Dynamics and unsteady morphologies at ice interfaces driven by D<sub>2</sub>O-H<sub>2</sub>O exchange.

Drori, Ran; Holmes-Cerfon, Miranda; Kahr, Bart; Kohn, Robert V; Ward, Michael D · Proc Natl Acad Sci U S A · 2017

basic_science · Level V

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Abstract

The growth dynamics of D<sub>2</sub>O ice in liquid H<sub>2</sub>O in a microfluidic device were investigated between the melting points of D<sub>2</sub>O ice (3.8 °C) and H<sub>2</sub>O ice (0 °C). As the temperature was decreased at rates between 0.002 °C/s and 0.1 °C/s, the ice front advanced but retreated immediately upon cessation of cooling, regardless of the temperature. This is a consequence of the competition between diffusion of H<sub>2</sub>O into the D<sub>2</sub>O ice, which favors melting of the interface, and the driving force for growth supplied by cooling. Raman microscopy tracked H/D exchange across the solid H<sub>2</sub>O-solid D<sub>2</sub>O interface, with diffusion coefficients consistent with transport of intact H<sub>2</sub>O molecules at the D<sub>2</sub>O ice interface. At fixed temperatures below 3 °C, the D<sub>2</sub>O ice front melted continuously, but at temperatures near 0 °C a scalloped interface morphology appeared with convex and concave sections that cycled between growth and retreat. This behavior, not observed for D<sub>2</sub>O ice in contact with D<sub>2</sub>O liquid or H<sub>2</sub>O ice in contact with H<sub>2</sub>O liquid, reflects a complex set of cooperative phenomena, including H/D exchange across the solid-liquid interface, latent heat exchange, local thermal gradients, and the Gibbs-Thomson effect on the melting points of the convex and concave features.