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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-26-8367-2026</article-id><title-group><article-title>Impacts of entrainment on secondary ice production in deep convective clouds</article-title><alt-title>Impacts of entrainment on secondary ice production in deep convective clouds</alt-title>
      </title-group>
      <contrib-group>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Portman</surname><given-names>Bowen Z.</given-names></name>
          
        <ext-link>https://orcid.org/0009-0003-0181-3425</ext-link></contrib>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Connolly</surname><given-names>Paul J.</given-names></name>
          <email>paul.connolly@manchester.ac.uk</email>
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Blyth</surname><given-names>Alan M.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-7115-2587</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>James</surname><given-names>Rachel L.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-5587-6590</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff3">
          <name><surname>Wu</surname><given-names>Huihui</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-6469-2892</ext-link></contrib>
        <aff id="aff1"><label>1</label><institution>Department of Earth and Environmental Sciences, The University of Manchester, Manchester, UK</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>National Centre for Atmospheric Science, University of Leeds, Leeds, UK</institution>
        </aff>
        <aff id="aff3"><label>a</label><institution>now at: Univ Paris Est Créteil and Université Paris Cité, CNRS, LISA, 94010 Créteil, France</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Paul J. Connolly (paul.connolly@manchester.ac.uk)</corresp></author-notes><pub-date><day>16</day><month>June</month><year>2026</year></pub-date>
      
      <volume>26</volume>
      <issue>11</issue>
      <fpage>8367</fpage><lpage>8385</lpage>
      <history>
        <date date-type="received"><day>21</day><month>January</month><year>2026</year></date>
           <date date-type="rev-request"><day>11</day><month>February</month><year>2026</year></date>
           <date date-type="rev-recd"><day>14</day><month>May</month><year>2026</year></date>
           <date date-type="accepted"><day>18</day><month>May</month><year>2026</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2026 Bowen Z. Portman et al.</copyright-statement>
        <copyright-year>2026</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/26/8367/2026/acp-26-8367-2026.html">This article is available from https://acp.copernicus.org/articles/26/8367/2026/acp-26-8367-2026.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/26/8367/2026/acp-26-8367-2026.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/26/8367/2026/acp-26-8367-2026.pdf</self-uri>
      <abstract><title>Abstract</title>

      <p id="d2e131">The accurate representation of secondary ice production (SIP) is essential for describing the microphysics of deep convective clouds, yet the exact mechanisms and efficiencies of SIP are still uncertain. In this study, we used the University of Manchester bin microphysics parcel model to investigate four SIP parameterisations: rime splintering, ice-ice collisional breakup, spherical freezing fragmentation of drops (mode 1), and fragmentation between supercooled droplets and more massive ice particles (mode 2). We simulated air trajectories through deep convective clouds observed during the Deep Convective Microphysics EXperiment (DCMEX) field campaign. Our results show that mode 2, as currently understood and represented in the model, is the key mechanism for explaining the high ice particle concentrations observed. We also present the first systematic study of how different entrainment conditions (homogeneous and inhomogeneous mixing) affect SIP mechanisms. In our simulations, homogeneous and inhomogeneous mixing with aerosol entrainment provide reasonable agreement with cloud-core and cloud-edge microphysical properties observed during DCMEX, respectively. In addition, the peak liquid water content values in the adiabatic simulations was approximately 300 % of that in the entraining simulations. The entrainment of external aerosols was also found to accelerate the collision-coalescence process under homogeneous mixing, leading to earlier ice enhancement. Our results show that SIP mechanisms, which are dependent on large droplets, such as mode 2, are highly sensitive to different entrainment conditions, emphasising the importance of representing entrainment correctly when including SIP processes in large-scale models.</p>
  </abstract>
    
<funding-group>
<award-group id="gs1">
<funding-source>Horizon 2020</funding-source>
<award-id>101137680</award-id>
</award-group>
</funding-group>
</article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d2e143">Ice formation in clouds significantly influences cloud properties and precipitation processes, thereby impacting weather systems and global climate <xref ref-type="bibr" rid="bib1.bibx62 bib1.bibx19 bib1.bibx71" id="paren.1"/>. However, the formation pathways of ice crystals in clouds remain uncertain, as observed concentrations of ice particles often far exceed what can be explained by primary ice nucleation alone <xref ref-type="bibr" rid="bib1.bibx29 bib1.bibx7 bib1.bibx12 bib1.bibx43 bib1.bibx48 bib1.bibx31" id="paren.2"/>. Several secondary ice production (SIP) mechanisms have therefore been proposed to explain this discrepancy <xref ref-type="bibr" rid="bib1.bibx60 bib1.bibx41" id="paren.3"/>. In our study, we focus on four SIP processes: rime splintering, ice-ice collisions, spherical freezing fragmentation of drops (mode 1), and fragmentation between supercooled droplets and more massive ice particles (mode 2).</p>
      <p id="d2e155">Rime Splintering (RS), also known as the Hallett–Mossop process, is currently the most widely implemented SIP mechanism in cloud microphysics models. In this process, secondary ice splinters are produced when supercooled droplets collide with and freeze onto riming ice particles. It is active only within a narrow temperature range of <inline-formula><mml:math id="M1" display="inline"><mml:mrow><mml:mi mathvariant="normal">−</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M2" display="inline"><mml:mrow><mml:mi mathvariant="normal">−</mml:mi><mml:mn mathvariant="normal">8</mml:mn></mml:mrow></mml:math></inline-formula> °C <xref ref-type="bibr" rid="bib1.bibx28" id="paren.4"/> and typically occurs when droplets smaller than 12 µm and larger than 24 µm in diameter are both present <xref ref-type="bibr" rid="bib1.bibx58 bib1.bibx30" id="paren.5"/>. However, the large amounts of ice observed in deep convective clouds cannot always be explained by RS, especially in cases where the increase in ice number is too rapid, the temperatures and crystal habits fall outside the RS window, or the necessary conditions for RS are not satisfied <xref ref-type="bibr" rid="bib1.bibx66 bib1.bibx49 bib1.bibx20" id="paren.6"/>. The interpretation is further complicated in deep convective clouds, where the role of RS may be difficult to identify because of cloud dynamics. A recent experiment by <xref ref-type="bibr" rid="bib1.bibx68" id="text.7"/> also failed to reproduce the high SIP rates reported in earlier RS studies, thereby questioning the significance of rime splintering under mixed-phase convective conditions. As noted in the review by <xref ref-type="bibr" rid="bib1.bibx41" id="text.8"/>, the physical mechanism of RS remains poorly quantified and understood, with the parameterisation still highly uncertain. Other potential SIP mechanisms therefore need to be considered to better understand ice enhancement in deep convective clouds.</p>
      <p id="d2e194">Ice–Ice Collisional Breakup (CB) is the second SIP mechanism investigated in this study. This process refers to the mechanical fragmentation of ice particles during collisions, leading to the formation of new ice crystals. This mechanism has been observed in both aircraft measurements <xref ref-type="bibr" rid="bib1.bibx67" id="paren.9"/> and laboratory experiments <xref ref-type="bibr" rid="bib1.bibx73 bib1.bibx70 bib1.bibx26" id="paren.10"/>. Laboratory studies found that CB is most active near <inline-formula><mml:math id="M3" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">16</mml:mn></mml:mrow></mml:math></inline-formula> °C <xref ref-type="bibr" rid="bib1.bibx70" id="paren.11"/>, and field observations also showed substantial secondary ice near <inline-formula><mml:math id="M4" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">15</mml:mn></mml:mrow></mml:math></inline-formula> °C <xref ref-type="bibr" rid="bib1.bibx54 bib1.bibx6" id="paren.12"/>. In simulations of deep convective clouds during the High Altitude Ice Crystals and High Ice Water Content (HAIC-HIWC) campaign, <xref ref-type="bibr" rid="bib1.bibx27" id="text.13"/> found that CB was a key contributor to ice enhancement, and that only when combined with RS could the observed high ice crystal concentrations be reproduced. However, the collision efficiency and fragmentation probability of this mechanism remain poorly understood, and future parameterisations will need to be improved accordingly (see the discussion in <xref ref-type="bibr" rid="bib1.bibx41" id="altparen.14"/>).</p>
      <p id="d2e236">Finally, we examine fragmentation of freezing drops, also known as drop shattering (DS), in which supercooled droplets fragment during freezing and produce secondary ice particles. To better characterise these processes, <xref ref-type="bibr" rid="bib1.bibx61" id="text.15"/> described DS as comprising two modes, with mode 1 (M1) representing fragmentation during the spherical freezing of droplets, and mode 2 (M2) representing fragmentation during collisions between supercooled droplets and more massive ice particles. According to <xref ref-type="bibr" rid="bib1.bibx61" id="text.16"/>, fragment numbers in M1 depend strongly on both temperature and droplet size, exhibiting a pronounced thermal peak near <inline-formula><mml:math id="M5" display="inline"><mml:mrow><mml:mi mathvariant="normal">−</mml:mi><mml:mn mathvariant="normal">15</mml:mn></mml:mrow></mml:math></inline-formula> °C and increasing with droplet size. In contrast, M2 shows no clear evidence of a thermal peak and instead increases with dimensionless collision energy and supercooling, requiring the presence of large supercooled droplets and more massive ice particles. DS has increasingly been incorporated into numerical studies of SIP in recent years, reflecting that it may represent an important source of secondary ice. For example, <xref ref-type="bibr" rid="bib1.bibx35" id="text.17"/> investigated M2 within the framework of <xref ref-type="bibr" rid="bib1.bibx61" id="text.18"/> in parcel model simulations of idealised shallow convective clouds, and compared it with RS, M1, and CB. Their results suggest that, under conditions where RS is limited, M2 may represent an important source of secondary ice in shallow convective clouds, whereas the contribution from M1 is relatively small. In this study, we follow the framework of <xref ref-type="bibr" rid="bib1.bibx61" id="text.19"/> and <xref ref-type="bibr" rid="bib1.bibx35" id="text.20"/> and examine DS by separately analysing M1 and M2, given their distinct physical characteristics.</p>
      <p id="d2e269">Many SIP mechanisms (e.g. RS, M1, and M2) are highly sensitive to warm-phase microphysical conditions in clouds, particularly liquid water content and droplet size distributions. Previous studies have shown that these properties can be strongly affected by entrainment in deep convective clouds, particularly by how entrained environmental air mixes with cloudy air <xref ref-type="bibr" rid="bib1.bibx57 bib1.bibx10" id="paren.21"/>. Homogeneous and inhomogeneous mixing are commonly regarded as two idealised limiting regimes of entrainment-mixing in clouds <xref ref-type="bibr" rid="bib1.bibx4 bib1.bibx51" id="paren.22"/>. Homogeneous mixing assumes that entrained air first mixes thoroughly with cloud air, after which the droplet population experiences an approximately uniform reduction in relative humidity, whereas in inhomogeneous mixing the mixing is incomplete and different droplets may be exposed to different local humidity conditions. <xref ref-type="bibr" rid="bib1.bibx77" id="text.23"/> found that the microphysical relationships in most cloud segments of continental stratocumulus were more consistent with homogeneous mixing. However, other observational studies have suggested that homogeneous and inhomogeneous mixing can both occur in real clouds, depending on cloud region, environmental conditions, and cloud life cycle stage. For example, <xref ref-type="bibr" rid="bib1.bibx51" id="text.24"/> showed that homogeneous mixing was more likely near the cloud core, whereas inhomogeneous mixing tended to dominate in more diluted cloud regions.</p>
      <p id="d2e284">Modelling studies of SIP in deep convective clouds have often reported contrasting conclusions regarding the dominant mechanisms. This may be because the relative importance of SIP processes can vary substantially over the cloud lifecycle. For example, <xref ref-type="bibr" rid="bib1.bibx32" id="text.25"/> found that DS dominated during the early stage of convection, whereas CB became more important at later stages, using the bulk P3 scheme in Weather Research and Forecasting (WRF). This variation in the dominant SIP mechanisms occurs even in studies based on the same observational case from the HAIC–HIWC campaign. For example, <xref ref-type="bibr" rid="bib1.bibx65" id="text.26"/> used a bulk microphysics scheme and suggested that DS was the dominant SIP mechanism during a later stage of their simulation (90 to 150 min). In contrast, <xref ref-type="bibr" rid="bib1.bibx27" id="text.27"/> used a 3D bin microphysics model and found that RS and CB were more important, with DS having only a limited effect at the mature stage of the simulated cloud. This discrepancy may be explained by differences in how warm microphysical processes and entrainment are represented across models, thereby affecting simulated SIP. In many commonly used microphysics schemes, especially those employing simplified bulk representations, entrainment is often treated as homogeneous mixing <xref ref-type="bibr" rid="bib1.bibx75" id="paren.28"/>. However, mixing can also be inhomogeneous in deep convective clouds because of their complex structure and strong spatial variability. It is therefore necessary to systematically examine how different representations of entrainment affect SIP.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>DCMEX</title>
      <p id="d2e307">The Deep Convective Microphysics EXperiment (DCMEX) campaign was conducted in July and August 2022 over the Magdalena Mountains near Socorro, New Mexico, with the aim of characterising the microphysics and dynamics of deep convective cloud formation, including improved understanding of SIP mechanisms <xref ref-type="bibr" rid="bib1.bibx21" id="paren.29"/>. Conditions in this region are highly favourable for the development of multiple-thermal cumulus congestus. These clouds are typically confined to the mountain range and can transition into deeper thunderstorms <xref ref-type="bibr" rid="bib1.bibx21" id="paren.30"/>. The occurrence of these clouds is strongly influenced by the North American Monsoon (NAM), during which moist inflows from the Gulf of Mexico and the eastern Pacific prevail between June and September <xref ref-type="bibr" rid="bib1.bibx2 bib1.bibx16" id="paren.31"/>.</p>
      <p id="d2e319">A number of studies have investigated cloud processes during the DCMEX campaign. Among these, <xref ref-type="bibr" rid="bib1.bibx74" id="text.32"/> conducted a combined modelling and observational analysis of warm cloud processes in two DCMEX cases and found that aerosol entrainment plays a key role in broadening the droplet size distribution (DSD), which has important implications for subsequent investigations of the ice phase in clouds. Previous work at the same site by <xref ref-type="bibr" rid="bib1.bibx7" id="text.33"/> suggested that RS was responsible for the high ice crystal concentrations observed in these clouds. The contributions and relative importance of different SIP mechanisms in deep convective clouds in this region remain to be systematically assessed.</p>
      <p id="d2e328">Section 2.1 describes the measurements used in this study, including the key instrumentation, while Sect. 2.2 introduces the case studies analysed in this work.</p>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>Measurements</title>
      <p id="d2e338">A key component of DCMEX was the Facility for Airborne Atmospheric Measurements (FAAM) British Aerospace Engineering-146 (BAe-146) aircraft, which was equipped with a comprehensive suite of aerosol and cloud microphysics instruments. During the DCMEX flights, the aircraft followed a kite-shaped pattern around the Magdalena Mountains for the INP and aerosol sampling parts of the flight, while straight and level passes were made through the clouds during cloud sampling. The right panel of Fig. <xref ref-type="fig" rid="F1"/> shows the flight track for Flight C300 on 22 July 2022, which is representative of the other flights that followed a similar plan view. All flights followed a similar pattern, starting with low-level aerosol runs to characterise the boundary-layer inflow, followed by cloud passes through developing convection to investigate microphysical properties within the mixed-phase region. In addition, dropsondes were released near the Magdalena Mountains to obtain vertical profiles of thermodynamic and wind fields <xref ref-type="bibr" rid="bib1.bibx21" id="paren.34"/>. Below, we briefly summarise the instruments used in this study.</p>

      <fig id="F1" specific-use="star"><label>Figure 1</label><caption><p id="d2e348">The left panel shows the time series of aircraft altitude for the three selected DCMEX cases, with shaded periods indicating cloud penetration. The right panel shows the corresponding flight track for the case on 22 July 2022 (C300).</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/26/8367/2026/acp-26-8367-2026-f01.jpg"/>

        </fig>

      <p id="d2e357">The Aerosol Mass Spectrometer (AMS) and the Scanning Mobility Particle Sizer (SMPS) were used to measure the composition and size distribution of sub-micron aerosol. The AMS provided estimates of the effective hygroscopicity parameter (<inline-formula><mml:math id="M6" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula>) of the aerosol, which were used to derive their cloud condensation nuclei (CCN) properties for input into the Bin Microphysics Model (BMM). The SMPS was employed to characterise the aerosol size distribution near the cloud base, as shown in <xref ref-type="bibr" rid="bib1.bibx74" id="text.35"/>.</p>
      <p id="d2e371">The cloud droplet probe (CDP-2) was used to measure the droplet size distribution (DSD) over the size range 2 to 50 <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 and to derive cloud droplet number concentration (CDNC) <xref ref-type="bibr" rid="bib1.bibx45" id="paren.36"/>. The relative dispersion of the DSD was also calculated as the ratio of the standard deviation of droplet diameter to the mean droplet diameter. Liquid water content (LWC) was obtained from a Nevzorov hot-wire probe following the Met Office processing method <xref ref-type="bibr" rid="bib1.bibx39 bib1.bibx1" id="paren.37"/>.</p>
      <p id="d2e388">The Cloud Particle Imager (CPI, version 2.5) was used to obtain high-resolution images of cloud particles larger than 8 µm and to derive ice particle concentration. Although the CPI has a relatively small sample volume compared with the 2D-S, data from multiple flight segments were averaged to make the results more reliable and representative. The high-resolution imagery was also used to identify potential SIP mechanisms in this study <xref ref-type="bibr" rid="bib1.bibx38 bib1.bibx42" id="paren.38"/>, with further discussion is provided in Sect. <xref ref-type="sec" rid="Ch1.S4.SS3"/>.</p>
</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>Case Study</title>
      <p id="d2e405">The data used in this study were collected from 19 July to 7 August 2022 (flight C298-C314). In the early phase of the campaign, from 19 to 22 July (Flight C298-C300), the airmass originated from north-western (NW) flow from the Pacific over the continent towards the Magdalena Mountains, resulting in relatively lower cloud-base temperatures (<inline-formula><mml:math id="M8" display="inline"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mi mathvariant="normal">cb</mml:mi></mml:msub><mml:mo>≈</mml:mo><mml:mn mathvariant="normal">1.5</mml:mn></mml:mrow></mml:math></inline-formula> °C) and lower humidity compared to later in the campaign. Around 24 July, a shift to south-eastern (SE) flow from the Gulf of Mexico introduced warmer and moister conditions, marking a transition observed in the subsequent flights (Flights C302-C314). After 28 July, the clouds generally maintained relatively high cloud-base temperatures (<inline-formula><mml:math id="M9" display="inline"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mi mathvariant="normal">cb</mml:mi></mml:msub><mml:mo>≈</mml:mo><mml:mn mathvariant="normal">5.67</mml:mn></mml:mrow></mml:math></inline-formula> °C) and relative humidity.  In this study, 15 flight cases were simulated, as listed in Table <xref ref-type="table" rid="T1"/>. Three representative cases, 22 July (C300), 25 July (C303), and 1 August (C309), are selected for detailed analysis based on the evolution of the airmass characteristics described above. The flight altitude for the three cases is shown in the left panel of Fig. <xref ref-type="fig" rid="F1"/>. The 22 July case was chosen as it represents typical convective clouds that developed under the NW flow during the early phase of the campaign, while the 25 July case represents the early stage of SE inflow.</p>
      <p id="d2e444">The 1 August case represents the later phase with SE flow.  It was selected because the cloud was in a relatively early stage of development, before the convection had penetrated the detrainment layer.  The in-situ sounding revealed a pronounced temperature inversion at around 7 km.  However, the observed cloud top reached approximately 14.4 km <xref ref-type="bibr" rid="bib1.bibx21" id="paren.39"/>, suggesting that the convection was strong enough to break through the inversion and later developed up to the tropopause.  Such inversion-breaking convection is commonly observed over the mountainous southwest United States during the summer monsoon <xref ref-type="bibr" rid="bib1.bibx3 bib1.bibx22" id="paren.40"/>.</p>

      <fig id="F2" specific-use="star"><label>Figure 2</label><caption><p id="d2e455">Schematic representation of the BMM parcel model. The left-hand side shows the main model framework, including the key microphysical processes and representations of the aerosol, droplet, and ice particle size bins from top to bottom. The right-hand side illustrates the two entrainment-mixing representations in the BMM, homogeneous mixing and inhomogeneous mixing.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/26/8367/2026/acp-26-8367-2026-f02.png"/>

        </fig>

</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Bin microphysics parcel model</title>
<sec id="Ch1.S3.SS1">
  <label>3.1</label><title>Model description</title>
      <p id="d2e480">The model used in this study is the University of Manchester BMM, based on an updated version of the framework developed in previous studies <xref ref-type="bibr" rid="bib1.bibx72 bib1.bibx23 bib1.bibx35" id="paren.41"/>, with the source code available at <uri>https://github.com/UoM-maul1609/bin-microphysics-model</uri> (last access: 11 June 2026). A simplified schematic overview of the main BMM framework is shown on the left side of Fig. <xref ref-type="fig" rid="F2"/>.</p>
      <p id="d2e491">In the BMM, particles are represented by two particle size distributions, droplet size bins and ice particle bins, each comprising 80 bins. Both distributions additionally include 60 aerosol bins (10 nm to 3 <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). The aerosol bins are not defined using linear or logarithmic spacing in particle size. Instead, the bin edges are defined from the initial aerosol number concentration so that each bin contains approximately equal particle numbers. This approach is intended to reduce discretisation artefacts during aerosol activation, thereby avoiding step-like increases in activated particle number concentration in response to changes in updraft or supersaturation.</p>
      <p id="d2e502">The aerosol population can be represented by one or more externally mixed components with different chemical compositions. For each externally mixed component, particles are assumed to be internally mixed across the size distribution, so that their chemical composition does not vary with particle size. In this study, only a single externally mixed component is considered. Its initial size distribution is represented as the sum of multiple lognormal modes, as follows:

            <disp-formula id="Ch1.E1" content-type="numbered"><label>1</label><mml:math id="M11" display="block"><mml:mrow><mml:msub><mml:mfenced close="]" open="["><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>N</mml:mi></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>ln⁡</mml:mi><mml:mi>D</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mfenced><mml:mi>j</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:munderover><mml:mo movablelimits="false">∑</mml:mo><mml:mi>i</mml:mi><mml:mi>M</mml:mi></mml:munderover><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mrow><mml:mi mathvariant="normal">ap</mml:mi><mml:mo>,</mml:mo><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub></mml:mrow><mml:mrow><mml:msqrt><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mi mathvariant="italic">π</mml:mi></mml:mrow></mml:msqrt><mml:mi>ln⁡</mml:mi><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mi>g</mml:mi><mml:mo>,</mml:mo><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mi>exp⁡</mml:mi><mml:mfenced open="(" close=")"><mml:mrow><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msup><mml:mi>ln⁡</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mfenced open="(" close=")"><mml:mrow><mml:mi>D</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi>d</mml:mi><mml:mrow><mml:mi>m</mml:mi><mml:mo>,</mml:mo><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:mfenced></mml:mrow><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:msup><mml:mi>ln⁡</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mi>g</mml:mi><mml:mo>,</mml:mo><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mfenced></mml:mrow></mml:math></disp-formula>

          where <inline-formula><mml:math id="M12" display="inline"><mml:mrow><mml:msub><mml:mfenced open="[" close="]"><mml:mstyle displaystyle="false"><mml:mfrac style="text"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>N</mml:mi></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>ln⁡</mml:mi><mml:mi>D</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mfenced><mml:mi>j</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the aerosol number size distribution (cm<sup>−3</sup>) for external mixture <inline-formula><mml:math id="M14" display="inline"><mml:mi>j</mml:mi></mml:math></inline-formula>, <inline-formula><mml:math id="M15" display="inline"><mml:mi>D</mml:mi></mml:math></inline-formula> is the particle diameter (m), <inline-formula><mml:math id="M16" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mrow><mml:mi mathvariant="normal">ap</mml:mi><mml:mo>,</mml:mo><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is the total aerosol number concentration (cm<sup>−3</sup>) of mode <inline-formula><mml:math id="M18" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula> within external mixture <inline-formula><mml:math id="M19" display="inline"><mml:mi>j</mml:mi></mml:math></inline-formula>, <inline-formula><mml:math id="M20" display="inline"><mml:mrow><mml:msub><mml:mi>d</mml:mi><mml:mrow><mml:mi>m</mml:mi><mml:mo>,</mml:mo><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is the geometric mean diameter (m), and <inline-formula><mml:math id="M21" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mi>g</mml:mi><mml:mo>,</mml:mo><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is the geometric standard deviation of the lognormal mode. In this study, <inline-formula><mml:math id="M22" display="inline"><mml:mrow><mml:mi>j</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> because only a single externally mixed component is considered, and <inline-formula><mml:math id="M23" display="inline"><mml:mrow><mml:mi>M</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> denotes the two lognormal modes used to represent the initial aerosol size distribution: the Aitken and accumulation modes.</p>
      <p id="d2e796">The hygroscopic growth of aerosol particles is described using <inline-formula><mml:math id="M24" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula>-Köhler theory, in which particle hygroscopicity is represented by the parameter <inline-formula><mml:math id="M25" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx59" id="paren.42"/>. In this study, <inline-formula><mml:math id="M26" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula> is assumed to remain constant across all size bins. The initial wet diameter and corresponding liquid water mass of aerosol particles are determined by assuming equilibrium with the prescribed environmental relative humidity, based on <inline-formula><mml:math id="M27" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula>-Köhler theory. This initial wet state is represented numerically on a mass-based bin structure, with the mass of adjacent bins increasing by a factor of <inline-formula><mml:math id="M28" display="inline"><mml:mrow><mml:msup><mml:mn mathvariant="normal">2</mml:mn><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>/</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>.</p>
      <p id="d2e848">The warm microphysical processes considered in this study include diffusional droplet growth and collision–coalescence of liquid particles. Diffusional growth rates account for kinetic effects and corrected diffusivity and thermal conductivity terms <xref ref-type="bibr" rid="bib1.bibx34 bib1.bibx64" id="paren.43"/>, whereas collision–coalescence is described by the stochastic collection equation and solved using the method of <xref ref-type="bibr" rid="bib1.bibx8" id="text.44"/>. In addition, the model also includes entrainment of dry air and external aerosol, as described in Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>.</p>
      <p id="d2e859">The cold microphysical processes considered in this study include homogeneous and heterogeneous freezing, vapour depositional growth of ice particles, ice-ice aggregation, riming, and secondary ice production. Homogeneous freezing of supercooled droplets is represented following the formulation of <xref ref-type="bibr" rid="bib1.bibx37" id="text.45"/>. Heterogeneous freezing in this study is represented using the parameterisation of <xref ref-type="bibr" rid="bib1.bibx14" id="text.46"/>, a recently developed formulation constrained by observations from the DCMEX campaign. To assess the sensitivity of the results to the representation of ice-nucleating particles, <xref ref-type="bibr" rid="bib1.bibx15" id="text.47"/> is also included for comparison. The differences between the two parameterisations are discussed in Sect. <xref ref-type="sec" rid="Ch1.S4.SS3"/>, with additional details provided in Sect. S2 of the Supplement.</p>
      <p id="d2e873">In the BMM, ice particles are represented by a separate set of bins from liquid particles. Additional prognostic properties are tracked in each ice bin, including the aspect ratio, particle volume, rime mass, and the number of ice crystal monomers per ice particle. Riming and ice–ice aggregation are also represented by numerically solving the stochastic collection equation (SCE) using the exponential flux method of <xref ref-type="bibr" rid="bib1.bibx8" id="text.48"/>. A more detailed description of the ice particle bin representation is provided by <xref ref-type="bibr" rid="bib1.bibx35" id="text.49"/>. The parameterisation of SIP is described in Sect. S1.</p>
</sec>
<sec id="Ch1.S3.SS2">
  <label>3.2</label><title>Entrainment Representation</title>
      <p id="d2e890">In this study, two types of entrainment processes are considered: homogeneous and inhomogeneous mixing. In the model, homogeneous mixing is represented by continuously incorporating environmental air into the parcel and instantaneously mixing it at each time step, leading to a dilution of the parcel thermodynamic properties. This is implemented by including additional equations in the solver routine, which are integrated using the variable-coefficient ordinary differential equation (VODE) solver. The theory is described in <xref ref-type="bibr" rid="bib1.bibx64" id="text.50"><named-content content-type="post">chapter 12</named-content></xref>.</p>
      <p id="d2e898">In this model, the parcel is represented as a jet, allowing entrainment to occur through the front interface of the plume. The evolution of the vertical velocity (<inline-formula><mml:math id="M29" display="inline"><mml:mi>W</mml:mi></mml:math></inline-formula>), parcel radius (<inline-formula><mml:math id="M30" display="inline"><mml:mrow><mml:msub><mml:mi>R</mml:mi><mml:mi>j</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>), and water vapour mixing ratio (<inline-formula><mml:math id="M31" display="inline"><mml:mrow><mml:msub><mml:mi>q</mml:mi><mml:mi mathvariant="normal">v</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) is explicitly represented, and the entrainment of ambient aerosol is also included. The entrainment rate (<inline-formula><mml:math id="M32" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">μ</mml:mi><mml:mi>J</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) for the jet parcel is therefore defined as

            <disp-formula id="Ch1.E2" content-type="numbered"><label>2</label><mml:math id="M33" display="block"><mml:mrow><mml:msub><mml:mi mathvariant="italic">μ</mml:mi><mml:mi>J</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>z</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi>C</mml:mi><mml:mi>J</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mi>R</mml:mi><mml:mi>J</mml:mi></mml:msub></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:math></disp-formula>

          where <inline-formula><mml:math id="M34" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi mathvariant="normal">m</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mi mathvariant="italic">π</mml:mi><mml:msubsup><mml:mi>R</mml:mi><mml:mi>J</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mi mathvariant="italic">ρ</mml:mi><mml:mi>W</mml:mi></mml:mrow></mml:math></inline-formula> is the total mass flux of the rising parcel (kg s<sup>−1</sup>), <inline-formula><mml:math id="M36" display="inline"><mml:mi mathvariant="italic">ρ</mml:mi></mml:math></inline-formula> is the parcel density, <inline-formula><mml:math id="M37" display="inline"><mml:mrow><mml:msub><mml:mi>C</mml:mi><mml:mi>J</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the entrainment parameter, set to 0.2 based on previous laboratory studies, and <inline-formula><mml:math id="M38" display="inline"><mml:mrow><mml:msub><mml:mi>R</mml:mi><mml:mi>J</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the jet radius, which is set to 1000 m in this model.</p>
      <p id="d2e1063">The evolution of the parcel’s vertical velocity <inline-formula><mml:math id="M39" display="inline"><mml:mi>W</mml:mi></mml:math></inline-formula> (m s<sup>−1</sup>) is described by

            <disp-formula id="Ch1.E3" content-type="numbered"><label>3</label><mml:math id="M41" display="block"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>W</mml:mi></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mi>g</mml:mi><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>+</mml:mo><mml:mi mathvariant="italic">γ</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mfenced open="(" close=")"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi>T</mml:mi><mml:mo>-</mml:mo><mml:msup><mml:mi>T</mml:mi><mml:mo>′</mml:mo></mml:msup></mml:mrow><mml:mrow><mml:msup><mml:mi>T</mml:mi><mml:mo>′</mml:mo></mml:msup></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>-</mml:mo><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">L</mml:mi></mml:msub></mml:mrow></mml:mfenced><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi mathvariant="italic">μ</mml:mi><mml:mi>J</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>+</mml:mo><mml:mi mathvariant="italic">γ</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:msup><mml:mi>W</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></disp-formula>

          where <inline-formula><mml:math id="M42" display="inline"><mml:mi>g</mml:mi></mml:math></inline-formula> is the gravitational acceleration (9.81 m s<sup>−2</sup>), <inline-formula><mml:math id="M44" display="inline"><mml:mrow><mml:mi mathvariant="italic">γ</mml:mi><mml:mo>≈</mml:mo><mml:mn mathvariant="normal">0.5</mml:mn></mml:mrow></mml:math></inline-formula> is the moisture correction parameter accounting for the virtual effect of water vapour, <inline-formula><mml:math id="M45" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M46" display="inline"><mml:mrow><mml:msup><mml:mi>T</mml:mi><mml:mo>′</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> are the temperatures of the parcel and the environment (K), respectively,  <inline-formula><mml:math id="M47" display="inline"><mml:mrow><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">L</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the liquid water mixing ratio (kg kg<sup>−1</sup>).</p>
      <p id="d2e1238">The evolution of the jet radius is given by

            <disp-formula id="Ch1.E4" content-type="numbered"><label>4</label><mml:math id="M49" display="block"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>R</mml:mi><mml:mi>J</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi>R</mml:mi><mml:mi>J</mml:mi></mml:msub></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:mfrac></mml:mstyle><mml:mfenced open="(" close=")"><mml:mrow><mml:msub><mml:mi mathvariant="italic">μ</mml:mi><mml:mi>J</mml:mi></mml:msub><mml:mi>W</mml:mi><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mi mathvariant="italic">ρ</mml:mi></mml:mfrac></mml:mstyle><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi mathvariant="italic">ρ</mml:mi></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mi>W</mml:mi></mml:mfrac></mml:mstyle><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>W</mml:mi></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mfenced></mml:mrow></mml:math></disp-formula>

          All variables are as defined above.</p>
      <p id="d2e1324">Finally, the water vapour mixing ratio is calculated by a statement of conservation of water substance

            <disp-formula id="Ch1.E5" content-type="numbered"><label>5</label><mml:math id="M50" display="block"><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">v</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>=</mml:mo><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">L</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>-</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">i</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:mi mathvariant="normal">d</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">μ</mml:mi><mml:mi>J</mml:mi></mml:msub><mml:mfenced close=")" open="("><mml:mrow><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">v</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>w</mml:mi><mml:mrow><mml:msup><mml:mi mathvariant="normal">v</mml:mi><mml:mo>′</mml:mo></mml:msup></mml:mrow></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">L</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">i</mml:mi></mml:msub></mml:mrow></mml:mfenced></mml:mrow></mml:math></disp-formula>

          where <inline-formula><mml:math id="M51" display="inline"><mml:mrow><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">v</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the water-vapour mixing ratio within the parcel (kg kg<sup>−1</sup>);  <inline-formula><mml:math id="M53" display="inline"><mml:mrow><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the ice-water mixing ratio (kg kg<sup>−1</sup>);  and <inline-formula><mml:math id="M55" display="inline"><mml:mrow><mml:msub><mml:mi>w</mml:mi><mml:mrow><mml:msup><mml:mi mathvariant="normal">v</mml:mi><mml:mo>′</mml:mo></mml:msup></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is the water-vapour mixing ratio of the entrained environmental air (kg kg<sup>−1</sup>).</p>
      <p id="d2e1497">The BMM also allows entrainment to be represented as inhomogeneous mixing <xref ref-type="bibr" rid="bib1.bibx4" id="paren.51"/>, in which environmental air is not instantaneously and uniformly mixed with the parcel air, but is instead entrained intermittently into the parcel in the form of discrete packets. The same mean entrainment rate as in the homogeneous case is applied. However, unlike the homogeneous mixing representation, the mixing process is not solved continuously within the VODE solver, but is instead implemented as discrete events over a longer 10 s timestep to represent intermittent entrainment. For inhomogeneous mixing, the droplet number concentrations in each size bin are adjusted to conserve parcel humidity, thereby preventing a uniform reduction in droplet size across the entire spectrum as occurs in homogeneous mixing. When inhomogeneous mixing causes droplet evaporation, the released aerosol particles are returned to the discrete packets of subsaturated air within the parcel, where they may become re-activated later.  A simplified schematic of the two entrainment representations in the BMM is shown on the right of Fig. <xref ref-type="fig" rid="F2"/>.</p>
</sec>
<sec id="Ch1.S3.SS3">
  <label>3.3</label><title>Initial conditions</title>
      <p id="d2e1513">In our study, simulations are initialised at cloud base with an initial relative humidity of 0.95. All simulations are run for about 2.2 h (8000 s) with a timestep of 10 s, and the parcel radius is set to 1000 m. The initial aerosol size distribution is represented by a two-mode lognormal fit derived from SMPS observations (see Fig. S1 and Table S1 in the Supplement). Table <xref ref-type="table" rid="T1"/> summarises the initial aerosol and cloud-base conditions used to initialise the simulations, including the cloud-base pressure (<inline-formula><mml:math id="M57" display="inline"><mml:mrow><mml:msub><mml:mi>P</mml:mi><mml:mi mathvariant="normal">cb</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>), aerosol density (<inline-formula><mml:math id="M58" display="inline"><mml:mi mathvariant="italic">ρ</mml:mi></mml:math></inline-formula>), and <inline-formula><mml:math id="M59" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula>.</p>

<table-wrap id="T1" specific-use="star"><label>Table 1</label><caption><p id="d2e1546">Cloud-base thermodynamic and aerosol properties for the simulated cases, including the lifting condensation level (LCL), cloud-base temperature (<inline-formula><mml:math id="M60" display="inline"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mi mathvariant="normal">cb</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>), temperature perturbation (<inline-formula><mml:math id="M61" display="inline"><mml:mrow><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi>T</mml:mi></mml:mrow></mml:math></inline-formula>), cloud-base pressure (<inline-formula><mml:math id="M62" display="inline"><mml:mrow><mml:msub><mml:mi>P</mml:mi><mml:mi mathvariant="normal">cb</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>), updraught velocity (<inline-formula><mml:math id="M63" display="inline"><mml:mrow><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">cb</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>), aerosol density (<inline-formula><mml:math id="M64" display="inline"><mml:mi mathvariant="italic">ρ</mml:mi></mml:math></inline-formula>), and hygroscopicity parameter (<inline-formula><mml:math id="M65" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula>).</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="9">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="center"/>
     <oasis:colspec colnum="4" colname="col4" align="center"/>
     <oasis:colspec colnum="5" colname="col5" align="center"/>
     <oasis:colspec colnum="6" colname="col6" align="center"/>
     <oasis:colspec colnum="7" colname="col7" align="center"/>
     <oasis:colspec colnum="8" colname="col8" align="right"/>
     <oasis:colspec colnum="9" colname="col9" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Date</oasis:entry>
         <oasis:entry colname="col2">Flight</oasis:entry>
         <oasis:entry colname="col3">LCL (km)</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M67" display="inline"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mi mathvariant="normal">cb</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (°C)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M68" display="inline"><mml:mrow><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi>T</mml:mi></mml:mrow></mml:math></inline-formula> (K)</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M69" display="inline"><mml:mrow><mml:msub><mml:mi>P</mml:mi><mml:mi mathvariant="normal">cb</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (hPa)</oasis:entry>
         <oasis:entry colname="col7"><inline-formula><mml:math id="M70" display="inline"><mml:mrow><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">cb</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M71" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">m</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">s</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>)</oasis:entry>
         <oasis:entry colname="col8"><inline-formula><mml:math id="M72" display="inline"><mml:mi mathvariant="italic">ρ</mml:mi></mml:math></inline-formula> (<inline-formula><mml:math id="M73" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kg</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">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>)</oasis:entry>
         <oasis:entry colname="col9"><inline-formula><mml:math id="M74" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Tue 19 Jul</oasis:entry>
         <oasis:entry colname="col2">C298</oasis:entry>
         <oasis:entry colname="col3">5.12</oasis:entry>
         <oasis:entry colname="col4">0.27</oasis:entry>
         <oasis:entry colname="col5">2.5</oasis:entry>
         <oasis:entry colname="col6">562.04</oasis:entry>
         <oasis:entry colname="col7">2.5</oasis:entry>
         <oasis:entry colname="col8">1566.84<sup>*</sup></oasis:entry>
         <oasis:entry colname="col9">0.3811<sup>*</sup></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Wed 20 Jul</oasis:entry>
         <oasis:entry colname="col2">C299</oasis:entry>
         <oasis:entry colname="col3">4.99</oasis:entry>
         <oasis:entry colname="col4">1.47</oasis:entry>
         <oasis:entry colname="col5">0.2</oasis:entry>
         <oasis:entry colname="col6">571.23</oasis:entry>
         <oasis:entry colname="col7">1.0</oasis:entry>
         <oasis:entry colname="col8">1566.84</oasis:entry>
         <oasis:entry colname="col9">0.3811</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Fri 22 Jul</oasis:entry>
         <oasis:entry colname="col2">C300</oasis:entry>
         <oasis:entry colname="col3">4.86</oasis:entry>
         <oasis:entry colname="col4">2.68</oasis:entry>
         <oasis:entry colname="col5">1.0</oasis:entry>
         <oasis:entry colname="col6">579.20</oasis:entry>
         <oasis:entry colname="col7">2.5</oasis:entry>
         <oasis:entry colname="col8">1484.95</oasis:entry>
         <oasis:entry colname="col9">0.2674</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Sun 24 Jul</oasis:entry>
         <oasis:entry colname="col2">C302</oasis:entry>
         <oasis:entry colname="col3">4.10</oasis:entry>
         <oasis:entry colname="col4">5.44</oasis:entry>
         <oasis:entry colname="col5">1.0</oasis:entry>
         <oasis:entry colname="col6">635.06</oasis:entry>
         <oasis:entry colname="col7">2.5</oasis:entry>
         <oasis:entry colname="col8">1606.81</oasis:entry>
         <oasis:entry colname="col9">0.4149</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Mon 25 Jul</oasis:entry>
         <oasis:entry colname="col2">C303</oasis:entry>
         <oasis:entry colname="col3">3.95</oasis:entry>
         <oasis:entry colname="col4">7.62</oasis:entry>
         <oasis:entry colname="col5">2.0</oasis:entry>
         <oasis:entry colname="col6">646.06</oasis:entry>
         <oasis:entry colname="col7">2.5</oasis:entry>
         <oasis:entry colname="col8">1617.27</oasis:entry>
         <oasis:entry colname="col9">0.4069</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Tue 26 Jul</oasis:entry>
         <oasis:entry colname="col2">C304</oasis:entry>
         <oasis:entry colname="col3">3.92</oasis:entry>
         <oasis:entry colname="col4">7.06</oasis:entry>
         <oasis:entry colname="col5">2.0</oasis:entry>
         <oasis:entry colname="col6">648.35</oasis:entry>
         <oasis:entry colname="col7">1.0</oasis:entry>
         <oasis:entry colname="col8">1637.87</oasis:entry>
         <oasis:entry colname="col9">0.4461</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Wed 27 Jul</oasis:entry>
         <oasis:entry colname="col2">C305</oasis:entry>
         <oasis:entry colname="col3">4.07</oasis:entry>
         <oasis:entry colname="col4">6.60</oasis:entry>
         <oasis:entry colname="col5">1.0</oasis:entry>
         <oasis:entry colname="col6">636.82</oasis:entry>
         <oasis:entry colname="col7">2.5</oasis:entry>
         <oasis:entry colname="col8">1650.06</oasis:entry>
         <oasis:entry colname="col9">0.4662</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Fri 29 Jul</oasis:entry>
         <oasis:entry colname="col2">C306</oasis:entry>
         <oasis:entry colname="col3">4.06</oasis:entry>
         <oasis:entry colname="col4">5.98</oasis:entry>
         <oasis:entry colname="col5">2.5</oasis:entry>
         <oasis:entry colname="col6">636.90</oasis:entry>
         <oasis:entry colname="col7">2.5</oasis:entry>
         <oasis:entry colname="col8">1603.63</oasis:entry>
         <oasis:entry colname="col9">0.3939</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Sat 30 Jul</oasis:entry>
         <oasis:entry colname="col2">C307</oasis:entry>
         <oasis:entry colname="col3">3.84</oasis:entry>
         <oasis:entry colname="col4">7.38</oasis:entry>
         <oasis:entry colname="col5">0.5</oasis:entry>
         <oasis:entry colname="col6">656.25</oasis:entry>
         <oasis:entry colname="col7">1.5</oasis:entry>
         <oasis:entry colname="col8">1571.12</oasis:entry>
         <oasis:entry colname="col9">0.4006</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Sun 31 Jul</oasis:entry>
         <oasis:entry colname="col2">C308</oasis:entry>
         <oasis:entry colname="col3">4.39</oasis:entry>
         <oasis:entry colname="col4">2.77</oasis:entry>
         <oasis:entry colname="col5">2.0</oasis:entry>
         <oasis:entry colname="col6">613.79</oasis:entry>
         <oasis:entry colname="col7">2.5</oasis:entry>
         <oasis:entry colname="col8">1569.68</oasis:entry>
         <oasis:entry colname="col9">0.3824</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Mon  1 Aug</oasis:entry>
         <oasis:entry colname="col2">C309</oasis:entry>
         <oasis:entry colname="col3">4.22</oasis:entry>
         <oasis:entry colname="col4">5.26</oasis:entry>
         <oasis:entry colname="col5">1.5</oasis:entry>
         <oasis:entry colname="col6">627.72</oasis:entry>
         <oasis:entry colname="col7">2.5</oasis:entry>
         <oasis:entry colname="col8">1547.22<sup>*</sup></oasis:entry>
         <oasis:entry colname="col9">0.3482<sup>*</sup></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Tue  2 Aug</oasis:entry>
         <oasis:entry colname="col2">C310</oasis:entry>
         <oasis:entry colname="col3">4.29</oasis:entry>
         <oasis:entry colname="col4">4.97</oasis:entry>
         <oasis:entry colname="col5">1.0</oasis:entry>
         <oasis:entry colname="col6">621.02</oasis:entry>
         <oasis:entry colname="col7">1.0</oasis:entry>
         <oasis:entry colname="col8">1547.22</oasis:entry>
         <oasis:entry colname="col9">0.3482</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Thu  4 Aug</oasis:entry>
         <oasis:entry colname="col2">C312</oasis:entry>
         <oasis:entry colname="col3">4.37</oasis:entry>
         <oasis:entry colname="col4">4.62</oasis:entry>
         <oasis:entry colname="col5">1.5</oasis:entry>
         <oasis:entry colname="col6">614.25</oasis:entry>
         <oasis:entry colname="col7">1.5</oasis:entry>
         <oasis:entry colname="col8">1591.61<sup>*</sup></oasis:entry>
         <oasis:entry colname="col9">0.3921<sup>*</sup></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Sat  6 Aug</oasis:entry>
         <oasis:entry colname="col2">C313</oasis:entry>
         <oasis:entry colname="col3">4.31</oasis:entry>
         <oasis:entry colname="col4">5.16</oasis:entry>
         <oasis:entry colname="col5">1.0</oasis:entry>
         <oasis:entry colname="col6">619.58</oasis:entry>
         <oasis:entry colname="col7">1.0</oasis:entry>
         <oasis:entry colname="col8">1591.61</oasis:entry>
         <oasis:entry colname="col9">0.3921</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Sun  7 Aug</oasis:entry>
         <oasis:entry colname="col2">C314</oasis:entry>
         <oasis:entry colname="col3">4.39</oasis:entry>
         <oasis:entry colname="col4">2.76</oasis:entry>
         <oasis:entry colname="col5">2.0</oasis:entry>
         <oasis:entry colname="col6">613.65</oasis:entry>
         <oasis:entry colname="col7">2.5</oasis:entry>
         <oasis:entry colname="col8">1541.35</oasis:entry>
         <oasis:entry colname="col9">0.3650</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table><table-wrap-foot><p id="d2e1607">Values marked with an asterisk (<sup>*</sup>) were taken from the closest available DCMEX case with similar atmospheric conditions because case-specific data were not available.</p></table-wrap-foot></table-wrap>

      <p id="d2e2280">Seven simulations were performed for each case to represent the seven mixing scenarios considered in this study (see Table <xref ref-type="table" rid="T2"/>). These scenarios include two primary types of mixing, homogeneous (HOM) and inhomogeneous (INHOM), each examined with or without entrained aerosol (EA). For the inhomogeneous scenarios, we further distinguished whether the entrained aerosol particles were released (RA) following the mixing process. In addition, a fully adiabatic reference case (ADIA) was included.</p>
      <p id="d2e2286">In the BMM, the initial parcel temperature was set to the potential temperature with an added perturbation (<inline-formula><mml:math id="M81" display="inline"><mml:mrow><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi>T</mml:mi></mml:mrow></mml:math></inline-formula>). The value of <inline-formula><mml:math id="M82" display="inline"><mml:mrow><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi>T</mml:mi></mml:mrow></mml:math></inline-formula> and the initial updraught velocity at cloud base (<inline-formula><mml:math id="M83" display="inline"><mml:mrow><mml:msub><mml:mi>w</mml:mi><mml:mi mathvariant="normal">cb</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) were both adjusted until the simulated liquid water content (LWC) agreed with the upper boundary of the observed profiles, which aimed to model the cloud core where liquid water contents are typically high <xref ref-type="bibr" rid="bib1.bibx51" id="paren.52"/>. For the adiabatic simulations, the ascent rate was constrained to match that in the non-adiabatic simulations, and the parcel was stopped at the same model cloud top. The entrainment parameter was set to 0 for the adiabatic simulations, while 0.2 was used for all non-adiabatic cases.</p>

<table-wrap id="T2" specific-use="star"><label>Table 2</label><caption><p id="d2e2326">Summary of the mixing scenarios considered in this study. HOM: homogeneous mixing; INHOM: inhomogeneous mixing; EA: entrained aerosol; RA: released aerosol; ADIA: adiabatic case.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="4">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Scenario</oasis:entry>
         <oasis:entry colname="col2">Mixing type</oasis:entry>
         <oasis:entry colname="col3">Entrain aerosol</oasis:entry>
         <oasis:entry colname="col4">Release aerosol</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">HOM+EA</oasis:entry>
         <oasis:entry colname="col2">Homogeneous</oasis:entry>
         <oasis:entry colname="col3">Yes</oasis:entry>
         <oasis:entry colname="col4">–</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">HOM</oasis:entry>
         <oasis:entry colname="col2">Homogeneous</oasis:entry>
         <oasis:entry colname="col3">No</oasis:entry>
         <oasis:entry colname="col4">–</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">INHOM+EA+RA</oasis:entry>
         <oasis:entry colname="col2">Inhomogeneous</oasis:entry>
         <oasis:entry colname="col3">Yes</oasis:entry>
         <oasis:entry colname="col4">Yes</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">INHOM+RA</oasis:entry>
         <oasis:entry colname="col2">Inhomogeneous</oasis:entry>
         <oasis:entry colname="col3">No</oasis:entry>
         <oasis:entry colname="col4">Yes</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">INHOM+EA</oasis:entry>
         <oasis:entry colname="col2">Inhomogeneous</oasis:entry>
         <oasis:entry colname="col3">Yes</oasis:entry>
         <oasis:entry colname="col4">No</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">INHOM</oasis:entry>
         <oasis:entry colname="col2">Inhomogeneous</oasis:entry>
         <oasis:entry colname="col3">No</oasis:entry>
         <oasis:entry colname="col4">No</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">ADIA</oasis:entry>
         <oasis:entry colname="col2">Adiabatic</oasis:entry>
         <oasis:entry colname="col3">–</oasis:entry>
         <oasis:entry colname="col4">–</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p id="d2e2470">For each sensitivity experiment, the SIP mechanisms (RS, CB, M1, and M2) were investigated individually, as well as in simulations with all mechanisms switched off and with all mechanisms activated. We also performed sensitivity tests with the heterogeneous freezing parameterisations of <xref ref-type="bibr" rid="bib1.bibx14" id="text.53"/> and <xref ref-type="bibr" rid="bib1.bibx15" id="text.54"/>, given that SIP processes depend on the availability of primary ice crystals.</p>
</sec>
</sec>
<sec id="Ch1.S4">
  <label>4</label><title>Results</title>
      <p id="d2e2488">We used the BMM to simulate the trajectories of individual air parcels for all 15 cases from the DCMEX campaign. Each parcel was initialised at the model cloud base and triggered by a thermal perturbation. Once the parcel reached buoyancy equilibrium, it remained at that level, while the internal microphysical processes and associated calculations continued throughout the simulation. Figures S3–S5 present the vertical profiles of cloud droplet number concentration (CDNC), liquid water content (LWC), and effective diameter (<inline-formula><mml:math id="M84" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) for all simulated cases. Figure S9 shows the total ice crystal number concentration in the control simulation, where all SIP mechanisms were switched off and only primary ice from INP activation was considered, based on DCMEX INP measurements <xref ref-type="bibr" rid="bib1.bibx14" id="paren.55"/>. Figures S10–S14 show the simulated ice enhancement for all 15 cases, for simulations in which each SIP mechanism (RS, CB, M1, M2) is activated individually and for the simulation in which all mechanisms are activated simultaneously.  This section is organised into four parts. Section <xref ref-type="sec" rid="Ch1.S4.SS1"/> presents the modelled evolution of liquid-phase properties (CDNC, LWC, and <inline-formula><mml:math id="M85" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) for the three selected cases, and Sect. <xref ref-type="sec" rid="Ch1.S4.SS2"/> shows the impact of entrainment on the droplet size distribution (DSD), including the vertical evolution of dispersion within the cloud. Section <xref ref-type="sec" rid="Ch1.S4.SS3"/> compares observed and simulated clouds with all SIP mechanisms activated, and Sect. <xref ref-type="sec" rid="Ch1.S4.SS4"/> analyses how individual SIP mechanisms contribute to ice enhancement.</p>
<sec id="Ch1.S4.SS1">
  <label>4.1</label><title>Bulk Liquid-Phase Cloud Properties</title>
      <p id="d2e2534">To quantify the effect of SIP on ice enhancement within the parcel, we first need to examine the liquid phase, including the vertical profiles of liquid water content (LWC), cloud droplet number concentration (CDNC), and <inline-formula><mml:math id="M86" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> from both observations and simulations under seven different mixing assumptions. The left panel of Fig. <xref ref-type="fig" rid="F3"/> presents the evolution of LWC for the three selected cases, showing only small differences among the non-adiabatic simulations because the parcel model entrains the same total mass of environmental air in each case. These simulations closely reproduce the observed peak LWC values, with maxima of approximately 1.0, 1.25, and 1.25 g m<sup>−3</sup> for the 22 July, 25 July, and 1 August cases, respectively, near the parcel maximum height. As expected, the observed values of LWC are much less than the adiabatic values due mainly to entrainment, while the ADIA simulations produce significantly higher LWC near the model cloud top, reaching approximately 300 % of those in the HOM and INHOM simulations.</p>

      <fig id="F3" specific-use="star"><label>Figure 3</label><caption><p id="d2e2564">Vertical profiles of (from left to right): liquid water content (LWC), cloud droplet number concentration (CDNC), effective diameter (<inline-formula><mml:math id="M88" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>), and dispersion for three representative cases, C300 (22 July 2022), C303 (25 July 2022), and C309 (1 August 2022). Coloured dots indicate observations; red lines denote ADIA; solid blue lines HOM+EA; dashed blue lines HOM; solid orange lines INHOM+EA+RA; dashed orange lines INHOM+RA; solid green lines INHOM+EA; and dashed green lines INHOM.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/26/8367/2026/acp-26-8367-2026-f03.jpg"/>

        </fig>

      <p id="d2e2584">It also should be noted that the CDP data collected during the DCMEX campaign represent instantaneous cloud measurements along the flight tracks, and the histories of the sampled cloud parcels cannot be determined. Therefore, the CDNC (middle-left panel), <inline-formula><mml:math id="M89" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (middle-right panel), and dispersion (right panel) distributions of Fig. <xref ref-type="fig" rid="F3"/> are interpreted in terms of LWC to identify cloud-core (yellow) and cloud-edge (blue) regions for each case. Following the findings of <xref ref-type="bibr" rid="bib1.bibx51" id="text.56"/>, cloud-core regions are characterised by high liquid water content, as well as droplet concentrations and droplet size distributions that are broadly consistent with homogeneous mixing, whereas cloud-edge regions experience stronger evaporation, lower LWC, and are characterised by inhomogeneous mixing.</p>
      <p id="d2e2604">The evolution of CDNC within the parcel is shown in the middle-left panel of Fig. <xref ref-type="fig" rid="F3"/>. For the ADIA simulations, the maximum CDNC values were reached near the model cloud base, with approximately 750, 850, and 900 cm<sup>−3</sup> for the 22 July, 25 July, and 1 August cases, respectively. CDNC then decreased by approximately 20 %–40 % across all three cases from the peak values near the model cloud base towards the cloud top, mainly due to collision–coalescence, which remained active in the ADIA simulations. In contrast, for the homogeneous mixing simulations, CDNC reached a peak of approximately 650, 700, and 850 cm<sup>−3</sup> near the model cloud base for the three cases, respectively. At temperatures warmer than <inline-formula><mml:math id="M92" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">10</mml:mn></mml:mrow></mml:math></inline-formula> °C, the HOM and HOM+EA simulations showed similar decreasing trends, with CDNC in HOM+EA remaining slightly higher. Around <inline-formula><mml:math id="M93" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">10</mml:mn></mml:mrow></mml:math></inline-formula> °C, a second CDNC peak of approximately 450, 500, and 550 cm<sup>−3</sup> appeared in HOM+EA, likely due to secondary droplet activation triggered by entrained aerosols. Near the model cloud top, CDNC in the HOM simulations was approximately 50 % lower than in the HOM+EA simulations. Overall, the homogeneous mixing simulations with external aerosol entrainment (HOM+EA) show reasonable agreement with the upper envelope of the observed CDNC.</p>
      <p id="d2e2666">For the inhomogeneous mixing simulations, both INHOM+EA+RA and INHOM+EA were in reasonable agreement with the observed CDNC values associated with relatively low LWC, as indicated by the blue and green dots. When the entrainment of external aerosols was disabled (i.e., with EA turned off), CDNC in the INHOM+RA and INHOM simulations decreased significantly, with only a small number of droplets remaining near the model cloud top. The effect of RA on CDNC under inhomogeneous mixing conditions was found to be limited, whereas the EA significantly enhanced CDNC. This is likely because released aerosols form in regions of evaporation, where decreasing relative humidity and strong subsaturation prevents them from reaching the critical supersaturation required for activation. Among the inhomogeneous mixing simulations, INHOM+EA+RA showed reasonable agreement with the average observed CDNC.</p>
      <p id="d2e2669">The evolution of <inline-formula><mml:math id="M95" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> within the parcel for the different simulations is shown in the middle-right panel of Fig. <xref ref-type="fig" rid="F3"/>. Across all simulations, <inline-formula><mml:math id="M96" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> generally increased with decreasing temperature as the cloud developed, as a result of continued droplet growth by collision–coalescence, and reached maximum values near the cloud top. For the ADIA simulations, maximum <inline-formula><mml:math id="M97" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> values reached approximately 22, 29, and 23 <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 for the 22 July, 25 July, and 1 August cases, respectively. In contrast, the HOM+EA simulations provided the best agreement with the observations, closely following the upper envelope, with peak <inline-formula><mml:math id="M99" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> values of approximately 18, 21, and 19 <inline-formula><mml:math id="M100" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m for the three cases. It is worth noting that, in the 25 July case, a pronounced increase in large droplets was observed near cloud top at temperatures of approximately <inline-formula><mml:math id="M101" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">15</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M102" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">20</mml:mn></mml:mrow></mml:math></inline-formula> °C, and a similar feature was reproduced by the HOM+EA simulations. Overall, the inhomogeneous mixing simulations produced larger <inline-formula><mml:math id="M103" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> values than both the homogeneous mixing and ADIA simulations. This effect was particularly evident under inhomogeneous mixing without any entrained aerosol or aerosol recycling, where <inline-formula><mml:math id="M104" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> became significantly larger, likely due to the removal of smaller droplets during inhomogeneous mixing, which shifted the droplet size distribution towards fewer but larger droplets.</p>
</sec>
<sec id="Ch1.S4.SS2">
  <label>4.2</label><title>Comparison of Observed and Modeled DSDs</title>
      <p id="d2e2785">Figures S6–S8 show the observed and simulated DSDs for three representative DCMEX cases, 22 July, 25 July, and 1 August, at nine selected temperature levels from cloud base to cloud top. In all three cases, the observed DSDs showed clear broadening with height, and bimodal, or even trimodal, structures were found at some temperature levels. This broadening of the DSD is also reflected in the dispersion, as shown in the right panel of Figure 3. The observed dispersion was generally smaller under higher-LWC conditions, which approximately correspond to cloud-core regions, and larger under lower-LWC conditions, shown in blue, which are more representative of cloud-edge regions.</p>
      <p id="d2e2788">This pattern suggests that the droplet distributions are likely broadened by entrainment, mixing, or turbulence. It should also be noted that some broadening in the observed DSDs may arise from measurement uncertainties, as discussed by <xref ref-type="bibr" rid="bib1.bibx44" id="text.57"/>. This is consistent with <xref ref-type="bibr" rid="bib1.bibx17" id="text.58"/>, who found that the mean diameters generally agree within a few percent, whereas the median diameters are overestimated by about 5 %–15 %, resulting in an artificial broadening and skewing of the spectra. Overall, ADIA and HOM simulations both show narrow DSDs, whereas the HOM+EA simulation reproduces key observed features of the in-situ DSDs, including a broader spectral width, the persistence of small droplets at higher altitudes, and a bimodal structure, which highlights the role of entrainment in DSD broadening, consistent with <xref ref-type="bibr" rid="bib1.bibx46" id="text.59"/> and <xref ref-type="bibr" rid="bib1.bibx56" id="text.60"/>.</p>
      <p id="d2e2803">The results show that homogeneous mixing (HOM+EA) alone cannot explain the observed droplet dispersion, particularly at the lower levels of the cloud. In contrast, inhomogeneous mixing (INHOM+EA+RA) can generate sufficiently broad droplet spectra but tends to overestimate the presence of large droplets, producing excessively wide distributions. This suggests that real cloud evolution may involve an initial inhomogeneous phase followed by more homogeneous mixing <xref ref-type="bibr" rid="bib1.bibx74" id="paren.61"/>. For the 22 July case, additional simulations were performed, applying INHOM+EA+RA followed by HOM+EA to examine the influence of early inhomogeneous mixing on cloud development. As shown in Fig. <xref ref-type="fig" rid="F4"/>, when the inhomogeneous phase lasts less than 30 s, the simulated results approach those of fully homogeneous mixing, while durations longer than 30 s result in behaviour consistent with inhomogeneous mixing. However, a major limitation of the parcel model in this study is its simplified treatment of ascending thermal trajectories. The model assumes isolated and internally uniform parcels, whereas in real thermals, parcel trajectories evolve dynamically, with varying turbulence, humidity, and mutual entrainment between neighbouring parcels. The transition from inhomogeneous to homogeneous mixing applied here should therefore be regarded as an idealised approximation.</p>

      <fig id="F4" specific-use="star"><label>Figure 4</label><caption><p id="d2e2814">Vertical profiles of observed and simulated CDNC (left), <inline-formula><mml:math id="M105" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (centre-left), and dispersion (centre-right), together with droplet size distributions (right) at four selected temperatures for the 22 July 2022 case. INHOM duration indicates the period of the INHOM+EA+RA phase in the combined INHOM+EA+RA–HOM+EA simulation.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/26/8367/2026/acp-26-8367-2026-f04.png"/>

        </fig>

</sec>
<sec id="Ch1.S4.SS3">
  <label>4.3</label><title>Observed and Simulated Ice-Phase Properties</title>
      <p id="d2e2842">Figure <xref ref-type="fig" rid="F5"/> shows box plots of observed ice number concentration in different temperature intervals for the three selected cases, based on CPI data. Representative CPI images for each case are shown in Figs. S15–S17. To further assess and quantify the impact of SIP on ice number concentration, SIP-off and SIP-on simulations are also shown for the three model configurations, ADIA, HOM+EA, and INHOM+EA+RA, with dashed and solid lines denoting simulations without SIP, referred to here as <inline-formula><mml:math id="M106" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">INP</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, and with SIP, referred to here as <inline-formula><mml:math id="M107" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">ICE</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, respectively. We also examine the temporal evolution of ice enhancement (here defined as <inline-formula><mml:math id="M108" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">ICE</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">INP</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) for six entrainment simulations together with the adiabatic reference, as shown in Fig. <xref ref-type="fig" rid="F6"/>.</p>

      <fig id="F5" specific-use="star"><label>Figure 5</label><caption><p id="d2e2891">Observed and simulated ice particle concentrations as a function of temperature for the three selected cases. In each panel, the boxplots show the observed ice concentrations based primarily on CPI data, and the coloured lines show the parcel model simulations under different entrainment scenarios. Blue, orange, and red lines represent the HOM+EA, INHOM+EA+RA, and ADIA simulations, respectively. Solid lines represent simulations with all SIP mechanisms activated, while dashed lines indicate simulations with SIP processes disabled.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/26/8367/2026/acp-26-8367-2026-f05.png"/>

        </fig>

      <fig id="F6" specific-use="star"><label>Figure 6</label><caption><p id="d2e2902">Time series of ice enhancement for three representative cases: C300 (left), C303 (middle), and C309 (right). The top row <bold>(a–c)</bold> shows simulations using the heterogeneous freezing parameterisation of <xref ref-type="bibr" rid="bib1.bibx14" id="text.62"/>, while the bottom row <bold>(d–f)</bold> shows results using the parameterisation of <xref ref-type="bibr" rid="bib1.bibx15" id="text.63"/>. Colour coding follows Fig. <xref ref-type="fig" rid="F5"/>.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/26/8367/2026/acp-26-8367-2026-f06.png"/>

        </fig>

      <p id="d2e2926">To assess the impact of SIP on ice number concentration, it is first necessary to establish the representation of primary ice production. In this study, primary ice production was parameterised following <xref ref-type="bibr" rid="bib1.bibx14" id="text.64"/>. The resulting <inline-formula><mml:math id="M109" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">INP</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> profiles from the different model configurations, plotted as dashed lines in Fig. <xref ref-type="fig" rid="F5"/>, were broadly consistent with the INP curve shown in the right panel of Fig. S2. For comparison, we also tested the parameterisation of <xref ref-type="bibr" rid="bib1.bibx15" id="text.65"/>. Only minor differences in ice enhancement were found between the two parameterisations, as shown in the upper and lower panels of Fig. <xref ref-type="fig" rid="F6"/>.</p>
      <p id="d2e2950">For the 22 July case, as shown in the left panel of Fig. <xref ref-type="fig" rid="F5"/>, <inline-formula><mml:math id="M110" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">INP</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> peaked at approximately 20, 10, and 25 L<sup>−1</sup> near <inline-formula><mml:math id="M112" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">26</mml:mn></mml:mrow></mml:math></inline-formula> °C in the ADIA, HOM+EA, and INHOM+EA+RA simulations, respectively. HOM+EA produced almost no ice enhancement, whereas both ADIA and INHOM+EA+RA showed increases of about 20 L<sup>−1</sup>, occurring at around 80 and 100 min, respectively, as shown in panel a of Fig. <xref ref-type="fig" rid="F6"/>. Figure S15 shows representative CPI images for the 22 July case. Near <inline-formula><mml:math id="M114" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">8</mml:mn></mml:mrow></mml:math></inline-formula> °C, the images were dominated by small, rounded particles, which are likely to be droplets. No obvious large droplets or well-developed ice crystals were observed at this temperature. At colder levels, some larger and more irregular ice particles were present. However, these were relatively few, and the particle population remained dominated overall by small, rounded particles.</p>
      <p id="d2e3013">For the 25 July case, panel (b) of Fig. <xref ref-type="fig" rid="F6"/> shows that ADIA, HOM+EA, and INHOM+EA+RA produced ice enhancement at around 50, 90, and 95 min, reaching approximately 60, 40, and 20 L<sup>−1</sup>, respectively. ADIA showed two peaks at about 25 and 50 min, with maxima of roughly 20 and 60 L<sup>−1</sup>. HOM showed a single peak of about 35 L<sup>−1</sup> near 105 min, whereas HOM+EA peaked earlier, at around 90 min, with a maximum of about 45 L<sup>−1</sup>. In contrast, INHOM+RA and INHOM+EA+RA both exhibited two peaks, at approximately 25 and 90 min, each reaching about 20 L<sup>−1</sup>. Figure S16 shows representative CPI images for the 25 July case. At approximately <inline-formula><mml:math id="M120" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">8</mml:mn></mml:mrow></mml:math></inline-formula> °C, the available CPI images were consistently dominated by rounded particles, with diameters mainly between 35 and 45 <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. No obvious faceted ice crystals were observed. At <inline-formula><mml:math id="M122" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">16</mml:mn></mml:mrow></mml:math></inline-formula> °C, larger rounded particles became clearly visible, with diameters generally exceeding 100 <inline-formula><mml:math id="M123" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m, and are inferred to represent large droplets. This may reflect the relatively warm cloud base in the 25 July case, which would provide sufficient liquid water for the droplets to grow to larger sizes before reaching colder levels. Potential inhomogeneous mixing may also have promoted a broader droplet size distribution, favouring the formation of larger droplets. In the representative CPI images shown for this temperature, irregular particles and some larger ice crystals were also visible, including hexagonal crystals, columnar crystals, and their aggregates. The red-boxed region may indicate a possible droplet–ice collision event, together with the presence of several small ice crystals and small supercooled raindrops in the surrounding area over a short period. At <inline-formula><mml:math id="M124" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">22</mml:mn></mml:mrow></mml:math></inline-formula> °C, larger droplets and irregular ice crystals were still observed, and partially developed hexagonal ice crystals were also present.</p>
      <p id="d2e3125">For the 1 August case, panel (c) of Fig. <xref ref-type="fig" rid="F6"/> shows that ADIA produced two peaks at around 40 and 70 min, both reaching approximately 40 L<sup>−1</sup>. INHOM+RA and INHOM+EA+RA also exhibited early ice enhancement at around 40 min, with their peak timing close to that of the first ADIA peak. HOM+EA reached a peak of about 40 L<sup>−1</sup> at approximately 100 min, whereas the HOM peak occurred about 10 min later and reached only around 20 L<sup>−1</sup>. Notably, the result for HOM and HOM+EA was reversed in panel (f), where HOM showed greater ice enhancement and reached its peak earlier than HOM+EA. Figure S17 shows representative CPI images for the 1 August case. At approximately <inline-formula><mml:math id="M128" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula> °C, relatively large particles were observed, with sizes reaching 300 to 400 <inline-formula><mml:math id="M129" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m. Columnar ice crystals and some small irregular ice particles were also present. At approximately <inline-formula><mml:math id="M130" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">8</mml:mn></mml:mrow></mml:math></inline-formula> °C, small supercooled raindrops were observed, while the images were dominated by aggregated ice particles, with the largest particle exceeding 500 <inline-formula><mml:math id="M131" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m in diameter. At the colder sampled level, at about <inline-formula><mml:math id="M132" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">11</mml:mn></mml:mrow></mml:math></inline-formula> °C, few obvious ice crystals were observed, and the images were dominated mainly by smaller supercooled raindrops.</p>
      <p id="d2e3213">It is worth noting that, for the three selected cases, the ice number concentrations simulated near the modelled cloud top when SIP was included were generally consistent with the observed ice number concentrations near the highest aircraft passes. However, at warmer levels during parcel development, the simulated ice concentrations were less consistent with the observations (Fig. <xref ref-type="fig" rid="F5"/>). This likely reflects limitations of the BMM as a one-dimensional model, which will be discussed in more detail in the Discussion section.</p>
</sec>
<sec id="Ch1.S4.SS4">
  <label>4.4</label><title>Analysis of Individual SIP Mechanisms</title>
      <p id="d2e3227">Figure <xref ref-type="fig" rid="F7"/> presents sensitivity tests for all three cases, designed to isolate the individual contribution of the four SIP mechanisms, RS, CB, M1, and M2. Primary ice formation was parameterised using <xref ref-type="bibr" rid="bib1.bibx14" id="text.66"/> in all simulations. In each test, only one SIP mechanism was activated, while the other three were switched off. Overall, RS and M1 were largely inactive and produced little ice enhancement in all three cases. By contrast, M2 was active in all cases, whereas CB was only active and produced ice enhancement in the 1 August case.</p>

      <fig id="F7" specific-use="star"><label>Figure 7</label><caption><p id="d2e3237">Time series of ice enhancement from individual SIP mechanisms for three representative cases: 22 July (C300, top row), 25 July (C303, middle row), and 1 August (C309, bottom row). Panels show the results for RS <bold>(a, e, i)</bold>, CB <bold>(b, f, j)</bold>, M1 <bold>(c, g, k)</bold>, and M2 <bold>(d, h, l)</bold>. Colour coding follows Fig. <xref ref-type="fig" rid="F5"/>.</p></caption>
          <graphic xlink:href="https://acp.copernicus.org/articles/26/8367/2026/acp-26-8367-2026-f07.png"/>

        </fig>

      <p id="d2e3260">For the 22 July case, when RS was activated, only INHOM+EA+RA produced a small ice enhancement of about 5 L<sup>−1</sup> at around 20 min. The available CPI images within the temperature range favourable for RS also show no clear large rimed particles (Fig. S15). When M1 was activated, only the inhomogeneous mixing simulations showed a very small ice enhancement during the first 20 min of the simulation, reaching about 7 L<sup>−1</sup>. When M2 was activated, no ice enhancement was observed in the homogeneous simulations. In contrast, ADIA produced a peak ice enhancement of about 20 L<sup>−1</sup> at around 80 min, while INHOM+EA and INHOM+EA+RA produced ice enhancements of about 18 L<sup>−1</sup> at around 100 min.</p>
      <p id="d2e3312">For the 25 July case, no clear ice enhancement was produced when RS, CB, or M1 was activated individually. When M2 was activated, ADIA showed a double peak, reaching about 20 and 40 L<sup>−1</sup> at around 30 and 50 min, respectively. The ice enhancements in INHOM and INHOM+RA occurred at times similar to the first peak in ADIA. By contrast, HOM+EA, INHOM+EA, and INHOM+EA+RA reached peak ice enhancements of about 40, 20, and 20 L<sup>−1</sup>, respectively, at around 85 min. HOM peaked about 10 min later than HOM+EA, and its peak ice enhancement was only about 25 L<sup>−1</sup>. In the CPI images for the 25 July case shown in Fig. S16, both large droplets and large ice particles were frequently observed, providing favourable conditions for M2. Within the red boxed region, a possible droplet–ice collision is visible, with numerous small ice crystals observed close to the possible collision feature. This feature is consistent with fragmentation during the freezing of supercooled droplets upon collision with a more massive ice particle, and this provides observational evidence that M2 may have occurred in this case. In addition, at around <inline-formula><mml:math id="M140" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">22</mml:mn></mml:mrow></mml:math></inline-formula> °C, partially broken ice crystals with an incomplete hexagonal shape were observed. These features may reflect mechanical damage associated with ice–ice collisions, and could suggest a minor contribution from CB.</p>
      <p id="d2e3361">For the 1 August case, no ice enhancement was observed when RS or M1 was activated individually. When CB was activated, ADIA showed no ice enhancement, whereas INHOM+EA and INHOM+EA+RA produced ice enhancements of about 15 L<sup>−1</sup> at around 65 min. HOM+EA and HOM reached about 30 and 15 L<sup>−1</sup> at around 100 and 110 min, respectively. When M2 was activated, ADIA showed a double peak, with ice enhancement occurring at around 40 and 75 min. The inhomogeneous mixing simulations produced ice enhancement at times similar to the first ADIA peak, while HOM+EA and HOM reached about 30 and 25 L<sup>−1</sup> at around 110 and 115 min, respectively. This is consistent with the CPI images shown in Fig. S17, in which large ice particles and relatively large droplets were frequently observed, providing favourable conditions for both M2 and CB.</p>
</sec>
</sec>
<sec id="Ch1.S5">
  <label>5</label><title>Discussion</title>
      <p id="d2e3410">In our study, we investigated four SIP mechanisms (RS, CB, M1, and M2) in 15 deep convective cloud cases observed during the DCMEX campaign from 22 July to 7 August 2022 using a parcel model. Two entrainment representations (homogeneous and inhomogeneous mixing) were incorporated into the model, extending the adiabatic framework of <xref ref-type="bibr" rid="bib1.bibx35" id="text.67"/> to better represent dilution effects on cloud microphysics. Our results suggest that M2 is likely a key mechanism for explaining the high ice particle concentrations observed in deep convective clouds during the DCMEX campaign (see Figs. S6–S10). As for the other mechanisms, RS and M1 remained largely inactive across all 15 cases, whereas CB contributed to ice enhancement in cases with warm cloud-top temperatures, as illustrated by the 1 August case (C309; Fig. S8). It should be noted that RS may be underestimated in our parcel model (see discussion later). However, observations during DCMEX indicate that RS contributed little to SIP in these clouds. This may partly result from the flight pattern adopted during the campaign, which could have limited sampling of regions where RS was active (P. J. Connolly, personal communication, 2026). The entrainment of aerosol was also found to accelerate the collision–coalescence process under homogeneous mixing conditions, leading to earlier ice enhancement, consistent with the hypothesis proposed by <xref ref-type="bibr" rid="bib1.bibx35" id="text.68"/>.</p>
      <p id="d2e3419">To investigate the role of each SIP mechanism, it is first necessary to examine the development of the liquid phase during the early stages of cloud evolution. In our simulations, large droplets with diameters greater than 150 µm are critical for initiating M2, since droplets of this size with higher relative velocities are more likely to produce splashing during collisions. M2 becomes more active as the ratio of collision kinetic energy to surface energy increases in our BMM <xref ref-type="bibr" rid="bib1.bibx60 bib1.bibx35" id="paren.69"/>. Previous studies have also shown that different representations of liquid-phase microphysics, especially the contrast between bulk and bin schemes <xref ref-type="bibr" rid="bib1.bibx50 bib1.bibx36" id="paren.70"/>, can substantially affect the simulated efficiency of SIP. <xref ref-type="bibr" rid="bib1.bibx27" id="text.71"/> and <xref ref-type="bibr" rid="bib1.bibx65" id="text.72"/> both analysed the same observational case of tropical deep convective clouds from the HAIC/HIWC campaign but reached contrasting conclusions regarding the contribution of DS (corresponding to our M1+M2) to ice enhancement, which they indicate differences in the availability of large droplets.</p>
      <p id="d2e3434">We found that representing aerosol entrainment was essential for simulating the observed breadth of the droplet size distribution during the DCMEX campaign. The observations revealed a bimodal spectrum with a distinct minimum near 10 <inline-formula><mml:math id="M144" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m, suggesting the presence of a secondary activation mechanism. This type of distribution has also been reported in previous studies <xref ref-type="bibr" rid="bib1.bibx56 bib1.bibx9 bib1.bibx11" id="paren.73"/>. <xref ref-type="bibr" rid="bib1.bibx35" id="text.74"/> also employed a parcel model to investigate the role of M2 in idealised shallow convective clouds. Their modelling setup is similar to our adiabatic configuration. Although adiabatic assumption can sometimes provide a reasonable approximation, observational and large-eddy simulation (LES) studies have shown that entrainment can begin almost immediately after cloud formation, with turbulent mixing potentially diluting the parcel even within a few hundred metres above cloud base <xref ref-type="bibr" rid="bib1.bibx25" id="paren.75"/>. We found that the adiabatic simulations produced narrower droplet size distributions and tended to substantially overestimate CDNC, as well as LWC by up to approximately 300 %. As a result, the efficiency of SIP was also overestimated, in some cases with relatively warm cloud-base temperatures and deeper cloud layers, such as C306 and C312 (see Fig. S14), the enhancement of ice production was even two to three times greater than in the simulations that included entrainment. Simulations with inhomogeneous mixing tend to lead to an underestimation of CDNC and an overestimation of <inline-formula><mml:math id="M145" display="inline"><mml:mrow><mml:msub><mml:mi>D</mml:mi><mml:mi mathvariant="normal">eff</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, as shown in Fig. <xref ref-type="fig" rid="F3"/>. Although many previous studies suggest that inhomogeneous mixing tends to become more prevalent during later stages of the cloud life cycle, this is likely due to increased entrainment and evaporation near the cloud edges as the updraft weakens <xref ref-type="bibr" rid="bib1.bibx51 bib1.bibx52 bib1.bibx76" id="paren.76"><named-content content-type="pre">e.g.</named-content></xref>. We did not find evidence supporting its dominance in our cases. This may be due to the aircraft tracking the developing clouds, thereby sampling them during the early stages of their lifecycle.</p>
      <p id="d2e3473">Despite the potential importance of entrainment for SIP, they have rarely been systematically evaluated in existing studies. <xref ref-type="bibr" rid="bib1.bibx24" id="text.77"/> used the mesoscale model WRF with the Morrison double-moment microphysics scheme to investigate three SIP mechanisms, RS, CB and DS (corresponding to our M1 and M2) in two alpine clouds. They found CB to be the dominant contributor to SIP, while DS was inactive, likely due to the lack of large droplets. However, the Morrison double-moment scheme in WRF is closer to the homogeneous mixing limit in its evaporation-dilution representation. In our colder cloud-base case (C300), homogeneous mixing likewise produced no active SIP, whereas M2 became active under inhomogeneous mixing due to the production of large droplets. This suggests that the efficiency of DS in <xref ref-type="bibr" rid="bib1.bibx24" id="text.78"/> may have been underestimated. A broad droplet size distribution can accelerate warm-rain formation through collision and coalescence, which can therefore affect SIP. Our results show that, across all SIP-active cases, HOM+EA leads to secondary ice enhancement occurring 15–20 min earlier and increasing in magnitude by approximately 30 %–40 % compared with HOM. <xref ref-type="bibr" rid="bib1.bibx69" id="text.79"/> used a high-resolution LES with double-moment bulk microphysics and explicitly resolved turbulent entrainment to investigate the effects of RS, CB and droplet fragmentation on summer Arctic stratocumulus. However, even at such high resolutions, the grid-scale microphysics in these models typically assumes instantaneous homogeneous mixing <xref ref-type="bibr" rid="bib1.bibx55" id="paren.80"><named-content content-type="pre">e.g.</named-content></xref>. They found DS to be ineffective, yet this assumption cannot resolve the detailed evolution of the droplet size distribution under local dilution and may underestimate spectral broadening caused by size-dependent evaporation, potentially leading to an underestimation of DS.</p>
      <p id="d2e3491">In this study, ice particle observations were primarily based on the processed CPI ice concentration variable, together with CPI imagery. The CPI imagery remains valuable for identifying larger particles and particle habits, and therefore for supporting the interpretation of SIP, as discussed in Sect. 4.4. For the three cases analysed in this study, the CPI images suggest that the coexistence of large droplets with small ice crystals was relatively uncommon, whereas coexistence with larger ice particles was observed more frequently, indirectly suggesting from an observational perspective that M1 may have been relatively inactive in these clouds, while M2 may have played a more important role. However, it should be acknowledged that the relatively limited sample volume of the CPI means that the inferred number concentrations are more strongly influenced by sampling noise, particularly when particle concentrations are low or spatial variability is pronounced <xref ref-type="bibr" rid="bib1.bibx5 bib1.bibx53" id="paren.81"/>. Further study including a more complete intercomparison across multiple probes would be useful to better constrain the observational uncertainty.</p>
      <p id="d2e3497">In an earlier study of summertime cumuli over the same region in New Mexico, <xref ref-type="bibr" rid="bib1.bibx7" id="text.82"/> observed high ice crystal concentrations. They concluded that this enhancement could be explained by the Hallett-Mossop (HM) process, based on the observed coexistence of graupel and supercooled drops larger than <inline-formula><mml:math id="M146" display="inline"><mml:mn mathvariant="normal">24</mml:mn></mml:math></inline-formula> <inline-formula><mml:math id="M147" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>m in diameter near the RS temperature range. However, we did not find this in our results (see Fig. S10), as RS remains inactive throughout all 15 simulated cases. The clouds investigated in their study are similar to those observed during the DCMEX project in 2022. It also should be noted that the ice crystal concentrations reported by <xref ref-type="bibr" rid="bib1.bibx7" id="text.83"/> were likely significantly overestimated due to probe-induced shattering <xref ref-type="bibr" rid="bib1.bibx40 bib1.bibx33" id="paren.84"/>. In our simulations, the model results indicate that RS is not the dominant SIP mechanism in the early stage of cloud development. We also acknowledge that the parcel model, due to its simplified structure, may underestimate the contribution of the RS mechanism. During the Ice in Clouds Experiment-Tropical (ICE-T) field campaign, <xref ref-type="bibr" rid="bib1.bibx47" id="text.85"/> reported cases in tropical maritime cumuli where graupel ascended near cloud tops and was later observed falling back into the rime-splintering zone, suggesting that RS could have been enhanced. Observations and simulations of tropical convective clouds during the Ice in Clouds Experiment-Dust (ICE-D) campaign by <xref ref-type="bibr" rid="bib1.bibx13" id="text.86"/> showed that RS was more active under multi-thermal conditions.</p>
      <p id="d2e3531">It should also be noted that the simplified framework of the parcel model introduces several limitations in the representation of cloud microphysical processes. The aerosol hygroscopicity parameter, <inline-formula><mml:math id="M148" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula>, used in this study was calculated following the Zdanovskii-Stokes-Robinson mixing rule described by <xref ref-type="bibr" rid="bib1.bibx74" id="text.87"/>. The resulting bulk <inline-formula><mml:math id="M149" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula>, which represents a volume-fraction-weighted average of the hygroscopicities of the individual aerosol components, was applied uniformly to all aerosol size bins. However, aerosol particles of different sizes may differ in chemical composition in the real atmosphere, and their <inline-formula><mml:math id="M150" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula> values are therefore not necessarily identical <xref ref-type="bibr" rid="bib1.bibx59 bib1.bibx75" id="paren.88"/>. Because it was derived using volume weighting, this bulk <inline-formula><mml:math id="M151" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula> value may be more reflective of the hygroscopicity of particles in the larger size bins than a number-weighted mean would be. However, applying a single <inline-formula><mml:math id="M152" display="inline"><mml:mi mathvariant="italic">κ</mml:mi></mml:math></inline-formula> value to all aerosol size bins neglects size-dependent aerosol hygroscopicity, introducing uncertainty into the simulated M2 activity, which is sensitive to the formation of larger cloud droplets.</p>
      <p id="d2e3576">Our 1D parcel model is also more representative of the evolution of a single local ascending trajectory than of the full cloud system, in which multiple air parcels interact continuously. In the observations (e.g. Figs. S15–S17), ice crystals observed in the lower part of the cloud may not arise solely from in situ formation within a single local ascending parcel, but may also reflect contributions from ice transported from other cloud regions through vertical or lateral exchange, together with redistribution associated with turbulent entrainment and mixing. In addition, as large ice particles formed in the model cannot leave the parcel through sedimentation, the local <inline-formula><mml:math id="M153" display="inline"><mml:mrow><mml:msub><mml:mi>N</mml:mi><mml:mi mathvariant="normal">ice</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> in the upper part of the cloud may be overestimated. These results are therefore more suitable for interpreting local processes and the relative contributions of individual mechanisms than for being regarded as a complete representation of the three-dimensional ice-phase structure of the whole deep convective cloud.</p>
      <p id="d2e3590">To assess the impact of primary ice nucleation on SIP, we tested two INP parameterizations, <xref ref-type="bibr" rid="bib1.bibx14" id="text.89"/> and <xref ref-type="bibr" rid="bib1.bibx15" id="text.90"/>. The former is more appropriate for this study, as it was developed from measurements in the inflow clear air below cloud bases and in the environment around clouds during the DCMEX project, whereas the latter is a more general parameterization. However, our simulations showed negligible differences in SIP efficiency between the two, suggesting that once secondary ice multiplication is triggered, the choice of INP parameterization has limited influence on the final ice particle concentrations under these convective conditions.</p>
</sec>
<sec id="Ch1.S6" sec-type="conclusions">
  <label>6</label><title>Conclusions</title>
      <p id="d2e3607">In this study, we implemented entrainment parameterisations in the bin microphysics parcel model, including two different mixing representations (homogeneous and inhomogeneous) and external aerosol entrainment. These schemes were applied to simulations of summer continental deep convective clouds over New Mexico to assess the impacts of dry air and aerosol entrainment on cloud microphysical properties and secondary ice production. The representation of entrainment leads to systematic differences in secondary ice production by modifying liquid-phase microphysical properties (e.g. cloud droplet number concentration, liquid water content, and droplet size distribution), thereby affecting both the efficiency and onset of ice enhancement.</p>
      <p id="d2e3610">Our results show that the observed broad and bimodal droplet size distribution can only be reproduced when entrainment is included, particularly aerosol entrainment, within the parcel model framework for individual air trajectories. This is consistent with previous studies on the effects of dilution on the warm phase of clouds. In our adiabatic parcel simulations, cloud droplet number concentration and liquid water content are much higher than in simulations that include entrainment, with liquid water content exceeding entrainment cases by up to <inline-formula><mml:math id="M154" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 300 %. As a result, ice enhancement is up to 2–3 times larger in some cases. Under homogeneous mixing, aerosol entrainment tends to result in a broader droplet size distribution, with the SIP peak occurring 15–20 min earlier and reaching a higher peak value (by about 25 %) than in simulations without aerosol entrainment. For shallow cloud cases, aerosol entrainment has little impact on SIP under inhomogeneous mixing. In deep cloud cases, inhomogeneous mixing results in an early SIP maximum (within <inline-formula><mml:math id="M155" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 20 min) associated with an excess of large droplets; however, aerosol entrainment shifts the SIP peak to a timing comparable to that under homogeneous mixing. In our simulations of the DCMEX cases over New Mexico, most cases are best represented by homogeneous mixing combined with aerosol entrainment. We also find no evidence that inhomogeneous mixing dominates in the simulated clouds, which may be due to the aircraft primarily sampling clouds during their early stages of development.</p>
      <p id="d2e3627">When the four SIP mechanisms (RS, CB, M1 and M2) are examined separately, our results suggest that M2, as currently understood and represented in the model, is the most important contributor to ice enhancement in the DCMEX deep convective cloud cases. M1 remains largely inactive, likely due to limitations of the parcel model in which the absence of sedimentation leads to an accumulation of ice crystals and a progressive reduction in supercooled liquid water, thereby suppressing collisions between large droplets and small ice crystals required for efficient M1. CB contributes to ice enhancement in some shallower cloud cases but produces little ice enhancement in the deeper cloud cases. Our results suggest that RS alone cannot account for the high ice crystal concentrations observed during DCMEX. This contrasts with earlier interpretations for summertime cumuli over the same region, which attributed ice enhancement mainly to the Hallett–Mossop process <xref ref-type="bibr" rid="bib1.bibx7" id="paren.91"/>. In our simulations, RS is inefficient during the early stages of cloud development because the temperature range favourable for rime splintering does not coincide with the presence of sufficiently large droplets and ice particles. The contribution of RS may be underestimated in the parcel model framework, as multi-thermal circulations and interactions between different air parcels are not represented. Future extensions of the model that include sedimentation and interactions between different air parcels will therefore be required to better assess the potential role of RS in deep convective clouds.</p>
      <p id="d2e3633">Further progress in understanding M2 will require improved laboratory constraints on freezing-drop fragmentation and continued development of idealised parcel modelling frameworks that include sedimentation and interactions between different air parcels. Incorporating the effects of entrainment on secondary ice production will also be critical for achieving an accurate representation of ice-phase processes in numerical weather prediction and other large-scale models.</p>
</sec>

      
      </body>
    <back><notes notes-type="codedataavailability"><title>Code and data availability</title>

      <p id="d2e3640">The version of the bin-microphysics model used in this study is archived on Zenodo at <ext-link xlink:href="https://doi.org/10.5281/zenodo.20646114" ext-link-type="DOI">10.5281/zenodo.20646114</ext-link> <xref ref-type="bibr" rid="bib1.bibx63" id="paren.92"/> and is also available from the corresponding GitHub repository at <uri>https://github.com/bowenzhuportman/bin-microphysics-model</uri> (last access: 11 June 2026). The FAAM aircraft observations used to initialise and evaluate the simulations are available from the Centre for Environmental Data Analysis (CEDA) archive at <ext-link xlink:href="https://doi.org/10.5285/B1211AD185E24B488D41DD98F957506C" ext-link-type="DOI">10.5285/B1211AD185E24B488D41DD98F957506C</ext-link> <xref ref-type="bibr" rid="bib1.bibx18" id="paren.93"/>.</p>
  </notes><app-group>
        <supplementary-material position="anchor"><p id="d2e3658">The supplement related to this article is available online at <inline-supplementary-material xlink:href="https://doi.org/10.5194/acp-26-8367-2026-supplement" xlink:title="pdf">https://doi.org/10.5194/acp-26-8367-2026-supplement</inline-supplementary-material>.</p></supplementary-material>
        </app-group><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d2e3667">BZP and PJC conceived the original study. PJC developed the model code. BZP performed the simulations, analysed the data, and wrote the manuscript. HW provided key observational data. PJC, AMB and RLJ contributed to scientific discussions and provided comments on the manuscript.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d2e3673">The contact author has declared that none of the authors has any competing interests.</p>
  </notes><notes notes-type="disclaimer"><title>Disclaimer</title>

      <p id="d2e3679">Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims made in the text, published maps, institutional affiliations, or any other geographical representation in this paper. The authors bear the ultimate responsibility for providing appropriate place names. Views expressed in the text are those of the authors and do not necessarily reflect the views of the publisher.</p>
  </notes><ack><title>Acknowledgements</title><p id="d2e3685">Airborne data were obtained using the FAAM Airborne Laboratory BAe-146 Atmospheric Research Aircraft, operated by Airtask Ltd, managed by the National Centre for Atmospheric Science, leased through the University of Leeds, and owned by UK Research and Innovation and the Natural Environment Research Council.</p><p id="d2e3687">The author used ChatGPT to assist with language editing and improving the clarity of the manuscript. All scientific analysis, interpretations, and conclusions were performed by the authors.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d2e3692">This research has been supported by the UK Natural Environment Research Council (grant nos. NE/T006420/1 and NE/T006439/1, Deep Convective Microphysics Experiment, DCMEX) and the European Union's Horizon Europe programme through the CERTAINTY project under grant agreement No. 101137680.</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d2e3699">This paper was edited by Greg McFarquhar and reviewed by two anonymous referees.</p>
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