Medium-Weight Euro Crunch

Reimer, Cody

doi:10.1145/3513130.3558986

Cited by 1 publication

(1 citation statement)

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“…But two-dimensional diffusion is not an abstract model and arises for gas atoms adsorbed to metal surfaces (Oura et al, 2013), so that the coherent particle diffusion indicated by the non-zero asymmetry parameter may be observed there. Meanwhile experiments are in progress (Fricke and Reimer, 2022) investigating three-site particle exchange in different systems including highly regular pore structures such as molecular organic frameworks (Stallmach et al, 2006;Forse et al, 2020). Moreover, future work aims at expanding the current models of vacancy and gas diffusion to three dimensions and different types of interactions between neighbor particles and walls to gain further insight into the details of local particle concentrations and thermodynamic equilibrium fluxes inside pores.…”

Section: Discussionmentioning

confidence: 99%

Monte-Carlo Analysis of Asymmetry in Three-Site Relaxation Exchange: Probing Detailed Balance

Bluemich

Parziale

Augustine

2023

Preprint

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Abstract. The question is investigated if three-site diffusive relaxation exchange in thermodynamic equilibrium can lead to exchange maps, which are asymmetric for fluids confined to pores. Asymmetry reports circular flow of particles between the relaxation sites which disagrees with detailed balance according to which the particle exchange between any pair of sites must be balanced. Vacancy diffusion and gas diffusion of particles confined to two-dimensional pores were modeled in Monte-Carlo simulations. For each particle move in vacancy diffusion on a 2D checkerboard grid, one of the eight neighboring destination cells was identified on the basis the jump probability calculated from an empirical approximation of the free energy. Gas diffusion was simulated without thermodynamic interaction on a simulation grid which was up to 104 times finer than the particle diameter. It was found that up to 1 % of all particles moves coherently in closed paths. This motion is attributed to pore resonance corresponding to diffusion eigenmodes. The study shows that detailed balance of multi-site exchange does not apply for a small fraction of particles when the exchange is impacted by topological constraints.

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