Pressure-induced ferroelectric-like transition creates a polar metal in defect antiperovskites Hg3Te2X2 (X = Cl, Br)
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 I213 to R3 induced by pressure in two isostructural defect antiperovskites Hg3Te2Cl2 (15.5 GPa) and Hg3Te2Br2 (17.5 GPa). First-principles calculations show that this transition is attributed to pressure-induced softening of the infrared phonon mode Γ4, similar to the archetypal ferroelectric material BaTiO3 at ambient pressure. Additionally, we observe a gradual band-gap closing from ~2.5 eV to metallic-like state of Hg3Te2Br2 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.
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Rochester, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Fusion Energy Sciences (FES)
- OSTI Identifier:
- 1769521
- Alternate Identifier(s):
- OSTI ID: 1787866; OSTI ID: 1924005
- Grant/Contract Number:
- AC02-06CH11357; SC0020340
- Resource Type:
- Published Article
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Name: Nature Communications Journal Volume: 12 Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Density functional theory; electronic materials; ferroelectrics and multiferroics
Citation Formats
Cai, Weizhao, He, Jiangang, Li, Hao, Zhang, Rong, Zhang, Dongzhou, Chung, Duck Young, Bhowmick, Tushar, Wolverton, Christopher, Kanatzidis, Mercouri G., and Deemyad, Shanti. Pressure-induced ferroelectric-like transition creates a polar metal in defect antiperovskites Hg3Te2X2 (X = Cl, Br). United Kingdom: N. p., 2021.
Web. doi:10.1038/s41467-021-21836-7.
Cai, Weizhao, He, Jiangang, Li, Hao, Zhang, Rong, Zhang, Dongzhou, Chung, Duck Young, Bhowmick, Tushar, Wolverton, Christopher, Kanatzidis, Mercouri G., & Deemyad, Shanti. Pressure-induced ferroelectric-like transition creates a polar metal in defect antiperovskites Hg3Te2X2 (X = Cl, Br). United Kingdom. https://doi.org/10.1038/s41467-021-21836-7
Cai, Weizhao, He, Jiangang, Li, Hao, Zhang, Rong, Zhang, Dongzhou, Chung, Duck Young, Bhowmick, Tushar, Wolverton, Christopher, Kanatzidis, Mercouri G., and Deemyad, Shanti. Mon .
"Pressure-induced ferroelectric-like transition creates a polar metal in defect antiperovskites Hg3Te2X2 (X = Cl, Br)". United Kingdom. https://doi.org/10.1038/s41467-021-21836-7.
@article{osti_1769521,
title = {Pressure-induced ferroelectric-like transition creates a polar metal in defect antiperovskites Hg3Te2X2 (X = Cl, Br)},
author = {Cai, Weizhao and He, Jiangang and Li, Hao and Zhang, Rong and Zhang, Dongzhou and Chung, Duck Young and Bhowmick, Tushar and Wolverton, Christopher and Kanatzidis, Mercouri G. and Deemyad, Shanti},
abstractNote = {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 I213 to R3 induced by pressure in two isostructural defect antiperovskites Hg3Te2Cl2 (15.5 GPa) and Hg3Te2Br2 (17.5 GPa). First-principles calculations show that this transition is attributed to pressure-induced softening of the infrared phonon mode Γ4, similar to the archetypal ferroelectric material BaTiO3 at ambient pressure. Additionally, we observe a gradual band-gap closing from ~2.5 eV to metallic-like state of Hg3Te2Br2 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.},
doi = {10.1038/s41467-021-21836-7},
journal = {Nature Communications},
number = 1,
volume = 12,
place = {United Kingdom},
year = {Mon Mar 08 00:00:00 EST 2021},
month = {Mon Mar 08 00:00:00 EST 2021}
}
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