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A Taxonomy of Snow Crystal Growth Behaviors: 1. Using c-axis Ice Needles as Seed Crystals

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 Publication date 2021
  fields Physics
and research's language is English




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I describe a new approach to the classification of snow crystal morphologies that focuses on the most common growth behaviors that appear in normal air under conditions of constant applied temperature and water-vapor supersaturation. The resulting morphological structures are generally robust with respect to small environmental changes and thus should be especially amenable to computational modeling. Because spontaneous structure formation depends on initial conditions, the choice of seed crystal can be an important consideration, and I have found that slender c-axis ice needles provide an exceptionally good starting point for this series of investigations. A sharp needle tip exposes a single basal surface that often simplifies subsequent morphological development, and the absence of a nearby substrate allows for the exploration of a broad range of supersaturations with well-controlled boundary conditions. The overarching goal of this endeavor is to facilitate detailed quantitative comparisons between laboratory ice-growth experiments and corresponding computational models, which will should greatly improve our understanding of the ice/vapor molecular attachment kinetics as well as our ability to model diffusion-limited growth dynamics in the ice/vapor system. This specific case-study of water ice connects broadly to many areas in aqueous chemistry, cryobiology, and environmental science, while the physical principles of molecular attachment kinetics and diffusion-limited growth apply more generally to other systems in crystal growth and materials science.



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I examine a variety of snow crystal growth measurements taken at a temperature of -5 C, as a function of supersaturation, background gas pressure, and crystal morphology. Both plate-like and columnar prismatic forms are observed under different conditions at this temperature, along with a diverse collection of complex dendritic structures. The observations can all be reasonably understood using a single comprehensive physical model for the basal and prism attachment kinetics, together with particle diffusion of water vapor through the surrounding medium and other well-understood physical processes. A critical model feature is structure-dependent attachment kinetics (SDAK), for which the molecular attachment kinetics on a faceted surface depend strongly on the nearby mesoscopic structure of the crystal.
I examine a variety snow crystal growth experiments performed at temperatures near -2 C, as a function of supersaturation, background gas pressure, and crystal morphology. Although the different experimental data were obtained using quite diverse experimental techniques, the resulting measurements can all be reasonably understood using a single comprehensive physical model for the basal and prism attachment kinetics, together with particle diffusion of water vapor through the surrounding medium and other well-understood physical processes. As with the previous paper in this series, comparing and reconciling different data sets at a single temperature yields significant insights into the underlying physical processes that govern snow crystal growth dynamics.
In this paper I examine snow crystal growth near -4 C in comparison with a comprehensive model that includes Structure-Dependent Attachment Kinetics (SDAK). Together with the previous paper in this series that investigated growth near 14 C, I show that a substantial body of experimental data now supports the existence of pronounced SDAK dips on basal surfaces near -4 C and on prism surfaces near -14 C. In both cases, the model suggests that edge-associated surface diffusion greatly reduces the nucleation barrier on narrow facet surfaces relative to that found on broad facets. The remarkable quantitative similarities in the growth behaviors near -4 C and -14 C suggest that these two SDAK features arise from essentially the same physical mechanism occurring at different temperatures on the two principal facets. When applied to atmospheric snow crystal formation, this comprehensive model can explain the recurrent morphological transitions between platelike and columnar growth seen in the Nakaya diagram.
In this paper I examine snow crystal growth near -14 C in comparison with a comprehensive model that includes Structure-Dependent Attachment Kinetics (SDAK). Analyzing a series of ice-growth observations in air, I show that the data strongly support the model, which stipulates that basal growth is described by classical terrace nucleation on faceted surfaces in this temperature region. In contrast, prism growth exhibits a pronounced SDAK dip that substantially reduces the nucleation barrier on narrow prism facets (relative to that found on broad prism facets). I use these measurements to further characterize and refine the SDAK model, which effectively explains the robust formation of platelike snow crystals in air near 14 C.
This monograph reviews our current understanding of the physical dynamics of ice crystal growth, focusing on the spontaneous formation of complex structures from water vapor (called snow crystals) as a function of temperature, supersaturation, background gas pressure, and other extrinsic parameters. Snow crystal growth is a remarkably rich and rather poorly understood phenomenon, requiring a synthesis of concepts from materials science, crystal-growth theory, statistical mechanics, diffusion-limited solidification, finite-element modeling, and molecular surface processes. Building upon recent advances in precision measurement techniques, computation modeling methods, and molecular dynamics simulations of crystalline surfaces, I believe we are moving rapidly toward the long-sought goal of developing a full physical model of snow crystal formation, using ab initio molecular dynamics simulations to create a semi-empirical characterization of the nanoscale surface attachment kinetics, and then incorporating that into a full computational model that reproduces the growth of macroscopic crystalline structures. Section 1 of this monograph deals mainly with the material properties of ice Ih in equilibrium, including thermodynamics quantities, facet surface structures, terrace step energies, and crystal twinning behaviors.
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