Pressure-induced ferroelectric-like transition creates a polar metal in defect antiperovskites Hg<sub>3</sub>Te<sub>2</sub>X<sub>2</sub> (X = Cl, Br).

Cai, Weizhao; He, Jiangang; Li, Hao; Zhang, Rong; Zhang, Dongzhou; Chung, Duck Young; Bhowmick, Tushar; Wolverton, Christopher et al. · Nat Commun · 2021

basic_science · Level V

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Abstract

Ferroelectricity is typically suppressed under hydrostatic compression because the short-range repulsions, which favor the nonpolar phase, increase more rapidly than the long-range interactions, which prefer the ferroelectric phase. Here, based on single-crystal X-ray diffraction and density-functional theory, we provide evidence of a ferroelectric-like transition from phase I2<sub>1</sub>3 to R3 induced by pressure in two isostructural defect antiperovskites Hg<sub>3</sub>Te<sub>2</sub>Cl<sub>2</sub> (15.5 GPa) and Hg<sub>3</sub>Te<sub>2</sub>Br<sub>2</sub> (17.5 GPa). First-principles calculations show that this transition is attributed to pressure-induced softening of the infrared phonon mode Γ<sub>4</sub>, similar to the archetypal ferroelectric material BaTiO<sub>3</sub> at ambient pressure. Additionally, we observe a gradual band-gap closing from ~2.5 eV to metallic-like state of Hg<sub>3</sub>Te<sub>2</sub>Br<sub>2</sub> with an unexpectedly stable R3 phase even after semiconductor-to-metal transition. This study demonstrates the possibility of emergence of polar metal under pressure in this class of materials and establishes the possibility of pressure-induced ferroelectric-like transition in perovskite-related systems.