Significant Enhancement of Thermoelectric Performance in Bi_0.5Sb_1.5Te₃ Thin Film via Ferroelectric Polarization Engineering

Abstract The Bi_0.5Sb_1.5Te₃ (BST) thin film shows great promise in harvesting low‐grade heat energy due to its excellent thermoelectric performance at room temperature. In order to further enhance its thermoelectric performance, specifically the power factor and output power, new approaches are highly desirable beyond the common “composition‐structure‐performance” paradigm. This study introduces ferroelectric polarization engineering as a novel strategy to achieve these goals. A Pb(Zr_0.52Ti_0.48)O₃/Bi_0.5Sb_1.5Te₃ (PZT/BST) hybrid film is fabricated via magnetron sputtering. Density functional theory calculations demonstrate PZT polarization's influence on charge redistribution and interlayer charge transfer at the PZT/BST interface, facilitating adjustable carrier transport behavior and power factor of the BST film. As a result, a 26.7% enhancement of the power factor, from unpolarized 12.0 to 15.2 µW cm⁻¹ K⁻², is reached by 2 kV out‐of‐plane downward polarization of PZT. Furthermore, a five‐leg generator constructed using this PZT/BST hybrid film exhibits a maximum output power density of 13.06 W m⁻² at ΔT = 39 K, which is 20.8% higher than that of the unpolarized one (10.81 W m⁻²). The research presents a new approach to enhance thermoelectric thin films’ power factor and output performance by introducing ferroelectric polarization engineering.