Impact of host phonons on interstitial diffusion

Abstract

The net effect of host phonons on interstitial diffusion has remained as a fundamental knowledge gap in our current theories since the motions of the host atoms and interstitials were coupled in these theories. Here we study this effect through molecular dynamics simulations of hydrogen diffusion in palladium, in which the motions can be decoupled through pinning the host atoms. Mathematically this decoupling corresponds to expanding the total diffusion coefficient into a Taylor series, which separates the phonon contribution from the intrinsic interstitial jumping. Our results clearly show that palladium phonons significantly promote hydrogen diffusion. The phonon contribution, being linear with temperature at high temperatures and exponential at low temperatures, is fitted with Brownian motion model. The total diffusion of interstitials can be understood as the intrinsic interstitial jumping in a pinned host plus phonon-induced Brownian diffusion. The generality of our findings is validated by examining the motion of lithium in manganese oxide and carbon in iron.