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Abstract. The onset of ice nucleation in mixed-phase clouds determines the lifetime and microphysical properties of ice clouds. In this work, we develop a novel method that differentiates between various phases of mixed-phase clouds, such as clouds dominated by pure liquid or pure ice segments, compared with those having ice crystals surrounded by supercooled liquid water droplets or vice versa. Using this method, we examine the relationship between the macrophysical and microphysical properties of Southern Ocean mixed-phase clouds at −40 to 0 °C (e.g. stratiform and cumuliform clouds) based on the in situ aircraft-based observations during the US National Science Foundation Southern Ocean Clouds, Radiation, Aerosol Transport Experimental Study (SOCRATES) flight campaign. The results show that the exchange between supercooled liquid water and ice crystals from a macrophysical perspective, represented by the increasing spatial ratio of regions containing ice crystals relative to the total in-cloud region (defined as ice spatial ratio), is positively correlated with the phase exchange from a microphysical perspective, represented by the increasing ice water content (IWC), decreasing liquid water content (LWC), increasing ice mass fraction, and increasing ice particle number fraction (IPNF). The mass exchange between liquid and ice becomes more significant during phase 3 when pure ice cloud regions (ICRs) start to appear. Occurrence frequencies of cloud thermodynamic phases show a significant phase change from liquid to ice at a similar temperature (i.e. −17.5 °C) among three types of definitions of mixed-phase clouds based on ice spatial ratio, ice mass fraction, or IPNF. Aerosol indirect effects are quantified for different phases using number concentrations of aerosols greater than 100 or 500 nm (N>100 and N>500, respectively). N>500 shows stronger positive correlations with ice spatial ratios compared with N>100. This result indicates that larger aerosols potentially contain ice-nucleating particles (INPs), which facilitate the formation of ice crystals in mixed-phase clouds. The impact of N>500 is also more significant in phase 2 when ice crystals just start to appear in the mixed phase compared with phase 3 when pure ICRs have formed, possibly due to the competing aerosol indirect effects on primary and secondary ice production in phase 3. The thermodynamic and dynamic conditions are quantified for each phase. The results show stronger in-cloud turbulence and higher updraughts in phases 2 and 3 when liquid and ice coexist compared with pure liquid or ice (phases 1 and 4, respectively). The highest updraughts and turbulence are seen in phase 3 when supercooled liquid droplets are surrounded by ice crystals. These results indicate both updraughts and turbulence support the maintenance of supercooled liquid water amongst ice crystals. Overall, these results illustrate the varying effects of aerosols, thermodynamics, and dynamics through various stages of mixed-phase cloud evolution based on this new method that categorizes cloud phases. 

Abstract Three climate models are evaluated using in situ airborne observations from the Southern Ocean Clouds, Radiation, Aerosol Transport Experimental Study (SOCRATES) campaign. The evaluation targets cloud phases, microphysical properties, thermodynamic conditions, and aerosol indirect effects from −40°C to 0°C. Compared with 580‐s averaged observations (i.e., 100 km horizontal scale), the Community Atmosphere Model version 6 (CAM6) shows the most similar result for cloud phase frequency distribution and allows more liquid‐containing clouds below −10°C compared with its predecessor—CAM5. The Energy Exascale Earth System Model (E3SM) underestimates (overestimates) ice phase frequencies below (above) −20°C. CAM6 and E3SM show liquid and ice water contents (i.e., LWC and IWC) similar to observations from −25°C to 0°C, but higher LWC and lower IWC than observations at lower temperatures. Simulated in‐cloud RH shows higher minimum values than observations, possibly restricting ice growth during sedimentation. As number concentrations of aerosols larger than 500 nm (Na₅₀₀) increase, observations show increases of LWC, IWC, liquid, and ice number concentrations (N_liq, N_ice). Number concentrations of aerosols larger than 100 nm (Na₁₀₀) only show positive correlations with LWC and N_liq. From −20°C to 0°C, higher aerosol number concentrations are correlated with lower glaciation ratio and higher cloud fraction. From −40°C to −20°C, large aerosols show positive correlations with glaciation ratio. CAM6 shows small increases of LWC and N_liqwith Na₅₀₀and Na₁₀₀. E3SM shows small increases of N_icewith Na₅₀₀. Overall, CAM6 and E3SM underestimate aerosol indirect effects on ice crystals and supercooled liquid droplets over the Southern Ocean.