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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. 

Cirrus cloud formation and evolution are subject to the influences of thermodynamic and dynamic conditions and aerosol indirect effects (AIEs). This study developed near global-scale in-situ aircraft observational datasets based on 12 field campaigns that spanned from the polar regions to the tropics, from 2008 to 2016. Cirrus cloud microphysical properties were investigated at temperatures ≤ ‑40 °C, including ice water content (IWC), ice crystal number concentration (Ni), and number-weighted mean diameter (Di). Positive correlations between the fluctuations of ice microphysical properties and the fluctuations of aerosol number concentrations for larger (> 500 nm) and smaller (> 100 nm) aerosols (i.e., Na500 and Na100, respectively) were found, with stronger AIE from larger aerosols than smaller ones. Machine learning (ML) models showed that using relative humidity with respect to ice (RHi) as a predictor significantly increases the accuracy of predicting cirrus occurrences compared with temperature, vertical velocity (w), and aerosol number concentrations. The ML predictions of IWC fluctuations showed higher accuracies when larger aerosols were used as an predictor compared with smaller aerosols, indicating the stronger AIE from larger aerosols than smaller ones, even though their AIEs are more similar when predicting the occurrences of cirrus. It is also important to capture the spatial variabilities of large aerosols at smaller scales as well as those of smaller aerosols at coarser scales to accurately simulate IWC in cirrus. These results can be used to improve understanding of aerosol-cloud interactions and evaluate model parameterizations of cirrus cloud properties and processes. 

Abstract High‐latitudinal mixed‐phase clouds significantly affect Earth's radiative balance. Observations of cloud and radiative properties from two field campaigns in the Southern Ocean and Antarctica were compared with two global climate model simulations. A cyclone compositing method was used to quantify “dynamics‐cloud‐radiation” relationships relative to the extratropical cyclone centers. Observations show larger asymmetry in cloud and radiative properties between western and eastern sectors at McMurdo compared with Macquarie Island. Most observed quantities at McMurdo are higher in the western (i.e., post‐frontal) than the eastern (frontal) sector, including cloud fraction, liquid water path (LWP), net surface shortwave and longwave radiation (SW and LW), except for ice water path (IWP) being higher in the eastern sector. The two models were found to overestimate cloud fraction and LWP at Macquarie Island but underestimate them at McMurdo Station. IWP is consistently underestimated at both locations, both sectors, and in all seasons. Biases of cloud fraction, LWP, and IWP are negatively correlated with SW biases and positively correlated with LW biases. The persistent negative IWP biases may have become one of the leading causes of radiative biases over the high southern latitudes, after correcting the underestimation of supercooled liquid water in the older model versions. By examining multi‐scale factors from cloud microphysics to synoptic dynamics, this work will help increase the fidelity of climate simulations in this remote region. 

Abstract Mixed‐phase clouds contribute to substantial uncertainties in global climate models due to their complex microphysical properties. Former model evaluations almost exclusively rely on satellite observations to assess cloud phase distributions globally. This study investigated mixed‐phase cloud properties using near global‐scale in situ observation data sets from 14 flight campaigns in combination with collocated output from a global climate model. The Southern Hemisphere (SH) shows significantly higher occurrence frequencies and higher mass fractions of supercooled liquid water than Northern Hemisphere (NH) based on observations at 0.2 and 100 km horizontal scales. Such hemispheric asymmetry is not captured by the model. The model also consistently overestimates liquid water content (LWC) in all cloud phases but shows ice water content (IWC) biases that vary with phase. Key processes contributing to model biases in phase partition can be identified through the combination of evaluation of phase frequency, liquid mass fraction, LWC and IWC. 

Abstract. Aerosols affect cirrus formation and evolution, yet quantificationof these effects remain difficult based on in situ observations due to thecomplexity of nucleation mechanisms and large variabilities in icemicrophysical properties. This work employed a method to distinguish fiveevolution phases of cirrus clouds based on in situ aircraft-basedobservations from seven U.S. National Science Foundation (NSF) and five NASAflight campaigns. Both homogeneous and heterogeneous nucleation werecaptured in the 1 Hz aircraft observations, inferred from the distributionsof relative humidity in the nucleation phase. Using linear regressions toquantify the correlations between cirrus microphysical properties andaerosol number concentrations, we found that ice water content (IWC) and icecrystal number concentration (Ni) show strong positive correlations withlarger aerosols (>500 nm) in the nucleation phase, indicatingstrong contributions of heterogeneous nucleation when ice crystals firststart to nucleate. For the later growth phase, IWC and Ni show similarpositive correlations with larger and smaller (i.e., >100 nm)aerosols, possibly due to fewer remaining ice-nucleating particles in thelater growth phase that allows more homogeneous nucleation to occur. Both200 m and 100 km observations were compared with the nudged simulations fromthe National Center for Atmospheric Research (NCAR) Community AtmosphereModel version 6 (CAM6). Simulated aerosol indirect effects are weaker thanthe observations for both larger and smaller aerosols for in situ cirrus,while the simulated aerosol indirect effects are closer to observations inconvective cirrus. The results also indicate that simulations overestimatehomogeneous freezing, underestimate heterogeneous nucleation andunderestimate the continuous formation and growth of ice crystals as cirrusclouds evolve. Observations show positive correlations of IWC, Ni and icecrystal mean diameter (Di) with respect to Na in both the Northern and SouthernHemisphere (NH and SH), while the simulations show negative correlations inthe SH. The observations also show higher increases of IWC and Ni in the SHunder the same increase of Na than those shown in the NH, indicating highersensitivity of cirrus microphysical properties to increases of Na in the SHthan the NH. The simulations underestimate IWC by a factor of 3–30 in theearly/later growth phase, indicating that the low bias of simulated IWC wasdue to insufficient continuous ice particle formation and growth. Sucha hypothesis is consistent with the model biases of lower frequencies of icesupersaturation and lower vertical velocity standard deviation in theearly/later growth phases. Overall, these findings show that aircraftobservations can capture both heterogeneous and homogeneous nucleation, andtheir contributions vary as cirrus clouds evolve. Future model developmentis also recommended to evaluate and improve the representation of watervapor and vertical velocity on the sub-grid scale to resolve theinsufficient ice particle formation and growth after the initial nucleationevent. 

Aerosols affect cirrus formation and evolution, yet quantification of these effects remain difficult based on in-situ observations due to the complexity of nucleation mechanisms and large variabilities in ice microphysical properties. This work employed a method to distinguish five evolution phases of cirrus clouds based on in-situ aircraft-based observations from seven U.S. National Science Foundation (NSF) and five NASA flight campaigns. Both homogeneous and heterogeneous nucleation were captured in the 1-Hz aircraft observations, inferred from the distributions of relative humidity in the nucleation phase. Using linear regressions to quantify the correlations between cirrus microphysical properties and aerosol number concentrations, we found that ice water content (IWC) and ice crystal number concentration (Ni) show strong positive correlations with larger aerosols (> 500 nm) in the nucleation phase, indicating strong contributions of heterogeneous nucleation when ice crystals first start to nucleate. For the later growth phase, IWC and Ni show similar positive correlations with larger and smaller (i.e., > 100 nm) aerosols, possibly due to fewer remaining ice nucleating particles in the later growth phase that allows more homogeneous nucleation to occur. Both 200-m and 100-km observations were compared with the nudged simulations from the National Center for Atmospheric Research (NCAR) Community Atmosphere Model version 6 (CAM6). Simulated aerosol indirect effects are weaker than the observations for both larger and smaller aerosols. Observations show stronger aerosol indirect effects (i.e., positive correlations between IWC, Ni and Na) in the Southern Hemisphere (SH) compared with the Northern Hemisphere (NH), while the simulations show negative correlations in the SH. The simulations underestimate IWC by a factor of 3 – 30 in the early/later growth phase, indicating that the low bias of simulated IWC was due to insufficient ice particle growth. Such hypothesis is consistent with the model biases of lower frequencies of ice supersaturation and lower vertical velocity standard deviation in the early/later growth phases. Overall, these findings show that aircraft observations can capture the competitions between heterogeneous and homogeneous nucleation, and their contributions vary as cirrus clouds evolve. Future model development is also recommended to evaluate and improve the representation of water vapor and vertical velocity on the sub-grid scale to resolve the insufficient ice particle growth. 

Abstract Understanding distributions of cloud thermodynamic phases is important for accurately representing cloud radiative effects and cloud feedback in a changing climate. Satellite‐based cloud phase data have been frequently used to compare with climate models, yet few studies validated them against in situ observations at a near‐global scale. This study aims to validate three satellite‐based cloud phase products using a compositive in situ airborne data set developed from 11 flight campaigns. Latitudinal‐altitudinal cross sections of cloud phase occurrence frequencies are examined. The Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) show the most similar vertical profiles of ice phase frequencies compared with in situ observations. The CloudSat data overestimate mixed‐phase frequencies up to 15 km but provide better sampling through cloud layers than lidar data. The DARDAR (raDAR/liDAR) data show a sharp transition between ice and liquid phase and overestimate ice phase frequency at most altitudes and latitudes. The satellite data are further evaluated for various latitudes, longitudes, and seasons, which show higher ice phase frequency in the extratropics in their respective wintertime and smaller impacts from longitudinal variations. The Southern Ocean shows a thicker mixing region where liquid and ice phases have similar frequencies compared with tropics and Northern Hemisphere (NH) extratropics. Two comparison methods with different spatiotemporal windows show similar results, which demonstrates the statistical robustness of these comparisons. Overall, this study develops a near global‐scale in situ observational data set to assess the accuracy of satellite‐based cloud phase products and investigates the key factors affecting the distributions of cloud phases. 

Abstract. Cirrus cloud radiative effects are largely affected byice microphysical properties, including ice water content (IWC), ice crystalnumber concentration (Ni) and mean diameter (Di). These characteristics varysignificantly due to thermodynamic, dynamical and aerosol conditions. Inthis work, a global-scale observation dataset is used to examine regionalvariations of cirrus cloud microphysical properties, as well as several keycontrolling factors, i.e., temperature, relative humidity with respect toice (RHi), vertical velocity (w) and aerosol number concentrations (Na).Results are compared with simulations from the National Center forAtmospheric Research (NCAR) Community Atmosphere Model version 6 (CAM6).Observed and simulated ice mass and number concentrations are constrained to≥62.5 µm to reduce potential uncertainty from shattered ice indata collection. The differences between simulations and observations arefound to vary with latitude and temperature. Comparing with averagedobservations at ∼100 km horizontal scale, simulations arefound to underestimate (overestimate) IWC by a factor of 3–10 in theNorthern (Southern) Hemisphere. Simulated Ni is overestimated in mostregions except the Northern Hemisphere midlatitudes. Simulated Di isunderestimated by a factor of 2, especially for warmer conditions(−50 to −40 ∘C), possibly due tomisrepresentation of ice particle growth/sedimentation. For RHi effects, thefrequency and magnitude of ice supersaturation are underestimated insimulations for clear-sky conditions. The simulated IWC and Ni show bimodaldistributions with maximum values at 100 % and 80 % RHi, differing fromthe unimodal distributions that peak at 100 % in the observations. For weffects, both observations and simulations show variances of w (σw) decreasing from the tropics to polar regions, but simulations show muchhigher σw for the in-cloud condition than the clear-sky condition.Compared with observations, simulations show weaker aerosol indirect effectswith a smaller increase of IWC and Di at higher Na. These findings provide anobservation-based guideline for improving simulated ice microphysicalproperties and their relationships with key controlling factors at variousgeographical locations. 

Abstract. Mixed-phase Southern Ocean clouds are challenging to simulate, and theirrepresentation in climate models is an important control on climatesensitivity. In particular, the amount of supercooled water and frozen massthat they contain in the present climate is a predictor of their planetaryfeedback in a warming climate. The recent Southern Ocean Clouds, Radiation, Aerosol Transport Experimental Study (SOCRATES) vastly increased theamount of in situ data available from mixed-phase Southern Ocean clouds usefulfor model evaluation. Bulk measurements distinguishing liquid and ice watercontent are not available from SOCRATES, so single-particle phaseclassifications from the Two-Dimensional Stereo (2D-S) probe are invaluablefor quantifying mixed-phase cloud properties. Motivated by the presence oflarge biases in existing phase discrimination algorithms, we develop a noveltechnique for single-particle phase classification of binary 2D-S images usinga random forest algorithm, which we refer to as the University of WashingtonIce–Liquid Discriminator (UWILD). UWILD uses 14 parameters computed frombinary image data, as well as particle inter-arrival time, to predict phase.We use liquid-only and ice-dominated time periods within the SOCRATES datasetas training and testing data. This novel approach to model training avoidsmajor pitfalls associated with using manually labeled data, including reducedmodel generalizability and high labor costs. We find that UWILD is wellcalibrated and has an overall accuracy of 95 % compared to72 % and 79 % for two existing phase classificationalgorithms that we compare it with. UWILD improves classifications of smallice crystals and large liquid drops in particular and has more flexibilitythan the other algorithms to identify both liquid-dominated and ice-dominatedregions within the SOCRATES dataset. UWILD misclassifies a small percentageof large liquid drops as ice. Such misclassified particles are typicallyassociated with model confidence below 75 % and can easily befiltered out of the dataset. UWILD phase classifications show that particleswith area-equivalent diameter (Deq)  < 0.17 mm are mostlyliquid at all temperatures sampled, down to −40 ∘C. Largerparticles (Deq>0.17 mm) are predominantly frozen at alltemperatures below 0 ∘C. Between 0 and 5 ∘C,there are roughly equal numbers of frozen and liquid mid-sized particles (0.17<0.33 mm), and larger particles (Deq>0.33 mm) are mostly frozen. We also use UWILD's phaseclassifications to estimate sub-1 Hz phase heterogeneity, and we showexamples of meter-scale cloud phase heterogeneity in the SOCRATES dataset.