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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-13-2335-2020</article-id><title-group><article-title>Atmospheric observations of the water vapour continuum in the near-infrared windows between 2500 and 6600 cm<inline-formula><mml:math id="M1" 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></article-title><alt-title>Atmospheric observations of the water vapour continuum</alt-title>
      </title-group><?xmltex \runningtitle{Atmospheric observations of the water vapour continuum}?><?xmltex \runningauthor{J. Elsey et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Elsey</surname><given-names>Jonathan</given-names></name>
          <email>jon.elsey@reading.ac.uk</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Coleman</surname><given-names>Marc D.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Gardiner</surname><given-names>Tom D.</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Menang</surname><given-names>Kaah P.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-7402-0141</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Shine</surname><given-names>Keith P.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-2672-9978</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Department of Meteorology, University of Reading, Reading, RG6 6BB, UK</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>National Physical Laboratory, Teddington, London, TW11 0LW, UK</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>National Department of Meteorology, Ministry of Transport,
Yaoundé, Cameroon</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Jonathan Elsey (jon.elsey@reading.ac.uk)</corresp></author-notes><pub-date><day>13</day><month>May</month><year>2020</year></pub-date>
      
      <volume>13</volume>
      <issue>5</issue>
      <fpage>2335</fpage><lpage>2361</lpage>
      <history>
        <date date-type="received"><day>28</day><month>October</month><year>2019</year></date>
           <date date-type="rev-request"><day>16</day><month>December</month><year>2019</year></date>
           <date date-type="rev-recd"><day>2</day><month>April</month><year>2020</year></date>
           <date date-type="accepted"><day>7</day><month>April</month><year>2020</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2020 </copyright-statement>
        <copyright-year>2020</copyright-year>
      <license license-type="open-access"><license-p>This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><self-uri xlink:href="https://amt.copernicus.org/articles/.html">This article is available from https://amt.copernicus.org/articles/.html</self-uri><self-uri xlink:href="https://amt.copernicus.org/articles/.pdf">The full text article is available as a PDF file from https://amt.copernicus.org/articles/.pdf</self-uri>
      <abstract><title>Abstract</title>
    <p id="d1e141">Water vapour continuum absorption is potentially
important for both closure of the Earth's energy budget and remote sensing
applications. Currently, there are significant uncertainties in its
characteristics in the near-infrared atmospheric windows at
2.1 and 1.6 <inline-formula><mml:math id="M2" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m. There have been several attempts to measure the continuum in the
laboratory; not only are there significant differences amongst these
measurements, but there are also difficulties in extrapolating the laboratory
data taken at room temperature and above to temperatures more widely
relevant to the atmosphere. Validation is therefore required using field
observations of the real atmosphere. There are currently no published
observations in atmospheric conditions with enough water vapour to detect a
continuum signal within these windows or where the self-continuum component
is significant. We present observations of the near-infrared water vapour
continuum from Camborne, UK, at sea level using a Sun-pointing,
radiometrically calibrated Fourier transform spectrometer in the window
regions between 2000 and 10 000 cm<inline-formula><mml:math id="M3" 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>. Analysis of these data is challenging,
particularly because of the need to remove aerosol extinction and the large
uncertainties associated with such field measurements. Nevertheless, we
present data that are consistent with recent laboratory datasets in the 4 and
2.1 <inline-formula><mml:math id="M4" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows (when extrapolated to atmospheric temperatures). These
results indicate that the most recent revision (3.2) of the
MT_CKD foreign continuum, versions of which are widely used
in atmospheric radiation models, requires strengthening by a factor of
<inline-formula><mml:math id="M5" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula> in the centre of the 2.1 <inline-formula><mml:math id="M6" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window. In the
higher-wavenumber window at 1.6 <inline-formula><mml:math id="M7" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m, our estimated self- and foreign-continua are significantly stronger than MT_CKD. The possible
contribution of the self- and foreign-continua to our derived total continuum
optical depth is estimated by using laboratory or MT_CKD
values of one, to estimate the other. The obtained self-continuum shows some
consistency with temperature-extrapolated laboratory data in the centres of
the 4 and 2.1 <inline-formula><mml:math id="M8" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows. The 1.6 <inline-formula><mml:math id="M9" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m region is more sensitive to
atmospheric aerosol and continuum retrievals and therefore more uncertain
than the more robust results at 2.1 and 4 <inline-formula><mml:math id="M10" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m. We highlight the
difficulties in observing the atmospheric continuum and make the case for
additional measurements in both the laboratory and field and discuss the
requirements for any future field campaign.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
<sec id="Ch1.S1.SS1">
  <label>1.1</label><title>Background</title>
      <p id="d1e239">The near-infrared spectrum (defined here in wavenumber space as 2000–10 000 cm<inline-formula><mml:math id="M11" 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 characterised by its spectral band-window structure, where
parts of the spectrum are completely opaque to radiation and others are
mostly transparent over typical (clear-sky) atmospheric paths. Within this
spectral region, in addition to the many discrete spectral lines of various
gases, there is additional absorption due to the water vapour continuum
absorption (henceforth simply continuum), a smoothly varying (with
wavenumber) component of the total absorption which underlies this
band-window structure. The cause of this continuum is not known but is
postulated to be due to a combination of far-wing broadening, e.g. by
collisional effects, and absorption due to<?pagebreak page2336?> water dimers (bound or
quasi-bound complexes of two water vapour molecules), as discussed in e.g. Shine et al. (2012). The continuum is normally
broken down into two components: a self-continuum component that depends on
the square of the vapour pressure and a foreign-continuum component that
depends linearly on vapour pressure and the pressure of the ambient air. The
foreign continuum is observed to have at most a weak temperature dependence (Ptashnik et al., 2012), while the
self-continuum has a negative exponential temperature dependence (Mondelain et al., 2014;
Ptashnik et al., 2011a). The temperature dependence of the self-continuum is
broadly consistent with a dimer-like theory, but this has not been verified
due to the difficulty of performing ab initio calculations of the water dimer
spectrum, and the strength of the temperature dependence varies amongst
different sets of measurements and may depend on wavenumber (e.g. Ptashnik et al., 2011b).</p>
      <p id="d1e254">Since the continuum absorbs radiation (particularly in the atmospheric
windows) which would otherwise penetrate further into the atmosphere or
reach the surface, it influences the surface–atmosphere partitioning of
energy and is therefore important for understanding the global energy
budget. In the more transparent window regions, most of the continuum
absorption occurs in the troposphere where water vapour is more abundant and
has a potential influence on the hydrological cycle. The continuum
contribution to climate feedbacks could also be enhanced in a warming
climate via the water vapour feedback; the strongly absorbing water vapour
bands are already close to saturation, meaning that the window regions, in
which the continuum is comparatively more important, could contribute more
to the change in absorption in a warming climate. For example, Rädel et
al. (2015) found that the near-IR continuum contributes <inline-formula><mml:math id="M12" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">10</mml:mn></mml:mrow></mml:math></inline-formula> %–20 % of the total water vapour shortwave feedback in a scenario with a
33 % increase in water vapour, depending on whether a weaker or a stronger
continuum is used. The continuum also impacts upon remote sensing of the
Earth's atmosphere and surface. Some remote sensing platforms, e.g. the
Orbiting Carbon Observatory 2 (OCO-2) (Oyafuso et al., 2017), have
channels observing in the 2.1 and 1.6 <inline-formula><mml:math id="M13" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m (<inline-formula><mml:math id="M14" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">4000</mml:mn></mml:mrow></mml:math></inline-formula> and 6300 cm<inline-formula><mml:math id="M15" 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) windows, as does the MODIS satellite (Platnick et al., 2017),
which is used to retrieve gas concentrations, cloud properties, surface
albedo, and aerosol optical depth.</p>
      <p id="d1e297">The strength of the near-infrared continuum is uncertain, particularly in
the 2.1 and 1.6 <inline-formula><mml:math id="M16" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows. There have been relatively few attempts to
measure the self-continuum in the laboratory, with observed absorption
coefficients that differ significantly (e.g. Shine et al., 2016) in the centres
of these windows at room temperature. Measuring the continuum in the
laboratory is problematic in some ways, due to the need to extrapolate in
temperature and pressure to conditions present in the atmosphere (which are
frequently below room temperature). The weak absorption strength of the
continuum in the windows makes it difficult to measure at typical
tropospheric temperatures (<inline-formula><mml:math id="M17" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">280</mml:mn></mml:mrow></mml:math></inline-formula> K) without long path lengths
(such as that from the top of atmosphere (TOA) to the surface), which are
difficult to attain in a laboratory. These issues can be mitigated using
certain high-precision techniques, e.g. cavity ring-down spectroscopy (CRDS), at the cost of wide spectral coverage. However, while CRDS
measurements exist at room temperature, there are none reported in the
literature at the lower temperatures considered here. Additionally, the weak
(and featureless) absorption means that the measurements are very sensitive
to the experimental conditions, such as the baseline stability of the
spectrometer when using Fourier transform spectroscopy (FTS) techniques
(e.g. Ptashnik et al., 2015).</p>
      <p id="d1e318">The continuum is parameterised in most radiative transfer codes used in
models and remote sensing by the MT_CKD
(Mlawer-Tobin_Clough-Kneizys-Davies) model (Mlawer et al., 2012),
typically using either version 2.5 or version 3.2 (Mlawer et al., 2019). MT_CKD is a semi-empirical model. Examples of codes using this model include
the Atmospheric Radiative Transfer Simulator (Buehler et al., 2018), the
Reference Forward Model (Dudhia et al., 2017), the Orbiting Carbon
Observatory-2 (O'Dell et al., 2018), the Met Office Unified Model (Walters et
al., 2019), and the GFDL Global Atmosphere and Land Model (Zhao et al., 2018).
In the window regions, the MT_CKD continuum mostly originates
from adjustment of the water vapour lineshape using a <inline-formula><mml:math id="M18" display="inline"><mml:mi mathvariant="italic">χ</mml:mi></mml:math></inline-formula> factor derived
primarily from measurements at wavenumbers in the mid- and far-infrared
(<inline-formula><mml:math id="M19" display="inline"><mml:mrow><mml:mi mathvariant="italic">&lt;</mml:mi><mml:mn mathvariant="normal">2000</mml:mn></mml:mrow></mml:math></inline-formula> cm<inline-formula><mml:math id="M20" 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 additional empirical adjustments. It is not
an ab initio calculation and uses selected observations to adjust its continuum
strength. Any such adjustment should therefore consider the uncertainty and
differences in the available measurements. A particularly important aspect
is the temperature dependence; atmospheric radiative transfer models
generally use the MT_CKD formulation to extrapolate the
self-continuum absorption to temperatures at which there are no laboratory
measurements.</p>
      <p id="d1e351">Measurements of the continuum in the atmosphere are therefore necessary to
supplement laboratory measurements. While field measurements present their
own issues, explained more in Sects. 3 and 6, they provide data with which
to test the experimentally implied temperature dependence, as well as that
of MT_CKD. Ideally, a combination of field and laboratory
measurements would converge on a set of continua at different temperatures
and pressures that could be included in spectroscopic databases such as
HITRAN (Gordon
et al., 2017) or at least provide a set of robust values (with agreement
within the uncertainties) that can be used to adjust MT_CKD.</p>
      <p id="d1e354">In this work, we present the first reported derivation of the near-IR
atmospheric continuum in the 4, 2.1, and 1.6 <inline-formula><mml:math id="M21" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows at mean sea
level with a well-constrained uncertainty budget, and the first to be
derived using a radiometrically calibrated spectrometer. These measurements
were made during the CAVIAR (Continuum Absorption at Visible and Infrared
wavelengths and its Atmospheric Relevance) field campaign<?pagebreak page2337?> in Camborne,
Cornwall, UK, in August–September 2008 (Gardiner et
al., 2012). Since these measurements are at mean sea level, it has been
estimated that the continuum absorption will be roughly evenly split between
the self- and foreign-continua at 1.6 <inline-formula><mml:math id="M22" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m and <inline-formula><mml:math id="M23" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">70</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="italic">%</mml:mi></mml:mrow></mml:math></inline-formula> self : 30<inline-formula><mml:math id="M24" display="inline"><mml:mrow><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="italic">%</mml:mi></mml:mrow></mml:math></inline-formula> foreign
in the 2.1 <inline-formula><mml:math id="M25" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window based on laboratory measurements (as calculated in Ptashnik et al.,
2012). Additionally, observing at sea level allows us to measure the
continuum within the windows, as the expected continuum contribution is
above the signal-to-noise of our spectrometer (see Sect. 2.2). These
conditions set our results apart from those of Reichert and
Sussmann (2016), who used an FTS at a high-altitude site to measure the
continuum. This allowed observations of the continuum within the bands but
restricted the ability to detect it within the windows. Additionally, our
measurements are radiometrically calibrated and traceable to SI (<italic>Système international d'unités</italic>, BIPM, 2006); this allows us to obtain the top-of-atmosphere
solar spectral irradiance (SSI) directly (Elsey
et al., 2017; Menang et al., 2013), which is itself uncertain to
<inline-formula><mml:math id="M26" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">8</mml:mn></mml:mrow></mml:math></inline-formula> % in the 4000–7000 cm<inline-formula><mml:math id="M27" 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> region.</p>
</sec>
<sec id="Ch1.S1.SS2">
  <label>1.2</label><title>Atmospheric observations of the near-IR continuum</title>
      <p id="d1e437">This section discusses the current literature in terms of field measurements
of the near-IR continuum. Reichert and Sussmann (2016), henceforth
“Zugspitze”, presented a continuum absorption obtained in atmospheric
conditions at a high-altitude site at the Zugspitze in the German Alps. This
used an FTS calibrated using a combination of Langley-derived TOA
irradiance, a medium-temperature (<inline-formula><mml:math id="M28" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">1970</mml:mn></mml:mrow></mml:math></inline-formula> K) blackbody and an
assumed SSI from a radiative transfer model (Reichert et
al., 2016). The high altitude allows for measurements of the continuum well
into the main water vapour absorption bands and ostensibly allows for an
upper limit to be set on the absorption in the windows. These are the most
immediately comparable measurements in the literature to the ones presented
here. There are several key differences between the two field campaigns,
which makes them difficult to compare directly. The Zugspitze measurements
were performed in conditions that had a significantly smaller water vapour
path, meaning that observations of the continuum in the windows are
extremely difficult, while allowing observations in the bands that sea-level
observations are not capable of. Additionally, the higher-altitude
measurements are dominated by the foreign continuum due to the lower vapour
pressures, whereas the sea-level observations are more of a mixture of
foreign- and self-continua. The higher-altitude measurements are above the
atmospheric boundary layer, mitigating the effect of aerosol extinction,
which is a significant problem for sea-level observations. To obtain a long
enough path length to mitigate the lack of water vapour, the Zugspitze
measurements were taken at large air-mass factors (<inline-formula><mml:math id="M29" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula>–9). This
may be problematic however since (a) the effects of atmospheric refraction
are more pronounced and (b) extrapolating from high air mass to zero air mass
using the Langley method increases the effect of the uncertainty in the
individual measurements, since these primarily use the closure method and
are therefore reliant on their calibration to a prescribed SSI.</p>
      <p id="d1e460">These factors mean that Zugspitze observations are available in the 2.1 <inline-formula><mml:math id="M30" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window and within several of the adjacent water vapour bands, but values
are not presented in the 1.6 <inline-formula><mml:math id="M31" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window (many of these are in fact
negative). Due to the large uncertainties, these are seemingly consistent
with both MT_CKD and contemporary laboratory measurements of
the foreign continuum (see Sect. 5.2), despite the considerable
differences between these datasets. These will be examined in more detail in
Sects. 4 and 5. Nevertheless, it should be emphasised that these
measurements are a significant advance in our understanding of the in-band
continuum. Additionally, as understanding of the near-IR SSI is improved,
the calibration used in the Zugspitze measurements could be used to measure
the continuum without the need for an expensive and time-consuming blackbody
calibration, which would allow for measurements in a wider variety of
conditions. This would both help validate radiative transfer models and
allow for separation of the foreign-continuum and self-continuum contributions in
atmospheric conditions; this task is extremely challenging to do with a
single field campaign at one location if only modest changes in water vapour
column occur.</p>
</sec>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Methods and experimental setup</title>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>Retrieval methods</title>
      <p id="d1e495">This work builds upon the work of Tallis et al. (2011), Menang et
al. (2013), and Elsey et al. (2017). These all used observations obtained
using an absolutely calibrated ground-based Sun-pointing Fourier transform
spectrometer (Gardiner et al., 2012) set up at a field site in Camborne,
Cornwall, UK (50.218<inline-formula><mml:math id="M32" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N, 5.327<inline-formula><mml:math id="M33" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E). Those papers focused on water
vapour spectral lines and SSI respectively. Gardiner et al. (2012) present
the calibration procedure and FTS setup in detail. The spectrometer measures
the centre of the solar disk (using dedicated solar tracker optics) in the
range 2000–10 000 cm<inline-formula><mml:math id="M34" 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 a spectral resolution of 0.03 cm<inline-formula><mml:math id="M35" 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 FTS is radiometrically calibrated, with traceability to SI via
calibration to the 3000 K Ultra High Temperature Blackbody (UHTBB) at the UK
National Physical Laboratory. The field-of-view of the FTS is
0.26<inline-formula><mml:math id="M36" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>.</p>
      <p id="d1e549">The total optical depth <inline-formula><mml:math id="M37" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">total</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> can be determined from the
irradiance <inline-formula><mml:math id="M38" display="inline"><mml:mi>I</mml:mi></mml:math></inline-formula> observed by the FTS at a given air-mass factor <inline-formula><mml:math id="M39" display="inline"><mml:mrow><mml:mi>m</mml:mi><mml:mo>=</mml:mo></mml:mrow></mml:math></inline-formula> sec(<inline-formula><mml:math id="M40" display="inline"><mml:mi mathvariant="italic">θ</mml:mi></mml:math></inline-formula>) (with <inline-formula><mml:math id="M41" display="inline"><mml:mi mathvariant="italic">θ</mml:mi></mml:math></inline-formula> the solar zenith angle). This is done using measurements
at a range of air masses via the Langley method or given a top-of-atmosphere
irradiance <inline-formula><mml:math id="M42" display="inline"><mml:mrow><mml:msub><mml:mi>I</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, the radiative closure method. Taking the logarithm of
the Beer–Bouguer–Lambert law,
            <disp-formula id="Ch1.E1" content-type="numbered"><label>1</label><mml:math id="M43" display="block"><mml:mrow><mml:mi>ln⁡</mml:mi><mml:mfenced open="(" close=")"><mml:mi>I</mml:mi></mml:mfenced><mml:mo>=</mml:mo><mml:mi>ln⁡</mml:mi><mml:mfenced open="(" close=")"><mml:mrow><mml:msub><mml:mi>I</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mfenced><mml:mo>-</mml:mo><mml:mi>m</mml:mi><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">total</mml:mi></mml:msub><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula>
         <?pagebreak page2338?> The radiative closure method is a simple inversion of this equation to solve
for <inline-formula><mml:math id="M44" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">total</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>. In this case, the SSI of Elsey et al. (2017) is
used, since this is determined directly by the spectrometer used in this
work. This does however introduce significant extra uncertainty, given the
large uncertainty in the near-IR SSI, particularly in the lower-wavenumber
windows.</p>
      <p id="d1e650">The Langley method exploits the fact that Eq. (1) can be solved as a linear
equation given observations at various air masses, assuming that the optical
depth does not vary significantly between these air masses. This means that
the aerosol optical depth (<inline-formula><mml:math id="M45" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) needs to be measured at the
same time as a spectrometer measurement and along the same atmospheric path,
as does the integrated water vapour (IWV). It also means that measurements
must be taken when there are no clouds present. <inline-formula><mml:math id="M46" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> was
measured using a handheld Microtops II sunphotometer (Solar
Light Company, 2001) at 0.38, 0.44, 0.675, 0.936, and 1.02 <inline-formula><mml:math id="M47" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m. The
Microtops has a field-of-view of 2.5<inline-formula><mml:math id="M48" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> and was operated by hand
rather than mounted on a solar tracker, which could lead to some additional
uncertainty (see Sect. 2.4). Integrated water vapour was measured using a
HATPRO microwave radiometer (Rose and Czekala, 2011). The effects
of clouds were minimised by visually checking for clouds at the time of
measurement and by using the variation in the observed voltage of the
spectrometer detector to determine whether any sub-visible clouds or haze
passed into the line-of-sight of the spectrometer during a measurement.</p>
      <p id="d1e692">The continuum optical depth, <inline-formula><mml:math id="M49" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">cont</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> derived from the total optical
depth <inline-formula><mml:math id="M50" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">total</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> obtained from the spectrometer measurements,
can be characterised as
            <disp-formula id="Ch1.E2" content-type="numbered"><label>2</label><mml:math id="M51" display="block"><mml:mtable columnspacing="1em" class="split" rowspacing="0.2ex" displaystyle="true" columnalign="right left"><mml:mtr><mml:mtd><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">cont</mml:mi></mml:msub></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">total</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mrow><mml:msub><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow><mml:mi mathvariant="normal">lines</mml:mi></mml:msub></mml:mrow></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mtext>other_gases</mml:mtext></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">Rayleigh</mml:mi></mml:msub></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">other</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub><mml:mo>.</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:math></disp-formula>
          The retrieval of the continuum mostly relies on accurate determination of
the line-by-line absorption from water vapour and other gases, and aerosol
extinction. Rayleigh scattering was modelled using the calculations of Bucholtz (1995). It is mostly negligible in the near-IR windows (Elsey et al., 2017)
and thus has minimal effect on the derived continuum. The line-by-line
optical depth was determined using the Reference Forward Model (version
5.01, Dudhia, 2017), the HITRAN2016
spectroscopic database (Gordon et al., 2017), and the Voigt lineshape cut off
at 25 cm<inline-formula><mml:math id="M52" 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 the line contribution at 25 cm<inline-formula><mml:math id="M53" 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> subtracted at
wavenumbers less than 25 cm<inline-formula><mml:math id="M54" 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>, as this is assumed to be part of the
continuum following the MT_CKD definition). It follows that
the choice of spectroscopic database has an effect on the derived continuum,
since a change in line parameters will affect the amount of absorption
attributed to the spectral lines rather than the continuum. This may also
affect our comparison with earlier studies, since these may use different
line databases to HITRAN2016. Since HITRAN2016 is one of the most up-to-date
line lists available, we believe it is the most suitable here.</p>
      <p id="d1e829">The atmospheric profiles were derived using co-located radiosonde ascents
and checked using ECMWF and Met Office analysis data. To minimise the effect
of solar lines, all regions within 0.1 cm<inline-formula><mml:math id="M55" 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> of a solar line (as
observed by Menang et al., 2013, and Elsey et al., 2017) are filtered
out. To minimise the effect of line shifting in the measurements or
misattributed line positions in HITRAN, the observed continuum is smoothed
over 15 cm<inline-formula><mml:math id="M56" 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>. This smoothing is suitable for observing the continuum,
as the continuum varies smoothly with wavenumber. This is necessary in
particular due to the high spectral resolution of the measurements, and also
filters out any high-frequency noise within these observations that may not
be accounted for otherwise. Regions with <inline-formula><mml:math id="M57" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">total</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> above 0.1 are also
filtered out to ensure that continuum derivation only takes place within
microwindows and in regions where the modelled spectral lines can be
reasonably subtracted from the observed ones (where the absorption is not
saturated).</p>
      <p id="d1e867">Continuum absorption by other molecules (<inline-formula><mml:math id="M58" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M59" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M60" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, and
<inline-formula><mml:math id="M61" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, defined here as <inline-formula><mml:math id="M62" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mtext>other</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>) was obtained from
MT_CKD_3.2 (Mlawer et al., 2012, 2019). This
non-water vapour continuum absorption is mostly important in the 1.25 <inline-formula><mml:math id="M63" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, where there is significant absorption due to a collision-induced
oxygen band; however, this window is not the focus of discussion here.
Figure 1 shows a schematic of how this information is put together to
retrieve the continuum from the FTS measurements.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1" specific-use="star"><?xmltex \currentcnt{1}?><label>Figure 1</label><caption><p id="d1e936">Schematic of the derivation process of the water vapour continuum
from the primary data (green), supplementary data (grey), computational
methods (orange), intermediate outputs (purple) and final output (red).</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f01.png"/>

        </fig>

</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>Best estimate of the continuum</title>
      <p id="d1e953">The best estimate of the continuum is from measurements made on 18 September 2008, with additional observations from other days. The IWV observed by the
HATPRO microwave radiometer on 18 September was <inline-formula><mml:math id="M64" display="inline"><mml:mrow><mml:mn mathvariant="normal">16.25</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.49</mml:mn></mml:mrow></mml:math></inline-formula> kg m<inline-formula><mml:math id="M65" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. The reliance on the observations of 18 September 2008 is due to
the need to observe in clear skies and to minimise the effects of
atmospheric aerosol; 18 September 2008 had clear skies for most of the day,
allowing observations at a wide range of air masses for Langley
extrapolation. Additionally, the aerosol optical depth was significantly
lower (observed via the sunphotometer) than the other days that fit this
criterion. This is a significant issue for a continuum derivation; when
deriving SSI a small absolute change in aerosol optical depth across the
course of a day has a minimal effect on the <inline-formula><mml:math id="M66" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> intercept of the Langley plot,
but the effect on the gradient (i.e. optical depth) is comparatively much
larger. Constraining the aerosol change throughout the day is a significant
challenge for such sea-level observations. Since the analysis is reliant
mostly on one day of observations, and given the large uncertainties, it is
not possible to<?pagebreak page2339?> retrieve the self- or foreign-continua separately. Therefore,
to compare with the laboratory measurements, an assumption needs to be made
about the relative strength of either the foreign continuum or self-continuum (see
Sect. 5). Figure 2 shows four Langley plots from the 18 September 2008
data, at 2500, 4500, 6500 and 9800 cm<inline-formula><mml:math id="M67" 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 4, 2.1, 1.6 and 1 <inline-formula><mml:math id="M68" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows respectively). These plots demonstrate the quality of fit (and
therefore the strong constraint on the observed total optical depth) we were
able to obtain from the observations of 18 September 2008.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2" specific-use="star"><?xmltex \currentcnt{2}?><label>Figure 2</label><caption><p id="d1e1009">Langley plots from selected wavenumbers in the near-infrared
atmospheric windows, along with the total optical depth obtained at that
wavenumber. Taken from observations of 18 September 2008.</p></caption>
          <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f02.png"/>

        </fig>

      <p id="d1e1018">Figure 3 shows the derivation process in the 1.6 <inline-formula><mml:math id="M69" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, starting
with the Langley-derived <inline-formula><mml:math id="M70" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">total</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> from the FTS observations (panel
a), subtracting the line-by-line contributions (panel b), smoothing using a
15 cm<inline-formula><mml:math id="M71" 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> boxcar filter and subtracting Rayleigh scattering and other
gaseous continua (panel c), and finally obtaining the water vapour continuum
by subtracting aerosol extinction (panel d).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><?xmltex \currentcnt{3}?><label>Figure 3</label><caption><p id="d1e1055">Example derivation of the water vapour continuum optical depth
<inline-formula><mml:math id="M72" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="bold">cont</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> from the total optical depth <inline-formula><mml:math id="M73" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">total</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> <bold>(a)</bold> via subtraction of <inline-formula><mml:math id="M74" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mrow><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow><mml:mtext>_lines</mml:mtext></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M75" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mtext>other_gases</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> <bold>(b)</bold>, smoothing and subtraction of
Rayleigh scattering <inline-formula><mml:math id="M76" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">Rayleigh</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> and continuum
absorption by other gases <inline-formula><mml:math id="M77" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">other</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> <bold>(c)</bold>,
and finally subtraction of <inline-formula><mml:math id="M78" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> to get the water
vapour continuum optical depth <bold>(d)</bold>.</p></caption>
          <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f03.png"/>

        </fig>

      <p id="d1e1163">Figure 4 shows the minimum detectable optical depth capable of being
observed by the FTS. This was calculated using the following method. For a
series of repeated observations from the calibration campaign (measurements
of the UHTBB; see Gardiner et al., 2012, for more details) the window
regions (2500–2800; 4400–4800; 6000–6400; 7900–8400; 9200–10 000 cm<inline-formula><mml:math id="M79" 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>) were selected. In each window region, the mean signal level
was calculated for each measurement. From this, the absolute difference
between these levels and the mean level across <italic>all</italic> the measurements was
obtained. The average difference gives a measure of the noise in each
region. We then take an observation of the Sun (one used in the Langley
analysis) and calculate the mean solar irradiance signal in each spectral
window. The ratio of the offset noise to the solar signal gives the
fractional offset noise in each window, which in the limit of small
absorption is approximately the optical depth noise in that region. The
minimum detectable offset is then assumed to be 3 times the optical depth
noise. It is found that the minimum detectable optical depth in each of the
atmospheric windows is typically 0.001, significantly below the derived
continuum optical depth in most cases.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><?xmltex \currentcnt{4}?><label>Figure 4</label><caption><p id="d1e1183">Minimum detectable optical depth in the various atmospheric
windows presented in this work (horizontal black line) against derived
continuum optical depth from 18 September 2008 (blue line). The shadings
indicate the <inline-formula><mml:math id="M80" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> (blue) and <inline-formula><mml:math id="M81" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> (cyan) uncertainty limits.</p></caption>
          <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f04.png"/>

        </fig>

</sec>
<sec id="Ch1.S2.SS3">
  <label>2.3</label><title>Uncertainty budget</title>
      <p id="d1e1224">The uncertainty budget on the continuum optical depth is obtained in a
similar way to Elsey et al. (2017). The Monte Carlo method used there was
extended to obtain the experimental uncertainty in the total optical depth.
Uncertainty in the optical depth from the line-by-line model comes from
sensitivity tests using the uncertainty limits in temperature, pressure and
water vapour from the radiosonde. Due to the increased sensitivity to the
atmospheric aerosol (when deriving continuum absorption rather than SSI),
<inline-formula><mml:math id="M82" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> was determined using the Microtops measurements and a
Mie scattering code based on Wiscombe (1980), in
addition to the Ångström exponent method described in Elsey et al. (2017). The Mie code was fed with a range of parameters for a comparable
atmosphere obtained from Dubovik et al. (2002). This allowed us to test the range of validity of the
Ångström exponent method by using a physically based wavelength
dependence. The uncertainty budget was more conservative than that of Elsey
et al. (2017), since this was estimated using the Mie scattering
calculations which were sensitive to various parameters (e.g. size
distribution) which had large ranges in Dubovik et al. (2002). Figure 5
shows the optical depth and <inline-formula><mml:math id="M83" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> (67 % confidence interval)
uncertainties of the <inline-formula><mml:math id="M84" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> used in this work and the relative
contribution this optical depth has to the combined continuum <inline-formula><mml:math id="M85" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> aerosol
optical depth.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><?xmltex \currentcnt{5}?><label>Figure 5</label><caption><p id="d1e1270"><bold>(a)</bold> Aerosol optical depth obtained from the Mie scattering
calculations for 18 September 2008 with the Microtops <inline-formula><mml:math id="M86" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mtext>aerosol</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> at 1 <inline-formula><mml:math id="M87" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m, along with the estimated <inline-formula><mml:math id="M88" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>
uncertainties (shaded region). <bold>(b)</bold> Relative contribution of the
continuum and aerosol in each of the near-infrared windows to the
combination of the two (<inline-formula><mml:math id="M89" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">continuum</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>).</p></caption>
          <?xmltex \igopts{width=355.659449pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f05.png"/>

        </fig>

</sec>
<?pagebreak page2341?><sec id="Ch1.S2.SS4">
  <label>2.4</label><?xmltex \opttitle{Comparison between FTS and Microtops observations at 1\,{$\unit{{\mu}}$}m}?><title>Comparison between FTS and Microtops observations at 1 <inline-formula><mml:math id="M90" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m</title>
      <p id="d1e1350">An issue with our derivation of <inline-formula><mml:math id="M91" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is our inability to
reconcile the observed variation in the sunphotometer <inline-formula><mml:math id="M92" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M93" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">cont</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> in the 1 <inline-formula><mml:math id="M94" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m channel, since this is not corrected for
in the Microtops processing algorithm) on 18 September 2008 with the
variation in the Langley-derived <inline-formula><mml:math id="M95" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">cont</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> from the
FTS. Figure 6 shows the time variation of the IWV and the continuum plus
aerosol optical depth from the FTS and the sunphotometer. The FTS showed a
consistent combined continuum and aerosol optical depth throughout the day,
while the Microtops showed a significant drop in aerosol optical depth over
the course of the day. This is very unlikely due to the continuum, since the
IWV observed by the HATPRO varied by only <inline-formula><mml:math id="M96" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula> % throughout
the day, which would not be enough to cause such large changes. The surface
temperature as observed by the radiosondes varied by less than 1 K
throughout the period of measurement. Additionally, the Microtops does not
contain a correction for the water vapour continuum; if there was a
significant change in continuum absorption, then this again should be seen in
both the Microtops and FTS data.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><?xmltex \currentcnt{6}?><label>Figure 6</label><caption><p id="d1e1427">Percentage variation across 18 September 2008 in integrated water
vapour as measured by the HATPRO microwave radiometer <bold>(a)</bold> and aerosol (<inline-formula><mml:math id="M97" display="inline"><mml:mo lspace="0mm">+</mml:mo></mml:math></inline-formula> continuum) optical depth as measured by the Microtops sunphotometer and the
FTS <bold>(b)</bold> in the 1.02 <inline-formula><mml:math id="M98" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m channel (9583 cm<inline-formula><mml:math id="M99" 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 FTS). The
FTS-observed aerosol optical depth (<inline-formula><mml:math id="M100" display="inline"><mml:mo lspace="0mm">+</mml:mo></mml:math></inline-formula> water vapour continuum) is
<inline-formula><mml:math id="M101" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">0.1</mml:mn></mml:mrow></mml:math></inline-formula> in this window, while the Microtops-observed aerosol
optical depth is <inline-formula><mml:math id="M102" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">0.05</mml:mn></mml:mrow></mml:math></inline-formula>.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f06.png"/>

        </fig>

      <p id="d1e1497">It is therefore unclear what is causing this discrepancy in the
time variation, but it may be due to uncertainties arising from the
operation of the sunphotometer or some systematic time-varying effect
impacting the FTS measurements. For the continuum derivation it was decided
to use the day average of the 18 September 2008 <inline-formula><mml:math id="M103" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>
measurements, with a corresponding increase in the uncertainty, since we
could not determine which aerosol variation was more likely to be the true
case.</p>
      <p id="d1e1512">In addition to the issue with the temporal variation, there is also an
irreconcilable difference between the optical depth observed by the FTS at 1 <inline-formula><mml:math id="M104" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m (<inline-formula><mml:math id="M105" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">0.1</mml:mn></mml:mrow></mml:math></inline-formula>) and that observed by the Microtops (0.03–0.08). Due to the small variation in IWV and temperature across the day, the
larger signal observed by the FTS is extremely unlikely to be due to water
vapour absorption. It is unclear why the FTS and the Microtops do not
observe the same signal. If the effect were physical, one would expect the
Microtops and FTS to both observe it. While the variability in the Microtops
is large, the absolute level of <inline-formula><mml:math id="M106" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is believed to be more
reliable than that from the FTS, particularly given the consistency with
shorter-wavelength Microtops measurements. This makes it a more reliable
instrument for extrapolating optical depth to lower wavenumbers. It was
postulated that the discrepancy may be due to a change in forward scattering
with wavenumber and the differences between the field-of-view of the
Microtops and the FTS (0.26<inline-formula><mml:math id="M107" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> and 2.5<inline-formula><mml:math id="M108" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> respectively), but
this correction to <inline-formula><mml:math id="M109" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is less than 10 % at all wavenumbers
observed by the FTS (Box and Deepak, 1979).</p>
      <?pagebreak page2343?><p id="d1e1574">Another issue is the assumptions made regarding the mirror reflectivity
correction. Since the mirrors were exposed to the elements, a correction is
made to the observed irradiance based on observations of the mirrors prior
to the field campaign and subsequent measurements afterward using the
National Reflectance Reflectometer (NRR) at NPL. However, the NRR
observations only cover the spectral region 4000–6600 cm<inline-formula><mml:math id="M110" 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
reflectance outside of these regions must be extrapolated based on the
observations within this spectral region. It is for this reason that we have
more confidence in the observations at these wavenumbers and in the
adjacent windows where the extrapolation takes place over fewer wavenumbers.
There is significant uncertainty in the behaviour in the 1 <inline-formula><mml:math id="M111" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window,
where the mirror correction is extrapolated further, which may be in excess
of the uncertainty estimate in Gardiner et al. (2012). The Supplement has more details on the possible effect of this mirror
extrapolation.</p>
      <p id="d1e1597">It was postulated that there could be significant uncertainty at higher
wavenumbers (<inline-formula><mml:math id="M112" display="inline"><mml:mrow><mml:mi mathvariant="italic">&gt;</mml:mi><mml:mn mathvariant="normal">7500</mml:mn></mml:mrow></mml:math></inline-formula> cm<inline-formula><mml:math id="M113" 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>) due to some uncertainty or
systematic offset in the phase correction used in the OPUS software used to
derive spectra from the FTS measurements (see Supplement). This
was motivated by the observation of systematic changes in the FTS phase
spectrum with respect to time across 18 September 2008 that were
particularly large at higher wavenumbers. It was found that uncertainties in
this phase correction would have small effects at lower wavenumbers but
could significantly impact the observed optical depth at higher wavenumbers.
However, we do not have a physical justification for why this may have been
the case and cannot ab initio determine the magnitude of this uncertainty.</p>
      <p id="d1e1622">We believe that the combination of the above factors (mirrors, phase
correction issues, larger aerosol effect) warrants significant caution being
used when interpreting the results at wavenumbers beyond <inline-formula><mml:math id="M114" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">6700</mml:mn></mml:mrow></mml:math></inline-formula> cm<inline-formula><mml:math id="M115" 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 observed optical depth (see Sect. 3) is seemingly
inconsistent with the (admittedly sparse) laboratory estimates or
MT_CKD. Therefore, the apparently high continuum optical
depth derived from the FTS near 1 <inline-formula><mml:math id="M116" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m (<inline-formula><mml:math id="M117" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">0.05</mml:mn></mml:mrow></mml:math></inline-formula> optical
depths; see Sect. 3) is regarded as an undiagnosed issue (potentially for the reasons postulated above) with the instrument sensitivity at high
wavenumbers, and henceforth we focus on the 1.6, 2.1, and 4 <inline-formula><mml:math id="M118" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows.
This is additionally motivated by the lack of laboratory measurements to
validate in the larger-wavenumber windows. However, we cannot rule out that
the large observed optical depth is some unexplained physical effect (or
indeed an unexpectedly large water vapour continuum signal). Further
clear-sky observations in this spectral region could affirm whether this is
the case.</p>
</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Results</title>
      <p id="d1e1682">Figure 7 shows the best estimate (henceforth referred to as
“CAVIAR-field”) of our continuum from 21 observations on 18 September 2008
using the Langley method. Also shown are the MT_CKD_3.2 and MT_CKD_2.5 modelled
continuum optical depth (self <inline-formula><mml:math id="M119" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> foreign) for atmospheric conditions on
this day. Since the uncertainties in our observations are large, there is
agreement with MT_CKD_3.2 and 2.5 within the
<inline-formula><mml:math id="M120" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> uncertainty limits in the centres of the 4, 2.1, 1.6, and 1.3 <inline-formula><mml:math id="M121" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m
windows. Note that the MT_CKD continuum does not provide any
uncertainties. The comparison between CAVIAR-field and MT_CKD
will be discussed further in Sect. 4. Section 5 focuses on a comparison of
these data to the available laboratory data. This section demonstrates the
consistency between the closure and Langley-derived data, which are
quasi-independent methods of deriving the continuum (see the Supplement for
more details). The Supplement also includes a comparison of the 18 September best estimate to data from other days from the field campaign,
which were less suitable for analysis of the continuum due to measurement
issues, increased aerosol extinction, and lack of data availability.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7" specific-use="star"><?xmltex \currentcnt{7}?><label>Figure 7</label><caption><p id="d1e1714">Langley-derived CAVIAR-field continuum optical depth and optical
depth for two versions of the MT_CKD water vapour continuum
for 18 September 2008. The blue shaded regions indicate the <inline-formula><mml:math id="M122" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>
uncertainties; the cyan regions indicate the <inline-formula><mml:math id="M123" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties. The
yellow shaded areas indicate spectral regions in which the CAVIAR-field-derived continuum is potentially spurious and should be treated with caution
(see Sect. 2.4).</p></caption>
        <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f07.png"/>

      </fig>

      <p id="d1e1747">Figure 8 shows the comparison of the Langley-derived and closure-derived
spectra from 18 September 2008. As with the Langley-derived spectrum, the
closure-derived spectrum is a mean of 21 spectra from this day. The green
and red lines overlap significantly in this figure, indicating that there is
excellent agreement between the two quasi-independent methods. This provides
additional confidence in the accuracy of the Langley retrieval. The
uncertainty in the closure-derived spectra is significantly larger, due to
the use of an assumed SSI (from Elsey et al., 2017) which itself has
uncertainties.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8" specific-use="star"><?xmltex \currentcnt{8}?><label>Figure 8</label><caption><p id="d1e1753">Comparison between the Langley and closure method derivations of
the continuum optical depth on 18 September 2008. Panel <bold>(a)</bold> shows absolute
values and panel <bold>(b)</bold> the residual of the two. Teal shaded region is the <inline-formula><mml:math id="M124" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>
Langley uncertainty, and green is the <inline-formula><mml:math id="M125" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> closure uncertainty. The optical
depth from two versions of MT_CKD is shown in panel <bold>(a)</bold>
for comparison.</p></caption>
        <?xmltex \igopts{width=426.791339pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f08.png"/>

      </fig>

      <p id="d1e1795">One way of assessing any potential aerosol contamination is to look at the
spectra at individual times, rather than the day-averaged continuum from the
Langley method or the mean continuum as measured via the closure method. The
closure-derived continua are calculated with aerosol extinction subtracted
as observed by the Microtops at the time of each measurement. They are shown
at different times across 18 September 2008 in Fig. 9. Figure 9a shows the
case with time-averaged aerosol as observed by the Microtops and Fig. 9b
the case with time-varying aerosol. The uncertainties are not plotted for
clarity, but are large (<inline-formula><mml:math id="M126" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.04</mml:mn></mml:mrow></mml:math></inline-formula>), meaning that, despite the observed
differences, the observations are consistent. Therefore, this change in
aerosol over the day cannot be confirmed with any degree of significance; it
is difficult to tell whether observed differences in central values are real or a
consequence of the uncertainties.</p>
      <p id="d1e1808">Assuming that the central values are well-characterised, they show that the
derived continuum (<inline-formula><mml:math id="M127" display="inline"><mml:mo lspace="0mm">+</mml:mo></mml:math></inline-formula> residual aerosol contribution) increases by a factor
of 2 across the day. It is clear from Fig. 6b that the time variation in
the aerosol extinction is not observed by the FTS. When using a
time-averaged aerosol (Fig. 9a), the different closure spectra are much
more consistent. The agreement between the Langley- and closure-derived
continua in this case indicates that there are not significant issues with
calibration of the instrument, unless such issues were strongly
time-varying.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F9"><?xmltex \currentcnt{9}?><label>Figure 9</label><caption><p id="d1e1820">Observed time-varying continuum optical depth derived from the
closure method at different times throughout 18 September 2008, <bold>(a)</bold> with
time-averaged aerosol as observed by the Microtops and <bold>(b)</bold> with time-varying
aerosol. The uncertainties are not shown for visual clarity, but are of the
order <inline-formula><mml:math id="M128" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">0.04</mml:mn></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M129" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>).</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f09.png"/>

      </fig>

      <p id="d1e1857">Given the level of uncertainty in these results, it is not certain whether the
differences between Fig. 9a and b are significant. However, one possible
source of difference that was considered was inaccuracy in the external
mirror reflectivity correction (explained in more detail in Gardiner et al.,
2012). However, as discussed in the Supplement, a change in the
reflectance will not lead to any change in the slope of a Langley fit and
therefore will not impact the Langley-derived continuum in any way, provided the
change is independent of angle. The Supplement shows that this cannot
account for the optical depth in the higher-wavenumber windows without<?pagebreak page2344?> an
undiagnosed change in the irradiance with angle, e.g. due to uncertainties
in the phase correction as discussed in Sect. 2.4.</p>
</sec>
<sec id="Ch1.S4">
  <label>4</label><?xmltex \opttitle{Comparison with MT\_CKD}?><title>Comparison with MT_CKD</title>
      <p id="d1e1869">Figure 7 shows that, in the centre of the 4 <inline-formula><mml:math id="M130" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, the CAVIAR-field
continuum optical depth appears to be in reasonable agreement with the
optical depth obtained using MT_CKD (and in better agreement
with version 2.5 than version 3.2), but less so toward the edges of the
window. This is further demonstrated in Fig. 10, which shows the ratio of
the CAVIAR-field continuum to two versions of MT_CKD. The
agreement at the centre of the window is indicative of agreement with
various FTS measurements in this region; this will be explored further in
Sect. 5. At the higher-wavenumber<?pagebreak page2345?> edge however there is no agreement
between MT_CKD and CAVIAR-field within the <inline-formula><mml:math id="M131" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula>
uncertainties; if our measurements are accurate (and in agreement with other
datasets), this indicates a strengthening to MT_CKD is
required in that region.</p>
      <p id="d1e1892">In the 2.1 <inline-formula><mml:math id="M132" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, CAVIAR-field is inconsistent with both versions
of MT_CKD within the <inline-formula><mml:math id="M133" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties in a significant
portion of the window and inconsistent within the <inline-formula><mml:math id="M134" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties in
the lower-wavenumber part of the window. The ratio of CAVIAR-field to
MT_CKD_3.2 is <inline-formula><mml:math id="M135" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula> in this region
(Fig. 10), but this is in significantly better agreement than would be the
case using the older MT_CKD_2.5 values; this
implies that either or both of the MT_CKD self- and foreign-continua need to be strengthened. Section 5 will further discuss the
relative contribution of the self- and foreign-continua to this discrepancy.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F10" specific-use="star"><?xmltex \currentcnt{10}?><label>Figure 10</label><caption><p id="d1e1939">Ratio of Langley-derived CAVIAR-field continuum optical depth
divided by MT_CKD optical depth (for two different versions
of MT_CKD) in the 2.1 and 1.6 <inline-formula><mml:math id="M136" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m atmospheric windows for
18 September 2008. Uncertainties (shaded regions) shown at <inline-formula><mml:math id="M137" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>.</p></caption>
        <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f10.png"/>

      </fig>

      <p id="d1e1969">The CAVIAR-field continuum is significantly stronger than either of the
recent versions of MT_CKD within the 1.6 <inline-formula><mml:math id="M138" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window,
disagreeing within the <inline-formula><mml:math id="M139" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties but consistent within the <inline-formula><mml:math id="M140" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula>
uncertainties. This is the region in which there is the most difference
between available laboratory spectra.</p>
</sec>
<sec id="Ch1.S5">
  <label>5</label><title>Comparison with other observations</title>
      <p id="d1e2013">This section describes the relevant laboratory and field measurements in
each of the 4, 2.1, and 1.6 <inline-formula><mml:math id="M141" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m atmospheric windows and compares them to
the continuum absorption from this work. The continuum absorption derived in
Sect. 3 is difficult to directly compare to the laboratory measurements of
the continuum absorption cross section, since our derived continuum optical
depth <inline-formula><mml:math id="M142" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">tot</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup></mml:mrow></mml:math></inline-formula> is the sum of the self <inline-formula><mml:math id="M143" display="inline"><mml:mo>+</mml:mo></mml:math></inline-formula> foreign continuum
optical depths. However, it is possible to compare these data indirectly,
via their ratio to MT_CKD_3.2 using
atmospheric conditions at the time of the measurements. Since
          <disp-formula id="Ch1.E3" content-type="numbered"><label>3</label><mml:math id="M144" display="block"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">tot</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup><mml:mo>=</mml:mo><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">self</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup><mml:mo>+</mml:mo><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
        either the self-continuum or foreign-continuum coefficient can be estimated by
subtracting the optical depth contribution from the other.</p>
      <p id="d1e2077">Consider the case in which <inline-formula><mml:math id="M145" display="inline"><mml:mrow><mml:msubsup><mml:mi>C</mml:mi><mml:mi mathvariant="normal">self</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup></mml:mrow></mml:math></inline-formula> (i.e. the CAVIAR-field
self-continuum cross section) is to be obtained. The foreign-continuum
optical depth <inline-formula><mml:math id="M146" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup></mml:mrow></mml:math></inline-formula> is an unknown which must be estimated. This
can be done by assuming either (a) <inline-formula><mml:math id="M147" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup><mml:mo>=</mml:mo><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mtext>MT_CKD</mml:mtext></mml:msubsup></mml:mrow></mml:math></inline-formula> (the MT_CKD_3.2 foreign-continuum optical depth derived for the conditions of 18 September 2008) or (b) by assuming
          <disp-formula id="Ch1.E4" content-type="numbered"><label>4</label><mml:math id="M148" display="block"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mi mathvariant="normal">lab</mml:mi></mml:msubsup><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msubsup><mml:mi>C</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mi mathvariant="normal">lab</mml:mi></mml:msubsup></mml:mrow><mml:mrow><mml:msubsup><mml:mi>C</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mtext>MT_CKD</mml:mtext></mml:msubsup></mml:mrow></mml:mfrac></mml:mstyle><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mtext>MT_CKD</mml:mtext></mml:msubsup><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
        where <inline-formula><mml:math id="M149" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mi mathvariant="normal">lab</mml:mi></mml:msubsup></mml:mrow></mml:math></inline-formula> is the foreign-continuum optical depth for the
atmospheric conditions of interest, <inline-formula><mml:math id="M150" display="inline"><mml:mrow><mml:msubsup><mml:mi>C</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mi mathvariant="normal">lab</mml:mi></mml:msubsup></mml:mrow></mml:math></inline-formula> is the foreign-continuum
cross section from laboratory observations, and <inline-formula><mml:math id="M151" display="inline"><mml:mrow><mml:msubsup><mml:mi>C</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mtext>MT_CKD</mml:mtext></mml:msubsup></mml:mrow></mml:math></inline-formula> is the MT_CKD_3.2 foreign-continuum cross section. The ratio
<inline-formula><mml:math id="M152" display="inline"><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mrow><mml:msubsup><mml:mi>C</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mi mathvariant="normal">lab</mml:mi></mml:msubsup></mml:mrow><mml:mrow><mml:msubsup><mml:mi>C</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mtext>MT_CKD</mml:mtext></mml:msubsup></mml:mrow></mml:mfrac></mml:mstyle></mml:math></inline-formula> effectively scales
the MT_CKD optical depth to the laboratory observations. This
is shown visually in Fig. 11.</p>
      <p id="d1e2233">There is no constraint on the total optical depth <inline-formula><mml:math id="M153" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">tot</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup></mml:mrow></mml:math></inline-formula> from
the laboratory observations or MT_CKD. Taking
<inline-formula><mml:math id="M154" display="inline"><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mrow><mml:msubsup><mml:mi>C</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mi mathvariant="normal">lab</mml:mi></mml:msubsup></mml:mrow><mml:mrow><mml:msubsup><mml:mi>C</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mtext>MT_CKD</mml:mtext></mml:msubsup></mml:mrow></mml:mfrac></mml:mstyle></mml:math></inline-formula> as the lab scaling
factor <inline-formula><mml:math id="M155" display="inline"><mml:mrow><mml:msub><mml:mi>k</mml:mi><mml:mi mathvariant="normal">f</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (for the foreign continuum), with a corresponding scaling
factor <inline-formula><mml:math id="M156" display="inline"><mml:mrow><mml:msub><mml:mi>k</mml:mi><mml:mi mathvariant="normal">s</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> for the self-continuum,
          <disp-formula id="Ch1.E5" content-type="numbered"><label>5</label><mml:math id="M157" display="block"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">tot</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup><mml:mo>=</mml:mo><mml:mi>a</mml:mi><mml:msub><mml:mi>k</mml:mi><mml:mi mathvariant="normal">s</mml:mi></mml:msub><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">self</mml:mi><mml:mtext>MT_CKD</mml:mtext></mml:msubsup><mml:mo>+</mml:mo><mml:mi>b</mml:mi><mml:msub><mml:mi>k</mml:mi><mml:mi mathvariant="normal">f</mml:mi></mml:msub><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mtext>MT_CKD</mml:mtext></mml:msubsup><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula>
        These parameters <inline-formula><mml:math id="M158" display="inline"><mml:mi>a</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M159" display="inline"><mml:mi>b</mml:mi></mml:math></inline-formula> determine the relative contribution of the self- and
foreign-continua to the offset between the CAVIAR-field optical depth and
the optical depth from MT_CKD (with or without the laboratory
scaling). However, as <inline-formula><mml:math id="M160" display="inline"><mml:mi>a</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M161" display="inline"><mml:mi>b</mml:mi></mml:math></inline-formula> are both unknowns, it is not possible to estimate
one or the other without making some assumptions. In this analysis, we
therefore assume that <inline-formula><mml:math id="M162" display="inline"><mml:mrow><mml:mi>b</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> when estimating the self-continuum and that
<inline-formula><mml:math id="M163" display="inline"><mml:mrow><mml:mi>a</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> when estimating the foreign continuum, i.e. that the
MT_CKD (with or without scaling to the laboratory
observations) optical depth accurately represents the self or foreign
component that is to be subtracted from the total to estimate the foreign or
self component respectively.</p>
      <p id="d1e2394">As will be demonstrated, for the conditions observed on 18 September 2008,
both the self- and foreign-continua make<?pagebreak page2346?> significant contributions in the
various windows to the total continuum. This is strongly dependent on
whether MT_CKD or the laboratory data are used to estimate the
self- or foreign-continua.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F11" specific-use="star"><?xmltex \currentcnt{11}?><label>Figure 11</label><caption><p id="d1e2400">Derivation process of the self-continuum absorption cross section
implied by the FTS optical depth. This process can be done for the foreign
continuum, in which case all references to the self-continuum in the figure apply to the foreign continuum and vice versa.</p></caption>
        <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f11.png"/>

      </fig>

      <p id="d1e2409">This approach is reasonably robust when estimating the self-continuum, as
this relies on the laboratory or MT_CKD foreign continuum,
which is believed to be relatively independent of temperature (Ptashnik et
al., 2012; Baranov, 2011). Therefore, high-temperature laboratory foreign-continuum measurements (with their lower uncertainties) can be used. In this
case, we use the average of the 350, 372, 402, and 431 K foreign-continuum measurements of Ptashnik et al. (2012), henceforth the CAVIAR-lab
foreign continuum, and assume that it is entirely independent of
temperature. However, a lack of broadband room-temperature measurements of
the foreign continuum in the windows means that there may be some additional
(and unquantifiable) uncertainty arising from this assumption.</p>
      <p id="d1e2412">When estimating the CAVIAR-field foreign continuum, due to the lack of
laboratory measurements at atmospheric temperatures (i.e. below room
temperature), one must assume a temperature dependence for the
self-continuum. This is done by extrapolating the high-temperature
laboratory data (above 374 K, even where lower-temperature data are
available due to their higher uncertainties) to atmospheric temperature
either by a statistical fit when scaling to the laboratory data or by
relying on the MT_CKD temperature dependence when scaling to
MT_CKD. This statistical fit assumes that the temperature
dependence is proportional to <inline-formula><mml:math id="M164" display="inline"><mml:mrow><mml:mi mathvariant="normal">exp</mml:mi><mml:mo>(</mml:mo><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow><mml:mi>T</mml:mi></mml:mfrac></mml:mstyle><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, where <inline-formula><mml:math id="M165" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> could be interpreted as relating to the dissociation energy of a water
dimer (e.g. Ptashnik et al., 2011a). For the axes used in Figs. 13, 14,
and 15 (<inline-formula><mml:math id="M166" display="inline"><mml:mrow><mml:mn mathvariant="normal">1000</mml:mn><mml:mo>/</mml:mo><mml:mi>T</mml:mi></mml:mrow></mml:math></inline-formula> vs. the logarithm of the continuum cross section), this shows
as a straight line. This temperature dependence is an assumption; this may
break down at lower temperatures due to e.g. a change in regime from bound
to quasi-bound dimers with increasing temperature (Ptashnik et al., 2011b, 2019). We apply this temperature dependence to the self-continuum
measurements of Ptashnik et al. (2011a), henceforth the CAVIAR-lab
self-continuum. This dataset was chosen due to its wide spectral coverage
and range of temperatures, making it more suited to such an extrapolation,
rather than using the room-temperature CRDS and OF-CEAS data (Sect. 5.1),
where there are measurements at room temperature, but only at specific
wavenumbers.</p>
<sec id="Ch1.S5.SS1">
  <label>5.1</label><title>Self-continuum</title>
      <p id="d1e2467">When deriving the CAVIAR-field self-continuum this way, a representative
temperature must be chosen to compare to the laboratory measurements, since
the continuum observed by the FTS is the integrated continuum across the
entire temperature and pressure range of the atmosphere. Figure 12 shows the
fractional contribution to the total continuum optical depth from the
surface upwards for selected wavenumbers, as calculated using
MT_CKD_3.2 and RFM for the conditions of 18 September 2008 at Camborne. This is calculated as the fractional
contribution at each layer as observed by our radiosonde profiles to the
total continuum absorption. This shows that more than 95 % of the
continuum optical depth is in the bottom 2 km of the atmosphere. This
corresponds to a temperature range of <inline-formula><mml:math id="M167" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">275</mml:mn></mml:mrow></mml:math></inline-formula>–290 K, which was
assumed to be the temperature for which the CAVIAR-field self-continuum is
representative.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F12"><?xmltex \currentcnt{12}?><label>Figure 12</label><caption><p id="d1e2482">Fractional contribution to the total continuum optical depth
(using MT_CKD_3.2) with height from the
surface up to 10 km at three wavenumbers. The temperature profile (top axis)
derived from radiosonde on 18 September 2008 is shown in red.</p></caption>
          <?xmltex \igopts{width=213.395669pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f12.png"/>

        </fig>

      <?pagebreak page2347?><p id="d1e2491">Shine et al. (2016) present a review of the laboratory data up to 2016 in
significant detail. The following paragraphs introduce the main data
available across multiple spectral windows used to compare the CAVIAR-field
self-continuum. Other datasets will be introduced as required for each
specific window.</p>
      <p id="d1e2495">Ptashnik et al. (2011a) (henceforth the
CAVIAR-lab self-continuum) presented laboratory observations of the
self-continuum taken by an FTS from 472 to 293 K between 2500 and 10 000 cm<inline-formula><mml:math id="M168" 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>;
because uncertainties become too large for the low-temperature measurements
(because of the lower vapour pressures that are necessary at low
temperatures), at wavenumbers greater than 5600 cm<inline-formula><mml:math id="M169" 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> their measurements
are restricted to 374 K and above, with the exception of a few 350 K
measurements at the edges of the windows where the continuum is stronger.
However, at all wavenumbers, uncertainties are larger at the lower
temperatures. Further sets of FTS measurements (Ptashnik
et al., 2013, 2015) were taken at the Institute for Atmospheric Optics in
Tomsk, Russia. However, recent and ongoing study has indicated that these
results may be spurious, due to reflectivity issues arising from adsorption
onto the gold mirrors used in their multipass cell (Ptashnik et al., 2019b). For this reason, these results have not been included in our
analysis.</p>
      <p id="d1e2522">Various sets of observations have been made by the Spectroscopy Group at
LiPhy (Laboratoire Interdisciplinaire de Physique) at the Université
Grenoble-Alpes (henceforth collectively “Grenoble”). Mondelain et al. (2013, 2014) presented observations of the near-IR self-continuum in the 1.6
and 2.1 <inline-formula><mml:math id="M170" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows at room temperature and above using a cavity
ring-down spectrometer (CRDS). Newer measurements (Lechevallier et al., 2018; Richard et al.,
2017) by this group in the 2.1 <inline-formula><mml:math id="M171" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window were presented, which
generally agree with the Mondelain et al. observations. Vasilchenko et al. (2019) present updated CRDS measurements at a range of wavenumbers at room
temperature in the 2.1 and 1.6 <inline-formula><mml:math id="M172" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows. Ventrillard et al. (2015) present
observations in the 2.1 <inline-formula><mml:math id="M173" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window (4302 and 4732 cm<inline-formula><mml:math id="M174" 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>) using an
optical feedback cavity enhanced absorption spectroscopy (OF-CEAS) technique
at 293–323 K, while Richard et al. (2017) use the same technique in the 4 <inline-formula><mml:math id="M175" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window (2491 cm<inline-formula><mml:math id="M176" 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>
<sec id="Ch1.S5.SS1.SSS1">
  <label>5.1.1</label><?xmltex \opttitle{4\,{$\unit{{\mu}}$}m window}?><title>4 <inline-formula><mml:math id="M177" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window</title>
      <p id="d1e2606">Figure 13 presents various estimates of the self-continuum from the
laboratory in the centre of the 4 <inline-formula><mml:math id="M178" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window (2491 cm<inline-formula><mml:math id="M179" 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
CAVIAR-lab measurements agree reasonably well at <inline-formula><mml:math id="M180" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">350</mml:mn></mml:mrow></mml:math></inline-formula> K with
the laboratory FTS data of Baranov and Lafferty (2011), taken at several
temperatures across the 4 <inline-formula><mml:math id="M181" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window. However, there is poor agreement
between these FTS data and both the measurements of Richard et al. (2017)
and grating spectrometer measurements of Burch and Alt (1984). Richard
et al. (2017) and Burch and Alt (1984) agree reasonably well and imply a
weaker temperature dependence than CAVIAR-lab and Baranov and Lafferty (2011). However, extrapolating only through the high-temperature CAVIAR-lab
data (i.e. excluding the point at 293 K) using an assumed
<inline-formula><mml:math id="M182" display="inline"><mml:mrow><mml:mi mathvariant="normal">exp</mml:mi><mml:mo>(</mml:mo><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow><mml:mi>T</mml:mi></mml:mfrac></mml:mstyle><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> temperature dependence yields excellent
agreement with the Burch and Alt (1984) and Richard et al. (2017) data.
These higher-temperature CAVIAR-lab measurements have smaller<?pagebreak page2348?> uncertainties
than the low-temperature CAVIAR-lab measurements and appear to lie on a
straight line, while the lower-temperature CAVIAR-lab data point does not
lie on this line. There are therefore two possible experimentally implied
temperature dependences, a lower one implied by the high-temperature
CAVIAR-lab, Richard et al. (2017) and Burch and Alt (1984) measurements, and
a stronger dependence implied by the less-certain lower-temperature
CAVIAR-lab and Baranov and Lafferty (2011) measurements. This reflects the
importance of making observations at lower temperature with well-constrained
uncertainty budgets.</p>
      <p id="d1e2669">Also shown in Fig. 13 are two estimates of the CAVIAR-field
self-continuum, derived using either the MT_CKD_3.2 foreign continuum (orange point) or the CAVIAR-lab
foreign continuum (green point). These estimates were obtained using the
method presented in Fig. 11. Since the CAVIAR-lab and MT_CKD_3.2 foreign continua differ significantly, these two
estimates are an order of magnitude different, with no agreement within the
<inline-formula><mml:math id="M183" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainty limits. The stronger CAVIAR-field self-continuum, derived
using the MT_CKD_3.2 foreign continuum, appears
to be more consistent with the temperature dependence implied by the
room-temperature CAVIAR-lab and Baranov and Lafferty measurements, whereas
the estimate using the CAVIAR-lab foreign continuum has better agreement
with the temperature dependence implied by the high-temperature CAVIAR-lab
and Richard et al. measurements, although it is somewhat weaker than the
implied data point at 280 K. It is also interesting to note that the
MT_CKD_3.2 self-continuum lies in between the
two CAVIAR-field estimates, with no agreement within the <inline-formula><mml:math id="M184" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainty
limits.</p>
      <p id="d1e2696">We believe that these estimates may provide some weak evidence for the
high-temperature CAVIAR-lab/Richard et al. temperature dependence, since
this lies closer to our estimate using real laboratory data (the CAVIAR-lab
foreign continuum) rather than the semi-empirical continuum from
MT_CKD. However, given the lack of agreement within the <inline-formula><mml:math id="M185" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainty limits and the high uncertainty in the room-temperature
CAVIAR-lab measurement, we are not able to make strong conclusions based on
the available data. A stronger constraint on the foreign continuum in this
spectral region would help to narrow down as to which of these estimates
(and which of the implied temperature dependences) is more robust.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F13"><?xmltex \currentcnt{13}?><label>Figure 13</label><caption><p id="d1e2714">Self-continuum absorption cross section against temperature for
various datasets at 2491 cm<inline-formula><mml:math id="M186" 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 error bars indicate the <inline-formula><mml:math id="M187" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>
uncertainties. Marker size is greater than the stated uncertainty where
error bars are not visible. The dashed black line of MT_CKD
above 350 K indicates the region outside of the expected applicability of
MT_CKD. The dashed blue line indicates extrapolation of the
high-temperature CAVIAR-lab temperature dependence, while the cyan dashed
line shows the extrapolation through all of the CAVIAR-lab data points
(including the low-temperature cyan data point).</p></caption>
            <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f13.png"/>

          </fig>

</sec>
<sec id="Ch1.S5.SS1.SSS2">
  <label>5.1.2</label><?xmltex \opttitle{2.1\,{$\unit{{\mu}}$}m window}?><title>2.1 <inline-formula><mml:math id="M188" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window</title>
      <p id="d1e2764">At 2.1 <inline-formula><mml:math id="M189" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m (Fig. 14), there is generally good agreement between the
various sets of laboratory data, particularly when extrapolating the
high-temperature CAVIAR-lab data to room temperature (blue dashed line)
rather than using the lower-temperature data point (cyan point and dashed line),
which has larger uncertainties. There is also good agreement between these
laboratory data and MT_CKD, within the temperature range in
which MT_CKD is expected to be valid (solid black line).
Figure 14 also shows the estimated CAVIAR-field at three wavenumbers at the edge
(4255 and 4302 cm<inline-formula><mml:math id="M190" 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 centre (4723 cm<inline-formula><mml:math id="M191" 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>) of the 2.1 <inline-formula><mml:math id="M192" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m
window. This is derived using both the MT_CKD_3.2 foreign continuum (orange data point) and the CAVIAR-lab foreign
continuum (green data point). The error bars show the <inline-formula><mml:math id="M193" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainty
limits. The error bars on the Mondelain et al. (2015) and Ventrillard et al. (2015) measurements are smaller than the marker size.</p>
      <p id="d1e2819">At the edge of the window (Fig. 14a, b), the CAVIAR-field estimated
continuum (assuming the MT_CKD foreign continuum) does not
overlap with the available laboratory data within the <inline-formula><mml:math id="M194" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties.
This suggests that, if the available data are robust and the assumed
temperature dependence of the self-continuum is correct, the
MT_CKD foreign continuum requires some strengthening at the
edge of this window. However, using the CAVIAR-lab foreign continuum at the
low-wavenumber edge of the window results in a negative implied
self-continuum, indicating that either the CAVIAR-lab foreign continuum is
too strong at the window edge, that there is a temperature dependence of the
foreign continuum<?pagebreak page2349?> that is neglected here, or that the observed optical depth
from this work is poorly characterised at the edge of the window. In the
centre of the 2.1 <inline-formula><mml:math id="M195" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window (Fig. 14c) the CAVIAR-field estimated
continuum shows reasonable agreement with the observed laboratory data
(extrapolated to 280 K) when using the CAVIAR-lab foreign continuum, with
overlap between the <inline-formula><mml:math id="M196" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties. This is not the case when using
the MT_CKD foreign continuum, providing further evidence that
this requires strengthening, particularly at the centre of the window. This
is consistent with laboratory analyses of the foreign continuum (Sect. 5.2).</p>
      <p id="d1e2854">It is important to note that there is good consistency between the 297 K
CAVIAR-lab data point and the CAVIAR-field estimated self-continuum when
using the MT_CKD foreign continuum. This would suggest that
if the self-continuum is as large as implied by this lower-temperature data
point, the foreign continuum would be robust in MT_CKD_3.2. However, given the agreement between the
high-temperature CAVIAR-lab data (which have lower uncertainties) and the
laboratory foreign-continuum data available in the 2.1 <inline-formula><mml:math id="M197" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m region
(Sect. 5.2), we believe that the likelihood is that the foreign continuum
requires strengthening rather than the self-continuum.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F14" specific-use="star"><?xmltex \currentcnt{14}?><label>Figure 14</label><caption><p id="d1e2868">Self-continuum absorption cross section against temperature for
various datasets at <bold>(a)</bold> 4255, <bold>(b)</bold> 4302, and <bold>(c)</bold> 4723 cm<inline-formula><mml:math id="M198" 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 error
bars indicate the <inline-formula><mml:math id="M199" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties. Marker size is greater than the
stated uncertainty where error bars are not visible. The dashed line of
MT_CKD above 350 K indicates the region outside of the
expected applicability of MT_CKD. The dashed blue, cyan, and
red lines indicate extrapolations of the CAVIAR-lab (with and without the
low-temperature data) and Grenoble temperature dependence respectively,
assuming an exponential temperature dependence. The green data points (CAVIAR-field with
CAVIAR-lab foreign continuum) are missing from frames <bold>(a)</bold> and <bold>(b)</bold> as the
inferred self-continuum is negative.</p></caption>
            <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f14.png"/>

          </fig>

</sec>
<sec id="Ch1.S5.SS1.SSS3">
  <label>5.1.3</label><?xmltex \opttitle{1.6\,{$\unit{{\mu}}$}m window}?><title>1.6 <inline-formula><mml:math id="M200" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window</title>
      <p id="d1e2934">Figure 15 shows the observed absorption cross section as a function of
temperature for three wavenumbers in the 1.6 <inline-formula><mml:math id="M201" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window (6050, 6177, and
6383 cm<inline-formula><mml:math id="M202" 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 panels a, b, and c respectively. These wavenumbers were
selected since these are the wavenumbers in which the Grenoble CRDS data are
available. The agreement in this window is generally lacking between
different laboratory datasets of the self-continuum. At room temperature,
the extrapolated CAVIAR-lab data imply significantly stronger absorption
than the Grenoble data (from Mondelain et al., 2014, and Vasilchenko et
al., 2019). The data indicate significantly different temperature
dependences between CAVIAR-lab and Grenoble; the latter shows a
significantly weaker temperature dependence across the window and a weaker
dependence relative to CAVIAR-lab than the Grenoble measurements in the 2.1 <inline-formula><mml:math id="M203" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window (Fig. 14). Both the Grenoble and CAVIAR-lab temperature
dependences are markedly different from the MT_CKD_3.2 temperature dependence. These discrepancies are
discussed in Shine et al. (2016). In addition to the data discussed at the
beginning of Sect. 5, we present an additional comparison at 6177 cm<inline-formula><mml:math id="M204" 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> (Fig. 15b) with the continuum derived in Kapitanov et al. (2018) using a photo-acoustic method. We note that the Kapitanov et al. (2018) data point lies in reasonable agreement with the extrapolated
CAVIAR-lab continuum, and to a lesser degree with the CAVIAR-field
self-continuum, particularly when using the CAVIAR-lab foreign continuum,
but has no agreement with the Grenoble measurements.</p>
      <p id="d1e2977">An additional issue arises when comparing the Mondelain et al. and
Vasilchenko et al. data; while the observed absorption cross sections are
similar, there is no agreement within their stated uncertainties. This can
be attributed to the differences in the fits used to obtain these
cross sections: both used a quadratic fit of vapour pressure versus
absorption to obtain their cross sections, but Mondelain et al. use an
additional linear term to account for supposed adsorption on the mirrors,
whereas Vasilchenko et al. did not need to use this additional term. The
Vasilchenko et al. (2019) data, being more recent, are regarded as the more
reliable, but are only available at one temperature.</p>
      <p id="d1e2980">The choice of foreign continuum has less of an effect on the CAVIAR-field
self-continuum in this window since the absolute difference between
MT_CKD and CAVIAR-lab foreign continuum is too small to
significantly affect the large observed optical depth. However, since the
associated uncertainties are large (the <inline-formula><mml:math id="M205" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties intersect with
zero), they are not entirely inconsistent with any of the observed data. The
Grenoble measurements imply an extremely weak temperature dependence which
is inconsistent with that of either CAVIAR-lab or MT_CKD_3.2 and less consistent with the estimated CAVIAR-field
data than CAVIAR-lab. While these results indicate a significantly stronger
continuum than that implied by the available laboratory data, the
uncertainties are too large to form firm conclusions. In addition, the
CAVIAR-field results do not reconcile the apparent large discrepancy between
the extrapolated CAVIAR-lab continuum and the Grenoble measurements; this
contrasts markedly with the situation in the centre of the 2.1 window (Fig. 14c), where there is consistency between these datasets and reasonable
consistency with CAVIAR-field when the CAVIAR-lab foreign continuum is
used.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F15" specific-use="star"><?xmltex \currentcnt{15}?><label>Figure 15</label><caption><p id="d1e2998">Self-continuum absorption cross section against temperature for
various datasets at <bold>(a)</bold> 6050, <bold>(b)</bold> 6177, and <bold>(c)</bold> 6383 cm<inline-formula><mml:math id="M206" 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 error
bars indicate the <inline-formula><mml:math id="M207" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties. Marker size is greater than the
stated uncertainty where error bars are not visible. The dashed black line
indicates the region outside of the expected applicability of
MT_CKD. The dashed blue and red lines indicate extrapolations
of the CAVIAR-lab and Grenoble temperature dependence respectively.</p></caption>
            <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f15.png"/>

          </fig>

</sec>
<sec id="Ch1.S5.SS1.SSS4">
  <label>5.1.4</label><title>Synthesis</title>
      <?pagebreak page2350?><p id="d1e3048">Figure 16 shows the spectrally resolved self-continuum from CAVIAR-field
(using the two foreign continua), alongside other sets of observations. The
CRDS measurements are shown at their original temperature, since for many
wavenumbers observations are only available at one temperature. Assuming the
MT_CKD temperature dependence holds, these can be scaled by a
factor of <inline-formula><mml:math id="M208" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">1.35</mml:mn></mml:mrow></mml:math></inline-formula> to be brought to 280 K. Figure 16 shows that
the estimated continuum does not vary particularly strongly spectrally in
the centres of the windows. However, there are clearly some issues in the 4 <inline-formula><mml:math id="M209" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, where at lower wavenumbers the derived continuum is
significantly stronger than MT_CKD_3.2 and the
extrapolated CAVIAR-lab self-continuum, and in the low-wavenumber edge of
the 2.1 <inline-formula><mml:math id="M210" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, where when estimating the self-continuum using the
CAVIAR-lab foreign continuum there is a significant decrease in the
self-continuum. As discussed previously, this is likely due to either the
CAVIAR-lab foreign continuum being too strong at this low-wavenumber edge
or some issue with the FTS field observations used in this work. In the 1.6 <inline-formula><mml:math id="M211" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, a significant strengthening of the foreign continuum of
over a factor of 100 would be required to bring the central values of the
CAVIAR-lab and CAVIAR-field self-continua into agreement, which is
inconsistent with the CAVIAR-lab foreign continuum in this window. However,
there is some agreement within the <inline-formula><mml:math id="M212" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainty limits between
CAVIAR-lab and CAVIAR-field at the centre of the window.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F16" specific-use="star"><?xmltex \currentcnt{16}?><label>Figure 16</label><caption><p id="d1e3099">Self-continuum from CAVIAR-field as estimated using <bold>(a)</bold> the
MT_CKD foreign continuum and <bold>(b)</bold> the CAVIAR-lab
foreign continuum, alongside MT_CKD_3.2 and
selected laboratory measurements. The grey shaded regions indicate the <inline-formula><mml:math id="M213" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> confidence limits in the CAVIAR-field self-continuum and the blue shaded
regions the uncertainty in the temperature-extrapolated (to 280 K)
CAVIAR-lab data. The darker shaded regions are where these uncertainty
limits overlap. The CAVIAR-lab uncertainties are obtained via Monte Carlo
fits using the uncertainties in the higher-temperature (<inline-formula><mml:math id="M214" display="inline"><mml:mrow><mml:mi mathvariant="italic">&gt;</mml:mi><mml:mn mathvariant="normal">350</mml:mn></mml:mrow></mml:math></inline-formula> K)
CAVIAR-lab data.</p></caption>
            <?xmltex \igopts{width=426.791339pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f16.png"/>

          </fig>

</sec>
</sec>
<sec id="Ch1.S5.SS2">
  <label>5.2</label><title>Foreign continuum</title>
<sec id="Ch1.S5.SS2.SSS1">
  <label>5.2.1</label><title>Current observations</title>
      <p id="d1e3152">Ptashnik et al. (2012) (CAVIAR-lab) presented foreign-continuum coefficients
in the 4, 2.1, 1.6, and 1.2 <inline-formula><mml:math id="M215" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows using FTS; these remain the only
laboratory dataset with a large wavenumber coverage. These observations are
made using a cell filled with an <inline-formula><mml:math id="M216" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math></inline-formula>–air mixture and then subtracting
the self-continuum contribution as measured by Ptashnik et al. (2011a). At
all temperatures, their foreign continuum is consistently stronger than all
versions of MT_CKD in the central parts of the 4–1.6 <inline-formula><mml:math id="M217" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m
windows (between 10 and 100 times stronger than MT_CKD_2.5), although there is better agreement at the edges of
these windows.</p>
      <p id="d1e3184">Baranov and Lafferty (2012) report foreign-continuum values in the 4 <inline-formula><mml:math id="M218" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m
window using an FTS technique, assuming the self-continuum as measured by
Baranov and Lafferty (2011). These agree very well with the measurements of
Baranov (2011), which were taken at four temperatures (326, 339, 352, and 363 K). In a similar way to the CAVIAR-lab foreign continuum, they observe a
factor of 100 stronger foreign continuum than MT_CKD_2.5 in the centre of the 4 <inline-formula><mml:math id="M219" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window and are in
reasonable agreement with Ptashnik et al. (2012). They also exhibit no
significant temperature dependence, in agreement with Ptashnik et al. (2012).</p>
      <p id="d1e3203">Mondelain et al. (2015) presented a
foreign-continuum measurement at one wavenumber (4250 cm<inline-formula><mml:math id="M220" 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 298 K
using the CRDS technique. Their reported values were a factor of
<inline-formula><mml:math id="M221" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">4.5</mml:mn></mml:mrow></mml:math></inline-formula> stronger than MT_CKD in this region and
a factor of <inline-formula><mml:math id="M222" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> weaker than CAVIAR-lab. Vasilchenko et al. (2019) present foreign-continuum data at 4435, 4522, 4720, and 4999 cm<inline-formula><mml:math id="M223" 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>
using CRDS. Their data do not agree within the <inline-formula><mml:math id="M224" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties of the
CAVIAR-lab FTS measurements (aside from at 4720 cm<inline-formula><mml:math id="M225" 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 are
systematically lower by a factor of 2–4. They do however agree within the
<inline-formula><mml:math id="M226" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties. The CRDS foreign continuum was measured at room
temperature; assuming that both the FTS and<?pagebreak page2351?> CRDS measurements are robust,
this would indicate a small positive temperature dependence for the foreign
continuum. The Vasilchenko et al. data are systematically a factor of 5
stronger than the MT_CKD foreign continuum; both the FTS and
CRDS data indicate that MT_CKD therefore requires some
strengthening, but by differing amounts.</p>
      <p id="d1e3287">The only existing dataset of pure foreign-continuum measurements in the 1.6 <inline-formula><mml:math id="M227" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window is the CAVIAR-lab data. We therefore focus our comparison
solely on MT_CKD and CAVIAR-lab in this region.</p>
      <p id="d1e3299">In addition to the laboratory measurements, Reichert and Sussmann (2016)
presented measurements of the water vapour continuum in the atmosphere
between 2500 and 7600 cm<inline-formula><mml:math id="M228" 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 Sect. 1.2 for more details). Given the
high altitude and low water vapour path of their measurements, Reichert and
Sussmann indicate that the foreign continuum is by far the dominant
contributor to the continuum in the majority of their measured spectral
regions; we therefore compare their measurements to our foreign-continuum
measurements directly, but there may be some small self-continuum component
which we do not account for in the Reichert and Sussmann data. The
domination of the foreign continuum is more likely to be the case in the
atmospheric windows, where the foreign-continuum contribution is larger
(e.g. Ptashnik et al., 2012). Reichert and Sussmann present data in the 4,
2.1, and 1.6 <inline-formula><mml:math id="M229" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows; however, due to the low atmospheric absorption
seen in their experiment, the results are negative for a significant portion
of the spectrum. However, their uncertainty limits provide an upper bound on
the strength of the foreign continuum.</p>
</sec>
<sec id="Ch1.S5.SS2.SSS2">
  <label>5.2.2</label><title>CAVIAR-field foreign continuum</title>
      <p id="d1e3330">The foreign continuum can be inferred from the CAVIAR-field measurements
using high-temperature observations of the self-continuum extrapolated down
to room temperature. This allows for comparison with the laboratory foreign-continuum data and with Reichert and Sussmann (2016). Figure 17 shows the
CAVIAR-field foreign continuum for two different cases, assuming (a) the
MT_CKD_3.2 self-continuum and (b) the
high-temperature CAVIAR-lab self-continuum extrapolated to 280 K. In this
case, only the data points above <inline-formula><mml:math id="M230" display="inline"><mml:mrow><mml:mi>T</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">297</mml:mn></mml:mrow></mml:math></inline-formula> K have been included in the
extrapolation, to better reflect the agreement (when extrapolated) with the
available Grenoble measurements in these windows, which have lower
uncertainties at low temperature.</p>
      <p id="d1e3345">We focus the discussion here on the 2.1 and 4 <inline-formula><mml:math id="M231" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows, since these
are the regions in which the most laboratory data are available. It is
important to emphasise here that the foreign continuum cannot be derived
from laboratory<?pagebreak page2352?> measurements without prior knowledge of the self-continuum
and that therefore the foreign-continuum values shown are sensitive to the
assumptions made about the self-continuum.</p>
      <p id="d1e3356">In the centre of the 4 <inline-formula><mml:math id="M232" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, Fig. 17 shows that the foreign
continuum is significantly stronger (<inline-formula><mml:math id="M233" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">20</mml:mn><mml:mo>×</mml:mo></mml:mrow></mml:math></inline-formula>) than
MT_CKD_3.2 regardless of the assumption made
about the self-continuum and agrees well with the CAVIAR-lab and Baranov (2011) foreign continua, which are plotted here at 326 K. It is also
consistent with Reichert and Sussmann (2016) within the <inline-formula><mml:math id="M234" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainty
limits. The weight of available data appears to indicate that a significant
strengthening of the MT_CKD foreign continuum is required in
the centre of this window. Given that Baranov and Lafferty (2012) retrieval
of the foreign continuum uses the Baranov and Lafferty (2011)
self-continuum, which may be an overestimate if the Grenoble measurements
are correct<?pagebreak page2353?> (Fig. 13), this strengthening could even be larger than
indicated.</p>
      <p id="d1e3391">Figure 17 shows that in the centre of the 2.1 <inline-formula><mml:math id="M235" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window there is
excellent agreement between the CAVIAR-lab and CAVIAR-field foreign continua
whether using either the MT_CKD_3.2 (panel a)
or CAVIAR-lab self-continuum (panel b). This provides evidence that,
assuming our knowledge of the self-continuum is robust, the foreign
continuum is better characterised by CAVIAR-lab than MT_CKD_ 3.2. As indicated in Reichert and Sussmann (2016), their
values can only represent an upper limit on the continuum in the windows.
Nevertheless, these results agree with ours within the <inline-formula><mml:math id="M236" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties,
indicating that the two are consistent. However, at the low-wavenumber edge
of the window (<inline-formula><mml:math id="M237" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">4200</mml:mn></mml:mrow></mml:math></inline-formula> cm<inline-formula><mml:math id="M238" 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>), our results show a somewhat
weaker (factor of <inline-formula><mml:math id="M239" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula>) foreign continuum than CAVIAR-lab. This
is consistent with the inference made in Sect. 5.1.2 when estimating the
self-continuum. Our results are consistent with the uncertainty limits of
Reichert and Sussmann (2016) at these wavenumbers. There is good agreement
between the various laboratory self-continuum data in this window (when
extrapolated to room temperature), which gives some confidence in the
analysis presented in Fig. 14. Our reported uncertainties are also smaller
in this region, and any unattributed aerosol effect would be smaller in this
window than at 1.6 <inline-formula><mml:math id="M240" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m. These results indicate that the foreign
continuum is stronger than the MT_CKD_3.2
foreign continuum by about a factor of 5 in the centre of the window, in
agreement with Ptashnik et al. (2012) and Vasilchenko et al. (2019).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F17" specific-use="star"><?xmltex \currentcnt{17}?><label>Figure 17</label><caption><p id="d1e3458">CAVIAR-field foreign continuum in the atmospheric windows across
the 2000–7000 cm<inline-formula><mml:math id="M241" 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> region alongside CAVIAR-lab, MT_CKD_ 3.2, and Reichert and Sussmann (2016) data. The shaded
regions and error bars indicate the <inline-formula><mml:math id="M242" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties. Panel <bold>(a)</bold> shows the
CAVIAR-field foreign continuum assuming the MT_CKD_3.2 self-continuum and panel <bold>(b)</bold> shows the CAVIAR-field
foreign continuum assuming the CAVIAR-lab self-continuum, which is derived
from extrapolating the high-temperature (<inline-formula><mml:math id="M243" display="inline"><mml:mrow><mml:mi mathvariant="italic">&gt;</mml:mi><mml:mn mathvariant="normal">350</mml:mn></mml:mrow></mml:math></inline-formula> K) data to 280 K.</p></caption>
            <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f17.png"/>

          </fig>

      <p id="d1e3507">The situation in the 1.6 <inline-formula><mml:math id="M244" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window (Fig. 17) is less clear. The
uncertainties in our measurements are greater, and there is less consistency
in this window between this work and the laboratory data. The agreement
improves when the stronger CAVIAR-lab self-continuum is used (Fig. 17b). This
could indicate that there is an issue with our measurements in this window
(such as aerosol contamination or a systematic calibration uncertainty) or
that the foreign continuum is significantly stronger than predicted by
CAVIAR-lab. Despite the large observed values, CAVIAR-field, CAVIAR-lab, and
Reichert and Sussmann (2016) are all consistent within their <inline-formula><mml:math id="M245" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula>
uncertainty limits. These results indicate a larger absorption than observed
in the CAVIAR-lab data. Such a large absorption could explain the results of
Oyafuso et al. (2017), who reported that “unrealistically large
multiplicative factors (<inline-formula><mml:math id="M246" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">8</mml:mn><mml:mo>×</mml:mo></mml:mrow></mml:math></inline-formula> for the 2.06 <inline-formula><mml:math id="M247" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m band and <inline-formula><mml:math id="M248" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">150</mml:mn><mml:mo>×</mml:mo></mml:mrow></mml:math></inline-formula> for the 1.6 <inline-formula><mml:math id="M249" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m band) for the water vapour continuum were
required”. This work strongly suggests that a strengthening of the foreign
continuum by a factor of <inline-formula><mml:math id="M250" display="inline"><mml:mrow><mml:mn mathvariant="normal">10</mml:mn><mml:mo>×</mml:mo></mml:mrow></mml:math></inline-formula> is necessary to MT_CKD_3.2 at 2.1 <inline-formula><mml:math id="M251" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m (consistent with laboratory
observations) and absorption a factor of <inline-formula><mml:math id="M252" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">100</mml:mn><mml:mo>×</mml:mo></mml:mrow></mml:math></inline-formula> stronger than
MT_CKD_3.2 in the 1.6 <inline-formula><mml:math id="M253" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window (which is
less consistent with laboratory observations). There appears to be an urgent
need for an independent set of foreign-continuum measurements in the
1.6 <inline-formula><mml:math id="M254" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window to resolve this discrepancy.</p>
</sec>
</sec>
<sec id="Ch1.S5.SS3">
  <label>5.3</label><title>Relative contributions of the self- and foreign-continua</title>
      <p id="d1e3626">An additional issue of importance is the relative contribution to the total
continuum absorption of the self- and foreign-continua, particularly for
atmospheric scientists, since the relative contribution of each is strongly
dependent on the atmospheric conditions at the time of measurement. Figure 18 shows the percentage of the optical depth originating from the self- and
foreign-continua for conditions of 18 September 2008 from MT_CKD_3.2 (the optical depth calculated using MT_CKD_3.2 is shown in Fig. 7). In these conditions (with an
integrated water vapour column of about 16 kg m<inline-formula><mml:math id="M255" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>; see Sect. 2), the
self-continuum dominates in the centres of the windows (<inline-formula><mml:math id="M256" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">95</mml:mn></mml:mrow></mml:math></inline-formula> % in the centre of the 4 <inline-formula><mml:math id="M257" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, 90 % in the centre of the
2.1 <inline-formula><mml:math id="M258" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, and <inline-formula><mml:math id="M259" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">80</mml:mn></mml:mrow></mml:math></inline-formula> % in the centre of the
1.6 <inline-formula><mml:math id="M260" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window), while the foreign continuum dominates in the bands.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F18" specific-use="star"><?xmltex \currentcnt{18}?><label>Figure 18</label><caption><p id="d1e3688">Proportion of the 18 September 2008 Camborne optical depth
attributable to the self- and foreign-continua as calculated using the
MT_CKD_3.2 model. The total optical depth is
shown by the red line in Fig. 7.</p></caption>
          <?xmltex \igopts{width=441.017717pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f18.png"/>

        </fig>

      <p id="d1e3697">Figure 19 shows the percentage contribution of the CAVIAR-field
self-continuum (panel a) and CAVIAR-field foreign continuum (panel b). Each
of these panels shows the proportion of the total 18 September 2008
continuum optical depth attributable to the self or foreign optical depth by
assuming the contribution from the other component via either CAVIAR-lab or
MT_CKD. The relative contribution in this case is as given by
Eq. (5). Unlike with MT_CKD, which is well-constrained (and
therefore the total contribution of the self- and foreign-continua sums up to
the total, as in Fig. 18), the CAVIAR-field estimated continuum is not, in
the case where <inline-formula><mml:math id="M261" display="inline"><mml:mrow><mml:mi>a</mml:mi><mml:mo>≠</mml:mo><mml:mi>b</mml:mi><mml:mo>≠</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>, as we do not have enough information to
derive independent values of the two components of the CAVIAR-field
continuum. Therefore, it should not be expected that <inline-formula><mml:math id="M262" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">for</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup><mml:mo>+</mml:mo><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">self</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup><mml:mo>=</mml:mo><mml:msubsup><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">tot</mml:mi><mml:mi mathvariant="normal">CAV</mml:mi></mml:msubsup></mml:mrow></mml:math></inline-formula>. Figure 19 should be
interpreted as the values implied by CAVIAR-field when assuming that the
self or foreign contribution is well-characterised by either CAVIAR-lab or
MT_CKD.</p>
      <p id="d1e3748">The self-continuum (panel a) contribution is large (<inline-formula><mml:math id="M263" display="inline"><mml:mrow><mml:mi mathvariant="italic">&gt;</mml:mi><mml:mn mathvariant="normal">95</mml:mn></mml:mrow></mml:math></inline-formula> %)
when using the MT_CKD foreign continuum across all of the
windows of interest, similar to the case shown in Fig. 18. However, when
using the CAVIAR-lab foreign continuum, this contribution decreases by an
amount depending on the window of interest. In the 4 <inline-formula><mml:math id="M264" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, the
contribution varies from <inline-formula><mml:math id="M265" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">50</mml:mn></mml:mrow></mml:math></inline-formula> % to almost 0 % in the
centre of the window. Similarly, in the 2.1 <inline-formula><mml:math id="M266" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, the
self-continuum drops from <inline-formula><mml:math id="M267" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">95</mml:mn></mml:mrow></mml:math></inline-formula> % to <inline-formula><mml:math id="M268" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">40</mml:mn></mml:mrow></mml:math></inline-formula> %
contribution when using the stronger CAVIAR-lab foreign continuum.
At 1.6 <inline-formula><mml:math id="M269" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m, almost all of the absorption when assuming the MT_CKD foreign continuum is implied to come from the self-continuum. This is
because the MT_CKD_3.2 foreign continuum is
extremely weak in this region, and the total CAVIAR-field optical depth is
much larger than the MT_CKD_3.2 optical depth
(see Fig. 7). Using the CAVIAR-lab foreign continuum decreases the
contribution of the self-continuum to <inline-formula><mml:math id="M270" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">80</mml:mn></mml:mrow></mml:math></inline-formula> % in the centre
of this window, comparable with the fraction implied when just using
MT_CKD (Fig. 18).</p>
      <?pagebreak page2355?><p id="d1e3826">Because of the lack of constraint on the CAVIAR-field optical depth, the
implied foreign-continuum contribution when assuming the MT_CKD or CAVIAR-lab self-continua (Fig. 17b) is also high (over 60 % across
all three windows). Unlike the self-continuum case, there is reasonable
consistency between the implied values using either CAVIAR-lab or
MT_CKD. At 4 <inline-formula><mml:math id="M271" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m, using the CAVIAR-lab self-continuum
increases the foreign contribution from <inline-formula><mml:math id="M272" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">60</mml:mn></mml:mrow></mml:math></inline-formula> %–80 % to
<inline-formula><mml:math id="M273" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">75</mml:mn></mml:mrow></mml:math></inline-formula> %–90 % in the centre of the window, since the CAVIAR-lab
self-continuum is smaller at room temperature than that of MT_CKD in this region (see Fig. 13). At 2.1 <inline-formula><mml:math id="M274" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m, the contribution drops
from <inline-formula><mml:math id="M275" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">80</mml:mn></mml:mrow></mml:math></inline-formula> % to <inline-formula><mml:math id="M276" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">70</mml:mn></mml:mrow></mml:math></inline-formula> % when using the
MT_CKD and CAVIAR-lab self-continua respectively. At 1.6 <inline-formula><mml:math id="M277" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m, the CAVIAR-field foreign continuum is almost 100 % in the centre of the window
when using the MT_CKD self-continuum, but drops to
<inline-formula><mml:math id="M278" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">80</mml:mn></mml:mrow></mml:math></inline-formula> %–90 % when using the CAVIAR-lab self-continuum.</p>
      <p id="d1e3904">The lack of consistency between the CAVIAR-field estimated self-continuum and foreign
continuum is an indication of the lack of constraint on <inline-formula><mml:math id="M279" display="inline"><mml:mi>a</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M280" display="inline"><mml:mi>b</mml:mi></mml:math></inline-formula>, meaning that
there are potentially issues with CAVIAR-field, with the laboratory
measurements, and/or MT_CKD.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F19" specific-use="star"><?xmltex \currentcnt{19}?><label>Figure 19</label><caption><p id="d1e3923">Proportion of the total continuum optical depth for 18 September 2008 from the CAVIAR-field self-continuum assuming the CAVIAR-lab and
MT_CKD_3.2 foreign continua (<bold>a</bold>) and the
CAVIAR-field foreign continuum assuming the CAVIAR-lab and MT_CKD_3.2 self-continua (<bold>b</bold>). As explained in the text,
these are insufficient data to constrain the field observations such that the
percentage contributions of the self-continuum and foreign continuum sum to 100 %, given the
methodology to derive the self and foreign components of the field
continuum.</p></caption>
          <?xmltex \igopts{width=398.338583pt}?><graphic xlink:href="https://amt.copernicus.org/articles/13/2335/2020/amt-13-2335-2020-f19.png"/>

        </fig>

</sec>
</sec>
<sec id="Ch1.S6">
  <label>6</label><title>Future steps</title>
      <p id="d1e3947">Given the uncertainties present in this analysis and the need to measure in
a wider range of conditions to more accurately separate the foreign- and
self-continua, more measurements are required to sufficiently constrain the
continuum absorption in atmospheric conditions. This section details how a
future field campaign might reduce the uncertainty in the derived continuum
when performing an analysis such as the one presented in this work.</p>
      <p id="d1e3950">The main contributor to the uncertainty was the lack of well-characterised
aerosol extinction. This is the most significant factor in the uncertainty
budget, and there were significant problems in characterising the variation
over time. This may have been due to operational problems with the Microtops
sunphotometer used to measure aerosol optical depth. While the stated
uncertainty is reasonably small (e.g. Ichoku et al., 2002, estimate an optical depth uncertainty of <inline-formula><mml:math id="M281" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula>
in the lower-wavenumber channels and <inline-formula><mml:math id="M282" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.01</mml:mn></mml:mrow></mml:math></inline-formula> or less in the higher
wavenumber channels), there was a clearly observed time variation in the
<inline-formula><mml:math id="M283" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> that was not present in the FTS measurements.
Additionally, the observations of <inline-formula><mml:math id="M284" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> were taken in channels
in the visible and near-infrared parts of the spectrum and extrapolated out
into the near-infrared. This means that, while the aerosol optical depth
decreases with decreasing wavenumber (e.g. Fig. 5), there is a higher
fractional uncertainty since there is a need to extrapolate further.</p>
      <p id="d1e3997">Ideally, any future campaign would use a more robust method of measuring
aerosol extinction, such as taking place close to an AERONET site (e.g. Giles et al.,
2019). Mounting our sunphotometer on a solar tracker may have aided our
analysis and possibly reduced some of the problems described in Sect. 2.4.
A future campaign should minimise the aerosol contamination by taking place
at higher altitude. High-altitude observations would take place in the
tropics to ensure there is enough water vapour for the continuum signal to
be detectable in the windows. Additionally, satellite products could be used
to measure <inline-formula><mml:math id="M285" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>; these have improved significantly in the
decade since the Camborne observations were taken and could be used in
conjunction with AERONET and in situ measurements to constrain aerosol. Some
caution should be warranted however, since satellites use atmospheric
windows to obtain aerosol which also contain the ill-constrained continuum
absorption.</p>
      <p id="d1e4011">Additionally, aircraft could be used to constrain the aerosol profile,
aiding in e.g. calculations using a Mie<?pagebreak page2356?> scattering code. Measuring the
aerosol profile in ambient conditions would be a significant step towards a
more robust representation of <inline-formula><mml:math id="M286" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mi mathvariant="normal">aerosol</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, e.g. from a research
aircraft. Aircraft could also be used to provide measurements of other
variables, such as temperature, or even for fully radiometric measurements. Green et al. (2012) and Newman et al. (2012) measured the mid- and
far-infrared continuum via aircraft measurements during the CAVIAR project
using the FAAM (Facility for Airborne Atmospheric Measurements). This method
works well for measuring the comparatively strong mid- and far-infrared
continuum, but could potentially be used to measure the in-band continuum in
the near-IR. However, this method relies on accurate calibration either to a
blackbody source or to a prescribed SSI to retrieve the continuum via the
closure method, since it is difficult to perform a Langley analysis using an
aircraft.</p>
      <p id="d1e4026">Future campaigns could use the calibration method described in Reichert et
al. (2016) to calibrate a spectrometer to the top of atmosphere solar
irradiance, rather than using a comprehensive radiometric calibration such
as that used in this work, once it is known to higher accuracy. This would
reduce the costs of such a campaign and potentially allow for observations
in a wider range of conditions, such as high-altitude sites where
maintaining good calibration is<?pagebreak page2357?> difficult. A significant limitation of this
study is the lack of measurements in different atmospheric conditions.
Measurements over a wide range of IWV would help significantly in
strengthening the constraints on the parameters <inline-formula><mml:math id="M287" display="inline"><mml:mi>a</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M288" display="inline"><mml:mi>b</mml:mi></mml:math></inline-formula> in Eq. (5),
particularly measurements where the continuum in the windows is dominated by
either the foreign continuum or self-continuum. It is in principle possible to derive
the absorption coefficients directly, given a set of atmospheric
observations over a range of conditions, since the self-continuum varies
with the square of the vapour pressure, while the foreign continuum varies with the
product of vapour pressure and the pressure of the ambient air. Such an
analysis would also have to take into account the temperature dependence of
the self-continuum.</p>
      <p id="d1e4043">If the relative contribution of the self- and foreign-continua was well-constrained, an analysis like that performed in Sect. 5 could be
performed, but with significantly more confidence in the results, and allow
a more direct comparison with the laboratory measurements without the strong
assumptions required in our analysis.</p>
      <p id="d1e4046">Alternatively, one could use a horizontal atmospheric path, using e.g. a
laser source rather than the Sun. This has been performed by e.g. Rieker et al. (2014) to observe carbon
dioxide and methane absorption in the centre and edges of the 1.6 <inline-formula><mml:math id="M289" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m
window using a frequency comb method over a 2 km path. Using a horizontal
path reduces the effect of clouds and aerosols and allows for in situ measurements
of humidity, temperature, and pressure directly in the beam path rather than
relying on potentially uncertain radiosonde measurements (which are directed
by the prevailing winds and not necessarily representative of the path
observed by a spectrometer). However, this would result in similar problems
to those found in a laboratory, namely the difficulty in constructing a path
length long enough to measure the comparatively weak continuum absorption in
the windows. In such a measurement, the experimenter would have
significantly less control over the conditions compared to a laboratory
measurement.</p>
</sec>
<sec id="Ch1.S7" sec-type="conclusions">
  <label>7</label><title>Conclusions</title>
      <p id="d1e4065">We have presented new field observations of the near-IR continuum in the
atmospheric windows at 4, 2.1, and 1.6, <inline-formula><mml:math id="M290" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m (2500–6600 cm<inline-formula><mml:math id="M291" 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>). These
measurements are, to our knowledge, the first and only published
measurements which characterise the water vapour continuum in the near-IR
windows at sea level. Our data show good agreement with laboratory spectra
in the first two of these windows, but the agreement worsens with increasing
wavenumber. This is consistent with signal contamination due to atmospheric
aerosol, which is more pronounced at higher wavenumbers. These measurements
provide some real-world validation of the extrapolated laboratory data and
semi-empirical models, which are relied on for radiative modelling purposes.</p>
      <p id="d1e4088">In the centre of the 4 <inline-formula><mml:math id="M292" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, there is good agreement between the
CAVIAR-field self-continuum and the various sets of laboratory data. The
laboratory self-continua exhibit two different temperature dependencies,
with Baranov and Lafferty (2011) showing a significantly steeper temperature
dependence than Richard et al. (2017). The CAVIAR-field data could agree
with either of these implied temperature dependences, depending on whether
the MT_CKD_3.2 or CAVIAR-lab foreign continuum
is assumed respectively. Given that CAVIAR-field is an experimental
estimate, and the high precision and accuracy of the Richard et al. (2017)
measurements, we believe that this is evidence of a weaker self-continuum
at the centre of this window than observed by Baranov and Lafferty (2011).
We also demonstrate that a strengthening is required to the
MT_CKD_3.2 foreign continuum in this window,
in agreement with the results of Ptashnik et al. (2012), Baranov (2011), and
Baranov and Lafferty (2012). This strengthening varies spectrally, but is a
factor of <inline-formula><mml:math id="M293" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">100</mml:mn></mml:mrow></mml:math></inline-formula> in the centre of the window at 2500 cm<inline-formula><mml:math id="M294" 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>
      <p id="d1e4121">We show that, assuming the (temperature-extrapolated) CAVIAR-lab
self-continuum is correct in the 2.1 <inline-formula><mml:math id="M295" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m window, the foreign continuum
in the centre of the window is underestimated by MT_CKD_3.2 by a factor of 5, in agreement with the laboratory
measurements of Ptashnik et al. (2012) and Vasilchenko et al. (2019). In
the centre of the window, assuming the CAVIAR-lab foreign continuum, our
data agree well with extrapolated self-continuum components from CAVIAR-lab
and the various Grenoble CRDS measurements. At the edge of the window, we
demonstrate that the MT_CKD foreign continuum is likely too
weak, but by less than a factor of 5 and not as strong as the window-edge
foreign continuum from CAVIAR-lab. Alternatively, there is a possibility
that the foreign continuum exhibits more temperature dependence than has
been inferred from the available laboratory studies.</p>
      <p id="d1e4132">At 1.6 <inline-formula><mml:math id="M296" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m, we show a significantly stronger implied self-continuum
than the extrapolated CAVIAR-lab and Grenoble laboratory measurements,
regardless of whether the MT_CKD_3.2 or CAVIAR
foreign continuum is used. This may indicate one of several things. There
may be some systematic error in our retrieval of the continuum optical depth
(whether due to aerosol or a calibration issue). It may also suggest that a
significantly stronger self-continuum is realistic, such as the large values
reported by Ptashnik et al. (2015). However, this is unlikely to be the
case, given that the authors of Ptashnik et al. (2015) believe their results
may be spurious (Ptashnik et al., 2019b). Alternatively, it may be that the
foreign continuum as measured by CAVIAR-lab is too weak, or some combination
of the above factors.</p>
      <p id="d1e4144">Across the spectrum, we observe a greater proportion of the total continuum
optical depth in the 4, 2.1, and 1.6 <inline-formula><mml:math id="M297" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m windows as likely coming from
the foreign continuum, rather than the self-continuum (for the atmospheric
conditions at the time of our observations). This may indicate that the
foreign continuum is being underestimated by MT_CKD_3.2 in<?pagebreak page2358?> these windows, which could have significant
implications for atmospheric radiative transfer calculations for both
climate modelling and remote sensing applications.</p>
      <p id="d1e4155">Given the challenges that come with making absolutely calibrated high-resolution results in the atmosphere, rather than a controlled laboratory
setting, our results are characterised by high uncertainties. We detail ways
in which a future field campaign should improve upon our characterisation of
atmospheric aerosol in particular, by either mitigating its effect or
measuring it with greater accuracy and precision.</p>
      <p id="d1e4158">This work represents a significant advance in understanding of the continuum
absorption in near-IR windows, as it is the only existing dataset of direct
atmospheric measurements with positive values in these windows. Our results
are consistent with the upper limits imposed by Reichert and Sussmann (2016). Our work and that of Reichert and Sussmann demonstrate that it is
possible to observe the near-IR continuum in the field within the bands and
windows to some degree of accuracy. We encourage future field measurements,
in as wide a range of conditions as possible, to more rigorously assess the
partition between the self- and foreign-continua in the atmosphere. Such
measurements should take steps to avoid the problems encountered in this
work, particularly regarding aerosol scattering, with careful consideration
of the calibration drift over the course of individual days of measurement
and over the course of a measurement campaign.</p>
</sec>

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

      <p id="d1e4165">The data from this work are available via online depository (<ext-link xlink:href="https://doi.org/10.5281/zenodo.3520519" ext-link-type="DOI">10.5281/zenodo.3520519</ext-link>, Elsey et al., 2019). Included is the best estimate of the continuum
optical depth (18 September 2008), provided with the <inline-formula><mml:math id="M298" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> uncertainties,
the ratio of this best estimate to the corresponding MT_CKD_3.2 optical depth from 18 September 2008, and the
CAVIAR-field estimated continuum absorption coefficients using both
MT_CKD and CAVIAR-lab. All data are provided at 1 cm<inline-formula><mml:math id="M299" 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>
resolution. Other data (including full resolution data) are available from
the corresponding author upon request.</p>
  </notes><app-group>
        <supplementary-material position="anchor"><p id="d1e4195">The supplement related to this article is available online at: <inline-supplementary-material xlink:href="https://doi.org/10.5194/amt-13-2335-2020-supplement" xlink:title="pdf">https://doi.org/10.5194/amt-13-2335-2020-supplement</inline-supplementary-material>.</p></supplementary-material>
        </app-group><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e4204">JE led the analysis of the measurements, building on the initial work of KPM,
both of whom were supervised and guided by KPS, MDC, and TDG. MDC and TDG designed
and calibrated the observing system and led the CAVIAR field measurements.
KPS was the overall principal investigator of the CAVIAR project and led the
formulation of the project goals. JE led the writing of the original draft,
with input from all the other authors over several cycles of revision.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e4210">The authors declare that they have no conflict of interest.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e4216">Jonathan Elsey would like to thank the NERC SCENARIO Doctoral Training Partnership for funding his PhD research (studentship number 1503015) and NPL for providing additional financial support. We thank Liam Tallis for his work in performing the initial measurements. We thank Nicolas Bellouin for his valuable input regarding the analysis of aerosol optical depth. We thank the referees for many useful comments.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e4222">This research was funded by the Natural Environment Research Council/Engineering and Physical Sciences Research Council (grant no. NE/D012082/1) as part of the CAVIAR (Continuum Absorption at Visible and Infrared wavelengths and its Atmospheric Relevance) project. The latter stages of the analysis and writing were supported by the Natural Environment Research Council “Advanced Spectroscopy for improved characterisation of the near-Infrared water vapour Continuum (ASPIC)” research grant (NE/R009848/1).</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e4228">This paper was edited by Christof Janssen and reviewed by two anonymous referees.</p>
  </notes><ref-list>
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    <!--<article-title-html>Atmospheric observations of the water vapour continuum in the near-infrared windows between 2500 and 6600&thinsp;cm<sup>−1</sup></article-title-html>
<abstract-html><p>Water vapour continuum absorption is potentially
important for both closure of the Earth's energy budget and remote sensing
applications. Currently, there are significant uncertainties in its
characteristics in the near-infrared atmospheric windows at
2.1 and 1.6&thinsp;µm. There have been several attempts to measure the continuum in the
laboratory; not only are there significant differences amongst these
measurements, but there are also difficulties in extrapolating the laboratory
data taken at room temperature and above to temperatures more widely
relevant to the atmosphere. Validation is therefore required using field
observations of the real atmosphere. There are currently no published
observations in atmospheric conditions with enough water vapour to detect a
continuum signal within these windows or where the self-continuum component
is significant. We present observations of the near-infrared water vapour
continuum from Camborne, UK, at sea level using a Sun-pointing,
radiometrically calibrated Fourier transform spectrometer in the window
regions between 2000 and 10&thinsp;000&thinsp;cm<sup>−1</sup>. Analysis of these data is challenging,
particularly because of the need to remove aerosol extinction and the large
uncertainties associated with such field measurements. Nevertheless, we
present data that are consistent with recent laboratory datasets in the 4 and
2.1&thinsp;µm windows (when extrapolated to atmospheric temperatures). These
results indicate that the most recent revision (3.2) of the
MT_CKD foreign continuum, versions of which are widely used
in atmospheric radiation models, requires strengthening by a factor of
 ∼ 5 in the centre of the 2.1&thinsp;µm window. In the
higher-wavenumber window at 1.6&thinsp;µm, our estimated self- and foreign-continua are significantly stronger than MT_CKD. The possible
contribution of the self- and foreign-continua to our derived total continuum
optical depth is estimated by using laboratory or MT_CKD
values of one, to estimate the other. The obtained self-continuum shows some
consistency with temperature-extrapolated laboratory data in the centres of
the 4 and 2.1&thinsp;µm windows. The 1.6&thinsp;µm region is more sensitive to
atmospheric aerosol and continuum retrievals and therefore more uncertain
than the more robust results at 2.1 and 4&thinsp;µm. We highlight the
difficulties in observing the atmospheric continuum and make the case for
additional measurements in both the laboratory and field and discuss the
requirements for any future field campaign.</p></abstract-html>
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