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High-Pressure Structural Evolution of Disordered Polymeric CS2

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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Phys. Chem. Lett. 2021, 12, 30, 7229-7235
    Physical Insights into Materials and Molecular Properties

    High-Pressure Structural Evolution of Disordered Polymeric CS2
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    • Jinwei Yan
      Jinwei Yan
      Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, 230031, China
      University of Science and Technology of China, Hefei 230026, China
      Center for High Pressure Science and Technology Advanced Research, 1690 Cailun Road, Shanghai, 201203, China
      More by Jinwei Yan
    • Ondrej Tóth
      Ondrej Tóth
      Department of Experimental Physics, Faculty of Mathematics, Physics and Informatics, Comenius University in Bratislava, Mlynská Dolina F2, 842 48 Bratislava, Slovakia
      More by Ondrej Tóth
    • Wan Xu
      Wan Xu
      Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, 230031, China
      University of Science and Technology of China, Hefei 230026, China
      More by Wan Xu
    • Xiao-Di Liu
      Xiao-Di Liu
      Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, 230031, China
      More by Xiao-Di Liu
    • Eugene Gregoryanz
      Eugene Gregoryanz
      Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, 230031, China
      School of Physics and Astronomy and Centre for Science at Extreme Conditions, University of Edinburgh, Edinburgh EH9 3JZ, U.K.
      Center for High Pressure Science and Technology Advanced Research, 1690 Cailun Road, Shanghai, 201203, China
      More by Eugene Gregoryanz
    • Philip Dalladay-Simpson
      Philip Dalladay-Simpson
      Center for High Pressure Science and Technology Advanced Research, 1690 Cailun Road, Shanghai, 201203, China
      More by Philip Dalladay-Simpson
    • Zeming Qi
      Zeming Qi
      National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
      More by Zeming Qi
    • Shiyu Xie
      Shiyu Xie
      National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
      More by Shiyu Xie
    • Federico Gorelli
      Federico Gorelli
      Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, 230031, China
      Center for High Pressure Science and Technology Advanced Research, 1690 Cailun Road, Shanghai, 201203, China
      Istituto Nazionale di Ottica (CNR-INO) and European Laboratory for non Linear Spectroscopy (LENS), via N. Carrara 1, 50019 Sesto Fiorentino, Italy
      More by Federico Gorelli
    • Roman Martoňák
      Roman Martoňák
      Department of Experimental Physics, Faculty of Mathematics, Physics and Informatics, Comenius University in Bratislava, Mlynská Dolina F2, 842 48 Bratislava, Slovakia
      More by Roman Martoňák
      Orcidhttps://orcid.org/0000-0002-4013-9117
    • Mario Santoro*
      Mario Santoro
      Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, 230031, China
      Istituto Nazionale di Ottica (CNR-INO) and European Laboratory for non Linear Spectroscopy (LENS), via N. Carrara 1, 50019 Sesto Fiorentino, Italy
      *E-mail: [email protected]
      More by Mario Santoro
      Orcidhttps://orcid.org/0000-0001-5693-4636
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2021, 12, 30, 7229–7235
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.1c01762
    Published July 26, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    Carbon disulfide is an archetypal double-bonded molecule belonging to the class of group IV–group VI, AB2 compounds. It is widely believed that, upon compression to several GPa at room temperature and above, a polymeric chain of type (−(C═S)–S−)n, named Bridgman’s black polymer, will form. By combining optical spectroscopy and synchrotron X-ray diffraction data with ab initio simulations, we demonstrate that the structure of this polymer is different. Solid molecular CS2 polymerizes at ∼10–11 GPa. The polymer is disordered and consists of a mixture of 3-fold (C3) and 4-fold (C4) coordinated carbon atoms with some C═C double bonds. The C4/C3 ratio continuously increases upon further compression to 40 GPa. Upon decompression, structural changes are partially reverted, while the sample also undergoes partial disproportionation. Our work uncovers the nontrivial high-pressure structural evolution in one of the simplest molecular systems exhibiting molecular as well as polymeric phases.

    Copyright © 2021 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.1c01762.

    • (I) Methods; (II) Ab initio molecular dynamics compression and decompression; (III) Partial VDOS; (IV) Polymerization mechanism (PDF)

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    This article is cited by 5 publications.

    1. Mario Santoro, Roberto Bini, Matteo Ceppatelli, Gaston Garbarino, Federico Aiace Gorelli, Michael Hanfland, Demetrio Scelta. High Pressure Structural Changes in Amorphous Polymeric Carbon Monoxide by Combined Infrared Spectroscopy and X-ray Diffraction. The Journal of Physical Chemistry C 2022, 126 (28) , 11840-11845. https://doi.org/10.1021/acs.jpcc.2c03204
    2. Demetrio Scelta, Matteo Ceppatelli, Roberto Bini, Anna Pakhomova, Gaston Garbarino, Mohamed Mezouar, Mario Santoro. High temperature decomposition of polymeric carbon monoxide at pressures up to 120 GPa. The Journal of Chemical Physics 2023, 159 (8) https://doi.org/10.1063/5.0157907
    3. Dominika Melicherová, Roman Martoňák. Study of polymerization of high-pressure nitrogen by ab initio molecular dynamics. The Journal of Chemical Physics 2023, 158 (24) https://doi.org/10.1063/5.0156014
    4. Heng Zhang, Junjie Wang, Frédéric Guégan, Gilles Frapper. First-principles structure prediction of two-dimensional HCN polymorphs obtained via formal molecular polymerization. Nanoscale 2023, 15 (16) , 7472-7481. https://doi.org/10.1039/D2NR07239D
    5. S. Klotz, B. Baptiste, T. Hattori, S.M. Feng, Ch Jin, K. Béneut, J.M. Guigner, I. Estève. Synthesis and characterisation of a new graphitic C–S compound obtained by high pressure decomposition of CS2. Carbon 2021, 185 , 491-500. https://doi.org/10.1016/j.carbon.2021.09.048
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2021, 12, 30, 7229–7235
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.1c01762
    Published July 26, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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