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Tailoring the degree of structural disorder in Ge-Sb-Te alloys is importantfor the development of non-volatile phase-change memory and neuro-inspiredcomputing. Upon crystallization from the amorphous phase, these alloys form acubic rocksalt-like structure with a high content of intrinsic vacancies.Further thermal annealing results in a gradual structural transition towards alayered structure and an insulator-to-metal transition. In this work, weelucidate the atomic-level details of the structural transition in crystallineGeSb2Te4 by in situ high-resolution transmission electron microscopy (HRTEM)experiments and ab initio density functional theory (DFT) calculations,providing a comprehensive real-time and real-space view of the vacancy orderingprocess. We also discuss the impact of vacancy ordering on altering theelectronic and optical properties of GeSb2Te4, which is relevant to multilevelstorage applications. The phase evolution paths in Ge-Sb-Te alloys areillustrated using a summary diagram, which serves as a guide for designingphase-change memory devices.

In situ characterization of vacancy ordering in Ge-Sb-Te phase-change memory alloys