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  <front>
    <journal-meta><journal-id journal-id-type="publisher">ACP</journal-id><journal-title-group>
    <journal-title>Atmospheric Chemistry and Physics</journal-title>
    <abbrev-journal-title abbrev-type="publisher">ACP</abbrev-journal-title><abbrev-journal-title abbrev-type="nlm-ta">Atmos. Chem. Phys.</abbrev-journal-title>
  </journal-title-group><issn pub-type="epub">1680-7324</issn><publisher>
    <publisher-name>Copernicus Publications</publisher-name>
    <publisher-loc>Göttingen, Germany</publisher-loc>
  </publisher></journal-meta>
    <article-meta>
      <article-id pub-id-type="doi">10.5194/acp-18-7827-2018</article-id><title-group><article-title>Aerosol–fog interaction and the transition to well-mixed<?xmltex \hack{\break}?>
radiation fog</article-title><alt-title>Aerosol–fog interaction</alt-title>
      </title-group><?xmltex \runningtitle{Aerosol--fog interaction}?><?xmltex \runningauthor{I.~Boutle et~al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Boutle</surname><given-names>Ian</given-names></name>
          <email>ian.boutle@metoffice.gov.uk</email>
        <ext-link>https://orcid.org/0000-0002-1485-4475</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Price</surname><given-names>Jeremy</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Kudzotsa</surname><given-names>Innocent</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Kokkola</surname><given-names>Harri</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-1404-6670</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Romakkaniemi</surname><given-names>Sami</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-9414-3093</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Met Office, Exeter, UK</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Atmospheric Research Centre of Eastern Finland, Finnish Meteorological Institute, Kuopio, Finland</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Ian Boutle (ian.boutle@metoffice.gov.uk)</corresp></author-notes><pub-date><day>4</day><month>June</month><year>2018</year></pub-date>
      
      <volume>18</volume>
      <issue>11</issue>
      <fpage>7827</fpage><lpage>7840</lpage>
      <history>
        <date date-type="received"><day>16</day><month>August</month><year>2017</year></date>
           <date date-type="rev-request"><day>13</day><month>October</month><year>2017</year></date>
           <date date-type="rev-recd"><day>4</day><month>May</month><year>2018</year></date>
           <date date-type="accepted"><day>17</day><month>May</month><year>2018</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2018 Ian Boutle et al.</copyright-statement>
        <copyright-year>2018</copyright-year>
      <license license-type="open-access"><license-p>This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><self-uri xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018.html">This article is available from https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018.pdf</self-uri>
      <abstract>
    <p id="d1e125">We analyse the development of a radiation fog event and its gradual
transition from optically thin fog in a stable boundary layer to
well-mixed optically thick fog. A comparison of observations and a
detailed large-eddy simulation demonstrate that aerosol growth and
activation is the key process in determining the onset of adiabatic
fog. Weak turbulence and low supersaturations lead to the growth of
aerosol particles which can significantly affect the visibility but
do not significantly interact with the long-wave radiation, allowing
the atmosphere to remain stable. Only when a substantial fraction of
the aerosol activates into cloud droplets can the fog
interact with the radiation, becoming optically thick and
well mixed. Modifications to the parameterisation of cloud droplet
numbers in fog, resulting in lower and more realistic
concentrations, are shown to give significant improvements to an NWP
model, which initially struggled to accurately simulate the
transition. Finally, the consequences of this work for common aerosol
activation parameterisations used in climate models are discussed,
demonstrating that many schemes are reliant on an artificial minimum
value when activating aerosol in fog, and adjustment of this minimum
can significantly affect the sensitivity of the climate system to
aerosol radiative forcing.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <title>Introduction</title>
      <p id="d1e135">Radiation fog is a challenging problem for numerical weather
prediction (NWP) models. To obtain an accurate forecast, models must
correctly represent the coupling between the land surface and
atmosphere, which leads to fog formation, and the coupling between
different atmospheric parameterisations (cloud microphysics,
turbulence, radiation), which determine the evolution of the fog. It is
therefore unsurprising that the quality of NWP fog forecasts remains
low.  Significant advancement in both the physical process
understanding and modelling is required to achieve forecasts of similar quality to those produced for other high-impact weather events.</p>
      <p id="d1e138">Several recent studies have focussed on large-eddy simulation (LES) of foggy
events <xref ref-type="bibr" rid="bib1.bibx3 bib1.bibx22 bib1.bibx20" id="paren.1"/> to investigate the systematic response
of fog to various dynamical and physical processes. All of these studies
showed how quantities such as wind speed, temperature, humidity or
land-surface characteristics, influence the initiation, peak intensity and
dissipation of fog, often in a fairly linear way. However,
<?xmltex \hack{\mbox\bgroup}?><xref ref-type="bibr" rid="bib1.bibx27" id="text.2"/><?xmltex \hack{\egroup}?> showed that fog can undergo more significant
bifurcations in its behaviour. He showed that, for a site in south-eastern
England, approximately 50 % of fog events remained as optically thin
condensed water in a stable boundary layer, whilst the other 50 % formed
optically thick (i.e. zero net surface radiation), well-mixed, adiabatic fog,
with the turbulence generated by radiative cooling giving the fog a distinct
structure of its own. Identifying this transition, and more importantly,
being able to forecast what causes it would be of significant value. Stable
fog generally persists throughout the night-time, dissipating quickly due to
solar heating in the morning. However, adiabatic fog has the ability to
persist for days, greatly increasing its potential to cause disruption to
infrastructure such as road traffic and airports.</p>
      <p id="d1e149">One possible mechanism for this non-linear response could arise from
atmospheric aerosol concentrations and their interaction with the
developing fog layer. <?pagebreak page7828?><xref ref-type="bibr" rid="bib1.bibx4" id="text.3"/> thoroughly studied the effect of
aerosol concentrations and properties on single-column model
simulations of the life cycle of radiation fog. He demonstrated that,
as aerosol concentrations were increased, the fog became deeper, with
higher condensed water content, and was less likely to be dissipated
by solar radiation. Despite the crucial importance of this conclusion
for NWP forecasts, most operational models used for fog prediction do
not consider variable aerosol or fog droplet number concentrations
<xref ref-type="bibr" rid="bib1.bibx14 bib1.bibx33 bib1.bibx35" id="paren.4"><named-content content-type="pre">e.g.</named-content></xref>, and therefore it may be
unsurprising that they struggle to obtain sufficient accuracy.</p>
      <p id="d1e160">The Local and Non-local Fog Experiment <xref ref-type="bibr" rid="bib1.bibx29" id="paren.5"><named-content content-type="pre">LANFEX,</named-content></xref> was a
recent UK attempt to gather new observations of foggy events to make
significant progress in their understanding and modelling. This paper
focusses on the first intensive observation period (IOP1), during
which a shallow, optically thin fog transitioned slowly into a
well-mixed, optically thick fog. This paper aims to extend the work of
<xref ref-type="bibr" rid="bib1.bibx4" id="text.6"/>, investigating the role aerosol plays in this transition
and establishing whether an NWP model is capable of reproducing the
observed behaviour. We discuss the current ability of an NWP model to
reproduce the observations (Sect. <xref ref-type="sec" rid="Ch1.S3"/>), investigate the
mechanisms causing the transition (supplementing the observational
analysis with process modelling from an LES; Sect. <xref ref-type="sec" rid="Ch1.S4"/>) and
evaluate some simple improvements to the NWP model
(Sect. <xref ref-type="sec" rid="Ch1.S5"/>). As we find that one of the key processes is
the representation of aerosol activation within the model, we conclude
(Sect. <xref ref-type="sec" rid="Ch1.S6"/>) with some interesting consequences of this work
for the climate system and climate modelling.</p>
</sec>
<sec id="Ch1.S2">
  <title>Case and model details</title>
      <p id="d1e186">IOP1 took place on the night of 24–25 November 2014 and was measured at the
Met Office field site at Cardington, UK (52.1015<inline-formula><mml:math id="M1" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N,
0.4159<inline-formula><mml:math id="M2" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W). Widespread radiation fog formed across much of the country
and remained stable for much of the night before becoming adiabatic later.
IOP1 was one of the cleanest examples of local fog development observed
during LANFEX, with no evidence that advective or non-local processes were
significant (this has been tested in single-column model simulations with and
without advective forcing; not shown). A detailed set of research-grade
observations are available from the Cardington site, including a 50 <inline-formula><mml:math id="M3" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>
flux tower, radiosonde launches, a cloud droplet probe flown on a tethered
balloon and standard surface and subsurface measurements (see  <xref ref-type="bibr" rid="bib1.bibx29" id="altparen.7"/>, for more
details).</p>
      <p id="d1e218">The NWP model considered in this paper is the Met Office Unified
Model, specifically the 1.5 <inline-formula><mml:math id="M4" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula> horizontal grid-length UKV
model. Details of this model and some discussion of its ability to
forecast fog can be found in <xref ref-type="bibr" rid="bib1.bibx7" id="text.8"/>, although several
aspects of the model dynamics <xref ref-type="bibr" rid="bib1.bibx41" id="paren.9"/>, turbulence
<xref ref-type="bibr" rid="bib1.bibx6" id="paren.10"/> and cloud microphysics <xref ref-type="bibr" rid="bib1.bibx5" id="paren.11"/>
parameterisations have been significantly upgraded. For the simulations
presented, the model is initialised from its own analysis at 12:00 UTC on
24 November 2014 and is free-running after this, forced only at the
boundaries by data from the Met Office global model
<xref ref-type="bibr" rid="bib1.bibx38" id="paren.12"/>. The model contains 70 vertical levels, 6 of which
are below 150 <inline-formula><mml:math id="M5" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> and the lowest of which are at 2.5 <inline-formula><mml:math id="M6" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>
for horizontal winds and 5 <inline-formula><mml:math id="M7" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> for temperature and humidity. As
discussed in <xref ref-type="bibr" rid="bib1.bibx8" id="text.13"/>, the model contains a single-species
prognostic aerosol, which is used in the diagnosis of near-surface
visibility, and converted to cloud droplet number
<xref ref-type="bibr" rid="bib1.bibx40 bib1.bibx26" id="paren.14"/> for use in the radiation and microphysical
parameterisations, i.e. the first and second indirect effects.</p>
      <p id="d1e275">To understand the physical processes leading to the observed
behaviour, we also consider simulations using UCLALES–SALSA
<xref ref-type="bibr" rid="bib1.bibx32" id="paren.15"/> as a process model. This model comprises an LES model
coupled to a detailed, interactive, aerosol–cloud microphysics model
and has been used previously to investigate the role aerosols play in
the development of radiation fog <xref ref-type="bibr" rid="bib1.bibx19" id="paren.16"/>. Within the LES
model, aerosol is partitioned into 10 bins covering the size range
3 <inline-formula><mml:math id="M8" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">nm</mml:mi></mml:mrow></mml:math></inline-formula> to 10 <inline-formula><mml:math id="M9" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>. Water condensation onto aerosol
particles is calculated by numerically solving the condensation
equation at every time step and grid point. Thus we are able to
explicitly simulate how radiative cooling and turbulence affect the
water saturation ratio and how this affects the size of the aerosol
particles. If aerosol becomes activated (i.e. its size exceeds the
critical size given by Köhler theory), it is transferred into a
separate sectional cloud droplet model, with bin sizes matching those
of the dry cloud condensation nuclei and diagnosed wet sizes,
typically between 0.7 and 50 <inline-formula><mml:math id="M10" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>. Thus we do not employ any
traditional parameterisation of activation commonly used in other
models but instead simulate the actual supersaturation and growth of
aerosol particles into droplets. Comparisons with a more detailed
parcel model <xref ref-type="bibr" rid="bib1.bibx18" id="paren.17"/> demonstrate that this growth is solved
with good accuracy for a range of air parcels and updraught velocities.</p>
      <p id="d1e316">For the simulations presented, the LES is initialised at 17:00 UTC with a
radiosonde profile and forced at the surface throughout the simulation with
the observed surface temperatures. This ensures that the simulation remains close
to the observations throughout, avoiding the large uncertainties in the
land-surface model discussed by <xref ref-type="bibr" rid="bib1.bibx20" id="text.18"/>. In this case, the surface
fluxes are very small and typically negative; therefore feedbacks from the
land to atmosphere are not expected to play a great role (although this will
not always be the case, particularly when fluxes are larger and positive).
The domain size is 500 <inline-formula><mml:math id="M11" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 500 <inline-formula><mml:math id="M12" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> in the horizontal with a
4 <inline-formula><mml:math id="M13" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> grid-length and 700 <inline-formula><mml:math id="M14" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> in the vertical with a
1.5 <inline-formula><mml:math id="M15" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> grid-length below 150 <inline-formula><mml:math id="M16" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, above which a stretching
factor of 1.05 is applied. The time step is variable but is typically around
0.25 <inline-formula><mml:math id="M17" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">s</mml:mi></mml:mrow></mml:math></inline-formula> after the turbulence has formed. As such, the cloud activation
within turbulent updraughts is<?pagebreak page7829?> well resolved, occurring on the timescale of a
few seconds. The aerosol distribution was initialised with
1000 <inline-formula><mml:math id="M18" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> number concentration of Aitken-mode aerosols (mean
diameter <inline-formula><mml:math id="M19" display="inline"><mml:mn mathvariant="normal">0.05</mml:mn></mml:math></inline-formula> <inline-formula><mml:math id="M20" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>), 100 <inline-formula><mml:math id="M21" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> accumulation-mode
aerosols (mean diameter <inline-formula><mml:math id="M22" display="inline"><mml:mn mathvariant="normal">0.15</mml:mn></mml:math></inline-formula> <inline-formula><mml:math id="M23" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>) and 2 <inline-formula><mml:math id="M24" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> coarse-mode
aerosols (mean diameter <inline-formula><mml:math id="M25" display="inline"><mml:mn mathvariant="normal">1</mml:mn></mml:math></inline-formula> <inline-formula><mml:math id="M26" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>), each following a log-normal
distribution with standard deviation of 2. Sadly, direct observations of
aerosol concentrations were not available for this case, but this
distribution is representative of the clean air typically found at
Cardington. Several different aerosol concentrations were tested and we
briefly discuss the sensitivity to this choice in the conclusions. During the
simulations, water condensation on cloud droplets is explicitly calculated,
and collision processes between differently sized hydrometeors are also
accounted for. Because radiation fog is relatively thin, and there is no
real precipitation formation, the autoconversion is turned off in the model.
Instead, hydrated aerosol particles and cloud droplets are allowed to
sediment onto the surface. Full details can be found in <xref ref-type="bibr" rid="bib1.bibx32" id="text.19"/> and
references within.</p>
</sec>
<sec id="Ch1.S3">
  <title>NWP model simulations</title>
      <p id="d1e482">The observations (Fig. <xref ref-type="fig" rid="Ch1.F1"/>a) showed
a drop in visibility to <inline-formula><mml:math id="M27" display="inline"><mml:mrow><mml:mo>≈</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M28" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula> as haze and patchy fog
formed just before 18:00 UTC, followed by the continuous onset of thicker
fog just after 20:00 UTC as the visibility dropped to near
100 <inline-formula><mml:math id="M29" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>. The fog persisted for approximately 12 h throughout
the night, clearing at around 08:00 UTC the following morning.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><caption><p id="d1e515">Time series of observations (black) and UKV experiments: control (blue), radiatively inactive cloud (cyan) and modified
droplet number (green), showing <bold>(a)</bold> visibility and
<bold>(b)</bold> grass-surface temperature.</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f01.pdf"/>

      </fig>

      <p id="d1e530">The control UKV shows a very good simulation of the pre-fog
conditions, tracing the observed surface temperature
(Fig. <xref ref-type="fig" rid="Ch1.F1"/>b) almost perfectly until the onset of fog at
20:00 UTC. The model then shows a sharp drop in median visibility, down
to <inline-formula><mml:math id="M30" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">100</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M31" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, at approximately the same time that the
observations show a drop in visibility to similar values. The model
also produced non-zero probabilities of visibility <inline-formula><mml:math id="M32" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M33" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula>
from 18:00 UTC; therefore it appears that the onset of fog, particularly
the timing, is reasonably well reproduced in this model. However,
after the onset of fog, there are noticeable differences between the
model and observations. The model shows a 2 <inline-formula><mml:math id="M34" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi></mml:mrow></mml:math></inline-formula> increase in
surface temperature immediately after the onset of fog, something
which is not apparent in reality. It also appears that the fog is too
thick in the model, with visibilities close to 60 <inline-formula><mml:math id="M35" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, compared
with 200 <inline-formula><mml:math id="M36" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> in the observations. The dissipation of fog also
occurs about 1–1.5 h too early, although this is due
to a bank of mid-level cloud arriving at the location too early in the
model. The cloud causes an increase in downwelling long-wave
radiation, which directly heats the surface and fog layer, causing its
dissipation. In reality, it is difficult to determine whether it was
the presence of this cloud or the onset of downwelling short-wave
radiation after sunrise (08:00 UTC) which caused dissipation, as both
occurred at approximately the same time.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><caption><p id="d1e599">Time series of observations (black), LES (red) and UKV
experiments: control (blue), radiatively inactive cloud (cyan) and
modified droplet number (green), showing <bold>(a)</bold> screen
(1.5 <inline-formula><mml:math id="M37" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>) temperature and <bold>(b)</bold> surface sensible heat
flux.</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f02.pdf"/>

      </fig>

      <p id="d1e622"><?xmltex \hack{\newpage}?>Figure <xref ref-type="fig" rid="Ch1.F2"/> shows the screen temperature and surface sensible heat
flux from the UKV simulation. The sharp rise in surface temperature after the
onset of fog leads to a positive sensible heat flux being formed throughout
the night. Although modest in size (10 <inline-formula><mml:math id="M38" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>), it is in clear
contrast to the observations which remain near zero throughout, and drives a
warming of the screen temperature, which therefore remains warmer than the
observations. Figure <xref ref-type="fig" rid="Ch1.F3"/> shows the effect this has throughout
the boundary layer. The positive heat flux exists through the lowest
50 <inline-formula><mml:math id="M39" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> of the atmosphere before dropping to zero at what is likely to
be the boundary layer top. The observations, by contrast, show a near-zero
flux throughout the depth of the boundary layer. The consequence of this for
the temperature profiles is that reality maintains a stable boundary layer,
whilst the model has a well-mixed temperature profile indicative of an
unstable boundary layer.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><caption><p id="d1e657">Profiles at 22:30 UTC showing observations (mast: black
circles, radiosonde: black line, tethered balloon: grey dots), LES
(red) and UKV experiments: control (blue), radiatively inactive
cloud (cyan) and modified droplet number (green), showing
<bold>(a)</bold> potential temperature and <bold>(b)</bold> sensible heat
flux. Model profiles show model-level data (crosses) and diagnosed
screen and surface-level temperature (filled circles).</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f03.pdf"/>

      </fig>

      <?pagebreak page7830?><p id="d1e672"><?xmltex \hack{\newpage}?>To understand what is going wrong in the model, it is useful to
consider the typical evolution of a real-world radiation fog event,
such as this one. Long-wave radiative cooling of the land surface
gives rise to a stable boundary layer profile, and a thin fog will
form within this profile when the relative humidity reaches
100 %. Initially this fog will only interact weakly with the
environment, allowing the surface and air temperature to continue to
cool and the fog to thicken. It will take several hours for the fog to
start to develop turbulent behaviour of its own. At this point,
long-wave radiative cooling from the fog top will generate negatively
buoyant air parcels, which will descend throughout the fog layer and
generate turbulence. Long-wave emission from the fog layer will also
act to heat the surface, which is now “insulated” from the clear sky
by the fog layer, and this in turn will maintain its temperature or
even allow it to warm, generating a positive surface sensible heat
flux. Upward heat flux from the soil is also a significant contributor
to surface heating once the surface net radiation has reached near
zero <xref ref-type="bibr" rid="bib1.bibx9" id="paren.20"/>. The combination of these processes is what leads
to the development of a well-mixed fog layer, but this process
normally takes many hours. However, the model appears to be simulating
this process almost instantaneously – mature, well-mixed fog is
formed within an hour of fog onset.</p>
      <p id="d1e679">The radiative effect of the fog appears to be a key feature in the process;
therefore as a sensitivity test we turn off the radiative effect of any fog
which forms in the model (i.e. by setting the absorption and scattering
coefficients for condensed water to zero, denoted “No Rad Cld”), shown in
Figs. <xref ref-type="fig" rid="Ch1.F1"/>–<xref ref-type="fig" rid="Ch1.F3"/>. The screen temperature and
sensible heat flux now show a very good agreement with observations, although
the surface temperature is now far too cold and no appreciable fog layer
actually forms; i.e. the visibility remains quite high. This demonstrates
that the radiative feedback is very important in both the development of the
fog and in maintaining the surface temperature. Although fog does form due to
the temperature dropping and relative humidity reaching 100 %, the lack
of any enhanced radiative cooling from the fog itself prevents further
development and thickening of the fog. There are also differences in the
temperature structure between the model and observations. The layer of
enhanced cooling near the surface is <inline-formula><mml:math id="M40" display="inline"><mml:mrow><mml:mo>≈</mml:mo><mml:mn mathvariant="normal">20</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M41" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> deep in reality,
whereas it sits entirely below the lowest model level in the model. This
means that the gradient is much sharper, explaining the colder surface
temperature for given (and approximately correct) free atmospheric
temperatures and screen-level<?pagebreak page7831?> temperature. It is unclear whether this is a
consequence of the fog interaction or the model vertical resolution, as
discussed in <?xmltex \hack{\mbox\bgroup}?><xref ref-type="bibr" rid="bib1.bibx36" id="text.21"/><?xmltex \hack{\egroup}?>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4"><caption><p id="d1e712">Time series of <bold>(a)</bold> surface water deposition rate,
and <bold>(b)</bold> liquid water path, showing observations
(<bold>a</bold> black; <bold>b</bold> tethered balloon: black dots,
radiometer: grey line), LES (red) and UKV experiments: control
(blue), radiatively inactive cloud (cyan) and modified droplet
number (green).</p></caption>
        <?xmltex \igopts{width=233.312598pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f04.pdf"/>

      </fig>

      <p id="d1e733">Whilst having radiatively inactive fog is clearly unrealistic, the
differences in temperature and heat-flux evolution from the control
simulation suggests that perhaps the fog is too radiatively
active. <xref ref-type="bibr" rid="bib1.bibx13" id="text.22"/> showed that errors in the development of
radiation fog can be caused by errors in dew deposition –
depositing too little dew onto the surface leaves too much condensed
water in the atmosphere, which in turn has too strong a radiative
effect. Figure <xref ref-type="fig" rid="Ch1.F4"/>a shows observations of dew deposition
from the instrument described in <xref ref-type="bibr" rid="bib1.bibx28" id="text.23"/> in comparison to the
model. During the main period analysed (20:00 to 04:00 UTC) the
control simulation is in reasonable agreement with the observations –
it is at the lower end of the observational range but certainly
within the uncertainty of the instrument. Before 20:00 UTC, the
control simulation underestimates the deposition, and this is likely
to be due to hygroscopic absorption, a process not accounted for in
the model's surface latent heat flux parameterisation, as discussed in
<xref ref-type="bibr" rid="bib1.bibx28" id="text.24"/>. There is also very shallow and inhomogeneous fog
present in reality at this time, which is not simulated by the model,
as it is only several metres deep and thus below the first model
level, but it will contribute to the observed deposition rate. The
radiatively inactive fog, by contrast, shows almost no deposition
throughout the simulation, and this is due to the fact that no
appreciable fog layer forms in the simulation, and the dominant
(model) process leading to surface dew deposition is sedimentation of
condensed water onto the surface.</p>
      <p id="d1e747">Hence the dew deposition may be slightly underestimated in the
control simulation, but the effect of this will only become
significant if it, in turn, leads to a significant overestimate in
the condensed water content. Figure <xref ref-type="fig" rid="Ch1.F4"/>b shows the liquid
water path (LWP) and Fig. <xref ref-type="fig" rid="Ch1.F5"/>a a profile through the
fog layer from the tethered balloon. The profile shows the kind of
variability which exists in the fog depth and water content and is
not indicative of any fog development between the two observation
times. The control simulation is in reasonable agreement with the
observations for much of the night, although generally at the higher
end of observed variability. The radiatively inactive fog is clearly
too thin when compared to all available observations. Hence it appears
that errors in dew deposition and the evolution of the condensed water
content are not the main causes of error in the radiative effect of
fog. However, the radiative effect of fog is not only controlled by the
liquid water content but also by the number of cloud droplets and
therefore their size. Figure <xref ref-type="fig" rid="Ch1.F5"/>b shows that the
number of droplets observed from the tethered balloon is significantly
lower than those predicted by the model.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5"><caption><p id="d1e758">Profiles at 00:30 UTC showing observations (00:00 UTC: grey,
00:30 UTC: black), LES (red) and UKV experiments: control (blue),
radiatively inactive cloud (cyan) and modified droplet number
(green), showing <bold>(a)</bold> cloud liquid water content and
<bold>(b)</bold> cloud droplet number concentration. For the LES droplet
number, we show only the activated droplets (solid) and all
particles <inline-formula><mml:math id="M42" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M43" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> (dashed).</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f05.pdf"/>

      </fig>

      <p id="d1e793">The model parameterisation <xref ref-type="bibr" rid="bib1.bibx40" id="paren.25"/> uses a fixed value of
75 <inline-formula><mml:math id="M44" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for the droplet concentration at the lowest model
level, tapering up to a value determined by the concentration of
aerosol <xref ref-type="bibr" rid="bib1.bibx26" id="paren.26"/> at 150 <inline-formula><mml:math id="M45" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>. This tapering process is a
pragmatic attempt at representing the fact that cloud droplet numbers in
fog tend to be lower than those observed higher up in the atmosphere
<xref ref-type="bibr" rid="bib1.bibx15 bib1.bibx27" id="paren.27"/>. However, it appears that it is failing to
represent some key features. The droplet numbers in fog are believed to
be low because, despite the abundance of aerosol near the surface from which
cloud droplets could form, the lack of any appreciable updraughts
in the near-surface stable boundary layer results in weak
supersaturations. This prevents the aerosol from being activated and
therefore only relatively few aerosol droplets become hydrated. The
observations also show the droplet numbers to be approximately
constant throughout the fog layer, whilst the model's (imposed)
profile increases quickly with height from its surface value, due to
the large value diagnosed higher up from the aerosol concentration.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6"><caption><p id="d1e830">Time series of surface downwelling long-wave radiation,
showing observations (black), LES (red) and UKV experiments: control
(blue), radiatively inactive cloud (cyan) and modified droplet
number (green).</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f06.pdf"/>

      </fig>

      <?pagebreak page7832?><p id="d1e839">The abundance of small cloud drops in the model will increase the
cloud absorptivity, making the fog optically thicker and more
radiatively important. This will drive stronger radiative cooling from
the fog top, enhancing the turbulence and causing the development of
well-mixed fog. It will also increase the downwelling long-wave
radiation at the surface, which will in turn heat the surface and
drive a positive sensible heat flux. However, observations of
downwelling long-wave radiation (Fig. <xref ref-type="fig" rid="Ch1.F6"/>) are not
available for much of the night due to ice formation on the dome of
the radiometer rendering the measurements unusable. The initial rise
in downwelling long-wave radiation (between 20:30 and 23:00 UTC,
before the ice formed) is representative of the fog, and it would not
be unreasonable to assume that values remained near
270 <inline-formula><mml:math id="M46" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> throughout the night, perhaps increasing
slightly as the fog developed. Therefore the model would appear to
have excessive downwelling long-wave radiation, but at this point we shall
appeal to the additional information that can be provided by the LES
model to support this conclusion.</p>
</sec>
<sec id="Ch1.S4">
  <title>LES analysis</title>
      <p id="d1e867">Figures <xref ref-type="fig" rid="Ch1.F2"/>–<xref ref-type="fig" rid="Ch1.F6"/> also showed results from the
LES, which generally appear to be in good agreement with the
observations, demonstrating that the LES is a representative proxy for
reality. They also confirm that the low cloud droplet number
(Fig. <xref ref-type="fig" rid="Ch1.F5"/>b) is responsible for a much lower
downwelling long-wave radiation (Fig. <xref ref-type="fig" rid="Ch1.F6"/>) than is simulated
by the UKV. The LES also provides the opportunity to explore the
mechanisms leading to cloud droplet activation (or lack thereof) in
the fog and therefore to suggest improvements to the NWP model.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7"><caption><p id="d1e880">Time series of vertical velocity variance at screen level
(2 <inline-formula><mml:math id="M47" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>), showing observations (black), LES (red) and UKV
experiments: control (blue), radiatively inactive cloud (cyan)
and modified droplet number (green). Also shown are the
<xref ref-type="bibr" rid="bib1.bibx29" id="text.28"/> value above which fog will not form (dashed) and
the minimum value used in most activation parameterisations (dotted).</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f07.pdf"/>

      </fig>

      <p id="d1e900">Figure <xref ref-type="fig" rid="Ch1.F7"/> shows the near-surface vertical velocity variance, which
is very low in the observations and all models. Indeed it is safely below the
0.005 <inline-formula><mml:math id="M48" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> suggested in <xref ref-type="bibr" rid="bib1.bibx29" id="text.29"/> for the threshold
value above which fog will not form. What this implies is that the peak
updraught speed driving aerosol activation is very low, typically
<inline-formula><mml:math id="M49" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.1</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M50" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">ms</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. This is<?pagebreak page7833?> much lower than the typical updraught speeds
found in “normal” clouds (i.e. those which do not contain a rigid surface
at their lower boundary). Because most models do not prognose or diagnose
supersaturation, most aerosol activation parameterisations
<xref ref-type="bibr" rid="bib1.bibx11 bib1.bibx23 bib1.bibx39" id="paren.30"><named-content content-type="pre">e.g.</named-content></xref> link this updraught speed directly to the
number of activated droplets. However, these parameterisations were not
developed in the weak updraught regime of radiation fog, instead typically
imposing a minimum updraught velocity or standard deviation of
0.1 <inline-formula><mml:math id="M51" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">ms</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> or higher. Therefore, if any schemes like this are used
to simulate aerosol activation in fog, they will systematically overestimate
the amount of aerosol activation and therefore the cloud droplet number,
with inevitable consequences such as those discussed in Sect. <xref ref-type="sec" rid="Ch1.S3"/>.</p>
      <p id="d1e974">For fog formation, updraughts are obviously not the only process that
will activate aerosol and lead to the formation of cloud droplets. The
fundamental process which drives activation is the ambient
supersaturation, driven by adiabatic cooling, which can be driven by
updraughts but in fog is also driven by direct cooling of the
atmosphere. The observed cooling rate during the first few hours of
fog formation (Fig. <xref ref-type="fig" rid="Ch1.F2"/>a) is 1 <inline-formula><mml:math id="M52" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">h</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, which
would be equivalent to an updraught speed of 0.04 <inline-formula><mml:math id="M53" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">ms</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>
assuming a temperature lapse rate of 6.5 <inline-formula><mml:math id="M54" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">km</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. This is
still significantly below the 0.1 <inline-formula><mml:math id="M55" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">ms</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> minimum used for
aerosol activation (even when added to the observed turbulent vertical
velocities), demonstrating that typical parameterisations do not even
indirectly represent the physical processes or amount of aerosol
activation correctly. Further work is clearly warranted to develop
schemes which are appropriate for this regime.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8"><caption><p id="d1e1044">Time–height contour plot from the LES showing water vapour
supersaturation with respect to the saturation vapour pressure over
liquid water.</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f08.pdf"/>

      </fig>

      <p id="d1e1053">Figure <xref ref-type="fig" rid="Ch1.F8"/> shows the supersaturation as predicted by
the LES throughout the simulation. The first point to note is that the
values are very low, <inline-formula><mml:math id="M56" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.1</mml:mn></mml:mrow></mml:math></inline-formula> %, which is much lower than values
typically found in clouds (0.3–1 %, <xref ref-type="bibr" rid="bib1.bibx11" id="author.31"/>,
<xref ref-type="bibr" rid="bib1.bibx11" id="year.32"/>; 0.2–1.5 %, <xref ref-type="bibr" rid="bib1.bibx31" id="author.33"/>,
<xref ref-type="bibr" rid="bib1.bibx31" id="year.34"/>). Low supersaturation values are also supported by
earlier observations in different fog campaigns. For example, in the
ParisFog campaign in France, the maximum effective supersaturation was
found to be less than 0.05 %, with the average activation diameter
of particles between 350 and 450 <inline-formula><mml:math id="M57" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">nm</mml:mi></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx16" id="paren.35"/>. Similar
findings were also obtained in the Po Valley, Italy, highlighting the
role of aerosol chemical composition <xref ref-type="bibr" rid="bib1.bibx12" id="paren.36"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F9"><caption><p id="d1e1097">Cloud droplet size spectra at <bold>(a)</bold> 00:30 UTC and
<bold>(b)</bold> 03:30 UTC, showing observations (black) and LES
(red). For the LES, we also show the number of activated drops
(blue) and number of aerosol particles (green).</p></caption>
        <?xmltex \igopts{width=233.312598pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f09.pdf"/>

      </fig>

      <p id="d1e1112">These low supersaturation values explain the very low levels of
aerosol activation and therefore low cloud droplet number
values. Figure <xref ref-type="fig" rid="Ch1.F9"/> shows the size spectra of
particles <inline-formula><mml:math id="M58" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M59" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, which shows that there are large
numbers of very small particles (<inline-formula><mml:math id="M60" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M61" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>) in both the
observations and LES. It is likely that these particles are not
activated cloud drops, but large aerosol particles which have absorbed
water and swollen in size. We note here that we have excluded the
lowest (1–2 <inline-formula><mml:math id="M62" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>) bin of the cloud droplet probe from our
analysis to avoid potential noise issues with large, dry aerosol
affecting the numbers. Because of the low supersaturation and therefore
high activation diameter, hydrated aerosol particles within fog can
grow larger than micrometre in size and can contribute up to 68 %
of total light scattering during different fog periods
<xref ref-type="bibr" rid="bib1.bibx16 bib1.bibx10" id="paren.37"/>. However, most of these hydrated particles
are still too small to<?pagebreak page7834?> considerably affect interaction with long-wave
radiation after fog has developed. This explains how the visibility
can become so low, and yet the fog remains optically thin and the
boundary layer stable.</p>
      <p id="d1e1171">The LES allows us to analyse this further, because we can break the
size spectra into their contributions from hydrated particles which
are still in the LES aerosol classes and particles which have been
activated into the LES cloud droplet classes, i.e. exceeded the
critical size given by Köhler theory. As shown in
Fig. <xref ref-type="fig" rid="Ch1.F9"/>, almost all particles in the LES with
diameter <inline-formula><mml:math id="M63" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">6</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M64" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> are wet aerosol, and only those with
diameter <inline-formula><mml:math id="M65" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">6</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M66" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> are activated cloud drops. This
distinction can also be seen in profiles of the cloud droplet number
(Figs. <xref ref-type="fig" rid="Ch1.F5"/>b and <xref ref-type="fig" rid="Ch1.F10"/>b), where we have
shown both the LES results for all particles <inline-formula><mml:math id="M67" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M68" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> (as
measured by the cloud droplet probe) and only those which are
activated cloud drops. There is approximately a factor of 2
difference between these two estimates of cloud droplet number, with
the all-particle estimate comparing best with the observations. In the
simulation, aerosol is assumed to be composed of ammonium sulfate,
which might be more hygroscopic than the actual aerosol observed
during IOP1. Less hygroscopic aerosol would have a lower growth factor
within fog, and thus the transition from hydrated aerosol to activated
fog droplets would be seen at a smaller diameter. However, less
hygroscopic aerosol would also activate less efficiently, thus
increasing the critical dry diameter of activating particles. Thus we
are confident that the small droplets seen in the observations are not
fully activated but are significantly hydrated aerosol. This suggests
that many observational estimates of fog droplet number, particularly
in clean air masses, could actually be overestimating the number of
activated droplets (i.e. those that are radiatively important in the long wave).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F10"><caption><p id="d1e1244">Profiles at 03:30 UTC showing observations, LES (red) and
UKV experiments: control (blue), radiatively inactive cloud (cyan)
and modified droplet number (green), showing <bold>(a)</bold> potential
temperature and <bold>(b)</bold> cloud droplet number
concentration. Model profiles show model-level data (crosses) and
diagnosed screen and surface-level temperature (filled circles). For
the LES droplet number, we show only the activated droplets (solid)
and all particles <inline-formula><mml:math id="M69" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M70" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> (dashed).</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f10.pdf"/>

      </fig>

      <p id="d1e1279">The supersaturation and turbulence levels remain remarkably constant
throughout the night (up to 04:00 UTC), resulting in a cloud droplet
number concentration which also remains reasonably constant throughout
the night (Figs. <xref ref-type="fig" rid="Ch1.F5"/>b
and <xref ref-type="fig" rid="Ch1.F10"/>b). This implies that the downwelling long-wave
radiation (and optical depth) of the fog is mainly driven by its
physical depth, which grows throughout the night (see
Fig. <xref ref-type="fig" rid="Ch1.F8"/>). The growth of the fog layer leads to a
gradual but continuous increase in the downwelling long-wave
radiation throughout the night (Fig. <xref ref-type="fig" rid="Ch1.F6"/>), with the
exception of a small decrease around 02:00 UTC. This occurs because
of a sharp decrease in the background specific humidity (not shown) at
around 80 <inline-formula><mml:math id="M71" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, and therefore the fog growth is temporarily
inhibited due to the entrainment of this drier air. This gradual rise
in the downwelling long-wave radiation is responsible for the surface
temperature ceasing to cool by 02:00 UTC and slowly warming
throughout the rest of the night, which in turn drives a slow
transition towards a well-mixed fog layer.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F11" specific-use="star"><caption><p id="d1e1300">Visibility forecasts from 00:00 UTC on 10 February 2015 at
3 h intervals from the UKV control <bold>(a)</bold> and with
modified droplet number <bold>(b)</bold>. Filled circles show
observations.</p></caption>
        <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f11.pdf"/>

      </fig>

      <p id="d1e1315">Figure <xref ref-type="fig" rid="Ch1.F10"/> shows that by 03:30 UTC, the surface is
warmer than the near surface and the lowest 20 <inline-formula><mml:math id="M72" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> of the
atmosphere is well mixed, with the top portion of the fog layer remaining
stable. It is interesting to note that once the fog becomes adiabatic,
the mixed layer temperature is very similar to that predicted by the
control NWP model, although the NWP model mixed layer is much deeper
because it has been developing for many hours. This can also be seen
by the convergence of screen temperature in all models around
04:00 UTC in Fig. <xref ref-type="fig" rid="Ch1.F2"/>a. After this time, the updraught
speeds within the fog begin to grow, leading to increased droplet
activation and a rise the observed and LES cloud droplet
numbers. Figure <xref ref-type="fig" rid="Ch1.F9"/>b shows a small secondary peak in the
size spectra around <inline-formula><mml:math id="M73" display="inline"><mml:mn mathvariant="normal">10</mml:mn></mml:math></inline-formula> <inline-formula><mml:math id="M74" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, developing due to the
increasing turbulence, and the evolution of the spectra and cloud
droplet numbers after this point is very similar to that already
reported in <xref ref-type="bibr" rid="bib1.bibx27" id="text.38"/> and <xref ref-type="bibr" rid="bib1.bibx32" id="text.39"/>; hence we do not focus on
it here. The well-mixed layer continues to grow throughout the night,
until the entire fog layer is well mixed and turbulent by 08:00 UTC.</p>
</sec>
<sec id="Ch1.S5">
  <title>NWP model improvement</title>
      <p id="d1e1363">To test whether improving the representation of aerosol activation
would improve the simulation of fog in the NWP model, we make a simple
adjustment to the cloud droplet profile used in the UKV (denoted
“Drop Taper”). Instead of tapering from a fixed value
(75 <inline-formula><mml:math id="M75" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>) at the surface to the aerosol-dependent value at
150 <inline-formula><mml:math id="M76" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, we keep the droplet number fixed throughout the lowest
50 <inline-formula><mml:math id="M77" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> of the atmosphere, before tapering towards the aerosol
value above this. This is motivated by the observations and LES
results, which show<?pagebreak page7835?> that the cloud droplet number is reasonably
uniform throughout the fog layer. We also reduce the fixed value used
in the lowest 50 <inline-formula><mml:math id="M78" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> to 50 <inline-formula><mml:math id="M79" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, which is more
representative of the observations, although still possibly too
high. Clearly this choice is likely to be location and case specific
and requires some adjustments for more polluted locations as discussed
in <xref ref-type="bibr" rid="bib1.bibx17" id="text.40"/>. A universal parameterisation would require some link
to aerosol.</p>
      <p id="d1e1422">Figures <xref ref-type="fig" rid="Ch1.F1"/>–<xref ref-type="fig" rid="Ch1.F7"/> and <xref ref-type="fig" rid="Ch1.F10"/> show
the results from this simulation and demonstrate that improvement is
possible. The downwelling long-wave radiation (Fig. <xref ref-type="fig" rid="Ch1.F6"/>)
now remains much lower throughout the night, which allows the surface
to remain cool and the sensible heat flux to remain near zero
(Fig. <xref ref-type="fig" rid="Ch1.F2"/>). The model can maintain a stable atmospheric
temperature profile for the early part of the night
(Fig. <xref ref-type="fig" rid="Ch1.F3"/>a), and eventually it transitions to a
well-mixed profile (Fig. <xref ref-type="fig" rid="Ch1.F10"/>a). Therefore, it would
appear that by having a realistic estimate of cloud droplet numbers in
fog we can significantly improve NWP fog simulations.</p>
      <p id="d1e1440">The mechanisms by which this improvement occur are twofold. Firstly,
the reduced cloud droplet number increases the bulk sedimentation
rate, which is calculated via Stokes Law <xref ref-type="bibr" rid="bib1.bibx40" id="paren.41"/>. This
increases the rate at which condensed water is removed from the fog
layer onto the surface, physically thinning the fog layer, i.e. the
LWP is reduced. This is shown in Fig. <xref ref-type="fig" rid="Ch1.F4"/>, where the LWP is
approximately halved, yet the water deposition rate (which is almost
entirely droplet settling) is largely unchanged. Secondly, the
increased effective radius, which comes from reducing the cloud
droplet number, reduces the cloud absorptivity to upwelling long-wave
radiation <xref ref-type="bibr" rid="bib1.bibx30" id="paren.42"/>. This allows more radiation to be emitted to
space, reducing the effectiveness of the fundamental process by which
radiation fog develops – long-wave emission from the fog itself
(Fig. <xref ref-type="fig" rid="Ch1.F6"/>), which is proportional to the
absorption. Cooling from the fog top is less efficient at turbulence
production, and downwelling long-wave radiation from the fog is less
efficient at heating the surface (and thus enabling surface-driven
turbulence to form). Both of these processes inhibit the transition to
well-mixed fog. The radiatively inactive cloud experiment is an
extreme example of this effect.</p>
      <p id="d1e1453">Given the simple nature of the aerosol representation in the UKV and
the current method of calculating cloud droplet numbers from this, the
solution proposed above may actually be a suitable candidate for
operational NWP implementation over the UK. To evaluate this, we run a
month-long trial of the full data assimilation and forecast system for
February 2015 with four forecasts per day (00:00, 06:00, 12:00,
18:00 UTC), each 36 h in length. This represented a typical UK
winter, comprising periods of high pressure with calm, potentially
foggy conditions, and periods of westerly flow bringing low-pressure
frontal systems across the country. The headline result is a small
improvement across all measures of forecast skill (wind speed,
temperature, cloud cover, precipitation, visibility). One of the more
interesting changes was a non-negligible improvement in screen
temperature forecasts. Despite the fact that there were only
relatively few foggy days during the month, the screen temperature
error (similar to Fig. <xref ref-type="fig" rid="Ch1.F2"/>a) is so great when fog is
present, that improvements to this can be seen in the mean temperature
error across the entire month.</p>
      <?pagebreak page7836?><p id="d1e1459">The main improvements, however, are seen in surface visibility
forecasts, such as those shown in Fig. <xref ref-type="fig" rid="Ch1.F11"/>. The figure
shows a widespread fog event over central and southern England on
10 February 2015. The fog onset occurs around 01:00 UTC in the
observations, and both forecasts reproduce this reasonably
well. However, once the fog is formed in the control simulation, it is
instantly thick, well-mixed fog with visibilities <inline-formula><mml:math id="M80" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">50</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M81" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>,
symptomatic of the problems discussed in Sect. <xref ref-type="sec" rid="Ch1.S3"/>. This is
not observed in reality, with many stations reporting visibilities
nearer to 100 <inline-formula><mml:math id="M82" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>. The control simulation maintains these low
visibilities throughout the night as the fog moves across the
country. By 09:00 UTC, the fog is dissipating in most places in
reality, whilst the model retains a large area of thick fog with very
low visibility.</p>
      <p id="d1e1492">With the revised droplet taper, the onset and dissipation phases of
the fog event are improved. The fog onset is slower, with visibilities
around 100 <inline-formula><mml:math id="M83" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> forecast at 03:00 UTC, in general agreement with
the observations. By 06:00 UTC, the fog has thickened, becoming
well mixed and with visibilities in places falling below
50 <inline-formula><mml:math id="M84" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>. Whilst this is still too thick compared to the
observations, it is certainly much better than the control. By
09:00 UTC, the fog has started to dissipate in the model, with
visibilities rising, again in better agreement with the observations.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F12"><caption><p id="d1e1513">NWP model verification of visibility from 5 February to
5 March 2015 utilising all observations and forecasts (4 per day)
over UK land areas. Panels show the equitable threat score (ETS),
frequency bias, probability of detection and probability of false
detection, for a visibility threshold of 200 <inline-formula><mml:math id="M85" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>, from the UKV
control (blue) and with modified droplet number (green).</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f12.pdf"/>

      </fig>

      <p id="d1e1530">Figure <xref ref-type="fig" rid="Ch1.F12"/> provides more quantitative support for these
conclusions, presenting categorical verification of all forecasts in
the trial period against all available surface observations. Following
<xref ref-type="bibr" rid="bib1.bibx21" id="text.43"/>, we define a 2 <inline-formula><mml:math id="M86" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 2 contingency table such that
<inline-formula><mml:math id="M87" display="inline"><mml:mi>a</mml:mi></mml:math></inline-formula> is the number of hits, <inline-formula><mml:math id="M88" display="inline"><mml:mi>b</mml:mi></mml:math></inline-formula> is the number of false alarms, <inline-formula><mml:math id="M89" display="inline"><mml:mi>c</mml:mi></mml:math></inline-formula> is
the number of misses and <inline-formula><mml:math id="M90" display="inline"><mml:mi>d</mml:mi></mml:math></inline-formula> is the number of correct negatives. We
then determine the equitable threat score (ETS) as <inline-formula><mml:math id="M91" display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:mi>a</mml:mi><mml:mo>-</mml:mo><mml:mi>X</mml:mi><mml:mo>)</mml:mo><mml:mo>/</mml:mo><mml:mo>(</mml:mo><mml:mi>a</mml:mi><mml:mo>-</mml:mo><mml:mi>X</mml:mi><mml:mo>+</mml:mo><mml:mi>b</mml:mi><mml:mo>+</mml:mo><mml:mi>c</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>
where <inline-formula><mml:math id="M92" display="inline"><mml:mrow><mml:mi>X</mml:mi><mml:mo>=</mml:mo><mml:mo>(</mml:mo><mml:mi>a</mml:mi><mml:mo>+</mml:mo><mml:mi>b</mml:mi><mml:mo>)</mml:mo><mml:mo>(</mml:mo><mml:mi>a</mml:mi><mml:mo>+</mml:mo><mml:mi>c</mml:mi><mml:mo>)</mml:mo><mml:mo>/</mml:mo><mml:mo>(</mml:mo><mml:mi>a</mml:mi><mml:mo>+</mml:mo><mml:mi>b</mml:mi><mml:mo>+</mml:mo><mml:mi>c</mml:mi><mml:mo>+</mml:mo><mml:mi>d</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, the frequency bias as <inline-formula><mml:math id="M93" display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:mi>a</mml:mi><mml:mo>+</mml:mo><mml:mi>b</mml:mi><mml:mo>)</mml:mo><mml:mo>/</mml:mo><mml:mo>(</mml:mo><mml:mi>a</mml:mi><mml:mo>+</mml:mo><mml:mi>c</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>,
probability of detection (hit rate) as <inline-formula><mml:math id="M94" display="inline"><mml:mrow><mml:mi>a</mml:mi><mml:mo>/</mml:mo><mml:mo>(</mml:mo><mml:mi>a</mml:mi><mml:mo>+</mml:mo><mml:mi>c</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> and the probability of
false detection (false alarm rate) as <inline-formula><mml:math id="M95" display="inline"><mml:mrow><mml:mi>b</mml:mi><mml:mo>/</mml:mo><mml:mo>(</mml:mo><mml:mi>a</mml:mi><mml:mo>+</mml:mo><mml:mi>b</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>. Perfect scores are 1
for the ETS, frequency bias and probability of detection, and 0 for
the probability of false detection. In Fig. <xref ref-type="fig" rid="Ch1.F12"/> we
consider the 200 <inline-formula><mml:math id="M96" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula> threshold for visibility, although results
are similar at other thresholds (e.g. 1 <inline-formula><mml:math id="M97" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula>). As shown, the
control simulation was overforecasting low-visibility events, with a
frequency bias <inline-formula><mml:math id="M98" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> and a probability of false
detection <inline-formula><mml:math id="M99" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">0</mml:mn></mml:mrow></mml:math></inline-formula>. Including the modified drop taper has clearly
improved both of these metrics. Importantly, it has done this without
significantly degrading the probability of detection, which remains
largely unchanged, and therefore the ETS is improved. These results
are consistent with the main results from IOP1 and the case study
from this trial period is presented in Fig. <xref ref-type="fig" rid="Ch1.F11"/>. The control
simulation produces fog which is too thick, too fast and tends to
persist for too long; i.e. it overforecasts. By improving the droplet
numbers, this behaviour is improved and can be seen in the
statistical analysis.</p>
      <p id="d1e1772">Therefore, although not a panacea, the changes presented here
certainly present a useful improvement in fog modelling and
highlight that an accurate representation of aerosol and its interaction
with fog are key challenges for NWP. Future work should look to
link the near-surface droplet number to aerosol for a more complete
and globally universal solution.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F13" specific-use="star"><caption><p id="d1e1778"><bold>(a)</bold> 20-year mean cloud droplet number concentration
at the lowest model level (20 <inline-formula><mml:math id="M100" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi></mml:mrow></mml:math></inline-formula>) from an atmosphere only
simulation of HadGEM3-GA7. <bold>(b)</bold> The difference from this
when reducing the minimum updraught speed used for aerosol activation
from 0.1 to 0.01 <inline-formula><mml:math id="M101" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">ms</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>.</p></caption>
        <?xmltex \igopts{width=497.923228pt}?><graphic xlink:href="https://acp.copernicus.org/articles/18/7827/2018/acp-18-7827-2018-f13.pdf"/>

      </fig>

</sec>
<sec id="Ch1.S6" sec-type="conclusions">
  <title>Conclusions</title>
      <p id="d1e1820">The manner in which atmospheric aerosol concentrations influence the
number and size of fog droplets created in a typical radiation fog
event, and how this influences the development of the fog, has been
discussed. For given aerosol concentrations, the number of activated
droplets is much lower in fog than usually found in clouds, due to the
absence of strong updraughts to force cooling of air parcels. Instead,
the activation of droplets relies on the very slow radiative cooling
of the air, which creates small supersaturations, resulting in
relatively few droplets becoming activated. The consequence of this
for fog development is that fog can remain optically thin for many
hours, relying on the physical growth of the fog<?pagebreak page7837?> layer to increase its
optical depth and force the transition to well-mixed fog with a
turbulent structure of its own. We can therefore summarise that key
factors affecting the development of well-mixed fog include (i) the
amount of time available for development before sunrise, i.e. the
length of the night and how soon after sunset the first fog forms;
(ii) the speed with which the fog layer can deepen, strongly governed
by the humidity profile – a moist environment will allow the fog to
grow quicker and transition faster; and (iii) the amount of
accumulation and coarse-mode aerosol present for activation, as
sensitivity tests with the LES demonstrated that considerably
increasing the initial concentrations of larger aerosol lead to a
faster transition to well-mixed fog. Non-local effects and advection
are other factors that have not been discussed in this work but are
likely to be important.</p>
      <p id="d1e1823">We have shown that accurate prediction of fog droplet number
concentrations is crucially important to the accurate simulation of
radiation fog. Excessive number concentrations, and therefore droplets
which are too small, too radiatively important and do not sediment out
fast enough, quickly lead to the fog becoming optically thick and
well mixed, in stark contrast to the observations. This may appear to
contradict the results of <xref ref-type="bibr" rid="bib1.bibx20" id="text.44"/>, who find little effect on
their simulations from changing the droplet number
concentration. However, we believe their results are broadly
consistent with our own. The simulations presented in <xref ref-type="bibr" rid="bib1.bibx20" id="text.45"/>
transition rapidly to well-mixed fog, i.e. within 30 min of the
first onset of fog. Therefore, their simulation is very similar to our
control simulation, and their sensitivity studies explore a range of
droplet numbers (100–200 <inline-formula><mml:math id="M102" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>) similar to our control
simulation. Our observations and LES show droplet numbers much lower than
this range (<inline-formula><mml:math id="M103" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">50</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M104" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>), and it is only when we reduce the
droplet numbers to this value that we achieve a simulation with a slow
transition to well-mixed fog. It is also worth noting that the
observations on which the <xref ref-type="bibr" rid="bib1.bibx20" id="text.46"/> simulations are based also
present a slow transition to well-mixed fog (approximately 5 h
from the first onset), and so it would be interesting rerun their
case with a much lower droplet concentration to see if the simulated
transition can be improved.</p>
      <p id="d1e1874">This threshold-type behaviour occurs because once the fog has become
optically thick, further changes to the cloud droplet number do little
to affect the surface radiation balance and therefore fog
development. It is only when the model can simulate fog in an
optically thin (i.e. upwelling and downwelling long-wave radiation not
in balance) and turbulently stable state, that the droplet number
has a greater influence as it can determine when the transition
between these states occurs. We believe that these results and
suggested model improvements should be applicable to any NWP model,
provided that the parameterisations of droplet settling and long-wave
cloud absorption correctly depend on the droplet number/size and so
are keen to conduct an intercomparison of NWP models for a fog case
like this to investigate these (and other) sensitivities.</p>
      <p id="d1e1877">Whilst we have shown that the use of a simple approach to represent low
droplet numbers in fog can lead to useful improvements in NWP skill,
this work has highlighted a key issue which has been overlooked in
many NWP and climate models – how aerosol activation and droplet
numbers in fog are calculated. More complex parameterisations of
aerosol activation, such as <xref ref-type="bibr" rid="bib1.bibx1" id="text.47"/>, are based around the
strength of updraughts. Yet in this paper, we have shown that the
minimum updraught speed often used in these parameterisations is
considerably larger than those found in<?pagebreak page7838?> radiation fog, and the
radiative cooling of the atmosphere is not sufficient to account for
this discrepancy. Therefore, it is likely that most models using these
types of activation parameterisation produce excessive aerosol
activation in their lowest model levels.</p>
      <p id="d1e1884">Poor representation of aerosol activation has notable consequences for
climate models and their simulation of the aerosol effective radiative
forcing of the climate system <xref ref-type="bibr" rid="bib1.bibx25" id="paren.48"/>. Figure <xref ref-type="fig" rid="Ch1.F13"/>a shows
the in-cloud mean cloud droplet number concentration in the lowest model
level of a 20-year present-day climate simulation using the Met Office
climate model HadGEM3-GA7 <xref ref-type="bibr" rid="bib1.bibx37" id="paren.49"/>. Throughout most of the Northern
Hemisphere land masses, when fog is present, the predicted droplet numbers
are in excess of 150 <inline-formula><mml:math id="M105" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, with peak values over
250 <inline-formula><mml:math id="M106" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. This model is typical of many climate models in using
the <xref ref-type="bibr" rid="bib1.bibx1" id="text.50"/> activation parameterisation with a minimum updraught speed
of 0.1 <inline-formula><mml:math id="M107" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">ms</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. Based on the results of Sect. <xref ref-type="sec" rid="Ch1.S4"/>,
Fig. <xref ref-type="fig" rid="Ch1.F13"/>b presents a sensitivity test where this minimum value
is reduced to 0.01 <inline-formula><mml:math id="M108" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">ms</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. As shown, there is a widespread reduction
in the fog droplet number, by up to 50–100 <inline-formula><mml:math id="M109" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">cm</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> in many regions.</p>
      <p id="d1e1973">Figure <xref ref-type="fig" rid="Ch1.F13"/> demonstrates that an artificial numerical minimum in
the aerosol activation code is actually responsible for a large proportion of
near-surface aerosol activation in HadGEM3-GA7. There is also potentially a
significant impact on the climate system from this process, as the regions
where the activation is happening are also predominantly the regions where
the aerosol concentrations have grown most significantly throughout the
20th century. To quantify this, we rerun the simulations with pre-industrial
aerosol concentrations, allowing us to estimate the effective radiative
forcing following the method of <xref ref-type="bibr" rid="bib1.bibx2" id="text.51"/>. The results show that reducing
the minimum updraught speed reduces (i.e. makes less negative) the aerosol
effective radiative forcing by 0.1 <inline-formula><mml:math id="M110" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. This is not an
insignificant change from a process which has been largely unconsidered by
climate models to date. Whilst it is beyond the scope of the current paper to
evaluate these changes to HadGEM3-GA7 (this will be done in
<xref ref-type="bibr" rid="bib1.bibx24" id="altparen.52"/>), it is clear that the representation of fog processes in
climate models is an area warranting further attention with high priority.
<xref ref-type="bibr" rid="bib1.bibx34" id="text.53"/> showed that recent reductions in fog occurrence over Europe
are a significant contributor to surface temperature warming, and therefore
missing or misrepresenting this process in climate projections is
problematic.</p>
</sec>

      
      </body>
    <back><notes notes-type="dataavailability">

      <p id="d1e2008">All data used in this study are available from the
authors upon request.</p>
  </notes><notes notes-type="competinginterests">

      <p id="d1e2014">The authors declare that they have no conflict of
interest.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e2020">Ian Boutle and Jeremy Price thank the UK Civil Aviation Authority
for providing some funding towards this research. Innocent Kudzotsa,
Harri Kokkola and Sami Romakkaniemi are supported by the Academy of
Finland (project nos. 283031 and 285068, and the Centre of Excellence in
Atmospheric Science, no. 272041). We also thank Adrian Hill for many
inspiring discussions on aerosol activation in fog and two
reviewers whose comments significantly improved the quality of the
manuscript.<?xmltex \hack{\newline}?><?xmltex \hack{\newline}?>
Edited by: Yafang Cheng<?xmltex \hack{\newline}?>
Reviewed by: Thierry Bergot and one anonymous referee</p></ack><ref-list>
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aerosol particles which can significantly affect the visibility but
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model, which initially struggled to accurately simulate the
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activation parameterisations used in climate models are discussed,
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value when activating aerosol in fog, and adjustment of this minimum
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