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1. Studies on the Competition Between Homogeneous and Heterogeneous Ice Nucleation in Cirrus Formation

   https://doi.org/10.1029/2021JD035805  

   Kärcher, B. ; DeMott, P. J. ; Jensen, E. J. ; Harrington, J. Y. ( February 2022 , Journal of Geophysical Research: Atmospheres)

   Cirrus ice crystals are produced heterogeneously on ice‐nucleating particles (INPs) and homogeneously in supercooled liquid solution droplets. They grow by uptake of water molecules from the ice‐supersaturated vapor. The precursor particles, characterized by disparate ice nucleation abilities and number concentrations, compete for available vapor during ice formation events. We investigate cirrus formation events systematically in different temperature and updraft regimes, and for different INP number concentrations and time‐independent nucleation efficiencies. We consider vertical air motion variability due to mesoscale gravity waves and effects of supersaturation‐dependent deposition coefficients for water molecules on ice surfaces. We analyze ice crystal properties to better understand the dynamics of competing nucleation processes. We study the reduction of ice crystal numbers produced by homogeneous freezing due to INPs in both, individual simulations assuming constant updraft speeds and in ensemble simulations based on a stochastic representation of vertical wind speed fluctuations. We simulate and interpret probability distributions of total nucleated ice crystal number concentrations, showing signatures of homogeneous and heterogeneous nucleation. At typically observed, mean updraft speeds (≈15 cm s⁻¹) competing nucleation should occur frequently, even at rather low INP number concentrations (<10 L⁻¹). INPs increase cirrus occurrence and may alter cirrus microphysical properties without entirely suppressing homogeneous freezingmore »events. We suggest to improve ice growth models, especially for low cirrus temperatures (<220 K) and low ice supersaturation (<0.3).

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2. Approximate Models for Lateral Growth on Ice Crystal Surfaces during Vapor Depositional Growth

   https://doi.org/10.1175/JAS-D-20-0228.1  

   Harrington, Jerry Y. ; Pokrifka, Gwenore F. ( March 2021 , Journal of the Atmospheric Sciences)

   Abstract Measurements show that after facets form on frozen water droplets, those facets grow laterally across the crystal surface leading to an increase in volume and surface area with only a small increase in maximum dimension. This lateral growth of the facets is distinctly different from that predicted by the capacitance model and by the theory of faceted growth. In this paper we develop two approximate theories of lateral growth, one that is empirical and one that uses explicit growth mechanisms. We show that both theories can reproduce the overall features of lateral growth on a frozen, supercooled water droplet. Both theories predict that the area-average deposition coefficient should decrease in time as the particle grows, and this result may help explain the divergence of some prior measurements of the deposition coefficient. The theories may also explain the approximately constant mass growth rates that have recently been found in some measurements. We also show that the empirical theory can reproduce the lateral growth that occurs when a previously sublimated crystal is regrown, as may happen during the recycling of crystals in cold clouds.
3. Effective Density Derived from Laboratory Measurements of the Vapor Growth Rates of Small Ice Crystals at −65° to −40°C

   https://doi.org/10.1175/JAS-D-22-0077.1  

   Pokrifka, Gwenore F. ; Moyle, Alfred M. ; Harrington, Jerry Y. ( February 2023 , Journal of the Atmospheric Sciences)

   Abstract An electrodynamic levitation thermal-gradient diffusion chamber was used to grow 268 individual, small ice particles (initial radii of 8–26 μ m) from the vapor, at temperatures ranging from −65° to −40°C, and supersaturations up to liquid saturation. Growth limited by attachment kinetics was frequently measured at low supersaturation, as shown in prior work. At high supersaturation, enhanced growth was measured, likely due to the development of branches and hollowed facets. The effects of branching and hollowing on particle growth are often treated with an effective density ρ eff . We fit the measured time series with two different models to estimate size-dependent ρ eff values: the first model decreases ρ eff to an asymptotic deposition density ρ dep , and the second models ρ eff by a power law with exponent P . Both methods produce similar results, though the fits with ρ dep typically have lower relative errors. The fit results do not correspond well with models of isometric or planar single-crystalline growth. While single-crystalline columnar crystals correspond to some of the highest growth rates, a newly constructed geometric model of budding rosette crystals produces the best match with the growth data. The relative frequency of occurrence ofmore »ρ dep and P values show a clear dependence on ice supersaturation normalized to liquid saturation. We use these relative frequencies of ρ dep and P to derive two supersaturation-dependent mass–size relationships suitable for cloud modeling applications.« less
4. Re-evaluating cloud chamber constraints on depositional ice growth in cirrus clouds – Part 1: Model description and sensitivity tests

   https://doi.org/10.5194/acp-23-6043-2023  

   Lamb, Kara D. ; Harrington, Jerry Y. ; Clouser, Benjamin W. ; Moyer, Elisabeth J. ; Sarkozy, Laszlo ; Ebert, Volker ; Möhler, Ottmar ; Saathoff, Harald ( January 2023 , Atmospheric Chemistry and Physics)

   Abstract. Ice growth from vapor deposition is an important process for the evolution of cirrus clouds, but the physics of depositional ice growth at the low temperatures (<235 K) characteristic of the upper troposphere and lower stratosphere is not well understood. Surface attachment kinetics, generally parameterized as a deposition coefficient αD, control ice crystal habit and also may limit growth rates in certain cases, but significant discrepancies between experimental measurements have not been satisfactorily explained. Experiments on single ice crystals have previously indicated the deposition coefficient is a function of temperature and supersaturation, consistent with growth mechanisms controlled by the crystal's surface characteristics. Here we use observations from cloud chamber experiments in the Aerosol Interactions and Dynamics in theAtmosphere (AIDA) aerosol and cloud chamber to evaluate surface kinetic models in realistic cirrus conditions. These experiments have rapidly changing temperature, pressure, and ice supersaturation such that depositional ice growth may evolve from diffusion limited to surface kinetics limited over the course of a single experiment. In Part 1, we describe the adaptation of a Lagrangian parcel model with the Diffusion Surface Kinetics Ice Crystal Evolution (DiSKICE) model (Zhang and Harrington, 2014) to the AIDA chamber experiments. We compare the observed ice water content andmore »saturation ratios to that derived under varying assumptions for ice surface growth mechanisms for experiments simulating ice clouds between 180 and 235 K and pressures between 150 and 300 hPa. We found that both heterogeneous and homogeneous nucleation experiments at higher temperatures (>205 K) could generally be modeled consistently with either a constant deposition coefficient or the DiSKICE model assuming growth on isometric crystals via abundant surface dislocations. Lower-temperature experiments showed more significant deviations from any depositional growth model, with different ice growth rates for heterogeneous and homogeneous nucleation experiments.« less
5. The University of Washington Ice–Liquid Discriminator (UWILD) improves single-particle phase classifications of hydrometeors within Southern Ocean clouds using machine learning

   https://doi.org/10.5194/amt-14-7079-2021  

   Atlas, Rachel ; Mohrmann, Johannes ; Finlon, Joseph ; Lu, Jeremy ; Hsiao, Ian ; Wood, Robert ; Diao, Minghui ( January 2021 , Atmospheric Measurement Techniques)

   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 accuracymore »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 (0.170.33 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.« less