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The role of fluctuations in the nucleation process.

Yuanpeng Deng1,2, Peilin Kang2, Xiang Xu1

  • 1Key Lab of Smart Prevention and Mitigation of Civil Engineering Disasters of the Ministry of Industry and Information Technology and Key Lab of Structures Dynamic Behavior and Control of the Ministry of Education, Harbin Institute of Technology, Harbin 150090, China.

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Researchers studied crystallization in liquids using a new sampling method. They found complex transition states and calculated a nucleation rate consistent with experiments, differing from prior estimates.

Keywords:
enhanced samplingmolecular dynamicsnucleationtransition state

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Area of Science:

  • * Physical Chemistry
  • * Computational Materials Science
  • * Statistical Mechanics

Background:

  • * The transition from liquid to solid states is a fundamental self-assembly process with significant practical applications.
  • * Understanding the nucleation mechanism is crucial for controlling crystallization.
  • * Previous computational methods have faced challenges in accurately simulating crystallization dynamics.

Purpose of the Study:

  • * To investigate the crystallization transition in a Lennard-Jones fluid using a novel committor-based enhanced sampling method.
  • * To analyze the detailed nucleation mechanism and identify key fluctuations leading to solid phase formation.
  • * To compute the nucleation rate and compare it with experimental data and previous theoretical estimates.

Main Methods:

  • * Employed a recently developed committor-based enhanced sampling technique.
  • * Utilized the variational principle derived from the backward Kolmogorov equation.
  • * Analyzed the structure of the transition state ensemble during crystallization.

Main Results:

  • * Detected and analyzed critical fluctuations driving the crystallization process.
  • * Characterized the transition state ensemble, revealing a disordered interface surrounding a nonspherical solid core.
  • * Calculated a nucleation rate that aligns with experimental observations, contrasting with earlier computational predictions.

Conclusions:

  • * The committor-based enhanced sampling method provides a powerful tool for studying complex phase transitions.
  • * The nucleation mechanism involves intricate transition states with unique interfacial properties.
  • * The computed nucleation rate offers a more accurate representation of experimental reality compared to previous estimates.