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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Crystallization Science

Background:

  • Molecules at liquid/vapor interfaces exhibit distinct organizations and mobilities compared to bulk phases.
  • These interfacial differences can influence crystal nucleation rates, but this effect is not fully understood.
  • Anisotropic molecules may preferentially orient at interfaces, impacting nucleation behavior.

Purpose of the Study:

  • To investigate the effect of liquid/vapor interfaces on crystal nucleation rates and polymorph selection.
  • To compare surface nucleation with bulk nucleation for amorphous poscaconazole.
  • To understand the molecular mechanisms driving interfacial nucleation enhancement and polymorph selection.

Main Methods:

  • Measurement of crystal nucleation rates at both the surface and in the bulk of amorphous poscaconazole.
  • Analysis of molecular organization and mobility at the liquid/vapor interface.
  • Comparison of nucleation behavior across different systems, including D-arabitol, acetaminophen, and water.

Main Results:

  • Surface nucleation of poscaconazole is enhanced by approximately 9 orders of magnitude compared to bulk nucleation.
  • Surface nucleation selects a different polymorph (II) than bulk nucleation (I).
  • This phenomenon is linked to the similarity between anisotropic surface molecular packing and the structure of the surface-nucleating polymorph.

Conclusions:

  • Liquid/vapor interfaces significantly enhance crystal nucleation rates, rather than suppress them.
  • Polymorphic changes during interfacial nucleation occur when surface structural reconstruction favors a different polymorph.
  • These findings aid in predicting interfacial effects on nucleation and polymorph selection, particularly for systems with high surface-area-to-volume ratios.