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Optimization of Crystal Growth for Neutron Macromolecular Crystallography
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Published on: March 13, 2021

Two-step vapor-crystal nucleation close below triple point.

J A van Meel1, A J Page, R P Sear

  • 1FOM Institute for Atomic and Molecular Physics, Amsterdam, The Netherlands. vanmeel@amolf.nl

The Journal of Chemical Physics
|December 3, 2008
PubMed
Summary

Crystal nucleation from vapor occurs in two steps: first liquid droplet formation, then crystal nucleation within the droplet. This two-step process, observed via Monte Carlo simulations, is independent of vapor supersaturation in the second stage.

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Area of Science:

  • Physical Chemistry
  • Computational Physics
  • Materials Science

Background:

  • Crystal nucleation from vapor is a fundamental process in materials science.
  • Understanding nucleation pathways is crucial for controlling material properties.
  • Previous studies suggest complex nucleation mechanisms, including surface melting phenomena.

Purpose of the Study:

  • To investigate the crystal nucleation pathway from the vapor phase using Monte Carlo simulations.
  • To analyze the dependence of nucleation rates on vapor supersaturation.
  • To compare simulation results with previous theoretical and computational findings.

Main Methods:

  • Monte Carlo simulations were employed to model crystal nucleation from the vapor phase.
  • The Lennard-Jones system was studied near the triple point.
  • Forward-flux sampling was used to directly compute nucleation rates.

Main Results:

  • A two-step nucleation pathway was observed: liquid droplet formation followed by crystal nucleation within the droplet.
  • The nucleation rate of the liquid droplet strongly depends on vapor supersaturation.
  • Crystal nucleation within the liquid droplet is independent of vapor supersaturation and requires a minimum droplet size.

Conclusions:

  • The observed two-step nucleation process can be described by quasiequilibrium theory.
  • Simulation results align with independent studies using different methodologies, confirming the two-step mechanism.
  • Quantitative comparison is limited due to differences in interaction potential cutoffs.