Intrinsically low thermal conductivity of stoichiometric lithium niobate:Experimental measurement and microscopic origin

Abstract

With the rapid development of integrated electro-optic and nonlinear optical devices based on lithium niobate (LiNbO$_3$, LN), thermal management is becoming a critical area of focus. However, experimental measurement of thermal transport in stoichiometric LiNbO$_3$ (sLN) remains scarce, and the intrinsic microscopic mechanisms remain to be established. Here, we combine the laser pump-probe technique of frequency-domain thermoreflectance (FDTR) with state-of-the-art machine-learned atomistic simulations to comprehensively investigate thermal transport in sLN. The measured and simulated room-temperature thermal conductivity ($κ$) values of sLN agree well, which are orders-of-magnitude lower than that of many classic and emerging semiconductors such as silicon. Furthermore, the temperature-dependent $κ$ exhibits a $T^{-α}$ scaling with $α$ near unity, suggesting that thermal transport is dominated by intrinsic phonon-phonon scattering. By comparing sLN with cubic boron arsenide (cBAs) which serves as an ultrahigh-$κ$ benchmark, we reveal that harmonic properties are not responsible for the low $κ$ of sLN, which feature phonon heat capacity and group velocities that are either higher than or comparable to those in cBAs. Instead, the low $κ$ originates from substantially stronger anharmonicity and larger scattering phase space. These two factors collectively suppress phonon lifetimes by 1-2 orders of magnitude, leading to a maximum phonon mean free path of approximately 140 nm. As a result, notable size effects emerge in thin-film sLN below 1 $μ$m, with $κ$ dropping to half the bulk value at 10 nm. Altogether, our findings establish a fundamental understanding of thermal transport in sLN and provide atomistic insights for thermal management in advanced lithium niobate technologies.