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Polyamorphism mirrors polymorphism in the liquid–liquid transition of a molecular liquid

DOI: 10.1021/jacs.0c01712 DOI Help

Authors: Finlay Walton (University of Glasgow) , John Bolling (University of Glasgow) , Andrew Farrell (University of Glasgow) , Jamie Macewen (University of Glasgow) , Christopher D. Syme (University of Glasgow) , Mario González-Jiménez (University of Glasgow) , Hans Martin Senn (University of Glasgow) , Claire Wilson (University of Glasgow) , Gianfelice Cinque (Diamond Light Source) , Klaas Wynne (University of Glasgow)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Journal Of The American Chemical Society

State: Published (Approved)
Published: April 2020
Diamond Proposal Number(s): 20351

Open Access Open Access

Abstract: Liquid-liquid transitions between two amorphous phases in a single-component liquid have courted controversy. All known examples of liquid–liquid transitions in molecular liquids have been observed in the supercooled state suggesting an intimate connection with vitrification and locally favored structures inhibiting crystallization. However, there is precious little information about the local molecular packing in supercooled liquids meaning that the order parameter of the transition is still unknown. Here, we investigate the liquid–liquid transition in triphenyl phosphite and show that it is caused by the competition between liquid structures that mirror two crystal polymorphs. The liquid–liquid transition is found to be between a geometrically frustrated liquid to a dynamically frustrated glass. These results indicate a general link between polymorphism and polyamorphism and will lead to a much greater understanding of the physical basis of liquid–liquid transitions and allow the systematic discovery of other examples.

Journal Keywords: Crystals; Crystallization; Liquids; Crystal structure; Phase transitions

Subject Areas: Chemistry

Instruments: B22-Multimode InfraRed imaging And Microspectroscopy

Added On: 06/04/2020 10:01


Discipline Tags:

Molecular Physics Physics Chemistry

Technical Tags:

Spectroscopy Infrared Spectroscopy Synchtron-based Fourier Transform Infrared Spectroscopy (SR-FTIR)