In situ optical spectroscopy of crystallization: One crystal nucleation at a time

  • Oscar Urquidi
    Department of Physical Chemistry, Sciences II, University of Geneva, 1211 Geneva, Switzerland
  • Johanna Brazard
    Department of Physical Chemistry, Sciences II, University of Geneva, 1211 Geneva, Switzerland
  • Natalie LeMessurier
    Department of Chemistry, McGill University, Montreal, QC H3A 0B8, Canada
  • Lena Simine
    Department of Chemistry, McGill University, Montreal, QC H3A 0B8, Canada
  • Takuji B. M. Adachi
    Department of Physical Chemistry, Sciences II, University of Geneva, 1211 Geneva, Switzerland

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<jats:title>Significance</jats:title><jats:p>It is of fundamental importance to establish the microscopic picture of crystal nucleation for both academic and industrial research. Here, we report an in situ time-resolved Raman spectroscopy to study crystallization from solution, one crystal nucleation at a time. The observed dynamics of α-glycine crystallization from water without any additive supports the nonclassical nucleation pathway, where prenucleation aggregates form and convert to a crystal. By the direct comparison of Raman spectrum of the aggregates between the experiment and simulation, we propose the structure of these aggregates as linear hydrogen-bonded networks. We demonstrate the power of studying one nucleation event at a time, which can accelerate the investigation of crystal nucleation by optical spectroscopy.</jats:p>

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