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Register a new userA Quantitative Physical Model of the Snow Crystal Morphology Diagram
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Added by
Kenneth G. Libbrecht
Publication date
2019
fields
Physics
and research's language is
English
Authors
Kenneth G. Libbrecht
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I describe a semi-empirical molecular model of the surface attachment kinetics governing ice crystal growth from water vapor as a function of temperature, supersaturation, and crystal mesostructure. An important new hypothesis in this model is surface-energy-driven molecular diffusion enabled by a leaky Ehrlich-Schwoebel barrier. The proposed surface-diffusion behavior is sensitive to facet width and surface premelting, yielding structure-dependent attachment kinetics with a complex temperature dependence. By incorporating several reasonable assumptions regarding the surface premelting behavior on basal and prism facets, this model can explain the overarching features of the snow crystal morphology diagram, which has been an enduring scientific puzzle for nearly 75 years.
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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.
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.
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.
I examine the molecular dynamics of ice growth from water vapor, focusing on how the attachment kinetics can be augmented by edge-dependent surface diffusion. Although there are significant uncertainties in developing an accurate physical model of this process, it is possible to make some reasonable estimates of surface diffusion rates and admolecule density enhancements, derived from our basic understanding of ice-crystal growth processes. A quantitative model suggests that edge-dependent surface diffusion could substantially enhance terrace nucleation on narrow faceted surfaces, especially at the onset of surface premelting. This result supports our hypothesized mechanism for structure-dependent attachment kinetics, which readily explains the changes in snow crystal growth morphology with temperature depicted in the well-known Nakaya diagram. Many of the model features described here may be amenable to further quantitative investigation using existing computational models of the molecular structure and dynamics of the ice surface.
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.
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