Pressure-induced amorphization and existence of molecular and polymeric amorphous forms in dense SO2

Anno: 2020

Autori: Zhang H., Toth O., Liu XD., Bini R., Gregoryanz E., Dalladay-Simpson P., De Panfilis S., Santoro M., Gorelli FA., Martonak R.

Affiliazione autori: 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.

Giornale/Rivista: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA

Volume: 117 (16)      Da Pagina: 8736  A: 8742

Maggiori informazioni: Experimental section of research was supported by the Chinese Academy of Sciences President´s 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 Director´s 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.
Parole chiavi: polyamorphism; sulfur dioxide; high pressure; polymeric form
DOI: 10.1073/pnas.1917749117

Citazioni: 15
dati da “WEB OF SCIENCE” (of Thomson Reuters) aggiornati al: 2025-06-29
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