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Optical Spectroscopy of Crystal Nucleation One Nucleus at a Time

preprint
submitted on 26.03.2021, 14:15 and posted on 29.03.2021, 07:18 by Oscar Urquidi, Johanna Brazard, Natalie LeMessurier, Lena Simine, Takuji Adachi

Crystallization is an important process in a wide range of disciplines from fundamental science to industrial application. Despite the importance of controlling the crystallization and its morphology (e.g. polymorphism), the lack of microscopic description of crystal nucleation often limits the rational approach to its engineering and control. The biggest challenge to experimentally track the nucleus formation is the stochastic and heterogeneous nature of the nucleation occurring at nanometer scale. To overcome this challenge, we developed a method we call “Single Nucleus Spectroscopy” or SNS and use it to follow the formation of single crystal glycine nucleus by Raman spectroscopy at 46 ms time resolution. The spectral evolution was analyzed by non-supervised spectral decomposition algorithm which unraveled the Raman spectrum of prenucleation aggregates. In order to gain microscopic insights into the structure of these aggregates we have established a direct comparison between the experiments and theoretical works. The outcome of our analysis is a new hypothesis of glycine crystal nucleation mechanism.

History

Email Address of Submitting Author

Takuji.Adachi@unige.ch

Institution

University of Geneva

Country

Switzerland

ORCID For Submitting Author

0000-0002-0577-1926

Declaration of Conflict of Interest

no conflict of interest

Version Notes

Version 1, 26.03.21

Exports