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  <front>
    <journal-meta>
<journal-id journal-id-type="publisher">AMT</journal-id>
<journal-title-group>
<journal-title>Atmospheric Measurement Techniques</journal-title>
<abbrev-journal-title abbrev-type="publisher">AMT</abbrev-journal-title>
<abbrev-journal-title abbrev-type="nlm-ta">Atmos. Meas. Tech.</abbrev-journal-title>
</journal-title-group>
<issn pub-type="epub">1867-8548</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/amt-9-4399-2016</article-id><title-group><article-title>Infrared limb emission measurements of aerosol in the troposphere and stratosphere</article-title>
      </title-group><?xmltex \runningtitle{Aerosol detection with infrared limb emission measurements}?><?xmltex \runningauthor{S. Griessbach et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Griessbach</surname><given-names>Sabine</given-names></name>
          <email>s.griessbach@fz-juelich.de</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Hoffmann</surname><given-names>Lars</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-3773-4377</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Spang</surname><given-names>Reinhold</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-2483-5761</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>von Hobe</surname><given-names>Marc</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-6034-6562</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Müller</surname><given-names>Rolf</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-5024-9977</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Riese</surname><given-names>Martin</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-6398-6493</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Jülich Supercomputing Centre (JSC), Forschungszentrum Jülich GmbH, Jülich, Germany</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Institute of Energy and Climate Research (IEK-7), Forschungszentrum Jülich GmbH, Jülich, Germany</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Sabine Griessbach (s.griessbach@fz-juelich.de)</corresp></author-notes><pub-date><day>7</day><month>September</month><year>2016</year></pub-date>
      
      <volume>9</volume>
      <issue>9</issue>
      <fpage>4399</fpage><lpage>4423</lpage>
      <history>
        <date date-type="received"><day>27</day><month>February</month><year>2015</year></date>
           <date date-type="rev-request"><day>29</day><month>April</month><year>2015</year></date>
           <date date-type="rev-recd"><day>29</day><month>June</month><year>2016</year></date>
           <date date-type="accepted"><day>28</day><month>July</month><year>2016</year></date>
      </history>
      <permissions>
<license license-type="open-access">
<license-p>This work is licensed under a Creative Commons Attribution 3.0 Unported License. To view a copy of this license, visit <ext-link ext-link-type="uri" xlink:href="http://creativecommons.org/licenses/by/3.0/">http://creativecommons.org/licenses/by/3.0/</ext-link></license-p>
</license>
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<self-uri xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016.pdf">The full text article is available as a PDF file from https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016.pdf</self-uri>


      <abstract>
    <p>Altitude-resolved aerosol detection in the upper troposphere and lower
stratosphere (UTLS) is a challenging task for remote sensing instruments.
Infrared limb emission measurements provide vertically resolved global
measurements at day- and nighttime in the UTLS. For high-spectral-resolution
infrared limb instruments we present here a new method to detect aerosol and
separate between ice and non-ice particles. The method is based on an
improved aerosol–cloud index that identifies infrared limb emission spectra
affected by non-ice aerosol or ice clouds. For the discrimination between
non-ice aerosol and ice clouds we employed brightness temperature difference
correlations. The discrimination thresholds for this method were derived from
radiative transfer simulations (including scattering) and Michelson
Interferometer for Passive Atmospheric Sounding (MIPAS)/Envisat measurements
obtained in 2011. We demonstrate the value of this approach for observations
of volcanic ash and sulfate aerosol originating from the Grímsvötn
(Iceland, 64<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N), Puyehue–Cordón Caulle (Chile,
40<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S), and Nabro (Eritrea, 13<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) eruptions in May and
June 2011 by comparing the MIPAS volcanic aerosol detections with Atmospheric
Infrared Sounder (AIRS) volcanic ash and SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> measurements.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p>Aerosol is omnipresent and highly variable in the atmosphere. In the upper
troposphere and lower stratosphere (UTLS) a large variety of aerosol
particles, comprising sulfate droplets, volcanic ash, mineral dust, wild fire
aerosol, organic material, and meteoritic dust, has been found
<xref ref-type="bibr" rid="bib1.bibx48 bib1.bibx62 bib1.bibx72 bib1.bibx63 bib1.bibx23 bib1.bibx59 bib1.bibx102" id="paren.1"><named-content content-type="pre">e.g.</named-content></xref>
(in this paper we do not refer to ice particles or liquid water droplets as
aerosol). The stratospheric aerosol is dominated by sulfate aerosol
<xref ref-type="bibr" rid="bib1.bibx48" id="paren.2"/> and is significantly influenced by volcanic eruptions
<xref ref-type="bibr" rid="bib1.bibx5 bib1.bibx97" id="paren.3"><named-content content-type="pre">e.g.</named-content></xref>. It has an impact on the radiation
budget of the Earth and hence influences climate
<xref ref-type="bibr" rid="bib1.bibx81 bib1.bibx75" id="paren.4"/>. The tropospheric background aerosol is also
dominated by sulfate aerosol but is disturbed by numerous irregular events,
such as volcanic eruptions, mineral dust outbreaks, and fires. In the
troposphere some specific aerosol particles serve as condensation nuclei and
hence influence cloud formation and precipitation
<xref ref-type="bibr" rid="bib1.bibx20 bib1.bibx104 bib1.bibx105" id="paren.5"/>. Aerosol events, such as mineral dust
outbreaks from the Sahara fertilising the Amazon forest <xref ref-type="bibr" rid="bib1.bibx55" id="paren.6"/> and
volcanic ash posing a danger to aircraft <xref ref-type="bibr" rid="bib1.bibx7" id="paren.7"/>, can be of
particular importance for specific questions. Lidar measurements indicate
that volcanic aerosol also can be a strongly variable load in the upper
troposphere <xref ref-type="bibr" rid="bib1.bibx14" id="paren.8"><named-content content-type="post">Fig. 12</named-content></xref>.</p>
      <p>Aerosol measurements in the stratosphere are available from a variety of
sources. In particular, satellite measurements provide global climatologies
and time series of stratospheric aerosol <xref ref-type="bibr" rid="bib1.bibx5 bib1.bibx97 bib1.bibx56" id="paren.9"/>. Global long-term observations of upper tropospheric aerosol are
rare because they are hampered by the presence of ice clouds
<xref ref-type="bibr" rid="bib1.bibx50 bib1.bibx94" id="paren.10"><named-content content-type="pre">e.g.</named-content></xref>. Hence, many stratospheric aerosol products are only
available above 15 km <xref ref-type="bibr" rid="bib1.bibx75" id="paren.11"/>.</p>
      <p>Satellite-based limb instruments, such as the Stratospheric Aerosol and Gas
Experiment (SAGE) series <xref ref-type="bibr" rid="bib1.bibx92 bib1.bibx5" id="paren.12"/>, Optical
Spectrograph and InfraRed Imaging System (OSIRIS) <xref ref-type="bibr" rid="bib1.bibx76" id="paren.13"/>, and the
Halogen Occultation Experiment (HALOE) <xref ref-type="bibr" rid="bib1.bibx93" id="paren.14"/>, have a long-standing history of measuring altitude-resolved global time series of
stratospheric aerosol. However, the spatial coverage of solar occultation
instruments (SAGE, HALOE) is limited. The solar scattering (OSIRIS)
measurements are limited to daytime and hence cannot provide measurements at
polar night. Also, due to the high sensitivity to low aerosol concentrations
of these instruments measuring in the ultraviolet to near-infrared spectral
range, their extinction profiles run into saturation for specific aerosol
events, such as moderate to major volcanic eruptions (with an volcanic
explosivity index of 4; e.g. Sarychev, 2009; Nabro, 2011) and impede
measurements below the plume top altitude <xref ref-type="bibr" rid="bib1.bibx24" id="paren.15"/>. The 750 nm
extinction coefficient thresholds range from about <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">3</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> to
0.02 km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> for OSIRIS and SAGE II respectively <xref ref-type="bibr" rid="bib1.bibx24" id="paren.16"/>.
Extending these aerosol measurements into the upper troposphere is also
challenging because the separation between ice clouds and aerosol is prone
to errors for SAGE and HALOE <xref ref-type="bibr" rid="bib1.bibx50 bib1.bibx94" id="paren.17"/> or is not done for
OSIRIS <xref ref-type="bibr" rid="bib1.bibx24" id="paren.18"/>.</p>
      <p>In contrast, satellite-based infrared (IR) emission measurements provide a
global coverage at day- and nighttime during all seasons. Furthermore, IR
nadir instruments have a better global and temporal coverage than ultraviolet (UV)/visible
(VIS)
nadir measurements or occultation measurements. IR nadir measurements have a
long-standing history in detecting aerosols and retrieving aerosol
composition and microphysics. The aerosol measurements from IR nadir
instruments mainly focus on volcanic ash
<xref ref-type="bibr" rid="bib1.bibx72 bib1.bibx35" id="paren.19"><named-content content-type="pre">e.g.</named-content></xref>, mineral dust
<xref ref-type="bibr" rid="bib1.bibx69 bib1.bibx53 bib1.bibx54 bib1.bibx59" id="paren.20"><named-content content-type="pre">e.g.</named-content></xref>, and smoke
<xref ref-type="bibr" rid="bib1.bibx22" id="paren.21"/>. There are several methods available to detect aerosol,
filter out ice clouds, and classify aerosol types. These methods comprise
the split window/reverse absorption technique for volcanic ash
<xref ref-type="bibr" rid="bib1.bibx72 bib1.bibx73 bib1.bibx80" id="paren.22"/>, trispectral approaches for volcanic
ash and mineral dust <xref ref-type="bibr" rid="bib1.bibx2 bib1.bibx1 bib1.bibx35" id="paren.23"/>, and
multispectral approaches for hyperspectral instruments
<xref ref-type="bibr" rid="bib1.bibx25 bib1.bibx8 bib1.bibx9" id="paren.24"/>. Although the established
methods are used for operational data products they are still subject to
improvements <xref ref-type="bibr" rid="bib1.bibx35" id="paren.25"/>. The capability of detecting sulfate
aerosol with IR nadir measurements has been demonstrated for band
measurements <xref ref-type="bibr" rid="bib1.bibx4 bib1.bibx1" id="paren.26"/> and for hyperspectral instruments
<xref ref-type="bibr" rid="bib1.bibx8 bib1.bibx25 bib1.bibx49" id="paren.27"/>. <xref ref-type="bibr" rid="bib1.bibx1" id="text.28"/> found
that sulfate droplets with an aerosol optical depth (AOD) larger than 0.01 at
11 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m should be detectable from IR nadir measurements. However, a
major disadvantage of IR nadir aerosol measurements is the lack of altitude
profile information. Another shortcoming is the limited sensitivity towards
thin aerosol. IR nadir instruments are not sensitive at low AODs, which are
characteristic for polar stratospheric clouds (PSCs) or diluted volcanic
sulfate aerosol. Considering UV/VIS solar occultation/scattering measurements
and IR nadir measurements together, there is a measurement gap for AODs
between 0.02 and 0.1 for sulfate aerosol: for UV/VIS solar
occultation/scattering measurements the maximum retrievable AOD is 0.02
<xref ref-type="bibr" rid="bib1.bibx24" id="paren.29"/> and for IR nadir measurements the minimum detectable AOD is
0.01 <xref ref-type="bibr" rid="bib1.bibx1" id="paren.30"/>, which corresponds to an AOD of about 0.1 in the
VIS range for the same scenario <xref ref-type="bibr" rid="bib1.bibx5" id="paren.31"><named-content content-type="pre">e.g.</named-content></xref>.</p>
      <p>IR limb emission measurements combine the advantages of occultation and IR
nadir measurements. They have better global coverage than occultation
measurements and provide altitude information. Limb emission measurements in
the IR are highly sensitive towards aerosol, yet only a few studies deal with
aerosol detection, aerosol classification, and ice cloud filtering of such
measurements. It has been shown that the stratospheric sulfate aerosol after
the Mt. Pinatubo eruption introduced a characteristic spectral signature
into IR limb spectra for the Improved Stratospheric And Mesospheric Sounder
(ISAMS) <xref ref-type="bibr" rid="bib1.bibx28 bib1.bibx57" id="paren.32"/>, the Cryogenic Limb Array Etalon
Spectrometer (CLAES) <xref ref-type="bibr" rid="bib1.bibx61 bib1.bibx58" id="paren.33"/>, and the balloon-borne
Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B)
<xref ref-type="bibr" rid="bib1.bibx15" id="paren.34"/>. Further, <xref ref-type="bibr" rid="bib1.bibx15" id="text.35"/> derived optical and
microphysical parameters of stratospheric aerosol from MIPAS-B measurements.
Studies using high-resolution IR spectra of the spaceborne IR limb
instruments Cryogenic Infrared Spectrometers and Telescopes for the
Atmosphere (CRISTA) <xref ref-type="bibr" rid="bib1.bibx67 bib1.bibx77" id="paren.36"/> and MIPAS <xref ref-type="bibr" rid="bib1.bibx18" id="paren.37"/>
present methods to detect PSCs and distinguish between the three PSC types
(ice, supercooled ternary solutions, and nitric acid trihydrate)
<xref ref-type="bibr" rid="bib1.bibx84 bib1.bibx86 bib1.bibx87 bib1.bibx44 bib1.bibx89" id="paren.38"/>. However, these
studies are restricted to the stratosphere and do not tackle the
discrimination between aerosol and ice clouds in the troposphere.
Measurements of the High Resolution Dynamics Limb Sounder (HIRDLS) <xref ref-type="bibr" rid="bib1.bibx26" id="paren.39"/> provide a flag for four different cloud types in the troposphere
and stratosphere (1 – unknown cloud, 2 – cirrus layer, 3 – extensive
PSC, 4 – opaque cloud) and 12 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m extinctions. HIRDLS
measurements are also sensitive towards volcanic aerosol and forest fire
smoke clouds, which the detection routine classifies as “unknown cloud”
<xref ref-type="bibr" rid="bib1.bibx60" id="paren.40"/>. However, not only aerosol is classified as “unknown
cloud”; multilayer cloud structures and clouds of intermediate
thickness between deep convection tower and isolated cirrus layer also fall into the
“unknown cloud” category <xref ref-type="bibr" rid="bib1.bibx60" id="paren.41"/>.</p>
      <p>For the detection of clouds and aerosol in the troposphere and stratosphere,
<xref ref-type="bibr" rid="bib1.bibx85" id="text.42"/> introduced the cloud index (CI) for CRISTA limb IR
measurements. Later, the CI was adapted to MIPAS <xref ref-type="bibr" rid="bib1.bibx86" id="paren.43"/> and to the
airborne CRISTA-New Frontiers (CRISTA-NF) <xref ref-type="bibr" rid="bib1.bibx88" id="paren.44"/>. The MIPAS CI
thresholds were optimized as a function of latitude and altitude
<xref ref-type="bibr" rid="bib1.bibx82" id="paren.45"/>. A first attempt to classify between tropospheric ice and
liquid clouds in MIPAS spectra was made by <xref ref-type="bibr" rid="bib1.bibx89" id="text.46"/>. Regarding the
discrimination between ice clouds and volcanic ash, <xref ref-type="bibr" rid="bib1.bibx31 bib1.bibx33" id="text.47"/> presented a method to detect volcanic ash in the troposphere
and stratosphere with MIPAS. Also for MIPAS, <xref ref-type="bibr" rid="bib1.bibx29" id="text.48"/> presented
methods to identify volcanic plumes containing sulfur dioxide, sulfate
aerosol, and volcanic ash.</p>
      <p>Aerosol detection and the separation from ice clouds for IR limb emission
measurements is by far not as elaborated as for IR nadir measurements. Also,
the nadir methods cannot be simply applied to limb emission measurements as
they have rather different sensitivities due to different measurement
geometries and principles (emission lines in the limb spectra and absorption
lines in the nadir spectra). However, the IR nadir classification techniques
mentioned above demonstrate the capability of IR measurements to provide a
separation between ice clouds and various aerosol types. Separating between
aerosol and ice clouds constitutes the first step towards altitude-resolved
IR limb emission aerosol measurements in the UTLS. This region is of
particular interest as in the past chiefly due to the lack of measurements
the impact of volcanic aerosol on radiative forcing in the lower stratosphere
at high and midlatitudes has been underestimated <xref ref-type="bibr" rid="bib1.bibx75" id="paren.49"/>.</p>
      <p>Here, we present a method to detect clouds and aerosol in the troposphere and
stratosphere and to separate between aerosol and ice clouds for IR limb
emission measurements. The paper describes the method and shows examples for
altitude-resolved aerosol detection for three volcanic eruptions at polar,
mid-, and tropical latitudes. First, we present the instruments and our
radiative transfer model (Sect. <xref ref-type="sec" rid="Ch1.S2"/>). Then we introduce a method
that allows aerosol and clouds to be detected in the troposphere as well as
in the stratosphere (Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/>). Starting with the new
aerosol and cloud detection we develop a method to distinguish between ice
clouds and aerosol (Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>). We apply the new method
to MIPAS measurements in 2011 and present the results for three volcanic
eruptions (the Grímsvötn (Iceland), Puyehue–Cordón Caulle
(Chile),
and the Nabro (Eritrea) eruptions) and compare them with Atmospheric Infrared
Sounder (AIRS) SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and volcanic ash measurements
(Sect. <xref ref-type="sec" rid="Ch1.S4"/>). Finally, we present our conclusions
(Sect. <xref ref-type="sec" rid="Ch1.S5"/>).</p>
</sec>
<sec id="Ch1.S2">
  <title>Instruments and forward model</title>
<sec id="Ch1.S2.SS1">
  <title>MIPAS</title>
      <p>The IR limb sounder MIPAS measured high-resolution spectra in the
thermal IR between 685 and 2410 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx18" id="paren.50"/>. In our
study we use the measurements of band A (685–970 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) and band B
(1215–1500 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>). MIPAS was mounted on ESA's Envisat and measured
atmospheric profiles between 6 and 68 km altitude from July 2002 to
March 2004 and between 7 and 72 km altitude from January 2005 to April 2012 in its
nominal mode. MIPAS measured in the thermal IR from a nearly polar
orbit providing complete latitudinal and longitudinal coverage at day- and
nighttime. Due to a malfunction in 2004 MIPAS's original nominal operation
mode, which comprised a spectral sampling of 0.025 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and a vertical
sampling of 3 km, had to be changed. In 2005 the spectral sampling was
reduced to 0.0625 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and the vertical sampling below 20 km was
increased to 1.5 km <xref ref-type="bibr" rid="bib1.bibx18" id="paren.51"/>. Also, the measurement geometry was
modified so that MIPAS sampled down to 7 km in the polar regions and down to
10 km in the tropics <xref ref-type="bibr" rid="bib1.bibx18" id="paren.52"/>. For developing a method to detect
aerosol and to demonstrate its viability we use MIPAS level 1b calibrated
radiances that are available at <xref ref-type="bibr" rid="bib1.bibx16" id="text.53"/>.</p>
</sec>
<sec id="Ch1.S2.SS2">
  <title>AIRS</title>
      <p>For the comparison with the MIPAS aerosol measurements we use the AIRS level
1b radiances that are available at <xref ref-type="bibr" rid="bib1.bibx64" id="text.54"/>. The IR nadir sounder
AIRS <xref ref-type="bibr" rid="bib1.bibx3" id="paren.55"/> is mounted on NASA's Aqua satellite launched in May
2002. The AIRS hyperspectral IR spectra between
3.7 and 15.4 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (649–2674 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) are obtained from
measurements in the nadir and sub-limb observation geometry. Each scan
consists of 90 footprints in the across-track direction and covers a distance
of 1765 km on the ground. The footprint size is 13.5 km <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 13.5 km
for nadir and 41 km <inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 21.4 km for the outermost sub-limb views.
AIRS measures 14.5 orbits and provides about 2.9 million spectra per day.
This provides an excellent horizontal resolution with global coverage twice a
day except for small gaps at mid- and low latitudes.</p>
</sec>
<sec id="Ch1.S2.SS3">
  <title>Juelich Rapid Spectral Simulation Code (JURASSIC)</title>
      <p>For radiative transfer simulations of the MIPAS measurements we use the
JURASSIC <xref ref-type="bibr" rid="bib1.bibx38" id="paren.56"/>. It
applies the emissivity growth approximation <xref ref-type="bibr" rid="bib1.bibx27" id="paren.57"/> for fast
simulations in the mid-infrared spectral region. JURASSIC has been used for
radiative transfer simulations and trace gas retrievals for various IR
limb instruments <xref ref-type="bibr" rid="bib1.bibx38 bib1.bibx39 bib1.bibx101 bib1.bibx96" id="paren.58"/> and for nadir sounders such as AIRS <xref ref-type="bibr" rid="bib1.bibx37 bib1.bibx34" id="paren.59"/>.</p>
      <p>JURASSIC has been extended with a scattering module that allows radiative
transfer simulations to be conducted including single and multiple scattering
on aerosol and cloud particles <xref ref-type="bibr" rid="bib1.bibx30 bib1.bibx32" id="paren.60"/>. In this
study, we use Mie calculations to determine the optical properties extinction
coefficient, scattering coefficient, and phase function of cloud and aerosol
particles. For the simulations presented here, we use a setup described in
detail by <xref ref-type="bibr" rid="bib1.bibx33" id="text.61"/> with slight modifications. Here, the
spectral sampling is 0.0625 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and the vertical sampling is 0.5 km.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <title>Aerosol detection and ice cloud filtering</title>
<sec id="Ch1.S3.SS1">
  <title>Aerosol and cloud detection</title>
<sec id="Ch1.S3.SS1.SSS1">
  <title>Index methods for aerosol and cloud detection</title>
      <p>The CI is the standard method to detect clouds and aerosol with MIPAS
<xref ref-type="bibr" rid="bib1.bibx85" id="paren.62"/>. It is defined as the ratio between the mean radiances
around the 792 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> band with strong CO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> emissions and the
atmospheric window region around 833 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>:
              <disp-formula id="Ch1.E1" content-type="numbered"><mml:math display="block"><mml:mrow><mml:mi mathvariant="normal">CI</mml:mi><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mi>I</mml:mi><mml:mo mathvariant="normal">¯</mml:mo></mml:mover><mml:mn mathvariant="normal">1</mml:mn></mml:msub><mml:mo>(</mml:mo><mml:mo>[</mml:mo><mml:mn>788.25</mml:mn><mml:mo>,</mml:mo><mml:mn>796.25</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>]</mml:mo><mml:mo>)</mml:mo></mml:mrow><mml:mrow><mml:msub><mml:mover accent="true"><mml:mi>I</mml:mi><mml:mo mathvariant="normal">¯</mml:mo></mml:mover><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>(</mml:mo><mml:mo>[</mml:mo><mml:mn>832.31</mml:mn><mml:mo>,</mml:mo><mml:mn>834.37</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>]</mml:mo><mml:mo>)</mml:mo></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
            where <inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mi>I</mml:mi><mml:mo mathvariant="normal">¯</mml:mo></mml:mover><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is the mean radiance of each window. The CI is a continuous
value, where large values indicate clear air conditions and small values
indicate the presence of clouds or aerosol. In previous studies CI values
below 1.8–6 have been used to indicate cloudy air and CI values above 6
indicate clear air <xref ref-type="bibr" rid="bib1.bibx86 bib1.bibx89 bib1.bibx82" id="paren.63"/>. The CI detection
threshold depends on altitude, latitude, and season, mainly because of the
water vapour continuum contributing to the 833 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> window radiance
<xref ref-type="bibr" rid="bib1.bibx86 bib1.bibx82" id="paren.64"/>. The effect of the water vapour continuum is
particularly pronounced at lower tropospheric altitudes.</p>
      <p>Because the water vapour continuum absorption decreases with higher
wavenumber <xref ref-type="bibr" rid="bib1.bibx79" id="paren.65"><named-content content-type="pre">e.g.</named-content></xref>, we looked for additional windows at
higher wavenumbers in MIPAS band A in order to achieve an altitude-,
latitude-,
and season-independent aerosol detection. For the selection of an appropriate
window, which cannot be directly adopted from IR nadir measurements due to
the strong trace gas emission lines measured in the IR limb geometry, we
considered MIPAS clear air radiance profiles between about 7 and 25 km
altitude. In the clear air profile in Fig. <xref ref-type="fig" rid="Ch1.F1"/> bright colours
indicate high radiances due to trace gas emissions and dark colours indicate
atmospheric window regions with low radiances. These atmospheric windows are
especially suited for aerosol detection, because trace gases have little
impact here. The broad window around 830 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> with low radiances at all
altitudes is already used for the CI. Between about 940 and 970 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>
there are many narrow windows with low radiances between CO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> lines. The
broadest of these windows is located between 960 and 961 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>.
Therefore, we average over the 17 spectral points measured by MIPAS in this
window and define the aerosol index (AI) as
              <disp-formula id="Ch1.E2" content-type="numbered"><mml:math display="block"><mml:mrow><mml:mi mathvariant="normal">AI</mml:mi><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mi>I</mml:mi><mml:mo mathvariant="normal">¯</mml:mo></mml:mover><mml:mn mathvariant="normal">1</mml:mn></mml:msub><mml:mo>(</mml:mo><mml:mo>[</mml:mo><mml:mn>788.25</mml:mn><mml:mo>,</mml:mo><mml:mn>796.25</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>]</mml:mo><mml:mo>)</mml:mo></mml:mrow><mml:mrow><mml:msub><mml:mover accent="true"><mml:mi>I</mml:mi><mml:mo mathvariant="normal">¯</mml:mo></mml:mover><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>(</mml:mo><mml:mo>[</mml:mo><mml:mn>960.00</mml:mn><mml:mo>,</mml:mo><mml:mn>961.00</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>]</mml:mo><mml:mo>)</mml:mo></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
            where <inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mi>I</mml:mi><mml:mo mathvariant="normal">¯</mml:mo></mml:mover><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is the mean radiance of each window.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><caption><p>MIPAS radiances measured in profile 89 of orbit 48509 (around
48<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>  S). This clear air case shows low radiances in the broad
window region around 830 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and multiple narrow windows between
950 and 970 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>.</p></caption>
            <?xmltex \igopts{width=195.129pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f01.pdf"/>

          </fig>

      <p>In the stratosphere at altitudes from about 50 km down to about 22 km we
found a seasonal and diurnal cycle in the radiances between 960 and
961 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and hence in the AI (Fig. <xref ref-type="fig" rid="App1.Ch1.F1"/>). This
diurnal cycle and the differences between the summer and the winter
hemisphere are most likely caused by non-local thermodynamic equilibrium
(non-LTE) effects of the CO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> laser bands between 950 and 970 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> at
altitudes of 50 km and above <xref ref-type="bibr" rid="bib1.bibx95" id="paren.66"><named-content content-type="pre">e.g.</named-content></xref>. In order to
filter out this non-LTE feature we combined the AI with the CI, which is not
affected by non-LTE effects, and defined the aerosol cloud index (ACI) as the
maximum value of both:
              <disp-formula id="Ch1.E3" content-type="numbered"><mml:math display="block"><mml:mrow><mml:mi mathvariant="normal">ACI</mml:mi><mml:mo>=</mml:mo><mml:mi mathvariant="normal">max</mml:mi><mml:mo>(</mml:mo><mml:mi mathvariant="normal">CI</mml:mi><mml:mo>,</mml:mo><mml:mi mathvariant="normal">AI</mml:mi><mml:mo>)</mml:mo><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula></p>
      <p>Below about 25 km the ACI generally corresponds to the AI and above about
25 km it corresponds to the CI (Fig. <xref ref-type="fig" rid="App1.Ch1.F1"/>).</p>
      <p>In order to demonstrate the benefits of the ACI and to derive a fixed
threshold value that is applicable to MIPAS measurements, we investigated the
behaviour of simulated and measured ACI profiles and compared them with the
corresponding CI profiles.</p>
</sec>
<sec id="Ch1.S3.SS1.SSS2">
  <title>Simulations</title>
      <p>In the radiative transfer simulations we focused on clear air and cloud
simulations at altitudes between 5.5 and 19.5 km with a 0.5 km vertical
sampling. We considered polar winter, polar summer, midlatitude, and tropical
atmospheric conditions <xref ref-type="bibr" rid="bib1.bibx74" id="paren.67"/> without any background aerosol.
The simulation results for clear air conditions
(Fig. <xref ref-type="fig" rid="App1.Ch1.F3"/>) show that the AI is significantly larger
than the CI. They also show an altitude dependence for the CI but also for
the AI/ACI especially at altitudes below 10 km. At altitudes above about
15 km the CI and AI converge towards each other. In the polar summer
atmosphere they intersect at 17 km, which means that the ACI corresponds to
the CI at altitudes above.</p>
      <p>For the cloud simulations we placed 1 km thick ice cloud, sulfate aerosol,
and volcanic ash layers at 6–7, 9–10, 13–14, and 17–18 km altitude in
polar winter, polar summer, midlatitude, and tropical atmospheric conditions.
For the ice cloud, volcanic ash, and sulfate aerosol simulations we assumed
various realistic combinations of particle sizes, concentrations, and
extinctions given at 948.5 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (see Tables 3–5 in
<xref ref-type="bibr" rid="bib1.bibx33" id="altparen.68"/>). The simulated extinction range was
<inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>–1, <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>–<inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">5</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, and
<inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">4</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>–<inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> for ice, volcanic ash, and
sulfate aerosol, respectively. The considered mode radii were 0.3–96,
0.1–5, and 0.01–1.5 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, respectively. Examples of simulated
profiles for ice, volcanic ash, and sulfate aerosol are shown in
Figs. <xref ref-type="fig" rid="App1.Ch1.F5"/> to <xref ref-type="fig" rid="App1.Ch1.F7"/>.</p>
      <p>While for clear air the AI/ACI values are systematically larger than the CI
values both have similar values in case of sulfate aerosol and volcanic ash
at cloud altitude. In some cases the AI becomes smaller than the CI, which
means that it is even more sensitive towards the aerosol. Also, the deviation
from the clear air profile is stronger for the AI than for the CI. For ice
clouds, however, the CI is systematically smaller than the AI/ACI, which
means that the CI is more sensitive towards ice. Since we focus on aerosol
detection, this is not an issue for our study. More details on the simulated
CI, AI, and ACI profiles and its sensitivity are discussed in the
Appendix Sect. <xref ref-type="sec" rid="App1.Ch1.S1.SS3"/>.</p>
      <p>To derive an ACI aerosol/cloud detection threshold value we considered the
simulated clear air profiles and the MIPAS measurement geometry after the
modification in 2005 that reached down to about 10 km in the tropics and
about 7 km in the polar regions. In the simulations the ACI is always larger
than 7 in the polar winter atmosphere. In the polar summer and midlatitude
atmosphere the ACI is larger than 7 at 7 km and above and in the equatorial
atmosphere it is larger than 7 at 9 km and above. This means that a fixed
ACI threshold value of 7 will be applicable to MIPAS measurements between
2005 and 2012 for the detection of aerosol.</p>
</sec>
<sec id="Ch1.S3.SS1.SSS3">
  <title>Measurements</title>
      <p>Examples of the CI (Fig. <xref ref-type="fig" rid="Ch1.F2"/>b), the AI
(Fig. <xref ref-type="fig" rid="Ch1.F2"/>c), and the ACI (Fig. <xref ref-type="fig" rid="Ch1.F2"/>d) are
shown as a function of altitude along a single MIPAS orbit
(Fig. <xref ref-type="fig" rid="Ch1.F2"/>a) measured on 18 August 2011. In mid-August most
of the northern hemispheric stratosphere was affected by a sulphate aerosol
layer caused by the Nabro eruption in June 2011
<xref ref-type="bibr" rid="bib1.bibx6 bib1.bibx24" id="paren.69"/>. Two months after the eruption of the Nabro
volcano this layer was diluted, so that it was invisible to IR nadir
measurements (Fig. <xref ref-type="fig" rid="Ch1.F2"/>f) and to the CALIPSO operational
product <xref ref-type="bibr" rid="bib1.bibx65" id="paren.70"/> but visible to OSIRIS solar scattering
measurements <xref ref-type="bibr" rid="bib1.bibx6" id="paren.71"/> and to MIPAS (Fig. <xref ref-type="fig" rid="Ch1.F2"/>d,
e) as discussed below.</p>
      <p>For the detection of aerosol and clouds along a MIPAS orbit we mainly rely on
the established CI. Here we briefly discuss the purposes and shortcomings of
the different CI thresholds for the example of a particular MIPAS orbit
(Fig. <xref ref-type="fig" rid="Ch1.F2"/>b). A fixed CI threshold of 1.8 (CI below 2 shown
in yellow) is used for cloud clearing for trace gas profile retrievals by ESA
<xref ref-type="bibr" rid="bib1.bibx86" id="paren.72"/>. This threshold captures tropospheric clouds only and PSCs
in the Antarctic but not a volcanic aerosol layer in the northern
hemispheric
UTLS like the one caused by Nabro. Also, a fixed CI threshold of 4.5 (yellow,
orange, red), which is used for more conservative cloud filtering, mainly
captures PSCs <xref ref-type="bibr" rid="bib1.bibx44" id="paren.73"/>, subvisible cirrus clouds (SVCs)
<xref ref-type="bibr" rid="bib1.bibx90" id="paren.74"/>, and tropospheric clouds but not the volcanic aerosol
layer. A fixed CI threshold of 6 (yellow, orange, red, dark red) captures
the UTLS aerosol layer but mistakes cloud-free regions (profiles 0–3,
56–60, and 92–95; see comparison with IR nadir data below) as cloudy. This
feature of the CI of becoming smaller at lower altitudes in cloud-free
conditions is addressed by <xref ref-type="bibr" rid="bib1.bibx82" id="text.75"/>, providing a variable CI
threshold definition at altitudes above 10 km. Here we used a simplified
variable CI threshold based on <xref ref-type="bibr" rid="bib1.bibx82" id="text.76"/>. The details are given in
Appendix <xref ref-type="sec" rid="App1.Ch1.S1.SS1"/>. This most advanced CI threshold definition
(black crosses in Fig. <xref ref-type="fig" rid="Ch1.F2"/>b and d) allows cloudy and cloud-free tropospheric regions as seen by IR nadir instruments
(Fig. <xref ref-type="fig" rid="Ch1.F2"/>f) to be discriminated and captures the UTLS
aerosol layer as observed by OSIRIS.</p>
      <p>Figure <xref ref-type="fig" rid="Ch1.F2"/> suggests that a fixed ACI with values smaller
than 7 allows tropospheric clouds as well as the stratospheric aerosol layer
caused by the Nabro eruption to be detected. Hence, we assessed the
performance of the ACI with a fixed threshold value of 7 for the detection of
aerosol and clouds by comparing the ACI aerosol/cloud detections with CI
cloud detections relying on the thresholds presented by <xref ref-type="bibr" rid="bib1.bibx82" id="text.77"/>
for altitudes above 10 km combined with a fixed CI threshold of 2 at 10 km
and below (black crosses in Fig. <xref ref-type="fig" rid="Ch1.F2"/>b and d). In
Fig. <xref ref-type="fig" rid="Ch1.F2"/>b and d the profiles 0–3, 56–60, and 92–95 are
identified as clear air by both the CI and the ACI. The UTLS aerosol layer is
also captured by both. However, the CI and the ACI cloud/aerosol detections
are not completely identical. Below 10 km the CI with a threshold of 2
identifies slightly less clouds than the ACI with a threshold of 7. Examples
can be found in profiles 16, 18, and 19 around 10 km and between profiles 30 and
40, where the CI detects clear air down to the lowest tangent altitude,
whereas the ACI indicates clouds at the lowest tangent altitude. Above 10 km
there are a few profiles where the CI identifies clouds/aerosol but not the
ACI and vice versa (e.g. profiles 5, 54, 41–44). However, the main differences
can be seen in profiles 16–18, where the CI indicates clouds/aerosol down to
the tropopause whereas the ACI indicates a stratospheric aerosol layer with
clear air below, and between profiles 23 and 35, where the CI indicates a thin
stratospheric aerosol layer whereas the ACI indicates aerosol down to the
tropopause.</p>
      <p>The tropospheric aerosol/cloud detections of the CI and ACI are confirmed by
geostationary IR nadir measurements by MTSAT (15:00 UTC), IODC (18:00 UTC),
and GOES East (15:00 UTC) (the IR nadir images were obtained from NERC
Satellite Receiving Station, Dundee University, Scotland,
<uri>http://www.sat.dundee.ac.uk/</uri>) along the orbit track
(Fig. <xref ref-type="fig" rid="Ch1.F2"/>f) and closest to the MIPAS measurement time
(15:05–16:45 UTC). In the IR nadir images clear air is indicated by
dark/black colours, high-altitude clouds are bright white, and low-altitude
clouds are indicated by greyish colours. For the clear air profiles 0–2
north west of Australia (22–20<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S), 53–60 west of South America
(2<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N–23<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S), and 92–95 over the Indian Ocean the IR
nadir images show only low-altitude clouds, which are below the lowest
tangent altitude of MIPAS. Over Asia (7<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–15<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) many
high-altitude clouds are present (profiles 4–15). Over northern China and
Mongolia there is a gap in the high-altitude clouds (profiles 17–18). Over
North and Central America (10–60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) there are patchy cloud
patterns, which is also reflected in the alternating cloudy and clear air
profiles (profiles 38–51) measured by MIPAS. From 26 to 60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S
(profiles 61–70) there is a large field of high-altitude clouds. At
latitudes higher than 60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>  the results from geostationary images
become uncertain, hence they are not discussed here. A more detailed
assessment of the detection sensitivity and altitude information accuracy of
the MIPAS measurements of the UTLS aerosol layer will be presented in a
future study.</p>

      <?xmltex \floatpos{p}?><fig id="Ch1.F2" specific-use="star"><caption><p>MIPAS profiles of orbit  49508 <bold>(a)</bold> measured on 18 August
2011 for <bold>(b)</bold> cloud index, <bold>(c)</bold> aerosol index, and <bold>(d)</bold>
aerosol–cloud index, <bold>(e)</bold> aerosol–cloud index. Black crosses denote
cloud/aerosol detections using a fixed CI threshold of 2 below 10 km and the
variable threshold definition following <xref ref-type="bibr" rid="bib1.bibx82" id="paren.78"/> above 10 km.
White curves denote the thermal tropopause according to the World
Meteorological Organization (WMO) definition along the orbit track derived
from ERA-Interim data <xref ref-type="bibr" rid="bib1.bibx12" id="paren.79"/>. In polar winter the thermal tropopause
is often not present <xref ref-type="bibr" rid="bib1.bibx106" id="paren.80"/>. Ice and optically thick clouds (grey
body radiators) are shown in grey. The IR nadir measurements of MTSAT, IODC,
and GOES-East <bold>(f)</bold> are shown temporally closest to the MIPAS
measurements. The IR nadir images were obtained from NERC Satellite Receiving
Station, Dundee University, Scotland, <uri>http://www.sat.dundee.ac.uk/</uri>.</p></caption>
            <?xmltex \igopts{width=426.791339pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f02.png"/>

          </fig>

</sec>
<sec id="Ch1.S3.SS1.SSS4">
  <title>Discussion of the ACI detection threshold value</title>
      <p>The simulations as well as the comparison with the most sensitive variable CI
threshold values indicated that a fixed ACI value of 7 is an appropriate
threshold value. Hence, in the following we use the ACI with a fixed
threshold value of 7 down to 7–9 km as an alternative to the CI with
variable thresholds above 10 km and a fixed threshold of 2 below 10 km. The
example (Fig. <xref ref-type="fig" rid="Ch1.F2"/>) shows the advantage of the ACI, namely
to have a fixed threshold that is sensitive to thin aerosol layers and
thick clouds, while not mistaking tropospheric clear air as cloudy.</p>
      <p>For the measurements before 2005 we also analysed altitudes below 7–9 km.
For these altitudes the simulations in Sect. <xref ref-type="sec" rid="Ch1.S3.SS1.SSS2"/>
indicated that the ACI for clear air falls below 7 at altitudes below
7–9 km. However, we often found ACI values significantly larger than 7 down
to the lowest tangent altitudes (Figs. <xref ref-type="fig" rid="App1.Ch1.F2"/>,
<xref ref-type="fig" rid="App1.Ch1.F4"/>) in the MIPAS measurements before 2005. As the
most likely reason for the discrepancy between the measurements and
simulations below 9 km we identified the water vapour continuum assumed in
the simulations. On the one hand, we used climatological water vapour profiles
that inherently do not cover the complete variability in the atmosphere;
on the other hand, in JURASSIC the Mlawer–Tobin–Clough–Kneizys–Davies 1.10
scheme (MT_CKD) <xref ref-type="bibr" rid="bib1.bibx10" id="paren.81"/> is used for the water vapour continuum
representation. This scheme was found to represent real conditions with
insufficient accuracy at lower altitudes <xref ref-type="bibr" rid="bib1.bibx32" id="paren.82"/>. Hence, the
ACI has the potential to be also applied to the MIPAS measurements before
2005, where the lowest tangent altitude reached down to nearly 5 km at all
latitudes.</p>
</sec>
</sec>
<sec id="Ch1.S3.SS2">
  <title>Ice cloud filtering</title>
<sec id="Ch1.S3.SS2.SSS1">
  <title>Window selection</title>
      <p>For the separation between aerosol and ice clouds by IR nadir measurements
spectral windows around 8.5, 11, and 12 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m (1176, 909,
833 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, respectively) are employed
<xref ref-type="bibr" rid="bib1.bibx1 bib1.bibx35" id="paren.83"/>. For these windows the optical properties
of ice differ most strongly from aerosol such as volcanic ash, soil-derived
aerosol, and sulfate aerosol <xref ref-type="bibr" rid="bib1.bibx1" id="paren.84"/>. For the IR limb emission
measurements of MIPAS we identified three narrow windows that have very
little interference with trace gases and exploit the spectral differences
between the optical properties of ice and, in our case, volcanic aerosol:
<list list-type="bullet"><list-item><p>830.6–831.1 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></p></list-item><list-item><p>960.0–961.0 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula></p></list-item><list-item><p>1224.1–1224.7 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>.</p></list-item></list>
Hereafter we refer to these windows as the 830, 960, and 1224 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> windows.</p>
      <p>The optical properties, i.e. extinction coefficient (<inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">β</mml:mi><mml:mi mathvariant="normal">e</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) and
single scattering albedo, are determined by the microphysical properties of
the particles, i.e. complex refractive index, particle size, and particle
shape. The imaginary and real parts of the complex refractive indices of ice
<xref ref-type="bibr" rid="bib1.bibx100" id="paren.85"/>, sulfate aerosol <xref ref-type="bibr" rid="bib1.bibx46" id="paren.86"/>, and two
representatives of volcanic ash (<xref ref-type="bibr" rid="bib1.bibx98" id="altparen.87"/>, volcanic ash;
<xref ref-type="bibr" rid="bib1.bibx71" id="altparen.88"/>, basalt) are shown in Fig. <xref ref-type="fig" rid="Ch1.F3"/>a and b,
where our windows are indicated by grey bars. The imaginary part of the
refractive index (Fig. <xref ref-type="fig" rid="Ch1.F3"/>a) has a positive spectral gradient
for ash and sulfate between 830 and 960 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, whereas the spectral
gradient of ice is negative. Also, between 830 and 1224 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> the
spectral gradient is positive for sulfate but negative for ice. For the real
part of the refractive indices (Fig. <xref ref-type="fig" rid="Ch1.F3"/>b), the spectral
gradient between 830 and 960 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> is positive for ash and sulfate but
negative for ice. The spectral gradient between 960 and 1224 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> is
negative for ash and sulfate but positive for ice.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><caption><p>Microphysical properties of sulfate aerosol, ice, and two types of
volcanic ash. <bold>(a, b)</bold> Complex refractive indices and their optical
properties. <bold>(c)</bold> Extinction coefficient. <bold>(d)</bold> Single
scattering albedo. The vertical lines indicate atmospheric window regions.</p></caption>
            <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f03.pdf"/>

          </fig>

      <p>As the imaginary part of the complex refractive index describes the
absorption and the real part describes the scattering, these differences
between ice clouds and aerosol (volcanic ash and sulfate aerosol) propagate
to the optical properties (Fig. <xref ref-type="fig" rid="Ch1.F3"/>c and d). To calculate the
extinction coefficient and single scattering albedo we used the same
log-normal size distributions as <xref ref-type="bibr" rid="bib1.bibx33" id="text.89"/> for sulfate aerosol,
volcanic ash, subvisible cirrus (small ice particles), and tropical cirrus
(large ice particles). The extinction coefficient spectra
(Fig. <xref ref-type="fig" rid="Ch1.F3"/>c) were normalised to 1 at 960 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. For
sulfate aerosol and ash they exhibit similar spectral gradients as the
imaginary part of the refractive index. However, in addition to the
refractive indices, the particle size has an impact on the optical
properties. For large ice particles the extinction coefficient spectrum is
flat and for small ice particles it exhibits a pronounced minimum around
960 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. The single scattering albedo depends on particle size and
wavenumber (Fig. <xref ref-type="fig" rid="Ch1.F3"/>d). The scattering contributions range
from 30 to 80 % for small ice particles and are nearly constant around
55 % for large ice particles. The scattering contribution of the sulfate
aerosol is generally below 10 % and for volcanic ash it ranges from 15 to
80 %. Hence, scattering effects can not be neglected for any particle type
discussed here.</p>
</sec>
<sec id="Ch1.S3.SS2.SSS2">
  <title>Simulations</title>
      <p>Having identified three window regions with small radiance contributions by
atmospheric trace gases and with significant differences in the optical
properties for ice and volcanic aerosol, we expected that these differences
could also be found in the radiance spectra measured by MIPAS. For IR nadir
measurements it is common practice to use brightness temperature differences
(BTDs) for the discrimination between volcanic or soil-derived aerosol and
ice clouds <xref ref-type="bibr" rid="bib1.bibx72 bib1.bibx2 bib1.bibx1" id="paren.90"><named-content content-type="pre">e.g.</named-content></xref>. In order
to identify characteristic patterns in BTD correlations for IR limb emission
measurements, we evaluated the radiative transfer simulations for clear air,
ice, volcanic ash, and sulfate aerosol under various atmospheric conditions
(<xref ref-type="sec" rid="Ch1.S3.SS1.SSS2"/>). In contrast to IR nadir BTD analyses that often
correlate 11–12 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m with 8–11 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m
<xref ref-type="bibr" rid="bib1.bibx2 bib1.bibx42" id="paren.91"><named-content content-type="pre">e.g.</named-content></xref>, we found for MIPAS IR limb spectra the
clearest correlation patterns for the BTDs between the 830 and
1224 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (12.0–8.2 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) windows and the 960 and
1224 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (10.4–8.2 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) windows.</p>
      <p>The simulation results are shown for all realistic ice cloud
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>a), sulfate aerosol (Fig. <xref ref-type="fig" rid="Ch1.F4"/>b),
volcanic ash (Fig. <xref ref-type="fig" rid="Ch1.F4"/>c), and “clear air”
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>d) scenarios. The tangent altitudes of the
simulations range from 6 to 19.5 km, which is from above to below the
simulated clouds. Except for the clear air simulations only the scenarios for
ACI <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 7 are shown. In the simulations, the individual results for the
BTDs are colour-coded by the ACI because we found a clear sensitivity to the
ACI in the simulations. The solid black lines are nearly identical to the
diagonal and split the plot into two parts (upper and lower part). Here, we
use them to guide the reader through each panel of
Fig. <xref ref-type="fig" rid="Ch1.F4"/>. In fact, these are our threshold functions that
will be derived in Sect. <xref ref-type="sec" rid="Ch1.S3.SS2.SSS4"/>.</p>
      <p>The ice simulations (Fig. <xref ref-type="fig" rid="Ch1.F4"/>a) comprise extinctions
ranging from 0.1 to 1 km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and mode radii ranging from 0.3 to
96 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. They fall in the middle of the BTD correlation plot,
forming a longish shape and reaching from negative BTDs to positive BTDs
(about <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>45 to 5 K) on both axes. Nearly all simulations fall into the
lower part (below the nearly diagonal separation lines). In the little inset
of Fig. <xref ref-type="fig" rid="Ch1.F4"/>a we filtered the comprehensive simulations for
realistic combinations of particle sizes and extinctions (number
concentrations). Hence, we removed all simulations with mode radii of
6 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and below and extinctions of <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">5</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>
and larger from the polar summer, midlatitude, and tropical atmosphere
because we consider such small ice particle sizes and high extinction (number
concentrations) only likely in PSCs <xref ref-type="bibr" rid="bib1.bibx13" id="paren.92"/>. SVCs may have such
small ice particle sizes, but they inherently have lower extinctions
<xref ref-type="bibr" rid="bib1.bibx47 bib1.bibx11 bib1.bibx19" id="paren.93"/>. The ice simulations show a dependence
on the ACI, where optically thick scenarios (ACI <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 2) form a narrow
cluster below the black line at BTDs between 0 and <inline-formula><mml:math display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn>20</mml:mn></mml:mrow></mml:math></inline-formula> K. Optically less
dense ice scenarios (ACI <inline-formula><mml:math display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> 2) usually have a lower BTD on both or only
one of both axes.</p>
      <p>The sulfate simulations (Fig. <xref ref-type="fig" rid="Ch1.F4"/>b) performed for
extinctions between <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">4</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and
mode radii between 0.01 and 1.5 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m have ACI values ranging from
larger than 2 to larger than 7. None of the scenarios that include
post-Pinatubo particle sizes and concentrations gets optically thick.
Scenarios for the 1 km thick sulfate aerosol layer with an extinction
coefficient of <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">4</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> at 947 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>
(10.5 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m) have ACIs larger than 7 and hence would be identified
as clear air. Scenarios with extinction coefficients of <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">5</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">4</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and higher have ACIs below 7. They cluster above the
diagonal at low BTDs (smaller than <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>20 K on the <inline-formula><mml:math display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> axis). The scenarios
that fall in the lower part of the plot are all for tangent altitudes below
8 km. Comparing the sulfate aerosol simulations with the ice cloud
simulations, there is nearly no overlap except for very few scenarios below
8 km.</p>
      <p>For the simulations of volcanic ash we used the “basalt” refractive indices
<xref ref-type="bibr" rid="bib1.bibx71" id="paren.94"/> (Fig. <xref ref-type="fig" rid="Ch1.F4"/>c) and the “volcanic ash”
refractive indices <xref ref-type="bibr" rid="bib1.bibx98" id="paren.95"/> (not shown). The simulations that were
performed for extinctions between <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">5</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> and mode radii between 0.1 and 5 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m cover
optically thick (ACI <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 2) to thin conditions. The simulated scenarios
form a diagonal shape in the middle of the BTD correlation plot and extend
from the lower left to the upper right of the plot. Also, a dependence on the
ACI, similar to the ice cloud simulations, with high values (optically
thin) at bottom left and small values (optically thick) at top right can be
seen. Several ash simulations fall in the lower part of the plot and are
congruent with the ice simulations. Hence, only the ash scenarios that fall
in the upper part of the plot are separable from ice clouds. In the
simulations we found a particle size dependency (not shown), where smaller
particles fall in the upper part and larger particles fall in the lower part
(ice region) of the plot. A size dependency for detecting volcanic ash with
IR limb emission measurements has also been reported by
<xref ref-type="bibr" rid="bib1.bibx33" id="text.96"/> with a maximum detectable mode radius of
1.5 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m for volcanic ash <xref ref-type="bibr" rid="bib1.bibx98" id="paren.97"/>. Here, for volcanic ash
we found scenarios with a mode radius of 5 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m that do not overlap
with ice. From the simulations presented here, we derived that volcanic ash
particles with mode radii between 0.3 and 5 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m and extinction
coefficients between <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">5</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> can
be discriminated from ice clouds at altitudes down to 6 km. Comparing the
ash simulations with the sulfate simulations, there is substantial overlap.
Hence, further criteria are required for the discrimination between sulfate
aerosol and volcanic ash. As the focus here is on filtering out ice spectra
from all cloudy spectra, we do not pursue an aerosol classification at this
point.</p>
      <p>Comparing the clear air simulations for the four atmospheres (polar winter,
polar summer, midlatitudes, equatorial) at altitudes between 6 and 19.5 km
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>d) with the ice and aerosol simulations shows that
there is an overlap. As already described in Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/>, there
are a few simulated clear air scenarios with ACI <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 7 below 9 km.
However, all clear air scenarios at altitudes below 14 km fall in the lower
part (ice region) of the BTD correlation plot and hence will be filtered out
together with the ice scenarios. Some scenarios above 14 km fall in the
upper part of the BTD correlation plot, but they all have an ACI <inline-formula><mml:math display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> 10.
Using an ACI <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 7 as a pre-condition, these clear air scenarios will be
filtered out also.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><caption><p>Simulated brightness temperature difference correlations for
<bold>(a)</bold> ice clouds, <bold>(b)</bold> sulfate aerosol, <bold>(c)</bold> volcanic
ash (here basalt from <xref ref-type="bibr" rid="bib1.bibx71" id="text.98"/> is shown), and <bold>(d)</bold> clear
air. The ice cloud simulations are shown for mode radii ranging from 0.3 to
96 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. In the small inset ice simulations are only shown for mode
radii ranging from 12 to 96 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. For the clear air simulations the
atmosphere type is indicated by the following symbols: polar winter –
crosses; polar summer – diamonds; midlatitudes – squares; equatorial –
circles. The black lines are the ice separation thresholds, where the solid
part of each line denotes the relevant part for the discrimination between
aerosol and ice.</p></caption>
            <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f04.pdf"/>

          </fig>

</sec>
<sec id="Ch1.S3.SS2.SSS3">
  <title>Measurements</title>
      <p>Having expectations from the simulations on what the BTD correlations look
like for ice clouds, sulfate aerosol, and volcanic ash, we show four selected
cases of UTLS aerosol measurements in order to verify the simulations
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>). For each case we used all measurements of an
entire day, which is about 14 orbits, in the latitude range given below and
at altitudes between MIPAS lowest tangent altitude (about 7 km) and 25 km.
For the longitude range we did not introduce a limitation in order to include
also clear air and ice clouds. In Fig. <xref ref-type="fig" rid="Ch1.F5"/> all spectra with
cloud/aerosol detections (ACI <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 7) are shown. Targeting at successfully
filtering out ice clouds, we expect that the aerosol clearly stands out from
the ice region as indicated by the simulations. For better comparison we also
added the nearly diagonal separation lines introduced in
Fig. <xref ref-type="fig" rid="Ch1.F4"/>.</p>
      <p>For 17 May 2011 (Fig. <xref ref-type="fig" rid="Ch1.F5"/>a) we expected to find only ice
clouds after filtering out the clear air spectra in the entire Southern
Hemisphere at latitudes between 0 and 60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S (since there are no
reports of volcanic eruptions; <xref ref-type="bibr" rid="bib1.bibx83" id="altparen.99"/>). As in the ice
cloud simulations (Fig. <xref ref-type="fig" rid="Ch1.F4"/>), the measurements with
ACI <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 7 form a relatively narrow diagonal group with BTDs ranging from 0
to <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>40 K on both axes.</p>
      <p>For 29 July 2011 (Fig. <xref ref-type="fig" rid="Ch1.F5"/>b) we expected to find sulfate
aerosol from the Nabro eruption covering the entire northern hemispheric UTLS
(0–90<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) <xref ref-type="bibr" rid="bib1.bibx6" id="paren.100"/> and ice clouds as well. In the
measurements with ACI <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 7 we again observe a relatively narrow diagonal
group just below the separations lines as in the ice simulations. In addition
there is a second cluster with ACI values between 5 and 7 and at BTDs between
<inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>30 and <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>50 K on the abscissa and between <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>20 and <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>40 K on the ordinate,
just as expected from the simulations for sulfate aerosol
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>b).</p>
      <p>For 16 June 2011 (Fig. <xref ref-type="fig" rid="Ch1.F5"/>c) we expected to find volcanic
ash at latitudes between 0 and 60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S originating from the eruption of
the Puyehue–Cordón Caulle <xref ref-type="bibr" rid="bib1.bibx52" id="paren.101"/> and ice clouds as well. As
seen in the two cases before, in the measurements with ACI <inline-formula><mml:math display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 7 there is
again a relatively narrow diagonal group just below the separation lines as
predicted by the ice simulations. Furthermore, there are many spectra above
the separation lines forming an arc-shaped structure and with ACI values
ranging from below 2 to 7. These measurements fall in the region covered by
the volcanic ash simulations (Fig. <xref ref-type="fig" rid="Ch1.F4"/>a).</p>
      <p>For 29 January 2011 (Fig. <xref ref-type="fig" rid="Ch1.F5"/>d) we again expected to find
tropospheric ice clouds after filtering out clear air spectra and polar
stratospheric clouds in the Northern Hemisphere (0–90<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N). As in
the cases before, there is the narrow diagonal ice group with ACI values
ranging from below 2 to 7, but there is also a second cluster just above the
separation lines with ACI values ranging from below 2 to 7. If only
measurements between 0 and 60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N are considered, the second cluster
disappears (Fig. <xref ref-type="fig" rid="App1.Ch1.F8"/>). This example demonstrates
that non-ice PSCs can also be separated from ice PSCs using this BTD
correlation. To determine the non-ice PSC types, particle sizes and
concentrations that can be separated from ice PSCs with this method require
detailed simulations which are not within the scope of this study. The
classification of PSCs measured by IR limb sounders is the subject of multiple
studies <xref ref-type="bibr" rid="bib1.bibx89 bib1.bibx90" id="paren.102"><named-content content-type="post">and references therein</named-content></xref>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><caption><p>MIPAS brightness temperature difference correlations for selected
scenarios: <bold>(a)</bold> ice clouds (0–60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S), <bold>(b)</bold> Nabro
sulfate aerosol (0–90<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) and ice clouds,
<bold>(c)</bold> Puyehue–Cordón Caulle volcanic ash (0–60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S) and
ice clouds, and <bold>(d)</bold> PSCs (0–90<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N) and tropospheric ice
clouds. All figures comprise all orbits (about 14) measured on the day given
on top of each plot. The black lines are the ice separation thresholds
derived from the observations, where the solid part of each line denotes the
relevant part for the discrimination between aerosol and ice.</p></caption>
            <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f05.pdf"/>

          </fig>

</sec>
<sec id="Ch1.S3.SS2.SSS4">
  <title>Definition of the ice filtering threshold and discussion</title>
      <p>As the simulations and measurements showed, the ice scenarios fall in the
lower half of the BTD correlation plot and a substantial number of the
aerosol simulations (volcanic ash and sulfate aerosol) falls in the upper
half (Figs. <xref ref-type="fig" rid="Ch1.F4"/> and <xref ref-type="fig" rid="Ch1.F5"/>). In order to
deduce an ice filtering threshold for MIPAS measurements, we analysed the
2011 MIPAS data on a day-by-day basis and analysed monthly and annual count
statistics. From these we found that filtering out the ice clouds is best
done with two threshold functions. For ACI values below 4 the upper edge of
the ice cluster (BTDs larger than 30.4 K on the <inline-formula><mml:math display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> axis) is very sharp in
the simulations (Fig. <xref ref-type="fig" rid="Ch1.F4"/>a) as well as in the measurements
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>). The corresponding threshold function is
              <disp-formula id="Ch1.E4" content-type="numbered"><mml:math display="block"><mml:mrow><mml:msub><mml:mi mathvariant="normal">BTD</mml:mi><mml:mrow><mml:mn>960</mml:mn><mml:mo>-</mml:mo><mml:mn>1224</mml:mn></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:mn>0.87</mml:mn><mml:mo>×</mml:mo><mml:msub><mml:mi mathvariant="normal">BTD</mml:mi><mml:mrow><mml:mn>830</mml:mn><mml:mo>-</mml:mo><mml:mn>1224</mml:mn></mml:mrow></mml:msub><mml:mo>+</mml:mo><mml:mn mathvariant="normal">6</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">K</mml:mi><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula>
            <?xmltex \hack{\newpage}?>For ACI values larger than 4 the BTD scatter plot can become
quite diffuse for 2011 because there were three volcanic eruptions
(Grímsvötn, Puyehue–Cordón Caulle, Nabro) that injected a
substantial amount of SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and volcanic ash into the atmosphere. We also
analysed the measurements from 2003, a year with very little volcanic
emissions during the MIPAS measurement period. For BTDs below <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>30.4 K we
obtained the following threshold function:
              <disp-formula id="Ch1.E5" content-type="numbered"><mml:math display="block"><mml:mrow><mml:msub><mml:mi mathvariant="normal">BTD</mml:mi><mml:mrow><mml:mn>960</mml:mn><mml:mo>-</mml:mo><mml:mn>1224</mml:mn></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:mn>1.33</mml:mn><mml:mo>×</mml:mo><mml:msub><mml:mi mathvariant="normal">BTD</mml:mi><mml:mrow><mml:mn>830</mml:mn><mml:mo>-</mml:mo><mml:mn>1224</mml:mn></mml:mrow></mml:msub><mml:mo>+</mml:mo><mml:mn>20</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">K</mml:mi><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula></p>
      <p>To identify aerosol in the MIPAS data we used the condition that the BTDs
must exceed at least one of the two threshold functions given in
Eqs. (<xref ref-type="disp-formula" rid="Ch1.E4"/>) and (<xref ref-type="disp-formula" rid="Ch1.E5"/>) (in Fig. <xref ref-type="fig" rid="Ch1.F5"/>
the black solid lines must be exceeded).</p>
      <p>For the MIPAS orbit discussed in Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/> the result using
our ice filtering thresholds is shown in Fig. <xref ref-type="fig" rid="Ch1.F2"/>e.
Figure <xref ref-type="fig" rid="Ch1.F2"/>e shows the ACI as in Fig. <xref ref-type="fig" rid="Ch1.F2"/>d
but indicating in grey all spectra that fall in the ice region. As expected
(see Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/>), nearly all aerosol/cloud detections in the
northern hemispheric troposphere are identified as ice clouds. On top of these
ice clouds there is a layer in the UTLS with ACI values between 4 and 7, which
is the Nabro sulfate aerosol. In the Antarctic region a large fraction of the
stratospheric clouds falls in the ice region, which can be expected in
southern hemispheric winter, but around profiles 83–85 non-ice PSCs are also
identified, consistent with the report of a NAT belt in the region downstream
of the Antarctic peninsula <xref ref-type="bibr" rid="bib1.bibx43" id="paren.103"/>.</p>
      <p>Considering Eqs. (<xref ref-type="disp-formula" rid="Ch1.E4"/>) and (<xref ref-type="disp-formula" rid="Ch1.E5"/>) derived from 2 years
of MIPAS measurements (2003, 2011) and the ice simulations
(Fig. <xref ref-type="fig" rid="Ch1.F4"/>a), it becomes obvious that the line corresponding
to Eq. (<xref ref-type="disp-formula" rid="Ch1.E4"/>) is very close to the simulations and that there is a
gap between the line corresponding to Eq. (<xref ref-type="disp-formula" rid="Ch1.E5"/>) and the
simulation results. Comparing the measurements (Fig. <xref ref-type="fig" rid="Ch1.F5"/>)
and the simulations in more detail, we found that the narrow ice pattern
below the threshold functions in the measurements is mostly reproduced by the
ice cloud simulations. Especially for ACI values below 2 simulations and
measurements agree well. However, for higher ACI values there are many
scenarios that fall in a range that was not covered by the measurements
(about 0 to <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>40 K on the abscissa and <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>20 to <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>50 K on the ordinate).
These scenarios have in common that the assumed mode radius of the particles
is 6 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m or smaller and the extinction coefficient is smaller than
or equal to 1<inline-formula><mml:math display="inline"><mml:mrow><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. We considered such small ice
particles to be likely for ice PSCs <xref ref-type="bibr" rid="bib1.bibx13" id="paren.104"/> and possibly SVCs
<xref ref-type="bibr" rid="bib1.bibx47 bib1.bibx11 bib1.bibx19" id="paren.105"/>. However, in the tropics and at
midlatitudes we could not find MIPAS measurements that fall into this range.
Hence, according to the MIPAS measurements 1 km thick ice clouds with mode
radii smaller than 6 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m seem very unlikely in the tropics and at
midlatitudes. Only in the polar regions, which are excluded in
Fig. <xref ref-type="fig" rid="Ch1.F5"/>a, b, c, did we find MIPAS measurements that show
the same BTDs as the ice cloud simulations for mode radii down to
3 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m.</p>
      <p>As already discussed in Sect. <xref ref-type="sec" rid="Ch1.S3.SS2.SSS2"/>, there are a few
simulated scenarios in the tropical atmosphere for the 18 km ice cloud that
slightly exceed the upper threshold function. For these particular scenarios
we assumed mode radii of 6 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m or less and the extinction
coefficients are between 5<inline-formula><mml:math display="inline"><mml:mrow><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> and 1 km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. In the tropics
mode radii of 6 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m or less can only be found in SVCs. However,
SVCs do not have such high particle concentrations and extinctions
<xref ref-type="bibr" rid="bib1.bibx47 bib1.bibx11 bib1.bibx19" id="paren.106"/>. Hence, in the inset of
Fig. <xref ref-type="fig" rid="Ch1.F4"/>a the simulation results are shown only for ice
particle size distributions with mode radii larger than 6 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. The
pattern of these ice cloud simulations is in very good agreement with the
measurements shown in Fig. <xref ref-type="fig" rid="Ch1.F5"/>. Further all, but 7 out of
3333, simulated scenarios fall below the threshold functions derived from the
measurements. These seven scenarios occur only for the ice cloud at 18 km
altitude in the tropics and they all have a BTD larger than <inline-formula><mml:math display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>25 K on the
abscissa. We checked the MIPAS measurements between 20<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>
(30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>) N and 20<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> (30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>) S and found that in 48 (62)
out of 58 945 (78 563) cloudy profiles in 2011 the upper threshold was
exceeded (both 0.08 %). In 2003, a year with less volcanic aerosol, only
15 (18) out of 56 375 (74 767) (0.02–0.03 %) cloudy profiles exceeded the
upper threshold. Although we do not consider 0.02–0.08 % to be a strong
evidence in the measurements that tropical high-altitude clouds consisting of
small ice particles could exceed the ice separation threshold, we would like
to point out that there is at least the theoretical possibility.</p>
      <p>The sulfate aerosol simulations (Fig. <xref ref-type="fig" rid="Ch1.F4"/>b) form a group
just above the lower threshold function. This group matches very well the
sulfate aerosol observations after the Nabro eruption
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>b). There are also a few scenarios for which the
simulated BTD does not exceed the aerosol detection threshold. These
scenarios occur all at tangent altitudes below 8 km. However, in the MIPAS
measurements we found numerous cases of aerosol detection below 8 km
altitude. This is most likely due to the fact that the aerosol layers in
reality have a larger vertical extent than the 1 km assumed in the
simulations. This effect and an analysis of the altitude information
including comparisons with lidar measurements will be discussed in detail in
a separate study.</p>
      <p>The volcanic ash simulations using “basalt” refractive indices reported by
<xref ref-type="bibr" rid="bib1.bibx71" id="text.107"/> (Fig. <xref ref-type="fig" rid="Ch1.F4"/>c) represent the volcanic ash
measurements after the Puyehue–Cordón Caulle eruption
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>c) better than simulations using the “volcanic
ash” refractive indices reported by <xref ref-type="bibr" rid="bib1.bibx98" id="text.108"/>. Thus, the volcanic ash
simulations are very sensitive to the refractive index data and therefore to
the type of volcanic ash present.</p>
</sec>
</sec>
</sec>
<sec id="Ch1.S4">
  <title>Examples for application and verification</title>
      <p>We applied our new aerosol detection method to the MIPAS measurements in
2011. We detected aerosol mainly after volcanic eruptions. In
Fig. <xref ref-type="fig" rid="Ch1.F6"/> three examples for aerosol detections after the
Grímsvötn, Puyehue–Cordón Caulle, and Nabro eruption are presented.
To verify our results we compared the MIPAS aerosol detections with SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>
and ash detections by AIRS. Note that gas-phase SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> is emitted by volcanic
eruptions and conversion to liquid sulfate (H<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:math></inline-formula>) starts immediately
after injection into the atmosphere by oxidation <xref ref-type="bibr" rid="bib1.bibx99" id="paren.109"/>. For our
comparisons of the horizontal plume locations we used the AIRS SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> index
and the AIRS ash index by <xref ref-type="bibr" rid="bib1.bibx40" id="text.110"/>. High SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> index values
indicate high SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> concentrations and high ash index values indicate high
ash concentrations.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><caption><p>AIRS volcanic emission contours and MIPAS aerosol detections
(coloured circles). <bold>(a)</bold> AIRS SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> index for Grímsvötn (27
May 2011, a.m.); <bold>(b)</bold> AIRS SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> index for Nabro (17 June 2011,
a.m.); <bold>(c)</bold> AIRS SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> index for Puyehue–Cordón Caulle
(9 June 2011, p.m.); <bold>(d)</bold> AIRS ash index for Puyehue–Cordón
Caulle (9 June 2011, p.m.). Non-ice PSCs in the Antarctic at altitudes above
18 km are coloured in black. The red triangles indicate the location of the
respective volcanoes. Please note the different altitude scales.</p></caption>
        <?xmltex \igopts{width=384.112205pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f06.png"/>

      </fig>

      <p>A U-shaped highly confined SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> filament was measured by AIRS on
27 May 2011, 6 days after the initial eruption of the Grímsvötn
volcano (Fig. <xref ref-type="fig" rid="Ch1.F6"/>a). The black dashed curves indicate the MIPAS
tracks measured between 00:00 and 12:00 UTC. Symbols along the MIPAS track
indicate aerosol detections. The symbols are coloured in shades of blue and
green representing the aerosol observation top altitude. In addition to our
new aerosol detection method, we looked for volcanic ash using the volcanic
ash detection method reported by <xref ref-type="bibr" rid="bib1.bibx33" id="text.111"/>. As we could not
detect volcanic ash in all four profiles, the volcanic aerosol particles are
most likely sulfate aerosol. The SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> measured by AIRS is the precursor gas
to sulfate aerosol measured by MIPAS. Since both SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and sulfate aerosol
can be detected, the SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> oxidised only partially during the 6 days after
the eruption and the AIRS and MIPAS measurements agree well in location.
While the AIRS data provide a high-horizontal-resolution picture of the
volcanic plume the MIPAS data add altitude information.</p>
      <p>In Fig. <xref ref-type="fig" rid="Ch1.F6"/>b the Nabro SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> plume is shown on 17 June 2011,
3 days after the initial eruption. The MIPAS tracks were measured between
00:00 and 12:00 UTC. The Nabro emissions were entrained in the Asian monsoon
circulation and first were transported northwards and later on eastwards.
Where the MIPAS tracks cross the SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> plume measured by AIRS, MIPAS detects
aerosol. In the MIPAS measurements we found mineral material using the MIPAS
ash detection method <xref ref-type="bibr" rid="bib1.bibx33" id="paren.112"/> in 2 out of 20 aerosol profiles
at altitudes below 10 km (over the Arabian peninsula and the Iranian
plateau). Based on this finding and studies by
<xref ref-type="bibr" rid="bib1.bibx17" id="text.113"/> and <xref ref-type="bibr" rid="bib1.bibx68" id="text.114"/> we conclude that the Nabro plume
mainly consists of sulfate aerosol, especially at higher altitudes. There are
also some aerosol detections over the North Sea and Siberia at altitudes
below 12 km that do not coincide with enhanced SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>. Based on MIPAS
measurements we deduced that these aerosol particles originated from the
Grímsvötn eruption about 1 month earlier. It is expected that 4
weeks after this eruption the emitted SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> is completely oxidised and
converted to sulfate aerosol <xref ref-type="bibr" rid="bib1.bibx99" id="paren.115"/> and hence can no longer be
seen in the AIRS SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> measurements <xref ref-type="bibr" rid="bib1.bibx41" id="paren.116"/>.</p>
      <p>The AIRS SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> index (Fig. <xref ref-type="fig" rid="Ch1.F6"/>c) and the ash index
(Fig. <xref ref-type="fig" rid="Ch1.F6"/>d) were measured on 9 June 2011, 3 days after the
initial eruption of the Puyehue–Cordón Caulle. The corresponding MIPAS
tracks were measured between 12:00 and 24:00 UTC. Aerosol detections above
18 km are coloured in black and are related to non-ice PSCs that are present
in each Antarctic winter <xref ref-type="bibr" rid="bib1.bibx70" id="paren.117"/>. Due to a strong jet stream the
volcanic emissions were transported eastwards very quickly. The SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> plume
(Fig. <xref ref-type="fig" rid="Ch1.F6"/>c) stretches from the southern tip of Africa to the
Indian Ocean just south-west of Australia. The Puyehue–Cordón Caulle
plume was rich in ash as shown by the AIRS ash index (Fig. <xref ref-type="fig" rid="Ch1.F6"/>d),
which shows an ash plume extending from west of Australia over South Africa
and along the way back to South America. Between South America and South
Africa there is no enhanced SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> visible in the AIRS data. The comparison
with the MIPAS aerosol detections based on the method presented here shows
that very close to the eastern plume front there are six MIPAS profiles in a
row indicating the presence of aerosol. These MIPAS detections are slightly
westward of the plume front measured by AIRS, which is due to a temporal
shift (up to 12 h) between the AIRS and MIPAS measurements. The comparison
of the MIPAS aerosol detections with the AIRS ash detections shows a good
agreement (Fig. <xref ref-type="fig" rid="Ch1.F6"/>d). Using the MIPAS ash detection technique
<xref ref-type="bibr" rid="bib1.bibx33" id="paren.118"/> we found ash in 10 out of 16 MIPAS aerosol profiles.</p>
      <p>For the three examples of fresh volcanic plumes in the polar, midlatitude,
and tropical atmosphere we found that the aerosol detection method introduced
for IR limb emission measurements (see Sect. <xref ref-type="sec" rid="Ch1.S3"/>) performs
well and also agrees well with AIRS volcanic emission measurements. However,
in contrast to AIRS volcanic emission measurements (ash and SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>) the MIPAS
volcanic emission measurements (comprising SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx45" id="paren.119"/>,
ash <xref ref-type="bibr" rid="bib1.bibx33" id="paren.120"/>, and sulfate aerosol from this study) can trace
volcanic emissions in the form of ash and sulfate aerosol for much longer
timescales (e.g. from June 2011 until April 2012 in case of the Nabro
eruption, not shown). This is due to a higher sensitivity of MIPAS to the
aerosol and due to the fact that SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> is converted to sulfate aerosol on a
timescale of about 4 weeks. These examples also demonstrate that IR
limb emission measurements provide valuable altitude information. In a recent
visualisation study, <xref ref-type="bibr" rid="bib1.bibx36" id="text.121"/> reconstructed 3-D volcanic emission
plumes of the Nabro and Puyehue–Cordón Caulle by combining MIPAS aerosol
and AIRS volcanic emission measurements with forward and backward
trajectories started at the location of MIPAS aerosol detections.</p>
</sec>
<sec id="Ch1.S5" sec-type="conclusions">
  <title>Summary and conclusions</title>
      <p>We introduced a two-step method to detect aerosol in the troposphere and
stratosphere with IR limb emission measurements. In the first step we
identified a window region in the MIPAS spectra that is sensitive towards
aerosol and clouds. In addition to the widely used  CI that is
very sensitive to clouds, we defined the AI that is more
sensitive to aerosol by using the identified window at 960 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. The AI
has the advantage of being less altitude dependent in the troposphere than
the CI. We combined the advantages of the AI in the troposphere and the CI in
the stratosphere in a new index, the ACI, which is the maximum of the CI and
the AI. The ACI is more sensitive towards aerosol and provides a better
contrast to clear air over the whole UTLS than the CI. Instead of varying CI
threshold values ranging from 2 to 6 depending on altitude, region, and
season, we found that a constant ACI threshold value of 7 is an appropriate
global value for the detection of enhanced aerosol and clouds.</p>
      <p>In the second step we developed a method to discriminate between ice clouds
and aerosol for IR limb emission spectra with an ACI below 7. We used
measured MIPAS spectra and simulations of optical properties for ice and
volcanic aerosol employing typical size distributions (volcanic ash and
sulfate aerosol) to identify appropriate windows for the discrimination.
Three windows at 830, 960, and 1224 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> that sample the contrasting
behaviour of ice and aerosol are combined by brightness temperature
difference correlations. We investigated the BTD correlations for the MIPAS
measurements and selected scenarios where we expected to find ice clouds
only, significant amounts of volcanic ash, volcanic sulfate aerosol, or
non-ice PSCs. From these measurements we derived two threshold functions that
separate between ice clouds and aerosol in MIPAS measurements.</p>
      <p>To corroborate and further characterise the threshold functions we conducted
radiative transfer simulations of ice clouds and aerosol layers. The
simulations showed that ice clouds fall below the thresholds and aerosol can
exceed the thresholds. Only for the rare case of optically thick
(<inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">β</mml:mi><mml:mi mathvariant="normal">e</mml:mi></mml:msub><mml:mo>≥</mml:mo><mml:mn mathvariant="normal">5</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) ice clouds at 18 km
altitude in the tropics could the threshold function be exceeded (7 out of
3333 scenarios). However, we consider these scenarios to be very unlikely and
found this confirmed by the measurements. The simulations further showed that
all realistic sulfate aerosol scenarios with
<inline-formula><mml:math display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">β</mml:mi><mml:mi mathvariant="normal">e</mml:mi></mml:msub><mml:mspace linebreak="nobreak" width="0.25em"/><mml:mo>(</mml:mo><mml:mn>948</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">4</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> above
8 km tangent altitude can be discriminated from ice clouds. For ash clouds
the simulations showed that several scenarios can be distinguished from ice
clouds. Detectable ash cloud scenarios had extinction coefficients (at
948 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) between <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">5</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> km<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>,
mode radii between 0.3 and 5 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m, and reached down to 6 km
tangent altitude. <?xmltex \hack{\newpage}?> A comparison of MIPAS measurements with
horizontal high-resolution AIRS SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> and ash index measurements for three
strong volcanic eruptions in 2011 that were either characterized by large
SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> (Grímsvötn, Nabro) or volcanic ash emissions
(Puyehue–Cordón Caulle) demonstrated the viability of our aerosol
detection method. This comparison and a recent study <xref ref-type="bibr" rid="bib1.bibx36" id="paren.122"/>
also point to the additional benefit of MIPAS altitude-resolved volcanic
aerosol detection. The IR limb emission measurements can be used to quickly
assign an altitude to the volcanic plume filaments measured by nadir
instruments.</p>
      <p>We consider our new aerosol detection method to be adaptable to other
hyper-spectral IR limb instruments such as CRISTA, CRISTA-NF, MIPAS
balloon (MIPAS-B) <xref ref-type="bibr" rid="bib1.bibx66" id="paren.123"/>, MIPAS-STRatospheric aircraft
(MIPAS-STR) <xref ref-type="bibr" rid="bib1.bibx103" id="paren.124"/>, and Gimballed Limb Observer for Radiance
Imaging of the Atmosphere (GLORIA) <xref ref-type="bibr" rid="bib1.bibx21 bib1.bibx78" id="paren.125"/>.
Although MIPAS is no longer operating there are 10 years of MIPAS
measurements available and the new aerosol detection method in conjunction
with the volcanic ash detection method <xref ref-type="bibr" rid="bib1.bibx33" id="paren.126"/> opens up new
perspectives for the analysis of enhanced aerosol in the UTLS and volcanic
eruptions based on IR limb emission measurements.</p>
</sec>
<sec id="Ch1.S6">
  <title>Data availability</title>
      <p>The data used for Figs. 1, 2, 4, 5, 6, A1, A2, A4, and A8 can be reproduced
by downloading the MIPAS Level 1b calibrated radiances from <xref ref-type="bibr" rid="bib1.bibx16" id="text.127"/> and
applying the methods described in this paper. The IR nadir images in Fig. 2f
were obtained from NERC Satellite Receiving Station, Dundee University,
Scotland (<uri>http://www.sat.dundee.ac.uk/</uri>). To generate Fig. 6 we used
AIRS level1b radiances that are available at <xref ref-type="bibr" rid="bib1.bibx64" id="text.128"/> and applied the
index methods described by <xref ref-type="bibr" rid="bib1.bibx40" id="text.129"/>. Access to the AIRS SO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>
and ash index data can be obtained by contacting Lars Hoffmann
(l.hoffmann@fz-juelich.de). Access to the complete data record of the MIPAS
aerosol detections and the radiative transfer simulation results can be
obtained by contacting the leading author (s.griessbach@fz-juelich.de).
<?xmltex \hack{\clearpage}?></p>
</sec>

      
      </body>
    <back><app-group>

<app id="App1.Ch1.S1">
  <title> </title>
<sec id="App1.Ch1.S1.SS1">
  <title>Variable CI thresholds</title>
      <p>The variable CI thresholds between 10 and 25 km used in this study were
derived from Fig. 2 in <xref ref-type="bibr" rid="bib1.bibx82" id="text.130"/>. Because of very similar threshold
profiles at these altitudes, we extracted the threshold profiles for three
latitude bands given in Table <xref ref-type="table" rid="App1.Ch1.T1"/> and used them for the
Northern and Southern hemispheres. At each altitude we used the smallest
integer threshold value in the corresponding latitude band. In the polar
region we neglected the simulated profile for Antarctic winter because it
“shows a large degree of uncertainty” <xref ref-type="bibr" rid="bib1.bibx82" id="paren.131"/>.</p>
</sec>
<sec id="App1.Ch1.S1.SS2">
  <title>Aerosol and cloud detection</title>
      <p>In the MIPAS measurements we found enhanced radiances in the 960 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>
window in the stratosphere at 50 km and below due to non-LTE effects of the
CO<inline-formula><mml:math display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> laser bands <xref ref-type="bibr" rid="bib1.bibx95" id="paren.132"/>. These radiances affect the AI and
cause low AI values that indicate incorrectly the presence of aerosol and
clouds at UTLS altitudes. The 830 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> window is not affected and
therefore, as discussed in Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/>, we defined the ACI.
Figure <xref ref-type="fig" rid="App1.Ch1.F1"/> illustrates the differences between the CI and
the AI in the middle stratosphere. Comparing the CI and AI with the ACI
illustrates that in the middle stratosphere the ACI is the CI and in the
troposphere the ACI is the AI. The spectra coloured in white are filtered
out because the radiances in at least one of the windows used in this study
were below the MIPAS noise:
            <disp-formula id="App1.Ch1.E1" content-type="numbered"><mml:math display="block"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mi>N</mml:mi><mml:msqrt><mml:mi>n</mml:mi></mml:msqrt></mml:mfrac></mml:mstyle><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
          where the MIPAS noise equivalent radiance <inline-formula><mml:math display="inline"><mml:mi>N</mml:mi></mml:math></inline-formula> is
<inline-formula><mml:math display="inline"><mml:mrow><mml:mn mathvariant="normal">3</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn>10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">4</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> W (m<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> sr cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>)<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in band A and
2<inline-formula><mml:math display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula>10<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">4</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> W (m<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> sr cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>)<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in band B
<xref ref-type="bibr" rid="bib1.bibx51" id="paren.133"/> and n is the number of spectral points.</p>
      <p>Figure <xref ref-type="fig" rid="App1.Ch1.F1"/> shows the characteristic MIPAS measurement
geometry after 2005 where the lowest tangent altitude follows the slope of
the tropopause with a high tropopause in the tropics and a low tropopause in
polar regions. The vertical sampling in the UTLS is 1.5 km. The measurement
geometry before 2005 is shown for the ACI in
Fig. <xref ref-type="fig" rid="App1.Ch1.F2"/>,
where the vertical sampling in the UTLS is 3 km and the lowest tangent
altitude reaches down to about 6 km at all latitudes.</p>

<?xmltex \floatpos{t!}?><table-wrap id="App1.Ch1.T1"><caption><p>Variable CI thresholds between 10 and 25 km derived from
<xref ref-type="bibr" rid="bib1.bibx82" id="text.134"/>.</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="center"/>
     <oasis:colspec colnum="3" colname="col3" align="center"/>
     <oasis:colspec colnum="4" colname="col4" align="center"/>
     <oasis:thead>
       <oasis:row rowsep="1">  
         <oasis:entry colname="col1">altitude/latitudes</oasis:entry>  
         <oasis:entry colname="col2">0–40</oasis:entry>  
         <oasis:entry colname="col3">40–65</oasis:entry>  
         <oasis:entry colname="col4">65–90</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>  
         <oasis:entry colname="col1">10</oasis:entry>  
         <oasis:entry colname="col2">3</oasis:entry>  
         <oasis:entry colname="col3">3</oasis:entry>  
         <oasis:entry colname="col4">3</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">11</oasis:entry>  
         <oasis:entry colname="col2">3</oasis:entry>  
         <oasis:entry colname="col3">4</oasis:entry>  
         <oasis:entry colname="col4">4</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">12</oasis:entry>  
         <oasis:entry colname="col2">4</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">5</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">13</oasis:entry>  
         <oasis:entry colname="col2">5</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">5</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">14</oasis:entry>  
         <oasis:entry colname="col2">5</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">5</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">15</oasis:entry>  
         <oasis:entry colname="col2">5</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">5</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">16</oasis:entry>  
         <oasis:entry colname="col2">5</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">5</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">17</oasis:entry>  
         <oasis:entry colname="col2">5</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">5</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">18</oasis:entry>  
         <oasis:entry colname="col2">5</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">5</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">19</oasis:entry>  
         <oasis:entry colname="col2">5</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">5</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">20</oasis:entry>  
         <oasis:entry colname="col2">6</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">4</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">21</oasis:entry>  
         <oasis:entry colname="col2">6</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">4</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">22</oasis:entry>  
         <oasis:entry colname="col2">6</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">3</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">23</oasis:entry>  
         <oasis:entry colname="col2">6</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">3</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">24</oasis:entry>  
         <oasis:entry colname="col2">6</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">2</oasis:entry>
       </oasis:row>
       <oasis:row>  
         <oasis:entry colname="col1">25</oasis:entry>  
         <oasis:entry colname="col2">6</oasis:entry>  
         <oasis:entry colname="col3">5</oasis:entry>  
         <oasis:entry colname="col4">2</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

<?xmltex \hack{\newpage}?>
</sec>
<sec id="App1.Ch1.S1.SS3">
  <title>Simulated and measured profiles</title>

      <?xmltex \floatpos{p}?><fig id="App1.Ch1.F1"><caption><p>CI <bold>(a)</bold>, AI <bold>(b)</bold>, and ACI <bold>(c)</bold> up to 50 km
altitude for MIPAS orbit 49508 measured on 18 August 2011. </p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f07.pdf"/>

        </fig>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.F2"><caption><p>ACI profiles for MIPAS orbit 7661 measured on 18 August 2003. The
black crossed denote cloudy regions identified by a fixed CI threshold of 2
below 10 km and by the variable thresholds above 10 km <xref ref-type="bibr" rid="bib1.bibx82" id="paren.135"/>.</p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f08.pdf"/>

        </fig>

      <p>In the following representative simulated and measured profiles for clear
air, ice clouds, and aerosol are shown in order to illustrate the behaviour of
the CI, AI, and ACI and to discuss their differences.</p>
      <p>The simulated clear air profiles for the CI and AI
(Fig. <xref ref-type="fig" rid="App1.Ch1.F3"/>a) show an altitude dependence for the CI
and the AI. In the simulations the CI is getting slightly smaller between 20
and about 12 km altitude whereas the AI is getting larger. Below 12 km
altitude the CI and the AI are getting significantly smaller with descending
altitude. At altitudes below 20 km the ACI
(Fig. <xref ref-type="fig" rid="App1.Ch1.F3"/>b) is the AI. The benefit of using the ACI
instead of the CI is that above about 10 km the ACI is not getting smaller
with decreasing altitude. This allows for a larger and altitude- and
latitude-independent threshold value, making this index more sensitive towards thin
aerosol layers.</p>
      <p>Comparing the clear air simulations (Fig. <xref ref-type="fig" rid="App1.Ch1.F3"/>) with
MIPAS measurements (Fig. <xref ref-type="fig" rid="App1.Ch1.F4"/>) shows a good
agreement of the shape of the vertical profile but systematically larger
values for the simulated CI and ACI above about 10 km (polar atmosphere:
Fig. <xref ref-type="fig" rid="App1.Ch1.F4"/>a, tropics:
Fig. <xref ref-type="fig" rid="App1.Ch1.F4"/>b, c). This difference is due to the fact
that in the clear air simulations no aerosol is considered, but in the real
atmosphere a variable amount of (background) aerosol is always present and
hence the index values are expected to be smaller. This effect is more
pronounced for the ACI than for the CI, because the 960 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> window
used for the ACI is only sensitive to the target species aerosol, whereas the
832 cm<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> window used for the CI is in addition slightly affected by the
water vapour continuum and some other trace gases. Below about 10 km in the
tropics the simulations of the CI and ACI show systematically smaller index
values than the measurements (Fig. <xref ref-type="fig" rid="App1.Ch1.F4"/>c).
Certainly the climatological data used in the simulations do not represent
the atmospheric state perfectly, but sensitivity tests showed that the ACI
simulations below 7.5 km at high and midlatitudes and 9.5 km in the
tropics are affected by the water vapour continuum. The water vapour scheme
used in JURASSIC is the MT_CKD scheme <xref ref-type="bibr" rid="bib1.bibx10" id="paren.136"/> that is known to
have a limited accuracy at the lowest altitudes (Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/>).
However, for the aerosol detection and ice filtering method presented here
this issue has no further implications, because the simulated clear air
spectra with low ACI values fall in the ice cloud group and hence will also
be filtered out.</p>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.F3"><caption><p>Simulated profiles for clear air in polar winter (dark blue), summer
(light blue), midlatitude (yellow), and equatorial (red) atmosphere.
<bold>(a)</bold> CI (solid lines) and AI (dashed lines). <bold>(b)</bold> ACI.</p></caption>
          <?xmltex \igopts{width=199.169291pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f09.pdf"/>

        </fig>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.F4"><caption><p>Measured ACI (solid lines) and CI (dashed lines) profiles for
<bold>(a)</bold> polar winter 2011 (70–90<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 0–2.5<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E),
<bold>(b)</bold> tropics 2011 (0–30<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S, 110–120<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E), and
<bold>(c)</bold> tropics 2003 (0–20<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 30–60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E). Grey dots
indicate clear air spectra and blue dots indicate spectra affected by ice
clouds according to the method presented in Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>.</p></caption>
          <?xmltex \igopts{width=199.169291pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f10.pdf"/>

        </fig>

      <p>Simulated profiles of the CI, AI, and ACI for a 1 km thick ice cloud,
volcanic ash, and sulfate aerosol are presented in Figs. <xref ref-type="fig" rid="App1.Ch1.F5"/>
to <xref ref-type="fig" rid="App1.Ch1.F7"/>. For the three particle types the deviation from
the clear air profile is more pronounced for the AI than for the CI. The CI
and AI minimum values due to the cloud layer are located slightly below cloud
altitude. For ice clouds (Fig. <xref ref-type="fig" rid="App1.Ch1.F5"/>) the AI is
systematically larger than the CI, whereas for volcanic ash
(Fig. <xref ref-type="fig" rid="App1.Ch1.F6"/>) and sulfate aerosol
(Fig. <xref ref-type="fig" rid="App1.Ch1.F7"/>) the AI can be smaller than the CI or both
values are similar. This is due to the spectral slope of the extinction
coefficient, where the extinction at 960 is larger than at 830 for sulfate
aerosol and ash and equal or smaller for ice. The simulations demonstrate
that the AI is highly sensitive not only to ice and aerosol but to aerosol
in particular.</p>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.F5" specific-use="star"><caption><p>Simulated profiles for a 1 km thick ice cloud for three extinctions
and the mode radius of 24 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m. Left column: CI (solid lines) and
AI (dashed lines). Right column ACI for cloud (coloured
lines) and clear air (black lines). The grey area indicates
the cloud layer. The colours indicate the atmosphere type: blue – polar
winter; light blue – polar summer; yellow – midlatitude; red – tropical
atmosphere.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f11.pdf"/>

        </fig>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.F6" specific-use="star"><caption><p>Same as Fig. <xref ref-type="fig" rid="App1.Ch1.F5"/> but for volcanic ash and the mode
radius of 0.8 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f12.pdf"/>

        </fig>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.F7" specific-use="star"><caption><p>Same as Fig. <xref ref-type="fig" rid="App1.Ch1.F5"/> but for sulfate aerosol and the
mode radius of 0.6 <inline-formula><mml:math display="inline"><mml:mi mathvariant="normal">µ</mml:mi></mml:math></inline-formula>m.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f13.pdf"/>

        </fig>

</sec>
<sec id="App1.Ch1.S1.SS4">
  <title>Separation between ice clouds and non-ice PSCs</title>
      <p>In Fig. <xref ref-type="fig" rid="Ch1.F5"/>d we show an example for PSCs where measurements
fall above the separation lines. On that particular day the polar vortex was
shifted towards about 60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N over Siberia (e.g. see MLS data at
<uri>http://mls.jpl.nasa.gov/</uri>) and temperatures were below 196 K and above
188 K so that STS and NAT PSCs can exist but not ice.
Figure <xref ref-type="fig" rid="App1.Ch1.F8"/>a shows the location and altitudes of MIPAS
particle detections that fall in the non-ice group. Most of these detections
are located in the polar region. As in
Fig. <xref ref-type="fig" rid="Ch1.F5"/>d, but for 0–60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N,
Fig. <xref ref-type="fig" rid="App1.Ch1.F8"/>b shows that the measurements above the
separation lines disappear, except for a few PSC detections south of
60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N over Siberia and some aerosol in the tropics. The fact that
the BTD correlation used here for filtering out ice clouds also improves the
discrimination between ice and non-ice PSCs has been investigated in a
separate study by <xref ref-type="bibr" rid="bib1.bibx91" id="text.137"/>.</p>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.F8" specific-use="star"><caption><p>Detection of non-ice particles on 29 January 2011. <bold>(a)</bold>
Location and altitudes of the particle detections. <bold>(b)</bold> Same as
Fig. <xref ref-type="fig" rid="Ch1.F5"/>d but for 0–60<inline-formula><mml:math display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://amt.copernicus.org/articles/9/4399/2016/amt-9-4399-2016-f14.pdf"/>

        </fig>

<?xmltex \hack{\clearpage}?>
</sec>
</app>
  </app-group><ack><title>Acknowledgements</title><p>We thank one anonymous reviewer for helpful comments and Mike Fromm for his
critical and constructive review. We are grateful to Thomas Kirchartz for
discussions and comments on the manuscript. We also thank W. Lahoz for a
grammatical and stylistic revision of the manuscript. The MIPAS data were
provided by the European Space Agency. The AIRS data were obtained from the
NASA Goddard Earth Sciences Data Information and Services Center (GES DISC).
The simulations were performed on JuRoPA at Forschungszentrum Jülich. We
gratefully acknowledge the computing time granted on the supercomputer at
Jülich Supercomputing Centre (JSC).<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?>The
article processing charges for this open-access <?xmltex \hack{\newline}?> publication
were covered by a Research <?xmltex \hack{\newline}?> Centre of the Helmholtz
Association.<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?>Edited by: E. Kyrölä
<?xmltex \hack{\newline}?> Reviewed by: two anonymous referees</p></ack><ref-list>
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    <!--<article-title-html>Infrared limb emission measurements of aerosol in the troposphere and stratosphere</article-title-html>
<abstract-html><p class="p">Altitude-resolved aerosol detection in the upper troposphere and lower
stratosphere (UTLS) is a challenging task for remote sensing instruments.
Infrared limb emission measurements provide vertically resolved global
measurements at day- and nighttime in the UTLS. For high-spectral-resolution
infrared limb instruments we present here a new method to detect aerosol and
separate between ice and non-ice particles. The method is based on an
improved aerosol–cloud index that identifies infrared limb emission spectra
affected by non-ice aerosol or ice clouds. For the discrimination between
non-ice aerosol and ice clouds we employed brightness temperature difference
correlations. The discrimination thresholds for this method were derived from
radiative transfer simulations (including scattering) and Michelson
Interferometer for Passive Atmospheric Sounding (MIPAS)/Envisat measurements
obtained in 2011. We demonstrate the value of this approach for observations
of volcanic ash and sulfate aerosol originating from the Grímsvötn
(Iceland, 64° N), Puyehue–Cordón Caulle (Chile,
40° S), and Nabro (Eritrea, 13° N) eruptions in May and
June 2011 by comparing the MIPAS volcanic aerosol detections with Atmospheric
Infrared Sounder (AIRS) volcanic ash and SO<sub>2</sub> measurements.</p></abstract-html>
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