Pressure-induced amorphization and existence of molecular and polymeric amorphous forms in dense SO<sub>2</sub>

ORAL

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 MD simulations, where both forward and reverse transitions were detected, allowing a detailed analysis of the respective local structures. The high-pressure polymeric amorphous form was found to consist mainly of disordered polymeric chains made of 3-coordinated sulfur atoms connected via oxygen atoms, with few residual intact molecules. Our study provides an example of polyamorphism in a system consisting of simple molecules with multiple bonds [1].

[1] Huichao Zhang et al., PNAS 2020, 117, 8736–8742.

*CAS President’s International Fellowship Initiative Fund (2018VMA0053,2019VMA0027), National Natural Science Foundation of China Grant (11874361, 51672279, 11774354, 51727806), CAS Innovation Grant (CXJJ-19-B08), Science Challenge Project (TZ2016001), Hefei Institutes of Physical Science CAS Director’s Fund Grant (YZJJ2017705), Slovak Research and Development Agency grant APVV-15-0496

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Presenters

  • Roman Martonak

    • Department of Experimental Physics, Comenius Univ, Bratislava, Slovakia
    • Department of experimental physics, Comenius university

Authors

  • Huichao Zhang

    • Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, China

  • Ondrej Tóth

    • Department of Experimental Physics, Comenius Univ, Bratislava, Slovakia
    • Department of experimental physics, Comenius university

  • Xiao-Di Liu

    • Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, China
    • Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences

  • Roberto Bini

    • Department of Chemistry, University of Florence, Florence, Italy

  • Eugene Gregoryanz

    • Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, China
    • Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences

  • Philip Dalladay-Simpson

    • Center for High Pressure Science Technology Advanced Research, Shanghai, China
    • Center for High Pressure Science Technology Advanced Research

  • Simone De Panfilis

    • Centre for Life Nano Science, Istituto Italiano di Tecnologia, Rome, Italy

  • Mario Santoro

    • National Institute of Optics, CNR-INO, and European Laboratory for Non-Linear Spectroscopy, LENS, Sesto Fiorentino, Italy
    • European Laboratory for Non-Linear Spectroscopy

  • Federico Aiace Gorelli

    • National Institute of Optics, CNR-INO, and European Laboratory for Non-Linear Spectroscopy, LENS, Sesto Fiorentino, Italy
    • European Laboratory for Non-Linear Spectroscopy

  • Roman Martonak

    • Department of Experimental Physics, Comenius Univ, Bratislava, Slovakia
    • Department of experimental physics, Comenius university