Mode-Decay Molecular Dynamics for Frequency-Dependent Phonon Scattering Rates

The thermal conductivity of crystalline materials can be determined in a statistical mechanical framework as long as phonon relaxation rates are known. Unfortunately, these quantities are difficult if not impossible to measure directly, and attempts to deduce these quantities yield gross averages not energy dependent relationships. Consequently, researchers often rely on heuristic models such as Holland’s suite of scattering rates for various phonon modes. A new molecular dynamics method was developed to estimate mode-dependent scattering rates by tracking the decay of an initially imposed standing wave. The wave vector is systematically changed and the corresponding decay is collected. Ultimately, the the thermal conductivity can be reconstructed using a Landauer formalism. The phonon scattering rates of a LJ crystal are calculated using this method. The standing wave decay approach allows scattering rates to be probed more directly than wave packet simulations, which are often used to obtain transmission coefficients.