Pressure-induced reversal of Peierls-like distortions elicits the polyamorphic transition in GeTe and GeSe

Tomoki Fujita, Yuhan Chen, Yoshio Kono, Seiya Takahashi, Hidetaka Kasai, Davide Campi, Marco Bernasconi, Koji Ohara, Hirokatsu Yumoto, Takahisa Koyama, Hiroshi Yamazaki, Yasunori Senba, Haruhiko Ohashi, Ichiro Inoue, Yujiro Hayashi, Makina Yabashi, Eiji Nishibori, Riccardo Mazzarello () and Shuai Wei ()
Additional contact information
Tomoki Fujita: Aarhus University
Yuhan Chen: Sapienza University of Rome
Yoshio Kono: Ehime University
Seiya Takahashi: University of Tsukuba
Hidetaka Kasai: University of Tsukuba
Davide Campi: University of Milano-Bicocca
Marco Bernasconi: University of Milano-Bicocca
Koji Ohara: Shimane University
Hirokatsu Yumoto: Japan Synchrotron Radiation Research Institute
Takahisa Koyama: Japan Synchrotron Radiation Research Institute
Hiroshi Yamazaki: Japan Synchrotron Radiation Research Institute
Yasunori Senba: Japan Synchrotron Radiation Research Institute
Haruhiko Ohashi: Japan Synchrotron Radiation Research Institute
Ichiro Inoue: RIKEN SPring-8 Center
Yujiro Hayashi: RIKEN SPring-8 Center
Makina Yabashi: RIKEN SPring-8 Center
Eiji Nishibori: University of Tsukuba
Riccardo Mazzarello: Sapienza University of Rome
Shuai Wei: Aarhus University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract While polymorphism is prevalent in crystalline solids, polyamorphism draws increasing interest in various types of amorphous solids. Recent studies suggested that supercooling of liquid phase-change materials (PCMs) induces Peierls-like distortions in their local structures, underlying their liquid-liquid transitions before vitrification. However, the mechanism of how the vitrified phases undergo a possible polyamorphic transition remains elusive. Here, using high-energy synchrotron X-rays, we can access the precise pair distribution functions under high pressure and provide clear evidence that pressure can reverse the Peierls-like distortions, eliciting a polyamorphic transition in GeTe and GeSe. Combined with simulations based on machine-learned-neural-network potential, our structural analysis reveals a high-pressure state characterized by diminished Peierls-like distortion, greater coherence length, reduced compressibility, and a narrowing bandgap. Our finding underscores the crucial role of Peierls-like distortions in amorphous octahedral systems including PCMs. These distortions can be controlled through pressure and composition, offering potentials for designing properties in PCM-based devices.

Date: 2023
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DOI: 10.1038/s41467-023-43457-y

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