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This study integrates second harmonic generation (SHG) imaging with differential scanning calorimetry (DSC) to observe stochastic phase transformations in crystals. The combined technique revealed complex thermal behaviors and a "cold phase transformation" in trehalose dihydrate.

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Area of Science:

  • Crystallography
  • Materials Science
  • Physical Chemistry

Background:

  • Crystalline phase transformations are crucial in materials science.
  • Conventional methods like differential scanning calorimetry (DSC) provide bulk information on phase transitions.
  • Observing single-particle stochastic transformations requires advanced imaging techniques.

Purpose of the Study:

  • To integrate second harmonic generation (SHG) imaging with DSC for studying stochastic phase transformations at the single-particle level.
  • To investigate the molecular packing arrangements and lattice transformations during dehydration/desolvation events.
  • To explore the complex phase behavior of trehalose dihydrate using stochastic differential scanning calorimetry (SDSC).

Main Methods:

  • Utilized second harmonic generation (SHG) imaging, a technique sensitive to molecular packing in noncentrosymmetric lattices.
  • Employed differential scanning calorimetry (DSC) to detect bulk phase transformations.
  • Developed and applied stochastic differential scanning calorimetry (SDSC) for single-particle analysis.

Main Results:

  • Successfully correlated SHG imaging observations of lattice transformations with DSC-detected phase transformations.
  • Observed stochastic phase transformations within individual crystalline particles.
  • SDSC revealed diverse single-particle thermal trajectories for trehalose dihydrate.
  • Provided direct evidence of a "cold phase transformation" in trehalose dihydrate, undetectable by conventional DSC.

Conclusions:

  • The integration of SHG imaging and DSC provides unprecedented insight into single-particle stochastic phase transformations.
  • SDSC is a powerful tool for characterizing complex phase behavior and uncovering subtle transformations like "cold phase transformations".
  • This approach advances the understanding of phase transitions in crystalline materials, particularly in biologically relevant molecules like trehalose.