A Metastable Amorphous Intermediate Is Responsible for Laser-Induced Nucleation of Glycine

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...

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Bibliographic Details
Published inJournal of the American Chemical Society Vol. 144; no. 15; pp. 6727 - 6733
Main Authors Liao, Zhiyu, Wynne, Klaas
Format Journal Article
LanguageEnglish
Published United States American Chemical Society 20.04.2022
Subjects
age
Americans
aqueous solutions
Crystallization
crystals
Glycine - chemistry
Lasers
Raman spectroscopy
Spectrum Analysis, Raman
Water
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Summary: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.
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ISSN:0002-7863
1520-5126
1520-5126
DOI:10.1021/jacs.1c11154