Crystal nucleation in a vapor deposited Lennard-Jones mixture

F Leoni and H Tanaka and J Russo, JOURNAL OF MOLECULAR LIQUIDS, 391, 123178 (2023).

DOI: 10.1016/j.molliq.2023.123178

Understanding the pathways to crystallization during the deposition of a vapor phase on a cold solid substrate is of great interest in industry, e.g., for the realization of electronic devices made of crystallites- free glassy materials, as well as in the atmospheric science in relation to ice nucleation and growth in clouds. Here we numerically investigate the nucleation process during the deposition of a glassformer by using a Lennard-Jones mixture, and compare the properties of this nucleation process with both its quenched counterpart and the bulk system. We find that all three systems homogeneously nucleate crystals in a narrow range of temperatures. However, the deposited layer shows a peculiar formation of ordered domains, promoted by the faster relaxation dynamics toward the free surface even in an as-deposited state. In contrast, the formation of such domains in the other systems occurs only when the structures are fully relaxed by quenching. Furthermore, the nucleus initially grows in an isotropic symmetrical manner, but eventually shows sub-3D growth due to its preference to grow along the basal plane, irrespective of the layer production procedure.

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