Optical Spectroscopy of Crystal Nucleation One Nucleus at a Time
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