3 years ago

Single-crystal Ih ice surfaces unveil connection between macroscopic and molecular structure [Chemistry]

Single-crystal Ih ice surfaces unveil connection between macroscopic and molecular structure [Chemistry]
Markus D. Mezger, Alexandra Brumberg, Mary Jane Shultz, Ellen H. G. Backus, Mischa Bonn, Charles P. Daghlian, Kevin Hammonds, Ian Baker, Patrick J. Bisson

Physics and chemistry of ice surfaces are not only of fundamental interest but also have important impacts on biological and environmental processes. As ice surfaces—particularly the two prism faces—come under greater scrutiny, it is increasingly important to connect the macroscopic faces with the molecular-level structure. The microscopic structure of the ubiquitous ice Ih crystal is well-known. It consists of stacked layers of chair-form hexagonal rings referred to as molecular hexagons. Crystallographic unit cells can be assembled into a regular right hexagonal prism. The bases are labeled crystallographic hexagons. The two hexagons are rotated 30° with respect to each other. The linkage between the familiar macroscopic shape of hexagonal snowflakes and either hexagon is not obvious per se. This report presents experimental data directly connecting the macroscopic shape of ice crystals and the microscopic hexagons. Large ice single crystals were used to fabricate samples with the basal, primary prism, or secondary prism faces exposed at the surface. In each case, the same sample was used to capture both a macroscopic etch pit image and an electron backscatter diffraction (EBSD) orientation density function (ODF) plot. Direct comparison of the etch pit image and the ODF plot compellingly connects the macroscopic etch pit hexagonal profile to the crystallographic hexagon. The most stable face at the ice–water interface is the smallest area face at the ice–vapor interface. A model based on the molecular structure of the prism faces accounts for this switch.

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