Molecular-Resolution Imaging of Ice Crystallized from Liquid Water

Abstract

Despite the ubiquity of ice, a molecular-resolution image of ice crystallized from liquid water or the resulting defect structure has never been obtained. Here, we report the stabilization and angstrom-resolution electron imaging of ice Ih crystallized from liquid water by developing cryogenic liquid-cell transmission electron microscopy (CRYOLIC-TEM). We combine lattice mapping with molecular dynamics simulations to reveal that ice formation is highly tolerant to nanoscale defects such as misoriented subdomains and trapped gas bubbles, which are stabilized by molecular-scale structural motifs. Importantly, bubble surfaces adopt low-energy nanofacets and create negligible strain fields in the surrounding crystal. These bubbles can dynamically nucleate, grow, migrate, dissolve, and coalesce under electron irradiation and be monitored in situ near a steady state. This work opens the door to understanding water crystallization behaviors at an unprecedented spatial resolution.

26 pages, 5 figures, and 1 table. Supplementary Information: 35 pages, 37 figures, and 9 tables

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