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A microscopic approach to crystallization: Challenging the classical/non-classical dichotomy.

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This study introduces a new framework for understanding crystallization, revealing that while crystal nucleation pathways can be non-classical, cluster size often remains a key factor, supporting classical nucleation theory in many cases.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Computational Physics

Background:

  • Classical nucleation theory (CNT) provides a foundational understanding of phase transitions.
  • However, experimental and simulation studies increasingly reveal non-classical crystallization pathways.
  • A unified theoretical framework is needed to reconcile these observations.

Purpose of the Study:

  • To develop a fundamental, parameter-free framework for studying crystallization.
  • To investigate colloidal crystal and droplet nucleation pathways using this framework.
  • To assess the applicability of classical nucleation theory to non-classical pathways.

Main Methods:

  • Combined classical density functional theory (DFT) and fluctuating hydrodynamics.
  • Studied nucleation of droplets and crystalline solids from colloidal solutions.
  • Analyzed critical clusters and computed unstable modes.

Main Results:

  • Nucleation pathways for droplets and crystals show early similarities, diverging due to rapid ordering in solids.
  • Despite non-classical pathways, cluster size consistently acts as the primary order parameter.
  • Nucleation rates can be systematically extracted from the developed formalism.

Conclusions:

  • The study provides a nuanced perspective on crystal nucleation, bridging classical and non-classical descriptions.
  • Classical nucleation theory can offer reasonable predictions for solids even with non-classical pathways.
  • The developed framework offers a systematic approach to studying crystallization dynamics.