Tailoring Mid–Gap States of Chalcogenide Glass by Pressure–Induced Hypervalent Bonding Towards the Design of Electrical Switching Materials

Xu, Meng; Xu, Qundao; Gu, Rongchuan; Wang, Songyou; Wang, Cai‐Zhuang; Ho, Kai‐Ming; Wang, Zhongrui; Xu, Ming; Miao, Xiangshui

doi:10.1002/adfm.202304926

Tailoring Mid–Gap States of Chalcogenide Glass by Pressure–Induced Hypervalent Bonding Towards the Design of Electrical Switching Materials

Journal Article · Tue Aug 01 00:00:00 EDT 2023 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202304926· OSTI ID:1998937

^[1]; Xu, Qundao ^[2]; Gu, Rongchuan ^[2]; ^[3]; ^[4]; ^[4]; ^[5]; ^[2]; ^[2]

Huazhong Univ. of Science and Technology, Wuhan (China); Univ. of Hong Kong (China)
Huazhong Univ. of Science and Technology, Wuhan (China)
Fudan Univ., Shanghai (China)
Ames Lab., and Iowa State Univ., Ames, IA (United States)
Univ. of Hong Kong (China)

Phase change memory (PCM) and ovonic threshold switching (OTS) materials using chalcogenide glass are essential elements in advanced 3D memory chips. The mid–gap states, induced by the disorder and defects in the glass, are the physical mechanisms of the electrical switching behavior, while the origin of these trap states is still under debate and the medium–range clusters that break the global octet rule, such as over–coordinated atoms, are known to be responsible in various glass. Here, it is discovered that a large fraction of over–coordinated clusters fails to generate mid–gap states, which are probably caused by hypervalent bonding, a multi–centered covalent bond participated by delocalized lone–pair electrons. This is confirmed by the pressure–driven simulations of amorphous GeSe models, in which it is found that octahedral motifs and hypervalent bonds prevent the over–coordinated medium–range clusters from providing excessive electrons. In practical applications, compatible dopants can be used to change the number of hypervalent bonds, thus controlling the number of mid–gap states and consequently the performance of PCM and OTS materials. Finally, these results reveal the origin of mid–gap states in chalcogenide glasses, enabling extensive control in the development of pioneering electrical switching materials.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Key Research and Development Plan of China; National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1998937

Report Number(s):: IS-J--11,127

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 45 Vol. 33; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Tailoring Mid–Gap States of Chalcogenide Glass by Pressure–Induced Hypervalent Bonding Towards the Design of Electrical Switching Materials

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