Anharmonic lattice dynamics via the special displacement method

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 thismethodology in the regime of strongly anharmonic materials, which exhibit a multiwell potential energy surface, like cubic SrTiO3, CsPbBr3, CsPbI3, CsSnI3, 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.

Automated summary

In this paper, we present an approach for the treatment of anharmonicity in solids based on the self-consistent phonon theory and the special displacement method. Our method allows for efficient calculation of temperature-dependent anharmonic phonon dispersions with minimal steps for minimizing the system's free energy. The results demonstrate good agreement with experiments and previous studies, and show promise for investigating strongly anharmonic systems.