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Structuring of Fluid Adlayers upon Ongoing Unimolecular Adsorption.

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  • 1Department of Physics, Durham University, South Road DH1 3LE, United Kingdom.

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Phenomenological models fail to describe fluid structuring during gradual destabilization. Kinetic Monte Carlo simulations reveal that region size strongly depends on adsorption rate, challenging existing theories in surface catalysis and polymer blends.

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Area of Science:

  • Biophysics
  • Soft Matter Physics
  • Materials Science
  • Surface Science
  • Chemical Engineering

Background:

  • Fluids with spatial density variations are crucial in biophysics, soft matter, and materials science.
  • Fluid structuring typically occurs via spinodal decomposition or nucleation after rapid destabilization (quench).
  • Instantaneous quenches are often impractical, necessitating the study of gradual destabilization processes.

Purpose of the Study:

  • To investigate the inadequacy of current phenomenological descriptions for fluid structuring under gradual destabilization conditions.
  • To explore fluid structuring in the context of surface catalysis using kinetic Monte Carlo (KMC) simulations.
  • To understand the influence of adsorption rate on phase separation dynamics in surface-adsorbed systems.

Main Methods:

  • Utilized kinetic Monte Carlo (KMC) simulations to model the unimolecular adsorption of gaseous molecules onto a metal surface.
  • Simulated adsorbate diffusion and lateral interactions leading to surface phase separation into low- and high-density regions.
  • Analyzed the dependence of the characteristic size of these regions on the rate of adsorption.

Main Results:

  • Demonstrated that commonly used phenomenological models are insufficient for describing fluid structuring during gradual destabilization.
  • Observed that the typical size of coexisting low- and high-density regions is significantly more sensitive to the adsorption rate than predicted by existing models.
  • Identified a strong dependence of domain size on adsorption rate in surface-catalyzed systems.

Conclusions:

  • The study highlights the limitations of current phenomenological models when applied to gradual destabilization scenarios.
  • Findings contribute to a fundamental understanding of how adsorption kinetics influence phase separation in surface-confined systems.
  • Provides insights into the crossover mechanisms between liquid-liquid and liquid-solid demixing in polymer blends.