Predicted alternative structure for tantalum metal under high pressure and high temperature

TL;DR

This study uses first-principles simulations to identify a new stable high-pressure phase of tantalum, called Pnma, which better explains experimental shock data than previously considered structures.

Contribution

The paper introduces a novel stable Pnma phase for tantalum under high pressure, identified through advanced crystal structure prediction and confirmed by phonon and elastic property analyses.

Findings

Pnma phase is more stable than ω and A15 structures.

ω phase is neither mechanically nor dynamically stable.

Pnma's shear sound velocities match experimental shock data.

Abstract

First-principles simulations have been performed to investigate the phase stability of tantalum metal under high pressure and high temperature (HPHT). We searched its low-energy structures globally using our developed multi-algorithm collaborative (MAC) crystal structure prediction technique. The body-centred cubic (bcc) was found to be stable at pressure up to 300 GPa. The previously reported $\omega$ and \textit{A}15 structures were also reproduced successfully. More interestingly, we observed another phase (space group: \textit{Pnma}, 62) that is more stable than $\omega$ and \textit{A}15. Its stability is confirmed by its phonon spectra and elastic constants. For $\omega$-Ta, the calculated elastic constants and high-temperature phonon spectra both imply that it is neither mechanically nor dynamically stable. Thus, $\omega$ is not the structure to which bcc-Ta transits before melting. On the contrary, the good agreement of \textit{Pnma}-Ta shear sound velocities with experiment suggests \textit{Pnma} is the new structure of Ta implied by the discontinuation of shear sound velocities in recent shock experiment [J. Appl. Phys. \textbf{111}, 033511 (2012)].