Ternary hypervalent silicon hydrides via lithium at high pressure

Tianxiao Liang, Zihan Zhang, Xiaolei Feng, Haojun Jia, Chris J. Pickard, Simon A. T. Redfern, and Defang Duan

Phys. Rev. Materials 4, 113607 – Published 18 November 2020

Abstract

Hydrogen is rarely observed as a ligand in hypervalent species, however, we find that high-pressure hydrogenation may stabilize hypervalent hydrogen-rich materials. Focusing on ternary silicon hydrides via lithium doping, we find anions composed of hypervalent silicon with H ligands formed under high pressure. Our results reveal two different hypervalent anions: layered ${SiH}_{5}^{-}$ and tricapped triangular prismatic ${SiH}_{6}^{2 -}$ . These differ from octahedral ${SiH}_{6}^{2 -}$ described in earlier studies. In addition, there are further hydrogen-rich structures, ${Li}_{3} {SiH}_{10}$ and ${Li}_{2} {SiH}_{6 + δ}$ , which may be stabilized at high pressure. Our work provides pointers to future investigations on hydrogen-rich materials.

Received 14 September 2020
Accepted 4 November 2020

DOI:https://doi.org/10.1103/PhysRevMaterials.4.113607

Physics Subject Headings (PhySH)

Charge Density of states Phase transitions

3-dimensional systems Complex materials Crystal structures

Density functional theory

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Tianxiao Liang¹, Zihan Zhang¹, Xiaolei Feng^2,3,*, Haojun Jia ⁴, Chris J. Pickard^5,6, Simon A. T. Redfern ^7,8, and Defang Duan ^1,†

¹College of Physics, Jilin University, Changchun 130012, China
²Institute for Disaster Management and Reconstruction, Sichuan University - the Hong Kong Polytechnic University, Chengdu 610207, China
³Department of Earth Science, University of Cambridge, Downing Site, Cambridge CB2 3EQ, United Kingdom
⁴Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA
⁵Department of Materials Science & Metallurgy, University of Cambridge, 27 Charles Babbage Road, Cambridge CB3 0FS, United Kingdom
⁶Advanced Institute for Materials Research, Tohoku University, 2-1-1 Katahira, Aoba, Sendai 980-8577, Japan
⁷Asian School of the Environment, Nanyang Technological University, Singapore 639798
⁸Center for High Pressure Science and Technology Advanced Research, Beijing 100094, China

^*xf232@cam.ac.uk
^†duandf@jlu.edu.cn

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Vol. 4, Iss. 11 — November 2020

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