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

Huichao Zhang, Ondrej Tóth, Xiaodi Liu, Roberto Bini, Eugene Gregoryanz, Philip Dalladay‐Simpson, Simone De Panfilis, Mario Santoro, Federico A. Gorelli, Roman Martoňák

2020Proceedings of the National Academy of Sciences24 citationsDOIOpen Access PDF

Abstract

: 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.

Topics & Concepts

PolyamorphismAmorphous solidChemical physicsMolecular dynamicsMaterials sciencePhase transitionHigh pressureAb initioMoleculePhase (matter)ThermodynamicsChemistryComputational chemistryCrystallographyPhysicsOrganic chemistryHigh-pressure geophysics and materialsCrystallography and molecular interactionsAdvanced Chemical Physics Studies