Reversible devitrification in amorphous As2Se3 under pressure

Azkar Saeed Ahmad, Hong-Bo Lou, Chuan-Long Lin, Ai-Guo Li, Ke Yang, K. Glazyrin, H. P. Liermann, Hermann Franz, Kenny Ståhl, Shuo Cui, Bruno Bureau, Dong-Xian Zhang, Xiao-Dong Wang, Qing-Ping Cao, A. Lindsay Greer, and Jian-Zhong Jiang
Phys. Rev. B 94, 195211 – Published 28 November 2016
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Abstract

In pressure-induced reversible structural transitions, the term “reversible” refers to the recovery of the virgin structure in a material upon complete decompression. Pressure-induced amorphous-to-crystalline transitions have been claimed to be reversible, but evidence that amorphous material recovers its virgin amorphous structure upon complete depressurization has been lacking. In amorphous As2Se3 (aAs2Se3) chalcogenide, however, we report a novel reversible amorphous-to-crystalline transition that provides compelling experimental evidence that upon complete decompression, the recovered amorphous phase is structurally the same as that of the virgin (as-cast) amorphous phase. Combining the experimental results with ab initio molecular dynamics simulations, we elucidate that the amorphization is mediated by a surplus of total free energy in the high-pressure face-centered cubic phase as compared to the virgin amorphous phase and that the structural recovery to the virgin amorphous phase is a consequence of an enhancement in covalent bonding character over interlayer forces upon complete decompression. Furthermore, we observed a two-dimensional to three-dimensional network transition under compression and its reversibility upon decompression.

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  • Received 20 April 2016

DOI:https://doi.org/10.1103/PhysRevB.94.195211

©2016 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Azkar Saeed Ahmad1, Hong-Bo Lou1, Chuan-Long Lin1, Ai-Guo Li2, Ke Yang2, K. Glazyrin3, H. P. Liermann3, Hermann Franz3, Kenny Ståhl4, Shuo Cui5, Bruno Bureau5, Dong-Xian Zhang6, Xiao-Dong Wang1, Qing-Ping Cao1, A. Lindsay Greer7, and Jian-Zhong Jiang1,*

  • 1International Center for New-Structured Materials and Laboratory of New-Structured Materials, State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, People's Republic of China
  • 2Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201203, People's Republic of China
  • 3Photon Science, Deutsches Elektronen-Synchrotron (DESY), Notkestraße 85, D-22603 Hamburg, Germany
  • 4Department of Chemistry, Building 207, Technical University of Denmark, DK-2800 Lyngby, Denmark
  • 5Sciences Chimiques de Rennes-EquipeVerres et Céramiques, Université de Rennes 1, France
  • 6State Key Laboratory of Modern Optical Instrumentation, Zhejiang University, Hangzhou 310027, People's Republic of China
  • 7Department of Materials Science & Metallurgy, 27 Charles Babbage Road, University of Cambridge, Cambridge CB3 0FS, United Kingdom

  • *Corresponding author: jiangjz@zju.edu.cn

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Issue

Vol. 94, Iss. 19 — 15 November 2016

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