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Non-Markovian dynamics in ice nucleation.

Pablo Montero de Hijes1, Sebastian Falkner2, Christoph Dellago3

  • 1Faculty of Physics, University of Vienna, A-1090 Vienna, Austria.

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|March 2, 2026
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Summary
This summary is machine-generated.

Classical nucleation theory assumes nucleus size dynamics are Markovian. This study reveals non-Markovian dynamics in homogeneous ice nucleation, suggesting nucleus size is not a sufficient reaction coordinate.

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Area of Science:

  • Physical Chemistry
  • Computational Physics
  • Materials Science

Background:

  • The size of the largest crystalline nucleus is a common reaction coordinate in crystallization simulations.
  • Classical nucleation theory often assumes Markovian dynamics for this coordinate.

Purpose of the Study:

  • To investigate if nucleus size dynamics in homogeneous ice nucleation are Markovian.
  • To identify slow modes and develop improved reaction coordinates.

Main Methods:

  • Molecular dynamics simulations of 300 independent ice nucleation trajectories.
  • Analysis of mean recurrence times and structural descriptors.
  • Neural network training to learn the committor function.
  • Symbolic regression for developing an approximate committor.

Main Results:

  • Nucleus size dynamics exhibit history dependence, indicating non-Markovian behavior.
  • Systematic differences observed in nucleus structures between early and late recurrences.
  • Identification of collective variables and a compact approximation of the committor.

Conclusions:

  • Nucleus size alone is insufficient as a reaction coordinate for homogeneous ice nucleation.
  • The identified collective variables and approximate committor offer improved descriptors for nucleation dynamics.