June 7, 2019
Journal Article

Crystallization Growth Rate and Front Propagation in Amorphous Solid Water Films

Abstract

The growth rate of crystalline ice in amorphous solid water (ASW) films was investigated using reflection absorption infrared spectroscopy (RAIRS). Two different experiments were setup to measure rates of the crystallization front propagation from the underlying crystalline template upward and from the vacuum interface downward. In one set of experiments, layers of ASW (5% D2O in H2O) were grown on a crystalline ice (CI) template and capped with a decane layer. In isothermal experiments from 140 to 150 K, crystallization was observed from the onset (no induction time) and the extent of crystallization increased linearly in time. In a second set of experiments, uncapped ASW films without a CI template were studied. The films were created by placing a 100 ML isotopic layer (5% D2O in H2O) at various positions in a 1000 ML ASW (H2O) film. The crystalline ice growth rates obtained from the two configurations (capped films with a CI template and uncapped films without a CI template) are in quantitative agreement. The results support the idea that for ASW films in a vacuum a crystalline layer forms at the surface that then acts as a CI template for a growth front that moves downward into the film.

Revised: July 10, 2019 | Published: June 7, 2019

Citation

Smith R.S., C. Yuan, N.G. Petrik, G.A. Kimmel, and B.D. Kay. 2019. Crystallization Growth Rate and Front Propagation in Amorphous Solid Water Films. Journal of Chemical Physics 150, no. 21:214703. PNNL-SA-142493. doi:10.1063/1.5098481