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Abstract Nanosized perovskite ferroelectrics are widely employed in several electromechanical, photonics, and thermoelectric applications. Scaling of ferroelectric materials entails a severe reduction in the lattice (phonon) thermal conductivity, particularly at sub‐100 nm length scales. Such thermal conductivity reduction can be accurately predicted using the information of phonon mean free path (MFP) distribution. The current understanding of phonon MFP distribution in perovskite ferroelectrics is still inconclusive despite the critical thermal management implications. Here, high‐quality single‐crystalline barium titanate (BTO) thin films, a representative perovskite ferroelectric material, are grown at several thicknesses. Using experimental thermal conductivity measurements and first‐principles based modeling (including four‐phonon scattering), the phonon MFP distribution is determined in BTO. The simulation results agree with the measured thickness‐dependent thermal conductivity. The results show that the phonons with sub‐100 nm MFP dominate the thermal transport in BTO, and phonons with MFP exceeding 10 nm contribute ≈35% to the total thermal conductivity, in significant contrast to previously published experimental results. The experimentally validated phonon MFP distribution is consistent with the theoretical predictions of other complex crystals with strong anharmonicity. This work paves the way for thermal management in nanostructured and ferroelectric‐domain‐engineered systems for oxide perovskite‐based functional materials. 

Abstract Acting like thermal resistances, ferroelectric domain walls can be manipulated to realize dynamic modulation of thermal conductivity (k), which is essential for developing novel phononic circuits. Despite the interest, little attention has been paid to achieving room‐temperature thermal modulation in bulk materials due to challenges in obtaining a high thermal conductivity switching ratio (k_high/k_low), particularly in commercially viable materials. Here, room‐temperature thermal modulation in 2.5 mm‐thick Pb(Mg_1/3Nb_2/3)O₃–xPbTiO₃(PMN–xPT) single crystals is demonstrated. With the use of advanced poling conditions, assisted by the systematic study on composition and orientation dependence of PMN–xPT, a range of thermal conductivity switching ratios with a maximum of ≈1.27 is observed. Simultaneous measurements of piezoelectric coefficient (d₃₃) to characterize the poling state, domain wall density using polarized light microscopy (PLM), and birefringence change using quantitative PLM reveal that compared to the unpoled state, the domain wall density at intermediate poling states (0<d₃₃<d_33,max) is lower due to the enlargement in domain size. At optimized poling conditions (d_33,max), the domain sizes show increased inhomogeneity that leads to enhancement in the domain wall density. This work highlights the potential of commercially available PMN–xPT single crystals among other relaxor‐ferroelectrics for achieving temperature control in solid‐state devices.