Probing Anharmonic Lattice Dynamics and Thermal Transport in Layered Perovskite LiYTiO4 Anode

Abstract

Layered perovskite lithium yttrium titanate ($\rm LiYTiO_4$) has recently emerged as a promising low-potential, ultrahigh-rate intercalation-type anode material for lithium-ion batteries; however, its lattice dynamics and thermal transport properties remain poorly understood, limiting a complete evaluation of its practical potential. Here, we combine experimental measurements with theoretical modeling to systematically investigate the anharmonic lattice dynamics and heat transport in $\rm LiYTiO_4$. We employ a neural evolution potential (NEP)-based framework that integrates the temperature-dependent effective potential method with the Wigner thermal transport (WTT) formalism, explicitly including both diagonal and off-diagonal terms of the heat-flux operator. Zero-temperature phonon calculations reveal dynamical instabilities associated with $\rm TiO_6$ octahedral rotation, which are stabilized at finite temperatures through anharmonic renormalization. Using the WTT approach with contributions from phonon propagation and coherence contributions, we predict a room-temperature lattice thermal conductivity ($\kappa_{\rm L}$) of 3.8 $\rm Wm^{-1}K^{-1}$ averaged over all crystal orientations, in close agreement with the measured value of 3.2 \pm 0.08 $\rm Wm^{-1}K^{-1}$ for polycrystalline samples. To further examine the possible influence of ionic motion on high-temperature thermal transport, we compute $\kappa_{\rm L}$ using a Green-Kubo equilibrium molecular dynamics approach based on the same NEP, which yields consistent results with both experiment and WTT predictions, confirming the negligible role of Li-ion mobility in heat conduction. Our study not only identifies the ultralow thermal conductivity of $\rm LiYTiO_4$ as a key limitation for its practical application but also establishes a reliable computational framework for studying thermal properties in battery materials.