Effects of high-order anharmonicity on anomalous lattice dynamics and thermal transport in fully filled skutterudite YbFe4Sb12

Abstract

Accurately describing the lattice dynamics and microscopic mechanism of thermal transport in materials with low-lying flat phonon modes remains an outstanding challenge due to the intrinsic strong anharmonicity. In this paper, we investigate the lattice dynamics and thermal transport in skutterudite ${\mathrm{YbFe}}_{4}{\mathrm{Sb}}_{12}$ using a state-of-the-art first-principles-based anharmonic phonon renormalization technique and a unified theory of lattice thermal transport. In contrast to the previous phenomenological models that introduce additional resonant scattering terms or hopping channels, we show that the unusual total lattice thermal conductivity in ${\mathrm{YbFe}}_{4}{\mathrm{Sb}}_{12}$ can be accurately predicted by considering anharmonic phonon renormalization and coherence contributions from the off-diagonal terms of heat flux operators. Both the cubic and quartic anharmonicities are essential for precisely predicting the significant shift in phonon energies. Specifically, the anharmonicity-induced phonon stiffening of the low-lying flat modes significantly enhances the thermal conductivity of particlelike phonons, e.g., by up to a factor of 1.6 at 300 K, by suppressing the cubic coupling strength and altering the scattering phase space, resulting in much-improved agreement with experiments. By further including the coherence contributions, the predicted total thermal conductivity increases by \ensuremath{\sim}22% throughout the entire temperature range, reproducing well the experimental values in both magnitude and temperature dependence. In this paper, we highlight the strong impact of higher-order anharmonicity on lattice dynamics and thermal transport in the filled skutterudite ${\mathrm{YbFe}}_{4}{\mathrm{Sb}}_{12}$. The insights gained in this paper will be helpful for manipulating the thermal properties of skutterudites and potentially other complex materials with strong anharmonicity, which can improve their performance in applications such as thermoelectrics, ferroelectrics, and photovoltaics.