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  3. Adsorbate Phase Transitions On Nanoclusters From Nested Sampling.

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Adsorbate phase transitions on nanoclusters from nested sampling.

Thanawitch Chatbipho1, Ray Yang2, Robert B Wexler2

  • 1Department of Chemistry, University of Warwick, Coventry CV4 7AL, United Kingdom.

The Journal of Chemical Physics
|November 3, 2025

View abstract on PubMed

Summary
This summary is machine-generated.

Nested sampling revealed two phase transitions in gas adsorption onto nanoclusters: condensation at high temperatures and layer rearrangement at low temperatures. Adsorbate size and interactions dictate site preference and arrangement on the cluster surface.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Computational Chemistry

Background:

  • Understanding gas adsorption on nanoclusters is crucial for catalysis and materials design.
  • Lennard-Jones (LJ) nanoclusters provide simplified models for studying adsorption phenomena.
  • Investigating phase transitions and site selectivity is key to controlling surface interactions.

Purpose of the Study:

  • To investigate adsorption equilibria on the LJ38 nanocluster using nested sampling.
  • To explore the effects of adsorbate-surface well depth and LJ size parameters on adsorption behavior.
  • To identify and characterize phase transitions occurring during gas adsorption.

Main Methods:

  • Nested sampling simulations were performed on the truncated-octahedral LJ38 nanocluster.
  • The canonical partition function was evaluated over a wide temperature range.
  • Systematic variation of adsorbate-surface well depth and LJ size parameters was conducted.

    • Main Results:

    • Two successive phase transitions were identified: gas condensation and lateral rearrangement of the adsorbed layer.
    • Adsorbate-adsorbate interactions influence site preference, shifting from hollow sites to four-coordinated (100) sites when interactions weaken.
    • Adsorbate size impacts low-temperature behavior, with smaller adsorbates aggregating and larger ones distributing evenly.

    Conclusions:

    • Nested sampling is an effective, automated tool for exploring surface configurational space.
    • Findings highlight trends in facet competition and lattice mismatch in nanocluster adsorption.
    • The study provides insights for designing interfaces with controlled adsorption properties.