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High-Pressure Structural Evolution of Disordered Polymeric CS2.

Jinwei Yan1,2,3, Ondrej Tóth4, Wan Xu1,2

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The Journal of Physical Chemistry Letters
|July 26, 2021
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High-pressure carbon disulfide (CS2) forms a disordered polymer with mixed 3-fold and 4-fold coordinated carbon atoms, challenging previous assumptions about Bridgman

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Area of Science:

  • Materials Science
  • Solid-state Chemistry
  • High-Pressure Physics

Background:

  • Carbon disulfide (CS2) is a simple AB2 molecule with double bonds.
  • Previous studies suggested CS2 forms Bridgman's black polymer under pressure.

Purpose of the Study:

  • To investigate the high-pressure polymerization structure of carbon disulfide.
  • To determine the actual structure of the polymer formed under compression.

Main Methods:

  • Combined optical spectroscopy and synchrotron X-ray diffraction.
  • Utilized ab initio simulations for theoretical analysis.

Main Results:

  • Solid CS2 polymerizes at 10-11 GPa.
  • The resulting polymer is disordered, containing 3-fold and 4-fold coordinated carbon atoms and C=C bonds.
  • The proportion of 4-fold coordinated carbons increases with pressure up to 40 GPa.
  • Partial structural reversion and disproportionation occur upon decompression.

Conclusions:

  • The high-pressure structure of carbon disulfide differs from previous models.
  • Reveals complex structural evolution in a simple molecular system under pressure.
  • Challenges the established understanding of Bridgman's black polymer formation.