A metastable amorphous intermediate is responsible for laser-induced nucleation of glycine

Liao, Z. and Wynne, K. (2022) A metastable amorphous intermediate is responsible for laser-induced nucleation of glycine. Journal of the American Chemical Society, 144(15), pp. 6727-6733. (doi: 10.1021/jacs.1c11154) (PMID:35384650)

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Abstract

Laser-induced crystal nucleation through optical tweezing, and in particular polymorph selection through laser polarization, promises unprecedented control over crystallization. However, in the absence of a nearby liquid–liquid critical point or miscibility gap, the origin of the required mesoscale clusters remains unclear. A number of recent studies of so-called nonclassical nucleation have suggested the presence of large amorphous clusters. Here, we show that supersaturated aqueous glycine solutions form metastable intermediate particles that are off the direct path to crystal nucleation. Laser-induced crystal nucleation only occurs when the laser “activates” one of these particles. In situ low-frequency Raman spectroscopy is used to demonstrate their amorphous or partially ordered character and transformation to various crystal polymorphs. The requirement for solution aging in many previously reported laser-induced crystal nucleation experiments strongly suggests that the presence of amorphous intermediates is a general requirement.

Item Type:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Liao, Dr Zhiyu and Wynne, Professor Klaas
Authors: Liao, Z., and Wynne, K.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Journal of the American Chemical Society
Publisher:American Chemical Society
ISSN:0002-7863
ISSN (Online):1520-5126
Published Online:06 April 2022
Copyright Holders:Copyright © 2022 American Chemical Society
First Published:First published in Journal of the American Chemical Society 144(15):6727–6733
Publisher Policy:Reproduced in accordance with the copyright policy of the publisher

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
166308Liquid-liquid transitions in molecular liquids: from supramolecular structure to phase separationKlaas WynneEngineering and Physical Sciences Research Council (EPSRC)EP/J004790/1Chemistry
190480University of Glasgow - Equipment AccountMuffy CalderEngineering and Physical Sciences Research Council (EPSRC)EP/J014478/1S&E - College Senior Management
304469CONTROLKlaas WynneEuropean Commission (EC)832703Chemistry