Anharmonic lattice dynamics via the special displacement method

TL;DR

This paper introduces an efficient method based on the self-consistent phonon theory and special displacement technique to accurately compute temperature-dependent anharmonic phonon dispersions in strongly anharmonic solids, aligning well with experimental data.

Contribution

The authors develop a novel, efficient approach for treating anharmonicity in solids using the special displacement method combined with self-consistent phonon theory, suitable for complex materials.

Findings

Accurate anharmonic phonon dispersions for strongly anharmonic materials.

Method requires few steps for free energy minimization.

Good agreement with experimental and previous computational results.

Abstract

On the basis of the self-consistent phonon theory and the special displacement method, we develop an approach for the treatment of anharmonicity in solids. We show that this approach enables the efficient calculation of temperature-dependent anharmonic phonon dispersions, requiring very few steps to achieve minimization of the system's free energy. We demonstrate this methodology in the regime of strongly anharmonic materials which exhibit a multi-well potential energy surface, like cubic SrTiO$_3$, CsPbBr$_3$, CsPbI$_3$, CsSnI$_3$, and Zr. Our results are in good agreement with experiments and previous first-principles studies relying on stochastic nonperturbative and molecular dynamics simulations. We achieve a very robust workflow by using harmonic phonons of the polymorphous ground state as the starting point and an iterative mixing scheme of the dynamical matrix. We also suggest that the phonons of the polymorphous ground state might provide an excellent starting approximation to explore anharmonicity. Given the simplicity, efficiency, and stability of the present treatment to anharmonicity, it is especially suitable for use with any electronic structure code and for investigating electron-phonon couplings in strongly anharmonic systems.