Pressure-Induced Synthesis and Properties of an H2S-H2Se-H2 Molecular Alloy
Year: 2021
Authors: Pesa-Alvarez M., Hu HX., Marquys M., Cooke PIC., Donnelly ME., Binns J., Gorelli FA., Gregoryanz E., Dalladay-Simpson P., Ackland GJ., Howie RT.
Autors Affiliation: Univ Edinburgh, Ctr Sci Extreme Condit, Edinburgh EH9 3FD, Midlothian, Scotland; Univ Edinburgh, Sch Phys & Astron, Edinburgh EH9 3FD, Midlothian, Scotland; Ctr High Pressure Sci Technol Adv Res HPSTAR, Shanghai, Peoples R China; RMIT Univ, Sch Sci, Melbourne, Vic 3000, Australia.
Abstract: The chalcogens are known to react with one another to form interchalcogens, which exhibit a diverse range of bonding and conductive behavior due to the difference in electronegativity between the group members. Through a series of high-pressure diamond anvil experiments combined with density functional theory calculations, we report the synthesis of an S-Se hydride. At pressures above 4 GPa we observe the formation of a single solid composed of both H2Se and H2S molecular units. Further compression in a hydrogen medium leads to the formation of an alloyed compound (H2SxSe1-x)(2)H-2, after which there is a sequence of pressure-induced phase transitions associated with the arrested rotation of molecules. At pressures above 50 GPa, there is a symmetrization of hydrogen bonds concomitantly with a closing band gap and increased reflectivity of the compound, indicative of a transition to a metallic state.
Journal/Review: JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume: 12 (24) Pages from: 5738 to: 5743
More Information: Parts of this research were performed at P02.2 at DESY, a member of the Helmholtz Association (HGF), and we thank H.-P. Liermann and K. Glazyrin for assistance. Parts of this research were performed at SPring8 , and we thank S. Kawaguchi for assistance. R.T.H. acknowledges the support of the National Science Foundation of China (Grant No. 11974034) and ERC Grant MetElOne Reference No. 948895. M.P.-A. acknowledges UKRI Future Leaders Fellowship Mrc-Mr/T043733/1. The research leading to this result has been supported by the project CALIPSOplus under Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. M.P.-A., G.J.A., E.G., and M.M. acknowledge the support of the European Research Council (ERC) Grant Hecate Ref. No. 695527. Computational resources provided by UK Materials and Molecular Modeling Hub partially funded by EPSRC (EP/P020194/1) and the UKCP consortium under the EPSRC grant (EP/P022561/1). Parts of this work was performed under Proposal No. 2017A1062 at SPring-8 and the UKCP collaboration EPSRC Grant PO22561.KeyWords: Density functional theory; Electronegativity; Energy gap; Hydrogen bonds; Hydrogen sulfide; Selenium compoundsDOI: 10.1021/acs.jpclett.1c01406Citations: 1data from “WEB OF SCIENCE” (of Thomson Reuters) are update at: 2024-10-20References taken from IsiWeb of Knowledge: (subscribers only)