Quantum diffusion at high interstitial concentrations: Application to surface diffusion

TL;DR

This paper investigates quantum diffusion in high interstitial concentrations within crystalline solids, focusing on surface diffusion of hydrogen isotopes on tungsten, considering quantum effects, interactions, and Monte Carlo simulations.

Contribution

It introduces a model combining quantum diffusion with interstitial interactions and surface diffusion, explaining isotope-dependent diffusion behaviors.

Findings

Quantum transition rates depend on temperature and concentration.

Surface diffusion behavior aligns qualitatively with low-temperature experiments.

Differences in hydrogen isotope diffusion are attributed to quantum statistics and interactions.

Abstract

In this work we first study the quantum diffusion in a volume of a crystalline solid at high interstitial concentrations when the effects of the short-range interactions between the diffusing particles are to be factors. Within the scope of the small-polaron formalism the transition rate depending on both the temperature and the interstitial concentration has been calculated. Then, using the obtained result, we consider the model of surface diffusion that reproduces qualitatively the diffusion behaviour of the hydrogen isotopes on W(110) surface, observed in the lowtemperature experiments [S.C. Wang and R. Gomer, J.Chem.Phys. v.83, 4193 (1985)]. The coverage dependence of the diffusion coefficient is determined by Monte Carlo simulation. The model allows to suppose that substantially the different diffusion of hydrogen (tritium) and deuterium can be the outcome of their different quantum statistic and the direct interactions between the adparticles.