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High-Pressure Structural Evolution of Disordered Polymeric CS2
Jinwei Yan1,2,3, Ondrej Tóth4, Wan Xu1,2
1Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, 230031, China.
High-pressure carbon disulfide (CS2) forms a disordered polymer with mixed 3-fold and 4-fold coordinated carbon atoms, challenging previous assumptions about Bridgman
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.
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