Best face forward: crystal-face competition at the ice-water interface.

Abstract

The ice-water interface plays an important role in determining the outcome of both biological and environmental processes. Under ambient pressure, the most stable form of ice is hexagonal ice (Ih). Experimentally probing the surface free energy between each of the major faces of Ih ice and the liquid is both experimentally and theoretically challenging. The basis for the challenge is the near-equality of the surface free energy for the major faces along with the tendency of water to supercool. As a result, morphology from crystallization initiated below 0 °C is kinetically controlled. The reported work circumvents supercooling consequences by providing a polycrystalline seed, followed by isothermal, equilibrium growth. Natural selection among seeded faces results in a single crystal. A record of the growth front is preserved in the frozen boule. Crystal orientation at the front is revealed by examining the boule cross section with two techniques: (1) viewing between crossed polarizers to locate the optical axis and (2) etching to distinguish the primary-prism face from the secondary-prism face. Results suggest that the most stable ice-water interface at 0 °C is the secondary-prism face, followed by the primary-prism face. The basal face that imparts the characteristic hexagonal shape to snowflakes is a distant third. The results contrast with those from freezing the vapor where the basal and primary-prism faces have comparable free energy followed by the secondary-prism face.