Extracting Phonon Quasiparticles from Molecular Dynamics Simulations

Abstract: Phonon anharmonicity are ubiquitous in real materials, creating finite phonon lifetimes. These effects are crucial for understanding thermal properties and phase stability. In this work, we define optimal phonon quasiparticles as those that maximize their lifetimes, and prove that the information about these quasiparticles is contained in two small matrices $\mathcal{S}$ and $\mathcal{Q}$, which can be constructed directly from molecular dynamics simulations. Based on these knowledge, we proposed an optimization scheme, which allows us to efficiently determine temperature-dependent phonon modes, frequencies and lifetimes. We applied this method to silicon and cubic CaSiO$_3$, revealing their temperature-dependent phonon behaviors and obtaining the well-known phonon softening in cubic CaSiO$_3$. This theory provides a convenient tool for investigating phonon quasiparticles and can be extended to study other quasiparticles, such as electrons and magnons.