Pressure-induced amorphization and existence of molecular and polymeric amorphous forms in dense SO2
Year: 2020
Authors: Zhang H., Toth O., Liu XD., Bini R., Gregoryanz E., Dalladay-Simpson P., De Panfilis S., Santoro M., Gorelli FA., Martonak R.
Autors Affiliation: Chinese Acad Sci, Inst Solid State Phys, Key Lab Mat Phys, Hefei 230031, Peoples R China; Univ Sci & Technol China, Hefei 230026, Peoples R China; Comenius Univ, Fac Math Phys & Informat, Dept Expt Phys, Bratislava 84248, Slovakia; Univ Florence, Dept Chem, I-50121 Florence, Italy; European Lab Nonlinear Spect, I-50019 Sesto Fiorentino, Italy; Univ Edinburgh, Sch Phys & Astron, Edinburgh EH9 3JZ, Midlothian, Scotland; Univ Edinburgh, Ctr Sci Extreme Condit, Edinburgh EH9 3JZ, Midlothian, Scotland; Ctr High Pressure Sci Technol Adv Res, Shanghai 201203, Peoples R China; Ist Italiano Tecnol, Ctr Life Nano Sci, I-00161 Rome, Italy; CNR, INO, I-50125 Florence, Italy.
Abstract: We report here the pressure-induced amorphization and reversible structural transformation between two amorphous forms of SO2: molecular amorphous and polymeric amorphous, with the transition found at 26 GPa over a broad temperature regime, 77 K to 300 K. The transformation was observed by both Raman spectroscopy and X-ray diffraction in a diamond anvil cell. The results were corroborated by ab initio molecular dynamics simulations, where both forward and reverse transitions were detected, opening a window to detailed analysis of the respective local structures. The high-pressure polymeric amorphous form was found to consist mainly of disordered polymeric chains made of three-coordinated sulfur atoms connected via oxygen atoms, with few residual intact molecules. This study provides an example of polyamorphism in a system consisting of simple molecules with multiple bonds.
Journal/Review: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume: 117 (16) Pages from: 8736 to: 8742
More Information: Experimental section of research was supported by the Chinese Academy of Sciences Presidentīs International Fellowship Initiative Fund (2018VMA0053 and 2019VMA0027), National Natural Science Foundation of China Grant (11874361, 51672279, 11774354, and 51727806), Chinese Academy of Sciences Innovation Grant (CXJJ-19-B08), Science Challenge Project (TZ2016001), and the Hefei Institutes of Physical Science Chinese Academy of Sciences Directorīs Fund Grant (YZJJ2017705). R.M. acknowledges stimulating discussions with P. Mach. R.M. and O.T. were supported by the Slovak Research and Development Agency under Contract APVV-15-0496. Calculations were performed at the Computing Center of the Slovak Academy of Sciences using the supercomputing infrastructure acquired in ITMS Projects 26230120002 and 26210120002 (Slovak Infrastructure for High-Performance Computing) supported by the Research and Development Operational Program funded by the European Regional Development Fund.KeyWords: polyamorphism; sulfur dioxide; high pressure; polymeric formDOI: 10.1073/pnas.1917749117Citations: 13data from “WEB OF SCIENCE” (of Thomson Reuters) are update at: 2024-11-17References taken from IsiWeb of Knowledge: (subscribers only)Connecting to view paper tab on IsiWeb: Click hereConnecting to view citations from IsiWeb: Click here