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Crystallization time scales for polydisperse hard-sphere fluids.

M Cristina Vargas1, Gabriel Pérez-Ángel

  • 1Departamento de Física Aplicada, CINVESTAV del IPN, A. P. 73 Cordemex, 97310 Mérida, Yucatán, Mexico.

Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics
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Summary

Crystallization in hard sphere fluids shows distinct stages: relaxation, nucleation, crystal growth, and coarsening. Increasing polydispersity sharply transitions fluids to a stable glassy state.

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Area of Science:

  • Physics
  • Materials Science
  • Chemical Engineering

Background:

  • Understanding the transition from amorphous to crystalline states is crucial for materials design.
  • Hard sphere fluids provide a fundamental model for studying phase transitions.

Purpose of the Study:

  • To investigate the dynamics of crystallization in dense mono- and polydisperse hard sphere fluids.
  • To characterize the evolution of order parameters and pressure during crystallization.
  • To explore the impact of polydispersity on fluid behavior and phase transitions.

Main Methods:

  • Simulations of initially amorphous hard sphere fluids.
  • Analysis of reduced pressure (Z) decay as a crystallization signature.
  • Monitoring of local and global orientational order parameters (Q[over ¯](6)).
  • Averaging over multiple realizations to identify common evolutionary trends.

Main Results:

  • Crystallization proceeds through distinct phases: fast relaxation, slow nucleation, rapid crystal growth, and slow domain coarsening.
  • Averaged data reveals a consistent crystallization pathway, despite apparent randomness in individual runs.
  • Increased polydispersity induces a sharp transition to a stable glassy fluid, suggesting first-order phase transition behavior.
  • No significant segregation effects were observed at high polydispersity.

Conclusions:

  • A well-defined crystallization pathway exists for hard sphere fluids, characterized by sequential dynamic processes.
  • A sharp boundary likely separates crystallizing and permanently amorphous states in a specific range of packing fractions.
  • Polydispersity plays a critical role in stabilizing amorphous states and influencing phase transition characteristics.