Abstract

Brain‐inspired computing, reconfigurable optical metamaterials, photonic tensor cores, and many other advanced applications require next‐generation phase change materials (PCMs) with better energy efficiency and a wider thermal and spectral range for reliable operations. Germanium ditelluride (GeTe2), with higher thermal stability and a larger bandgap compared to current benchmark PCMs, appears promising for THz metasurfaces and the controlled crystallization of atomically thin 2D materials. Using high‐energy X‐ray diffraction supported by first‐principles simulation, we investigate the atomic structure in semiconducting pulsed laser deposition films and metallic high‐temperature liquids. The results suggest that the structural and chemical metastability of GeTe2, leading to disproportionation into GeTe and Te, is related to high internal pressure during a semiconductor‐metal transition, presumably occurring in the supercooled melt. Similar phenomena are expected for canonical GeS2 and GeSe2 under high temperatures and pressures.This article is protected by copyright. All rights reserved.

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