Frustration vs prenucleation: understanding the surprising stability of supersaturated sodium thiosulfate solutions

Reichenbach, J. and Wynne, K. (2018) Frustration vs prenucleation: understanding the surprising stability of supersaturated sodium thiosulfate solutions. Journal of Physical Chemistry B, 122(30), pp. 7590-7596. (doi:10.1021/acs.jpcb.8b04112) (PMID:29993246)

Reichenbach, J. and Wynne, K. (2018) Frustration vs prenucleation: understanding the surprising stability of supersaturated sodium thiosulfate solutions. Journal of Physical Chemistry B, 122(30), pp. 7590-7596. (doi:10.1021/acs.jpcb.8b04112) (PMID:29993246)

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Abstract

Gibbs classical nucleation theory predicts that a supersaturated solution will have transient nuclei that flitter in and out of existence. Only when one of these nuclei becomes larger than a critical size, will the solution crystalize. Recently, nonclassical nucleation theories have invoked the presence of prenuclei possibly associated with a liquid–liquid phase separation. However, there are few experimental observations of such prenuclei. Here, we use ultrafast optical Kerr-effect spectroscopy to measure the temperature-dependent low-frequency (sub-gigahertz to terahertz) anisotropic Raman spectra of supersaturated aqueous sodium thiosulfate solutions. Clear evidence of clusters is obtained in the spectra. However, on the basis of the inferred stability of these clusters, it appears that they frustrate rather than promote the formation of crystals. This would explain the surprising stability of supersaturated sodium thiosulfate and similar solutions.

Item Type:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Reichenbach, Judith and Wynne, Professor Klaas
Authors: Reichenbach, J., and Wynne, K.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Journal of Physical Chemistry B
Publisher:American Chemical Society
ISSN:1520-6106
ISSN (Online):1520-5207
Published Online:11 July 2018
Copyright Holders:Copyright © 2018 American Chemical Society
First Published:First published in Journal of Physical Chemistry B 122(30):7590-7596
Publisher Policy:Reproduced under a Creative Commons License
Data DOI:10.5525/gla.researchdata.636

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
563561Terahertz spectroscopy of aqueous ionic solutions to understand the role of hydrogen-bond network breaking and strengthening in the HofmeisterKlaas WynneEngineering and Physical Sciences Research Council (EPSRC)EP/E046541/2CHEM - CHEMISTRY
559071Two-dimensional terahertz/IR spectroscopy: a unique probe of ultrafast hydrogen-bond dynamics of liquid water and model systems.Klaas WynneEngineering and Physical Sciences Research Council (EPSRC)EP/F06926X/2CHEM - CHEMISTRY
582891The structure and dynamics of water confined in nanoscale pools: the dynamic crossoverKlaas WynneEngineering and Physical Sciences Research Council (EPSRC)EP/J009733/1CHEM - CHEMISTRY
619561Solvation dynamics and structure around proteins and peptides: collective network motions vs. weak interactionsKlaas WynneEngineering and Physical Sciences Research Council (EPSRC)EP/K034995/1CHEM - CHEMISTRY