Carbon diffusion in alpha-iron: Evidence for quantum mechanical tunneling

TL;DR

This study provides evidence that quantum mechanical tunneling significantly influences carbon diffusion in alpha-iron at low temperatures, explaining the temperature-independent diffusion behavior observed experimentally.

Contribution

The paper introduces a quantum tunneling model for carbon diffusion in alpha-iron, aligning theoretical predictions with experimental data at low temperatures.

Findings

Diffusion constant becomes temperature-independent below LNT.

Quantum tunneling dominates carbon migration at low temperatures.

The model accurately predicts vibrational frequencies and migrational barriers.

Abstract

Recent experimental data on the diffusion coefficient of carbon in alpha-iron below liquid nitrogen temperature (LNT) question the classical approach to the observed temperature dependence. As the temperature is lowered below LNT, the diffusion constant tends to a nearly temperature-independent value rather than continuing its activated trend. The low temperature branch is apparently characteristic of a quantum mechanical process dominated by tunneling in ground state. Concommitantly, we apply an occurrence probability approach to describing the overall temperature dependence as a single continuous rate. Within the adiabatic approximation the electronic eigenvalue depending parametrically on the nuclear coordinates is taken to be the potential energy to control the motion of the nuclei. The resulting rate involves all horizontal-tunneling energy-conserving elastic transitions at the quantized energy levels of the migrating atom. A small though not negligible slope of in the temperature dependence as the temperature is raised below 100 K is dealt with by complementing for the rate of a parallel one-phonon inelastic tunneling process in excess to the basic elastic-tunneling rate. Our combined approach agrees well with the experimental data. In particular, the frequency of the coupled vibration is obtained virtually identical to the carbon vibrational frequency from inelastic neutron-scattering data. The migrational barrier is also found to be within the limits expected for alpha-iron.