its variability.
Impacts on ice crystal concentrations, cloud droplet number concentrations, and effective crystal radii are found to be negligible.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e489">Aerosols play a pivotal role in both air pollution and climate change.
They have large impact on human health <xref ref-type="bibr" rid="bib1.bibx39 bib1.bibx41" id="paren.1"/>,
impose a negative (net) effective radiative forcing <xref ref-type="bibr" rid="bib1.bibx6" id="paren.2"/>, and
are a large source of uncertainty in climate change assessments.
A reduction in the cooling effect by a decreased aerosol burden necessitates stronger reductions of
greenhouse gases (GHGs) for a targeted net radiative forcing <xref ref-type="bibr" rid="bib1.bibx35 bib1.bibx53" id="paren.3"/>.</p>
      <p id="d1e501">Owing to the central importance of aerosol particles, the reduced emissions resulting from drastic restrictions on mobility,
industry, and public life during the COVID-19 “lockdowns” in early 2020
(hereafter referred to as “lockdown”) <xref ref-type="bibr" rid="bib1.bibx4 bib1.bibx13 bib1.bibx20 bib1.bibx36" id="paren.4"/> sparked a plethora of publications on
the subsequent effects on local, regional, and global air pollution <xref ref-type="bibr" rid="bib1.bibx21 bib1.bibx42 bib1.bibx56 bib1.bibx73 bib1.bibx77 bib1.bibx51" id="paren.5"><named-content content-type="pre">see, for instance,</named-content></xref>.</p>
      <p id="d1e512">We recognize that reduced emissions during lockdown do not necessarily translate into improved air quality,
as primary pollutants take part in a complex set of chemical processes,
which need to be included in a thorough analysis <xref ref-type="bibr" rid="bib1.bibx31" id="paren.6"/>.
For instance, although ozone  was reported to be reduced in the free troposphere in the Northern Hemisphere <xref ref-type="bibr" rid="bib1.bibx70" id="paren.7"/>,
the reduced emissions of the nitrogen oxides <inline-formula><mml:math id="M3" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M4" 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>
led to an increase in ozone concentrations in urban locations,
as an important short-term sink (reaction with <inline-formula><mml:math id="M5" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow></mml:math></inline-formula>) was reduced <xref ref-type="bibr" rid="bib1.bibx18 bib1.bibx69 bib1.bibx51" id="paren.8"><named-content content-type="pre">e.g.,</named-content></xref>.
This illustrates how the complex (photo-)chemistry and the nonlinearity of the underlying
chemical system have to be described and analyzed within the framework of a dynamic atmospheric chemistry model.
A chemistry climate model with appropriate chemistry furthermore enables
a direct comparison of baseline and reduced emissions
within the same synoptic background conditions, complementary to a purely observation-based approach.
Many works are present in the literature that investigate the climatic effect of COVID-19 lockdown
<xref ref-type="bibr" rid="bib1.bibx37 bib1.bibx14 bib1.bibx17" id="paren.9"><named-content content-type="pre">e.g.,</named-content></xref>.
Of particular importance is the CovidMIP intercomparison project,
where 12 global chemistry climate model were used to investigate the impact of COVID-19 lockdown
on the radiation <xref ref-type="bibr" rid="bib1.bibx27 bib1.bibx34" id="paren.10"/>, with special focus on aerosol–radiation interaction.</p>
      <p id="d1e562">The interaction of aerosols with radiation and their climatic impact
can be categorized into two types:
(i) direct effects by impact on radiation fluxes and (ii) indirect effects through
changes in cloud physical and optical properties.</p>
      <p id="d1e566">The direct effects include absorption and scattering of electromagnetic waves, whereby
aerosol particles, most prominently black carbon (BC), absorb incoming solar radiation,
which leads to warming of the ambient air and decreases solar irradiance in the layers below.
In addition, aerosols scatter incident radiation back to space,
leading to a net cooling of the climate system on average.
These processes depend on the size, shape,
and chemical composition of the aerosols and on the wavelength of the radiation.
In addition, the net effect depends on the surface albedo <xref ref-type="bibr" rid="bib1.bibx68 bib1.bibx80 bib1.bibx6" id="paren.11"/>.
The reduced emissions in spring 2020 are thus expected to affect aerosol radiative forcing.
A reduction in the backscattering of solar radiation is expected to result in warming,
which is offset by the anticipated cooling effect through a
reduction of black carbon emissions, and the net effect may vary vertically and horizontally.
For instance, <xref ref-type="bibr" rid="bib1.bibx17" id="text.12"/> reported a simulated net warming
at the surface and in the lower troposphere in most regions
caused by enhanced  insolation at the surface
and cooling in upper layers of the troposphere due to reduced absorption by black carbon.
They also determined a difference in the clear-sky net shortwave (SW) flux at the top of the atmosphere (TOA)
of up to 0.1 <inline-formula><mml:math id="M6" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> globally in May 2020 between simulations with and without reduced emissions,
i.e., less outgoing SW radiation due to the lockdown.
Complementing the analyses regarding these more immediate effects,
<xref ref-type="bibr" rid="bib1.bibx14" id="text.13"/> estimate a short-term warming driven
by a weakened aerosol cooling through reduced sulfur dioxide (<inline-formula><mml:math id="M7" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) emissions,
followed by a cooling of 0.010 <inline-formula><mml:math id="M8" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.005 <inline-formula><mml:math id="M9" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi></mml:mrow></mml:math></inline-formula> by 2030
in reference to a baseline scenario.</p>
      <p id="d1e622">In addition to the aerosol direct effects on the radiation budget, aerosol particles have several indirect effects.
Aerosol particles serve as cloud condensation nuclei and thus can potentially alter cloud properties, such as cloud albedo, cloud droplet number concentration,
formation processes, precipitation, and cloud lifetime <xref ref-type="bibr" rid="bib1.bibx6 bib1.bibx8 bib1.bibx44 bib1.bibx76" id="paren.14"><named-content content-type="pre">see, for instance,</named-content></xref>.
In turn, clouds also affect aerosols. Clouds convert precursor gases into aerosol particles through heterogeneous chemistry
<xref ref-type="bibr" rid="bib1.bibx12 bib1.bibx38 bib1.bibx50" id="paren.15"/> and, at the same time, remove aerosols and soluble gases from the atmosphere by precipitation (“wet deposition”).
Radiative forcing from aerosol cloud interactions is very challenging to quantify, and it is strongly
model dependent  <xref ref-type="bibr" rid="bib1.bibx23 bib1.bibx16 bib1.bibx53" id="paren.16"/>.
Recently, satellite data have been used to quantify changes in clouds in regions with COVID-reduced
air traffic in 2020 <xref ref-type="bibr" rid="bib1.bibx61 bib1.bibx17" id="paren.17"/>.
With respect to contrails, <xref ref-type="bibr" rid="bib1.bibx65 bib1.bibx66" id="text.18"/> find a substantial reduction
of contrail cirrus optical thickness and radiative forcing during the lockdown period.</p>
      <p id="d1e642">Complex models like as the one used by the CovidMIP, however, are most effective when accompanied by observational data,
as the capability of the models to reproduce the real
atmosphere is unclear, especially when the anthropogenic emissions are strongly perturbed as in the
case of the COVID-19 lockdown. Furthermore, as the reduced emissions have different effect
on the atmospheric composition depending also on the altitude, the observational data should
cover large regions of the troposphere.
Despite the large presence of observations at the surface during the COVID-19 lockdown <xref ref-type="bibr" rid="bib1.bibx18" id="paren.19"/>,
the free and upper troposphere presented comparably almost no in situ measurements against which
the model could be validated.
One notable exception is the BLUESKY field campaign <xref ref-type="bibr" rid="bib1.bibx78" id="paren.20"/>:
from 16 May to 9 June 2020 in situ measurements of trace gases and trace particles were conducted
in the atmosphere over European urban areas and the North Atlantic flight corridor
with the High Altitude and Long Range (HALO)
research aircraft and a second research aircraft, Falcon
(see Fig. <xref ref-type="fig" rid="Ch1.F1"/> for flight paths).
Comprehensive measurements of trace gas and aerosol compositions were conducted, providing
a unique set of observations that can be used to validate model results.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><?xmltex \currentcnt{1}?><?xmltex \def\figurename{Figure}?><label>Figure 1</label><caption><p id="d1e655">Tracks of conducted flights during the BLUESKY campaign (16 May to 9 June 2020). Colors denote the aircraft: Falcon (blue) and HALO (red).</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/10901/2022/acp-22-10901-2022-f01.png"/>

      </fig>

      <p id="d1e664">Using an observation-guided model, the COVID-19 lockdown provided an opportunity to examine
how the climate system reacts to perturbations such as abruptly reduced air pollution emissions.
The COVID-19 lockdown may also serve to assess the impact of economic recovery with respect to climate change mitigation:
for instance, <xref ref-type="bibr" rid="bib1.bibx14" id="text.21"/> show that investments aimed at a “green” opposed to a fossil-fueled recovery
can reduce projected warming by 0.3 <inline-formula><mml:math id="M10" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi></mml:mrow></mml:math></inline-formula> by 2050, with only negligible contributions from the lockdown.</p>
      <p id="d1e679">In the present study, we simulate the chemical composition of the atmosphere in Europe in spring 2020
under a reduced-emission scenario and a baseline scenario with a state-of-the-art
climate and chemistry simulation system, constraining atmospheric dynamics by reanalysis meteorological data.
We use the BLUESKY observational data set of trace gases and aerosols obtained during
an aircraft measurement campaign in Europe during the COVID-19 lockdown in summer 2020 to evaluate the model results.
We then quantify the effects of the lockdown on radiative transfer in the atmosphere,
particularly the change in shortwave fluxes and shortwave heating rates attributable to a reduced aerosol burden in Europe.
Furthermore, we examine the impacts of the reduced emissions on cloud properties,
including potential changes of the radiative forcing caused by indirect aerosol effects.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Data and methods</title>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>Model data</title>
      <p id="d1e697">The ECHAM5/MESSy Atmospheric Chemistry (EMAC) model is a numerical chemistry
and climate simulation system that includes submodels describing tropospheric
and middle-atmospheric processes and their
interaction with oceans, land, and human influences <xref ref-type="bibr" rid="bib1.bibx26" id="paren.22"/>.
It uses the second version of the Modular Earth Submodel System (MESSy2)
to link multi-institutional computer codes.
The core atmospheric model is the fifth-generation European Centre Hamburg general circulation model <xref ref-type="bibr" rid="bib1.bibx64" id="paren.23"><named-content content-type="pre">ECHAM5,</named-content></xref>.</p>
      <p id="d1e708">For the present study we applied EMAC (ECHAM5 version 5.3.02, MESSy version 2.55.0) in T63L47MA resolution,
i.e., with a spherical truncation of T63 (corresponding to a quadratic Gaussian grid of approx.
1.8<inline-formula><mml:math id="M11" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> by 1.8<inline-formula><mml:math id="M12" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> in latitude and longitude) with 47 vertical hybrid pressure levels up to 1 Pa.
Roughly 22 levels are included in the troposphere, and the model has a time step of 300 s.
The dynamics of the EMAC model has been weakly nudged in the troposphere
<xref ref-type="bibr" rid="bib1.bibx24 bib1.bibx25 bib1.bibx43" id="paren.24"/>
towards the ERA5 meteorological reanalysis data <xref ref-type="bibr" rid="bib1.bibx22" id="paren.25"/>
of the European Centre for Medium-Range Weather Forecasts (ECMWF) to represent
the actual day to day meteorology in the troposphere.</p>
      <p id="d1e735"><?xmltex \hack{\newpage}?>The setup of the chemistry submodels for this study is similar to the one presented by
<xref ref-type="bibr" rid="bib1.bibx26" id="text.26"><named-content content-type="post">simulation RC1–aero–07</named-content></xref>
but with the addition of the submodel ORACLE <xref ref-type="bibr" rid="bib1.bibx75" id="paren.27"/> for the organic
chemistry calculation and with stratospheric heterogeneous chemistry neglected.
Initial conditions for the meteorology were also taken from the ERA-Interim reanalysis data,
while the ones for the chemical composition were from previous EMAC simulations <xref ref-type="bibr" rid="bib1.bibx59" id="paren.28"/>.
In addition, the anthropogenic emissions used are based on CAMS-GLOB-ANTv4.2 <xref ref-type="bibr" rid="bib1.bibx19" id="paren.29"/>.
To reproduce the effect of lockdown on the emissions, we adopted the reduction coefficient for
Europe as in <xref ref-type="bibr" rid="bib1.bibx20" id="text.30"/> for the sectors of energy production (ENE), road transport (TRO),
and industrial processes (IND). The reduced emissions were
averaged for the period 19 to 26 April (i.e., the last available week in the data set),
and applied (for each country) for March, April, May, and June.
For aviation (AVI) we adopted the same method, although we applied the estimated
factor to the entire aviation emissions, without any country distinction.</p>
      <p id="d1e756">Atmospheric aerosols are described via a two-moment aerosol scheme,
which predicts number concentration and mass mixing ratio of the aerosol modes <xref ref-type="bibr" rid="bib1.bibx60" id="paren.31"/>.
This scheme takes into account various physical and chemical processes of aerosols,
such as coagulation, aging, condensation, and gas–aerosol
partitioning <xref ref-type="bibr" rid="bib1.bibx15" id="paren.32"/>.
Convective cloud processes are accounted for using the framework of <xref ref-type="bibr" rid="bib1.bibx74" id="text.33"/>,
based on the convection schemes of <xref ref-type="bibr" rid="bib1.bibx72" id="text.34"/> and <xref ref-type="bibr" rid="bib1.bibx55" id="text.35"/>.
Convective cloud microphysics does not take into account the influence of aerosols
on liquid droplet or ice formation processes and is solely based on temperature and vertical velocity.
In EMAC, the vertical velocity is given by the sum of the grid mean vertical velocity and
the turbulent contribution <xref ref-type="bibr" rid="bib1.bibx7" id="paren.36"/>, and thus one single updraft velocity is used for the whole grid cell.
Large-scale stratiform clouds are described by the CLOUD submodel,
which, in the setup applied here, uses a two-moment cloud
microphysics scheme for cloud droplets and ice crystals
<xref ref-type="bibr" rid="bib1.bibx48 bib1.bibx49 bib1.bibx46" id="paren.37"/>
and solves the prognostic equations for specific humidity, liquid cloud mixing ratio,
ice cloud mixing ratio, cloud droplet number concentration (CDNC),
and ice crystal number concentration (ICNC).
The model setup without cloud–aerosol interactions
uses the original ECHAM5 cloud microphysical scheme
<xref ref-type="bibr" rid="bib1.bibx47" id="paren.38"/> and a statistical cloud cover scheme including prognostic equations
for the distribution moments <xref ref-type="bibr" rid="bib1.bibx71" id="paren.39"/>.
Details on the cloud microphysical scheme can be found in
<xref ref-type="bibr" rid="bib1.bibx63" id="text.40"><named-content content-type="post">and references therein</named-content></xref>.</p>
      <p id="d1e793">Cloud droplet formation in the model setup without cloud–aerosol interaction
is computed by the “unified activation framework”,
an advanced physically based parameterization <xref ref-type="bibr" rid="bib1.bibx33 bib1.bibx28" id="paren.41"/>
that combines the <inline-formula><mml:math id="M13" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula>-Köhler theory
<xref ref-type="bibr" rid="bib1.bibx57" id="paren.42"/>
for the activation of soluble aerosols with the Frenkel–Halsey–Hill
adsorption activation theory <xref ref-type="bibr" rid="bib1.bibx33" id="paren.43"/>
for the droplet activation due to water adsorption onto insoluble aerosols.
Ice formation occurs via homogeneous ice nucleation following the parameterization
of <xref ref-type="bibr" rid="bib1.bibx3" id="text.44"/> and heterogeneous ice nucleation of insoluble dust,
insoluble black carbon, and glassy organics following <xref ref-type="bibr" rid="bib1.bibx58" id="text.45"/>.
In the cirrus regime (<inline-formula><mml:math id="M14" display="inline"><mml:mrow><mml:mi>T</mml:mi><mml:mo>≤</mml:mo><mml:mn mathvariant="normal">238.15</mml:mn></mml:mrow></mml:math></inline-formula> K), the effect of preexisting ice crystals
and the competition for the available water vapor between homogeneous and
heterogeneous ice nucleation mechanisms are taken into account <xref ref-type="bibr" rid="bib1.bibx1" id="paren.46"/>.
Given the high contribution of instantaneous freezing <xref ref-type="bibr" rid="bib1.bibx2" id="paren.47"/>,
the ICNC in the cirrus regime was modified according to <xref ref-type="bibr" rid="bib1.bibx54" id="text.48"/>
in order to reduce the artificial homogeneous freezing of dry aerosol particles
independent of the availability of water vapor.
Other microphysical processes related to cloud droplets and ice crystals,
like phase transitions, autoconversion, aggregation, accretion, evaporation, and
melting, are also taken into account by the CLOUD submodel.
The cloud cover is computed diagnostically with the scheme of <xref ref-type="bibr" rid="bib1.bibx71" id="text.49"/>,
which is based on the grid-mean relative humidity.</p>
      <p id="d1e843">The aerosol forcing of the EMAC model has been investigated,
and here we report the effective radiative forcing of the aerosol–radiation interaction
(ERF<inline-formula><mml:math id="M15" display="inline"><mml:msub><mml:mi/><mml:mtext>ari</mml:mtext></mml:msub></mml:math></inline-formula>) and the effective radiative forcing of the aerosol–cloud interaction
(ERF<inline-formula><mml:math id="M16" display="inline"><mml:msub><mml:mi/><mml:mtext>aci</mml:mtext></mml:msub></mml:math></inline-formula>), based on the definition of <xref ref-type="bibr" rid="bib1.bibx53" id="text.50"/>.
Following the work of <xref ref-type="bibr" rid="bib1.bibx40" id="text.51"/>,
the EMAC model, in a setup very similar to ours, simulates
a radiative forcing global mean of all anthropogenic aerosols
at TOA (top of the atmosphere)
of <inline-formula><mml:math id="M17" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.46</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M18" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.01 and <inline-formula><mml:math id="M19" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1.2</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M20" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1 <inline-formula><mml:math id="M21" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>
for ERF<inline-formula><mml:math id="M22" display="inline"><mml:msub><mml:mi/><mml:mtext>ari</mml:mtext></mml:msub></mml:math></inline-formula> and
ERF<inline-formula><mml:math id="M23" display="inline"><mml:msub><mml:mi/><mml:mtext>ari</mml:mtext></mml:msub></mml:math></inline-formula> + ERF<inline-formula><mml:math id="M24" display="inline"><mml:msub><mml:mi/><mml:mtext>aci</mml:mtext></mml:msub></mml:math></inline-formula>, respectively.
At the BOA (bottom of the atmosphere) the model simulates <inline-formula><mml:math id="M25" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1.6</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M26" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.02
and <inline-formula><mml:math id="M27" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2.1</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M28" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.1 <inline-formula><mml:math id="M29" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for ERF<inline-formula><mml:math id="M30" display="inline"><mml:msub><mml:mi/><mml:mtext>ari</mml:mtext></mml:msub></mml:math></inline-formula> and ERF<inline-formula><mml:math id="M31" display="inline"><mml:msub><mml:mi/><mml:mtext>ari</mml:mtext></mml:msub></mml:math></inline-formula> + ERF<inline-formula><mml:math id="M32" display="inline"><mml:msub><mml:mi/><mml:mtext>aci</mml:mtext></mml:msub></mml:math></inline-formula>, respectively.</p>
      <p id="d1e1029">We performed four simulations, all covering the period from January 2019 to July 2020.
<list list-type="bullet"><list-item>
      <p id="d1e1034">BASE, i.e., standard (“baseline”) emissions, without cloud–aerosol interaction;</p></list-item><list-item>
      <p id="d1e1038">RED, i.e., reduced emissions due to lockdown, without cloud–aerosol interaction;</p></list-item><list-item>
      <p id="d1e1042">BASECLOUD, which was like BASE but with aerosol–cloud interaction;</p></list-item><list-item>
      <p id="d1e1046">REDCLOUD, which was like RED but with aerosol–cloud interaction.</p></list-item></list></p>
      <p id="d1e1049">In all simulations performed, the impact of different aerosol concentrations
on the radiation (discussed in Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS1"/>) is
diagnosed but not used by the general circulation model, which instead
adopts an aerosol climatology <xref ref-type="bibr" rid="bib1.bibx60" id="paren.52"/>.
Similarly, changes in the tracers (e.g., ozone)
do not influence the radiation, which is calculated with a greenhouse gas climatology.</p>
      <p id="d1e1057">The model evaluation is performed with the RED simulation, while its difference with the BASE simulation
is used to evaluate the impact of the reduced emissions during the lockdown.
Simulation RED and BASE have identical binary dynamics <xref ref-type="bibr" rid="bib1.bibx10" id="paren.53"/>, i.e., they
reproduce numerically exactly the same dynamics, as no feedback between chemistry and dynamic is present.
In contrast, in REDCLOUD and BASECLOUD the aerosol–cloud interaction is activated
following the work of <xref ref-type="bibr" rid="bib1.bibx45 bib1.bibx1" id="text.54"/>,
leading to modification of cloud
properties and therefore to changes in radiation and dynamics.
The simulations REDCLOUD and BASECLOUD are only used for estimating the indirect effects of aerosols
(see Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS2"/>).</p>
</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>BLUESKY observational data</title>
      <p id="d1e1076">We compare simulated trace gas and aerosol abundances to a comprehensive set of observations
obtained during the BLUESKY campaign <xref ref-type="bibr" rid="bib1.bibx78" id="paren.55"/>.
In situ measurements of trace gases and trace particles were conducted at the end of May 2022
in the atmosphere over Europe with the Falcon and HALO
research aircraft.
In total 8 and 12 flights were conducted with the HALO and the Falcon,
respectively (Fig. <xref ref-type="fig" rid="Ch1.F1"/>).</p>
      <p id="d1e1084">We compare aerosol mass concentrations of black carbon (BC, size range between 70 and 500 <inline-formula><mml:math id="M33" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">nm</mml:mi></mml:mrow></mml:math></inline-formula>), sulfate (<inline-formula><mml:math id="M34" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>), nitrate (<inline-formula><mml:math id="M35" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>-</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula>), ammonium (<inline-formula><mml:math id="M36" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">NH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mo>+</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula>), organic aerosol particles
(ORG, all from 40 to 800 <inline-formula><mml:math id="M37" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">nm</mml:mi></mml:mrow></mml:math></inline-formula>), and aerosol particle number concentrations (between 250 <inline-formula><mml:math id="M38" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">nm</mml:mi></mml:mrow></mml:math></inline-formula> to 40 <inline-formula><mml:math id="M39" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>).
These are complemented by volume mixing ratios of carbon monoxide (<inline-formula><mml:math id="M40" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula>),
ozone (<inline-formula><mml:math id="M41" display="inline"><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:math></inline-formula>), nitric oxide (<inline-formula><mml:math id="M42" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow></mml:math></inline-formula>), hydrogen peroxide (<inline-formula><mml:math id="M43" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>),
peroxyacetyl nitrate (PAN), nitric acid (<inline-formula><mml:math id="M44" 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>),
and sulfur dioxide (<inline-formula><mml:math id="M45" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>). Details regarding instrumentation are provided by <xref ref-type="bibr" rid="bib1.bibx78" id="text.56"/>.
We additionally use air temperature <inline-formula><mml:math id="M46" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula>, wind speed, and specific humidity <inline-formula><mml:math id="M47" display="inline"><mml:mi>q</mml:mi></mml:math></inline-formula>
to assess the quality of the reproduced synoptic conditions
that are constrained (nudged) in the model.
For the comparison, the model output was sampled during runtime
by the submodel S4D <xref ref-type="bibr" rid="bib1.bibx26" id="paren.57"/>,
following the flight tracks of the field campaign and with a time frequency of 5 min.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Model evaluation</title>
      <p id="d1e1262">The ambient air temperature <inline-formula><mml:math id="M48" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula> is reproduced very well by the model;
the average ratio of observed and simulated <inline-formula><mml:math id="M49" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula> is equal to 1.00
with a normalized root-mean-squared error of 0.04 (NRMSE; RMSE divided by range of observations).
The vertical temperature profile is matched in the lower and free troposphere
with a slight underestimation of observed temperatures towards the upper troposphere (Fig. <xref ref-type="fig" rid="Ch1.F2"/>),
which confirms the quality of the nudged data.
Specific humidity <inline-formula><mml:math id="M50" display="inline"><mml:mi>q</mml:mi></mml:math></inline-formula>, a quantity that is not subject to nudging, is also captured reasonably well in the model,
(<inline-formula><mml:math id="M51" display="inline"><mml:mrow><mml:mtext>NRMSE</mml:mtext><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.06</mml:mn></mml:mrow></mml:math></inline-formula>), as 85.9 % of simulated values lie within a factor of 2 of the observations, and
yet they are slightly overestimated (see Fig. <xref ref-type="fig" rid="Ch1.F2"/> and Table <xref ref-type="table" rid="Ch1.T1"/>).
In addition, horizontal wind speed <inline-formula><mml:math id="M52" display="inline"><mml:mrow><mml:mo>‖</mml:mo><mml:msub><mml:mi mathvariant="bold-italic">u</mml:mi><mml:mi mathvariant="normal">h</mml:mi></mml:msub><mml:mo>‖</mml:mo></mml:mrow></mml:math></inline-formula> is also reproduced accurately
with a low NRMSE (0.06) and an average ratio of 1.02.</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="d1e1322">Vertical distribution of simulated (red, simulation RED) and observed (blue) tracer mixing ratios and two meteorological variables (<inline-formula><mml:math id="M53" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M54" display="inline"><mml:mi>q</mml:mi></mml:math></inline-formula>), represented by box–whisker plots for pressure bins. The white line marks the median, the box corresponds to lower and upper quartiles, the whiskers represent the 5th–95th percentile. The grey numbers on the right indicate the sample size (number of observed and interpolated simulated data points) for each pressure bin.
Simulated values are from the RED simulation, i.e., with reduced emissions and no aerosol–cloud interactions.
For <inline-formula><mml:math id="M55" 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> and <inline-formula><mml:math id="M56" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> (measured onboard the Falcon aircraft, shown by the grey number marked with asterisks) the domain average
of the model results over Europe at the corresponding altitude were used, not the values sampled online on the flight track.
</p></caption>
        <?xmltex \igopts{width=455.244094pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/10901/2022/acp-22-10901-2022-f02.png"/>

      </fig>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1"><?xmltex \currentcnt{1}?><label>Table 1</label><caption><p id="d1e1370">Summary of model–observation comparison. The same spatiotemporal location was used
for all simultaneously available points.
NRMSE is the root-mean-squared error normalized by the range of the observations.
PF2 denotes the percentage of model points within a factor of 2 of the observations.
The column <inline-formula><mml:math id="M57" display="inline"><mml:mover accent="true"><mml:mrow><mml:mtext>MOD</mml:mtext><mml:mo>/</mml:mo><mml:mtext>OBS</mml:mtext></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:math></inline-formula> is the average of the simulated and observed data ratios.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="4">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Variable</oasis:entry>
         <oasis:entry colname="col2">NRMSE</oasis:entry>
         <oasis:entry colname="col3">PF2</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M58" display="inline"><mml:mover accent="true"><mml:mrow><mml:mtext>MOD</mml:mtext><mml:mo>/</mml:mo><mml:mtext>OBS</mml:mtext></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Trace gases</oasis:entry>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M59" display="inline"><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:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.04</oasis:entry>
         <oasis:entry colname="col3">94.7</oasis:entry>
         <oasis:entry colname="col4">1.25</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M60" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.14</oasis:entry>
         <oasis:entry colname="col3">99.3</oasis:entry>
         <oasis:entry colname="col4">0.98</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M61" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.08</oasis:entry>
         <oasis:entry colname="col3">65.0</oasis:entry>
         <oasis:entry colname="col4">0.99</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M62" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.32</oasis:entry>
         <oasis:entry colname="col3">61.5</oasis:entry>
         <oasis:entry colname="col4">2.01</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M63" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">PAN</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.13</oasis:entry>
         <oasis:entry colname="col3">60.3</oasis:entry>
         <oasis:entry colname="col4">1.91</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M64" 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></oasis:entry>
         <oasis:entry colname="col2">0.37</oasis:entry>
         <oasis:entry colname="col3">12.9</oasis:entry>
         <oasis:entry colname="col4">0.46</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"><inline-formula><mml:math id="M65" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.40</oasis:entry>
         <oasis:entry colname="col3">25.9</oasis:entry>
         <oasis:entry colname="col4">0.43</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Aerosols</oasis:entry>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">BC</oasis:entry>
         <oasis:entry colname="col2">0.09</oasis:entry>
         <oasis:entry colname="col3">18.6</oasis:entry>
         <oasis:entry colname="col4">0.68</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M66" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>-</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.14</oasis:entry>
         <oasis:entry colname="col3">20.6</oasis:entry>
         <oasis:entry colname="col4">0.92</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M67" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">NH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mo>+</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.22</oasis:entry>
         <oasis:entry colname="col3">28.8</oasis:entry>
         <oasis:entry colname="col4">0.83</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M68" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.16</oasis:entry>
         <oasis:entry colname="col3">26.8</oasis:entry>
         <oasis:entry colname="col4">0.72</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Organics</oasis:entry>
         <oasis:entry colname="col2">0.45</oasis:entry>
         <oasis:entry colname="col3">40.6</oasis:entry>
         <oasis:entry colname="col4">1.73</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Number conc.</oasis:entry>
         <oasis:entry colname="col2">0.11</oasis:entry>
         <oasis:entry colname="col3">42.8</oasis:entry>
         <oasis:entry colname="col4">2.60</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Meteorology</oasis:entry>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
         <oasis:entry colname="col4"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M69" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.04</oasis:entry>
         <oasis:entry colname="col3">100.0</oasis:entry>
         <oasis:entry colname="col4">1.00</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M70" display="inline"><mml:mi>q</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.06</oasis:entry>
         <oasis:entry colname="col3">85.9</oasis:entry>
         <oasis:entry colname="col4">1.27</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M71" display="inline"><mml:mrow><mml:mo>‖</mml:mo><mml:msub><mml:mi mathvariant="bold-italic">u</mml:mi><mml:mi mathvariant="normal">h</mml:mi></mml:msub><mml:mo>‖</mml:mo></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.06</oasis:entry>
         <oasis:entry colname="col3">100.0</oasis:entry>
         <oasis:entry colname="col4">1.02</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p id="d1e1837">Overall, the agreement between the meteorological variables from the model and
those observed in the BLUESKY campaign
indicates successful initialization and nudging
of meteorological variables and that the meteorological conditions
during the relevant time period are simulated adequately.
As the model is not nudged in the stratosphere or boundary layer (the nudging
coefficient is maximal in the free troposphere, <xref ref-type="bibr" rid="bib1.bibx25" id="altparen.58"/>),
the deviation in the upper troposphere between model results and observational data
are to be expected due to the intrinsic model dynamics, which deviates from the nudging data.
Nevertheless, the temperature bias is much lower than in other EMAC studies, despite the use of same nudging method
and coefficients <xref ref-type="bibr" rid="bib1.bibx26" id="paren.59"/>, due to the initialization and shorter simulation time in this work.
As temperature and humidity are important quantities regarding cloud formation
and accurate wind vectors are key for representing advective processes,
the following analyses of atmospheric composition and the effects on radiative transfer
build on an accurate representation of the meteorological state of the model.</p><?xmltex \hack{\newpage}?>
<sec id="Ch1.S3.SS1">
  <label>3.1</label><title>Trace gases</title>
      <p id="d1e1854">More than 94 % of simulated ozone (<inline-formula><mml:math id="M72" display="inline"><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:math></inline-formula>) mixing ratios are within a factor of 2 of the observations
(“PF2” value) and the normalized root-mean-squared error of 0.04 is low,
with improvements from previous evaluation of the same model <xref ref-type="bibr" rid="bib1.bibx26" id="paren.60"/>.
Nevertheless, the model seems to slightly overestimate the observations,
as already pointed out in various studies <xref ref-type="bibr" rid="bib1.bibx26" id="paren.61"><named-content content-type="pre">e.g.,</named-content></xref>.</p>
      <p id="d1e1876">Simulated carbon monoxide (<inline-formula><mml:math id="M73" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula>) mixing ratios are also in good agreement with the observations,
and virtually all simulated values lie within a factor of 2 of the observations.
However, especially at lower altitudes, the simulated mixing ratios underestimate the observed values,
although the difference between average observations and average model results are well within their respective variability,
and the shape of the vertical profile is qualitatively well reproduced.
The same holds for nitric oxide (<inline-formula><mml:math id="M74" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow></mml:math></inline-formula>), which exhibits a C-shaped profile.
The NRMSE for <inline-formula><mml:math id="M75" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow></mml:math></inline-formula> is low (0.08) and the average ratio of simulated to observed mixing ratio is 0.99;
however, more than a third of simulated values deviate more than a factor of 2 from the observations
due to the high variability of this tracer.
Specifically, the range of the observed mixing ratios close to the surface is not well reproduced by the model,
which results from the short lifetime of <inline-formula><mml:math id="M76" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow></mml:math></inline-formula> and the challenge in reproducing
its local variation by a global model.</p>
      <p id="d1e1911">Hydrogen peroxide (<inline-formula><mml:math id="M77" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) and peroxyacetyl nitrate (PAN) are less well represented,
the average ratios of simulated to observed mixing ratio (2.01 for <inline-formula><mml:math id="M78" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and 1.91 for <inline-formula><mml:math id="M79" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">PAN</mml:mi></mml:mrow></mml:math></inline-formula>)
indicate an overestimation by the model.
Nevertheless, for both species about two-thirds of the simulated points
are still within a factor of 2 of the observations
(see Fig. <xref ref-type="fig" rid="Ch1.F2"/>),
and the measured dependence on altitude is captured by the model.</p>
      <p id="d1e1956">Sulfur dioxide (<inline-formula><mml:math id="M80" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) was sampled predominantly at high altitudes
between 370 to 170 <inline-formula><mml:math id="M81" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>, where it is strongly underestimated by the model.
We hypothesize that the systematic underestimation of <inline-formula><mml:math id="M82" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>
concentrations is due to model shortcomings within the stratospheric aerosol chemistry,
which will be discussed briefly as part of the following Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>.
All in all, as summarized in Table <xref ref-type="table" rid="Ch1.T1"/>, there is reasonable agreement
between observed and simulated mixing ratios of the trace gases investigated.</p>
</sec>
<sec id="Ch1.S3.SS2">
  <label>3.2</label><title>Aerosols</title>
      <p id="d1e2001">In the comparison between model results and aerosol observations, the instrumental
cutoffs have been taken into account; the aerosol log-normal modes in the model have been
integrated only in the appropriate range to have a reasonable comparison.
In addition, all the measurements and model results are based on location
pressure and temperature and are not normalized to Standard Temperature and Pressure (STP).</p>
      <p id="d1e2004">The vertical profile of the measured aerosol number concentration is qualitatively reproduced
(see Fig. <xref ref-type="fig" rid="Ch1.F3"/>, with logarithmic scale on the <inline-formula><mml:math id="M83" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> axis),
with a minimum at <inline-formula><mml:math id="M84" display="inline"><mml:mrow><mml:mo>≃</mml:mo><mml:mn mathvariant="normal">300</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M85" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> and a maximum at the surface.
In the lowest-altitude pressure bin, the range and median of the observations and
model results match very well.
There are some deviations between 850 and 480 <inline-formula><mml:math id="M86" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>, where simulated number concentrations
are larger than the observed ones, although this overestimation is well within the observations' variability.
This overestimation dominates the average ratio of modeled to measured values
(2.60, see Table <xref ref-type="table" rid="Ch1.T1"/>).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><?xmltex \currentcnt{3}?><?xmltex \def\figurename{Figure}?><label>Figure 3</label><caption><p id="d1e2047">The same as Fig. <xref ref-type="fig" rid="Ch1.F2"/> but for aerosols. Please note the logarithmic scale on the <inline-formula><mml:math id="M87" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> axis.</p></caption>
          <?xmltex \igopts{width=455.244094pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/10901/2022/acp-22-10901-2022-f03.png"/>

        </fig>

      <p id="d1e2066">The measured black carbon (BC) concentrations are captured well by the model close to the surface,
while the observational variability is underestimated at high altitudes.
The NRMSE of 0.09 is relatively low, as the higher abundance closer to the surface
– that is, closer to the sources – is well represented, both in terms of magnitude
and variability.
A detail analysis of the black carbon concentration simulated with the EMAC model
during the BLUESKY campaign can be found in <xref ref-type="bibr" rid="bib1.bibx32" id="text.62"/>.</p>
      <p id="d1e2072">Sulfate (<inline-formula><mml:math id="M88" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>) exhibits qualitatively similar features to BC;
the relatively high concentrations observed in the lower troposphere are matched by the simulated concentrations,
yet there is a significant underestimation of sulfate aerosol concentrations in the upper troposphere.</p>
      <p id="d1e2092">Between 1050 and 625 <inline-formula><mml:math id="M89" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> simulated organic aerosol concentrations are somewhat
larger in the model than in reality;
the shape of the vertical profile is, however, qualitatively reproduced.</p>
      <p id="d1e2103">Nitrate (<inline-formula><mml:math id="M90" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>-</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula>) and ammonium (<inline-formula><mml:math id="M91" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">NH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mo>+</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula>) concentrations close to the surface are generally
well reproduced.
While at higher altitudes the simulated <inline-formula><mml:math id="M92" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">NH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mo>+</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> agrees with the observations,
simulated nitrate is too high, which is probably related to the co-located underestimation of sulfate.</p>
      <p id="d1e2148">The results of the model–measurement comparison are summarized in Table <xref ref-type="table" rid="Ch1.T1"/>.
We can observe that there is generally reasonable agreement between simulated and observed
trace gases and aerosols with some deviation of the aerosol concentrations,
especially in the mid-upper troposphere.</p>
      <p id="d1e2153">A single emission source causing the model underestimation of BC and sulfate aerosol concentrations in the upper troposphere,
e.g., a localized plume of pollution, is judged unlikely, as BC and <inline-formula><mml:math id="M93" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> do not correlate (<inline-formula><mml:math id="M94" display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M95" display="inline"><mml:mrow><mml:mi>p</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.90</mml:mn></mml:mrow></mml:math></inline-formula>):
in fact, mapping observed <inline-formula><mml:math id="M96" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> concentrations to ozone (a tracer of stratospheric air)
and carbon monoxide (a tracer of tropospheric air) reveals that high <inline-formula><mml:math id="M97" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> concentrations
coincide with high ozone (<inline-formula><mml:math id="M98" display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.83</mml:mn></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M99" display="inline"><mml:mrow><mml:mi>p</mml:mi><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula>) and low carbon monoxide (<inline-formula><mml:math id="M100" display="inline"><mml:mrow><mml:mi>r</mml:mi><mml:mo>=</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.65</mml:mn></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M101" display="inline"><mml:mrow><mml:mi>p</mml:mi><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula>) (Fig. <xref ref-type="fig" rid="Ch1.F4"/>).
A similar, yet weaker, correspondence can be found in the simulated data (see  Fig. <xref ref-type="fig" rid="Ch1.F4"/>).
The strong correlation with ozone in the upper troposphere implies a stratospheric source of sulfate aerosols in both model and reality.
It is noteworthy that a precursor for sulfate aerosols, sulfur dioxide, is also systematically underestimated.
We assume hence that the high <inline-formula><mml:math id="M102" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> abundance measured in the upper troposphere has stratospheric
origin and is from volcanic eruptions.
Many small- and medium-sized eruptions were reported in the year prior to the BLUESKY
campaign (<uri>https://volcano.si.edu</uri>, last access: 30 October 2021),
but their influence on the  upper troposphere and lower stratosphere
is yet to be quantified.
We tested this by injecting high levels of <inline-formula><mml:math id="M103" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> in the stratosphere in additional simulations,
mimicking volcanic eruptions that had enough energy to reach the
stratosphere, i.e., Raikoke (June) and Ulawun (June and August) in 2019
<xref ref-type="bibr" rid="bib1.bibx9 bib1.bibx30" id="paren.63"><named-content content-type="pre">see</named-content></xref>.
However, this did not affect the concentrations of <inline-formula><mml:math id="M104" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M105" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>-</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula>
significantly (not shown).
A partial increase of <inline-formula><mml:math id="M106" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> was obtained by including the volcanic eruption
of Taal in January 2020.
Nevertheless, this is still not enough to bring the model results close to the observations.
We therefore conclude that our observed underestimation of <inline-formula><mml:math id="M107" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>
is of stratospheric origin, although it is not fully clear what caused it.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><?xmltex \currentcnt{4}?><?xmltex \def\figurename{Figure}?><label>Figure 4</label><caption><p id="d1e2386">Scatter plot of co-located <inline-formula><mml:math id="M108" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M109" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula> (red), and <inline-formula><mml:math id="M110" display="inline"><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:math></inline-formula> (blue)
abundance between 350 and 150 <inline-formula><mml:math id="M111" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula> from observations <bold>(a)</bold> and the RED simulation <bold>(b)</bold>.</p></caption>
          <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/10901/2022/acp-22-10901-2022-f04.png"/>

        </fig>

      <p id="d1e2440">A further partition of the region of interest into three subregions (central Europe, southern Europe, Atlantic)
did not reveal substantial spatial dependencies of model deviation from observations (not shown).</p>
</sec>
</sec>
<sec id="Ch1.S4">
  <label>4</label><title>Impact of reduced emissions</title>
      <p id="d1e2452">To quantify the effect of the lockdown, we use the baseline simulations (BASE and BASECLOUD)
in the analyses.
We focus on May 2020, as this time period is covered by the measurement campaign
and the atmosphere can be expected to have adjusted to the impact of abruptly reduced emissions.
We also analyze the impact in an area encompassing Europe (the region of study),
i.e., over a longitude–latitude box from <inline-formula><mml:math id="M112" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">20</mml:mn></mml:mrow></mml:math></inline-formula> to 20<inline-formula><mml:math id="M113" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E and 30 to 60<inline-formula><mml:math id="M114" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N
(exactly the depicted map sector in Fig. <xref ref-type="fig" rid="Ch1.F1"/>).</p>
<sec id="Ch1.S4.SS1">
  <label>4.1</label><title>Impact on tracers and aerosols</title>
      <p id="d1e2492">As no difference in dynamics between RED and BASE simulations are present,
any chemical differences between these simulations are purely attributable
to the different emissions during the lockdown period, as these are the only
changes between these two simulations, and the consequent different chemical regimes.</p>
      <p id="d1e2495">In general, while large absolute changes are expected at the surface, in the upper troposphere (UT) we find the largest relative changes
due to the strong influence of the local emissions and
to the low mixing ratios of most of the species investigated (see Fig. <xref ref-type="fig" rid="Ch1.F5"/>).
Large relative changes in the UT are found for <inline-formula><mml:math id="M115" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M116" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, and BC,
with a strong reduction (<inline-formula><mml:math id="M117" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">50</mml:mn></mml:mrow></mml:math></inline-formula> % or more)
in the region between 200 and 300 <inline-formula><mml:math id="M118" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>,
i.e., the typical aircraft cruise altitude.
The reduced air traffic during the lockdown period greatly decreased
the emissions of nitrogen oxides into the UT,
and the effects of the lockdown on other tracers in the UT are mostly a result of this strong reduction.
Hydroxyl radicals (<inline-formula><mml:math id="M119" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">OH</mml:mi></mml:mrow></mml:math></inline-formula>) decrease by roughly 20 % in the UT and
5 % elsewhere in the troposphere, a direct effect of a reduced
<inline-formula><mml:math id="M120" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">OH</mml:mi></mml:mrow></mml:math></inline-formula> recycling by <inline-formula><mml:math id="M121" 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>.
Despite the reduced OH, carbon monoxide does not increase due to the decrease in the direct emissions.
The overall effect of the lockdown for most tracers is a combination of reduced emissions and
reduced sinks (i.e., oxidation via <inline-formula><mml:math id="M122" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">OH</mml:mi></mml:mrow></mml:math></inline-formula>):
while this is well balanced for <inline-formula><mml:math id="M123" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula> (changes on the order of few percent),
for <inline-formula><mml:math id="M124" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> the emission reductions are larger than the decrease in the reaction with <inline-formula><mml:math id="M125" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">OH</mml:mi></mml:mrow></mml:math></inline-formula>,
causing its mixing ratio to be reduced (up to 50 % in the UT) compared to the baseline scenario.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><?xmltex \currentcnt{5}?><?xmltex \def\figurename{Figure}?><label>Figure 5</label><caption><p id="d1e2603">Vertical profiles from BASE and RED simulations and their relative difference (<inline-formula><mml:math id="M126" display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:mtext>RED</mml:mtext><mml:mo>-</mml:mo><mml:mtext>BASE</mml:mtext><mml:mo>)</mml:mo><mml:mo>/</mml:mo><mml:mtext>BASE</mml:mtext></mml:mrow></mml:math></inline-formula>). The grey area represents 1 standard deviation of the spatial–temporal mean (grey line).
Please note the different scales for the relative differences.</p></caption>
          <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/10901/2022/acp-22-10901-2022-f05.png"/>

        </fig>

      <p id="d1e2633">Similar to the trace gases, for most aerosols the lockdown reduces their concentration mostly at the surface,
although the largest relative differences are simulated in the UT
due to the low concentration at these altitudes.
For example, sulfate is subject to a large relative change in the UT
but to much larger absolute changes close to the surface, mimicking the changes in <inline-formula><mml:math id="M127" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> (see also Fig. <xref ref-type="fig" rid="Ch1.F6"/>).
Furthermore, BC decreases significantly in the whole troposphere
due to the strong reduction of the emissions both at the surface and in the UT (from aircraft).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><?xmltex \currentcnt{6}?><?xmltex \def\figurename{Figure}?><label>Figure 6</label><caption><p id="d1e2651">Vertical profiles of the difference in monthly mean sulfate mass concentration (<inline-formula><mml:math id="M128" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>), black carbon mass concentration (BC), heating rate (<inline-formula><mml:math id="M129" display="inline"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>T</mml:mi><mml:mo>/</mml:mo><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:math></inline-formula>), and net shortwave flux (<inline-formula><mml:math id="M130" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mtext>SW</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>) between the reduced emission scenario RED and the standard emission scenario BASE. Shortwave flux and shortwave heating are derived under clear-sky conditions. The shading indicates 1 standard deviation of the monthly mean difference. Note the logarithmic horizontal axis for the two plots on the left.</p></caption>
          <?xmltex \igopts{width=455.244094pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/10901/2022/acp-22-10901-2022-f06.png"/>

        </fig>

      <p id="d1e2704">While the changes in CO and NO can be considered significant and
representative of the real atmospheric changes (due to the low
bias at all tropospheric levels between model results and observations),
changes in the aerosol components should be considered with caution,
as these are generally smaller than the bias between the model results and the observations.</p>
</sec>
<sec id="Ch1.S4.SS2">
  <label>4.2</label><title>Impact on shortwave radiation</title>
      <p id="d1e2715">As the model is nudged in the troposphere (i.e., constrained air temperature with prescribed sea surface temperatures)
and free to adjust dynamics of the stratosphere, we report here RF (radiative forcing) values <xref ref-type="bibr" rid="bib1.bibx53" id="paren.64"/>.
For the same reason (i.e. tropospheric nudging), we mostly focus the analyses on the shortwave flux
<inline-formula><mml:math id="M131" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mtext>SW</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> and its induced heating rate <inline-formula><mml:math id="M132" display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:mo>∂</mml:mo><mml:mi>T</mml:mi><mml:mo>/</mml:mo><mml:mo>∂</mml:mo><mml:mi>t</mml:mi><mml:msub><mml:mo>)</mml:mo><mml:mtext>SW</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>
in the area encompassing Europe, as these are directly influenced
by the aerosols changes and are not strongly influenced by the numerical forcing.</p><?xmltex \hack{\newpage}?>
<sec id="Ch1.S4.SS2.SSS1">
  <label>4.2.1</label><title>Direct effects</title>
      <p id="d1e2763">Aerosols directly impact the radiation balance by absorption and scattering of electromagnetic waves.
Compared to the baseline emissions, the monthly mean sulfate (and inorganic aerosols, not shown)
and black carbon concentrations are reduced in the entire troposphere, with a strong
relative reduction at the commercial flight level
(around 200 <inline-formula><mml:math id="M133" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>; see Fig. <xref ref-type="fig" rid="Ch1.F6"/>).
Furthermore, the mean aerosol (number) concentrations
were reduced in the scenario with reduced emissions due to lockdown throughout the whole air column
(see Fig. <xref ref-type="fig" rid="Ch1.F8"/> and Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS2"/>),
with the reduction being most pronounced between 300 and 200 <inline-formula><mml:math id="M134" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>.
Based on  model results from  a sensitivity simulation,
where only the aircraft emissions were reduced compared to the BASE simulation,
we estimated that more than 90 % of the reduced aerosol numbers between 300 and 200 <inline-formula><mml:math id="M135" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>
over Europe are due to reduced aircraft emissions.</p>
      <p id="d1e2797">We calculate the simulated difference in the downwelling shortwave flux between simulation RED and STD,
i.e., the impact of the reduced emissions on the SW radiation.
Here only the aerosol contribution is estimated, removing any radiative effect from
changes in trace gases (e.g., ozone) within the Europe longitude–latitude box for May 2020.
The differences are largest over continental central Europe and lowest over northern Scandinavia (Fig. <xref ref-type="fig" rid="Ch1.F7"/>),
with no large spatial gradients over Europe.
In virtually all regions there is more downwelling shortwave radiation in the reduced-emission scenario.
Spatially averaged at ground level within the European domain,
there is an increase of 0.33 <inline-formula><mml:math id="M136" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.10 <inline-formula><mml:math id="M137" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>
under clear-sky conditions (i.e., no clouds)
compared to the baseline scenario, while at the TOA the increase
is 0.20 <inline-formula><mml:math id="M138" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09 <inline-formula><mml:math id="M139" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>.
This increase, together with the reduced heating rates of ambient air,
is indicative of a reduction in shortwave scattering and absorption,
due to the reduced inorganic aerosol and black carbon concentrations,
i.e., the lockdown contributed to make the atmosphere more
transparent to SW radiation.
The column-integrated contribution of backscatter and absorption can
be estimated from the radiation values at TOA and surface, indicating that
during lockdown the total backscatter (clear sky)
of SW radiation has been decreased by 0.26 <inline-formula><mml:math id="M140" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.07 <inline-formula><mml:math id="M141" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>,
while the total absorption (clear sky) was decreased by
0.06 <inline-formula><mml:math id="M142" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.05 <inline-formula><mml:math id="M143" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>.
Based on an additional sensitivity simulations,
in which only individual emissions (i.e., of BC, <inline-formula><mml:math id="M144" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, NO) have been reduced,
we found that slightly more than one-third of the absorption reduction
is caused by the BC decrease.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7"><?xmltex \currentcnt{7}?><?xmltex \def\figurename{Figure}?><label>Figure 7</label><caption><p id="d1e2912">Difference in monthly mean clear-sky shortwave radiation (May 2020) at the surface between RED and BASE simulation. Positive (red) values indicate more incoming radiation at the surface due to less absorption and backscattering in the “lockdown” atmosphere than in the baseline scenario. Note that we used a common reduction factor for emissions from countries outside Europe.</p></caption>
            <?xmltex \igopts{width=184.942913pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/10901/2022/acp-22-10901-2022-f07.png"/>

          </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8" specific-use="star"><?xmltex \currentcnt{8}?><?xmltex \def\figurename{Figure}?><label>Figure 8</label><caption><p id="d1e2924">Vertical profiles of the monthly mean ice crystal number concentration (ICNC), cloud droplet number concentration (CDNC), aerosol number concentration (<inline-formula><mml:math id="M145" display="inline"><mml:mi>N</mml:mi></mml:math></inline-formula>), and ice crystal effective radius (<inline-formula><mml:math id="M146" display="inline"><mml:mi>r</mml:mi></mml:math></inline-formula>) of the reduced-emission scenario REDCLOUD (red), the standard emission scenario BASECLOUD (blue), and their relative difference (grey line) for May 2020 over Europe. The grey area denotes the spatial and temporal standard deviation of the relative difference.</p></caption>
            <?xmltex \igopts{width=483.69685pt}?><graphic xlink:href="https://acp.copernicus.org/articles/22/10901/2022/acp-22-10901-2022-f08.png"/>

          </fig>

      <p id="d1e2947">Reduced scattering by aerosol particles plays a larger role, as the “net”
(i.e., the difference attributable to the lockdown) shortwave flux is positive
in the whole air column;
on the other hand, reduced absorption dominates the shortwave component
of direct aerosol effects in the boundary layer,
as clearly shown in Fig. <xref ref-type="fig" rid="Ch1.F6"/>.
The heating of ambient air exhibits a local minimum in the upper troposphere,
which is, however, small compared to that in the lower troposphere.
We calculate the surface integral of the accumulated heating due to shortwave fluxes,
only attributable to aerosols under clear-sky conditions:
the difference in the atmospheric layer directly above the surface is <inline-formula><mml:math id="M147" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.005</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M148" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.001 <inline-formula><mml:math id="M149" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">d</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>,
i.e., less heating of the boundary layer in the lockdown conditions compared to normal emissions.
Based on a sensitivity simulation similar to RED but without any reduction in BC,
we found that the decreased heating is by 40 % to the reduced absorption by BC during the lockdown conditions,
causing a cooling of the atmosphere (through SW radiation)
despite an increase of the incoming radiation.
Both the changes in heating and shortwave flux are solely attributable to the different aerosol burden in the BASE and RED simulations.</p>
      <p id="d1e2986">We also estimated the RF<inline-formula><mml:math id="M150" display="inline"><mml:msub><mml:mi/><mml:mtext>ari</mml:mtext></mml:msub></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx53" id="text.65"/> due to COVID-19 lockdown
against the baseline scenario,  by also including the longwave radiation.
We obtained an RF<inline-formula><mml:math id="M151" display="inline"><mml:msub><mml:mi/><mml:mtext>ari</mml:mtext></mml:msub></mml:math></inline-formula> equal to 0.08 <inline-formula><mml:math id="M152" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.03
for all-sky measurements over Europe in May 2020 at the TOA.
This value, despite only accounting for a limited amount of the anthropogenic aerosols
(the lockdown did not remove all anthropogenic emissions) and only referring to Europe,
is within the range suggested by <xref ref-type="bibr" rid="bib1.bibx6" id="text.66"><named-content content-type="post">see Table 5</named-content></xref>.</p>
</sec>
<sec id="Ch1.S4.SS2.SSS2">
  <label>4.2.2</label><title>Aerosol–cloud interactions</title>
      <p id="d1e3030">In Fig. <xref ref-type="fig" rid="Ch1.F8"/>, the vertical distributions of the total aerosol number concentration
(N, including all aerosol sizes),
ice crystal number concentration (ICNC),
cloud droplet number concentration (CDNC), and ice crystal radius (<inline-formula><mml:math id="M153" display="inline"><mml:mi>r</mml:mi></mml:math></inline-formula>)
are shown for Europe for both simulations, BASECLOUD and REDCLOUD.
Additionally, the SW flux at the TOA and the surface have been calculated
from these coupled aerosol–cloud simulations (see Table <xref ref-type="table" rid="Ch1.T2"/>)
for both the total effect (i.e., direct plus indirect) and the indirect effect
(i.e., neglecting any direct radiation influence of the aerosol particles).
Due to the short simulation period, the difference between these simulations
is much smaller than its variability, represented by its spatial and temporal standard deviation.
Nevertheless, comparing the vertical distribution of number concentrations of aerosols, ice crystals, and cloud droplets,
the largest relative difference between BASECLOUD and REDCLOUD
(i.e., the two simulations where the aerosol–cloud feedback is activated)
is found for the aerosol number concentration between 200 and 300 <inline-formula><mml:math id="M154" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>.
These are the cruise altitudes at which the largest aircraft emissions are injected in the model,
and therefore these differences can be directly connected
to the reduced air traffic present during the lockdown (REDCLOUD).
As this altitude is somewhat higher than the typical (cold) cloud altitude,
the effect on clouds is less pronounced.
At the highest level of these clouds (see Fig. <xref ref-type="fig" rid="Ch1.F8"/>) the ICNC
are reduced (by <inline-formula><mml:math id="M155" display="inline"><mml:mrow><mml:mo>≃</mml:mo><mml:mn mathvariant="normal">30</mml:mn></mml:mrow></mml:math></inline-formula> % at 250 hPa, although with large variability),
while no visible effect is found for CDNC.
These results are in line with those obtained by <xref ref-type="bibr" rid="bib1.bibx62" id="text.67"/>,
who showed that aircraft emissions do increase ice crystal number concentration,
although their results were not statistically significant.
The ice crystal effective radius seems to be the least affected
by the reduced emissions during the COVID-19 lockdown,
with a negligible absolute and relative difference.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T2"><?xmltex \currentcnt{2}?><label>Table 2</label><caption><p id="d1e3071">Aerosol direct and indirect effects on the shortwave radiation flux at the top of atmosphere (TOA) and surface (SRF) over Europe for May compared to baseline scenario.
Note that direct effects are derived from BASE and RED simulations, and indirect and total (i.e., direct plus indirect) effects from BASECLOUD and REDCLOUD.
The indirect effect of clear-sky estimation is obviously equal to zero, but it was included to confirm the validity of the calculations.</p></caption><oasis:table frame="topbot"><?xmltex \begin{scaleboxenv}{0.9}[0.9]?><oasis:tgroup cols="4">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:thead>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M156" display="inline"><mml:mrow><mml:mtext>RED</mml:mtext><mml:mo>-</mml:mo><mml:mtext>BASE</mml:mtext></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry rowsep="1" namest="col3" nameend="col4" align="center"><inline-formula><mml:math id="M157" display="inline"><mml:mrow><mml:mtext>REDCLOUD</mml:mtext><mml:mo>-</mml:mo><mml:mtext>BASECLOUD</mml:mtext></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"><inline-formula><mml:math id="M158" display="inline"><mml:mrow><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi>F</mml:mi><mml:mtext>SW</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M159" display="inline"><mml:mrow class="unit"><mml:mo>[</mml:mo><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup><mml:mo>]</mml:mo></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">direct</oasis:entry>
         <oasis:entry colname="col3">indirect</oasis:entry>
         <oasis:entry colname="col4">total</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">TOA</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M160" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.09</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.03</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M161" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.19</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.76</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M162" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.28</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.93</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">TOA clear sky</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M163" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.20</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.09</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M164" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.00</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M165" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.19</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.11</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">SRF</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M166" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.21</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.05</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M167" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.23</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">1.09</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M168" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.44</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">1.06</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">SRF clear sky</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M169" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.33</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.10</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M170" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.00</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M171" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.31</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.11</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup><?xmltex \end{scaleboxenv}?></oasis:table></table-wrap>

      <p id="d1e3352">To investigate the effect of reduced aircraft emissions on the SW flux via the indirect aerosol effect at the TOA and surface (SRF),
the mean differences in SW flux between REDCLOUD and BASECLOUD for May were calculated over Europe.
Positive values indicate greater reflection of SW radiation back to space (for TOA)
or more absorption through the troposphere (for surface values) in the BASECLOUD simulation
compared to the REDCLOUD simulation.
The mean surface differences are 0.31 <inline-formula><mml:math id="M172" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11 <inline-formula><mml:math id="M173" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for the clear-sky case
and 0.44 <inline-formula><mml:math id="M174" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.06 <inline-formula><mml:math id="M175" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for the all-sky case.
At the TOA the mean differences in shortwave fluxes are 0.19 <inline-formula><mml:math id="M176" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.11 <inline-formula><mml:math id="M177" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> (clear sky)
and 0.28 <inline-formula><mml:math id="M178" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.93 <inline-formula><mml:math id="M179" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> (all sky, Table <xref ref-type="table" rid="Ch1.T2"/>).
We should note that the clear-sky results agree with the direct effect estimated
in Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS1"/> but with different simulations, confirming the consistency of the calculations.
Thus, the indirect effect of aerosols enhances
the direct effect on the SW radiation during the lockdown,
even with larger intensity.
However, those values are associated with large standard deviations
related to the strong spatial variability of the upward shortwave radiation
difference between the simulations.</p>
      <p id="d1e3457">The total RF<inline-formula><mml:math id="M180" display="inline"><mml:msub><mml:mi/><mml:mtext>aci</mml:mtext></mml:msub></mml:math></inline-formula> due to COVID-19 lockdown
against the baseline scenario was also estimated.
We obtained a value of 0.19 <inline-formula><mml:math id="M181" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.92
for all-sky measurements over Europe in May 2020 at the TOA.
Similarly to RF<inline-formula><mml:math id="M182" display="inline"><mml:msub><mml:mi/><mml:mtext>ari</mml:mtext></mml:msub></mml:math></inline-formula>, this value
is also in line with the range suggested by <xref ref-type="bibr" rid="bib1.bibx6" id="text.68"><named-content content-type="post">see Table 5</named-content></xref>,
keeping in mind that only a partial reduction of anthropogenic aerosols
took place during the COVID-19 lockdown.
Although the average value agrees with the literature,
a large standard deviation is associated to RF<inline-formula><mml:math id="M183" display="inline"><mml:msub><mml:mi/><mml:mtext>aci</mml:mtext></mml:msub></mml:math></inline-formula>,
and thus the estimate should be used with caution as it is not
statistically significant.</p>
</sec>
</sec>
</sec>
<sec id="Ch1.S5" sec-type="conclusions">
  <label>5</label><title>Conclusions</title>
      <p id="d1e3510">We simulated the effects of drastically reduced anthropogenic emissions
on the atmospheric composition in Europe during the COVID-19 lockdown in spring 2020.
We evaluated the model simulations with observations obtained during the aircraft measurement campaign BLUESKY.
The overall agreement between the observations and the simulated aerosol concentrations
and trace gas mixing ratios is reasonable. Nevertheless, problems remain regarding stratosphere–troposphere transport,
especially of volcanic influence,
which resulted in systematically underestimated <inline-formula><mml:math id="M184" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M185" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>-</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>
of stratospheric origin
and a consequent overestimation of <inline-formula><mml:math id="M186" display="inline"><mml:mrow class="chem"><mml:msup><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub><mml:mo>-</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula>
<xref ref-type="bibr" rid="bib1.bibx5 bib1.bibx67 bib1.bibx79" id="paren.69"><named-content content-type="pre">which substitutes the underestimated sulfate in ammonium salts; see</named-content></xref>
in the upper troposphere.</p>
      <p id="d1e3560">Focusing on the effects of aerosol particles on the shortwave radiation budget,
we find that their reduction due to lockdown leads to a net clear-sky SW flux increase
of 0.33 <inline-formula><mml:math id="M187" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.10 and 0.20 <inline-formula><mml:math id="M188" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.09 <inline-formula><mml:math id="M189" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>
at surface level and TOA over Europe, respectively.
The increase of the SW radiation during the lockdown period is due to the
decrease in both black carbon and inorganic aerosols, which made the atmosphere more
transparent to the incoming solar radiation by reducing SW absorption and SW backscatter,
with the latter dominating.
It must be stressed that although this BC reduction causes an increase
in the SW incoming radiation, the SW heating has also been reduced by up to 0.005 <inline-formula><mml:math id="M190" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">d</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>
due to the lowered BC absorption.</p>
      <p id="d1e3611">With reduced emissions, the model simulates a lower number
concentration of aerosols between 300 and 50 hPa;  this reduction is located at an altitude
too high to influence the cloud droplet formation <xref ref-type="bibr" rid="bib1.bibx29" id="paren.70"/>
and heterogeneous ice nucleation from black carbon and dust; glassy organics freeze at these altitudes,
but their contribution is totally negligible
in comparison with homogeneous nucleation <xref ref-type="bibr" rid="bib1.bibx2" id="paren.71"/>.
The analysis of the indirect aerosol effect did not give any conclusive results
due to the large variability in the calculations caused by the short duration of the lockdown “experiment”.</p>
      <p id="d1e3620">Note that contrails and their contribution to radiative forcing are not considered in this study.
Contrails are expected to reduce solar radiation reaching the Earth surface
and to reduce outgoing longwave radiation.
The mean changes induced by reduced air traffic in 2020 compared to 2019, computed
in two model studies, were of the order of <inline-formula><mml:math id="M191" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.1</mml:mn></mml:mrow></mml:math></inline-formula> to 0.5 <inline-formula><mml:math id="M192" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> over Europe
<xref ref-type="bibr" rid="bib1.bibx17 bib1.bibx66" id="paren.72"/>, with a magnitude comparable to what is found in this study.
The differences between these studies can partly be attributed to the
applied methodologies and general difficulties in
discriminating anthropogenic effects from interannual variability.
Hence, a study which considers contrail and aerosol effects simultaneously
and covers a longer time period is recommended to better attribute
the causes of the observed changes .</p>
</sec>

      
      </body>
    <back><notes notes-type="codeavailability"><title>Code availability</title>

      <p id="d1e3657">The Modular Earth Submodel System (MESSy) is continuously further developed and applied by a consortium of institutions.
The usage of MESSy and access to the source code is licensed to all affiliates of institutions that are members of the MESSy Consortium.
Institutions can become a member of the MESSy Consortium by signing the MESSy Memorandum of Understanding.
More information can be found on the MESSy Consortium Website
(<uri>http://www.messy-interface.org</uri>, last access: 22  July 2022; <xref ref-type="bibr" rid="bib1.bibx52" id="altparen.73"/>).
The code presented here has been based on MESSy version 2.55 and is available as git commit #dcdc3ed8 in the MESSy repository.</p>
  </notes><notes notes-type="dataavailability"><title>Data availability</title>

      <p id="d1e3669">The observational data and the model results are available on the HALO
(High Altitude Long RAnge research aircraft) database
(<ext-link xlink:href="https://doi.org/10.17616/R39Q0T" ext-link-type="DOI">10.17616/R39Q0T</ext-link>, <xref ref-type="bibr" rid="bib1.bibx11" id="altparen.74"/>),
upon signing the data protocol.</p>
  </notes><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e3681">AP and SR planned the research.
AP and SR collected and prepared the emission data.
AM implemented code corrections for aerosol–cloud interactions.
AP performed the model simulations.
PJ contributed to the overall model development and helped with the preparation of the model setups.
SB helped the interpretation of aerosol–cloud interactions.
MK provided the script for the aerosol mass estimation in the model.
ZH, IT, LR, DJC, and HF provided the data for <inline-formula><mml:math id="M193" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M194" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">NO</mml:mi></mml:mrow></mml:math></inline-formula>, and <inline-formula><mml:math id="M195" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>.
JS and KK provided observational aerosol composition data.
RD and JNC were responsible for the PAN measurements.
CV, LT, and AM provided observational data of <inline-formula><mml:math id="M196" 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> and <inline-formula><mml:math id="M197" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">SO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>.
AZ provided the ozone data.
OK, BH, CP, MP, and UP conducted, analyzed, and interpreted the BC data.
BB contributed to the campaign.
MD organized the field campaign logistically.
JC planned the flight tracks during the campaign.
HS coordinated the measurements on the FALCON.
SR and AP performed the model evaluation and analysis of direct effects.
AM and AP performed the analysis of indirect effects.
US and AP discussed the results on the radiative forcing.
SR, AM, and AP wrote the manuscript with the help of SB, JC, MK, and JW.
AP and JL supervised the project.
All authors discussed the results and contributed to the review and editing of the manuscript.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e3741">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="d1e3750">Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.</p>
  </notes><notes notes-type="sistatement"><title>Special issue statement</title>

      <p id="d1e3756">This article is part of the special issues “BLUESKY atmospheric composition measurements by aircraft during the COVID-19 lockdown in spring 2020” and “The Modular Earth Submodel System (MESSy) (ACP/GMD inter-journal SI)”. It is not associated with a conference.</p>
  </notes><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e3762">Christiane Voigt, Laura Tomsche, and Andreas Marsing have been supported by the Helmholtz-Gemeinschaft (grant no. W2/W3-060) and the Deutsche Forschungsgemeinschaft (grant nos. TRR 301 – Project-ID 428312742 and SPP 1294 HALO – VO 1504/7-1).
Birger Bohn received funding from the grant BO 1580/5-1 within the HALO-SPP.
<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?>
The article processing charges for this open-access <?xmltex \notforhtml{\newline}?> publication were covered by the Max Planck Society.</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e3773">This paper was edited by Pedro Jimenez-Guerrero and reviewed by two anonymous referees.</p>
  </notes><ref-list>
    <title>References</title>

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