Energetics and diffusion of gold in bismuth telluride

TL;DR

This study combines microscopy, spectroscopy, and ab-initio modeling to investigate gold's solubility and diffusion in bismuth telluride, revealing higher-than-expected concentrations and anisotropic diffusion mechanisms.

Contribution

It provides new insights into gold diffusion mechanisms in Bi₂Te₃, highlighting the role of substitutional defects and anisotropic diffusion pathways.

Findings

Gold concentrations exceed previous solubility limits.

Diffusion into Bi₂Te₃ is slower than expected.

Interstitial and substitutional defects influence diffusion behavior.

Abstract

We have coupled electron microscopy and energy dispersive spectroscopy experiments with \textit{ab-initio} modeling to study the solubility and diffusion of Au in Bi$_2$Te$_3$. We found that thermal annealing of Au films results in Au concentrations in Bi$_2$Te$_3$ above the previously reported solubility limit. The time scale of Au diffusion into Bi$_2$Te$_3$ is also much greater than expected. To explain our observations, we calculate defect formation energies and diffusion barriers within DFT. We identify an interstitial mechanism consistent with the previously observed low solubility and (rapid) anisotropic diffusion. However, the lower formation energies of substitutional defects suggest that they may be active in our experiments and explain the high observed concentrations.