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中国物理学会期刊

极性纳米微区诱导畴翻转增强电卡效应的机理研究

Investigation on the mechanism of enhanced electrocaloric effect via polar nanoregion-induced domain switching

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  • 为揭示极性纳米微区(PNRs)增强无铅铁电薄膜电卡效应的微观机理,采用金属有机物分解法制备Na0.5Bi0.5TiO3-7BaTiO3(NBT-7BT)薄膜,结合变温压电力显微镜、铁电性能测试与三维相场模拟,系统研究PNRs的电场/温度驱动畴演化规律及其对电卡性能的调控机制。结果表明:在30 ℃退极化温度附近,PNRs被热激活,可显著降低畴翻转能垒,高效诱导面内ab畴向面外c畴定向翻转,使体系饱和极化强度与极化温度敏感性显著提升;在500 kV/cm电场下,基于麦克斯韦关系间接法计算得到薄膜于20~30 ℃区间获得最大绝热温变|ΔT|=2.0 K。理论上三维相场模拟精准复现了PNRs诱导的畴翻转过程,与实验结果高度吻合,从理论上验证了PNRs热-电协同激活到畴结构演化到极化增强再到电卡效应提升的完整物理机制。本研究阐明了PNRs调控畴结构增强电卡效应的微观本质,为设计高性能无铅铁电固态制冷材料提供了实验与理论支撑。

     

    To uncover how polar nanoregions (PNRs) regulate the electrocaloric effect in lead-free ferroelectric thin films, we fabricated Na0.5Bi0.5TiO3-7BaTiO3 (NBT-7BT) films via metal-organic decomposition. Using variable-temperature piezoresponse force microscopy (PFM), ferroelectric characterization, and three-dimensional phase-field simulations, we systematically probed the electric field- and temperature-driven domain evolution of PNRs. Our results reveal that near the depolarization temperature (Td≈30 °C), thermally activated PNRs substantially reduce the domain switching energy barrier, efficiently inducing directional switching from in-plane ab domains to out-of-plane c domains. Consequently, both the saturation polarization (Ps) and its temperature sensitivity are substantially enhanced. Under an applied electric field of 500 kV/cm, the film achieves a maximum adiabatic temperature change |ΔT|= 2.0 K in the range of 20-30 °C, as determined by the indirect method based on Maxwell relations. The three-dimensional phase-field simulations accurately reproduce this PNR-induced switching process, showing excellent agreement with experiments and theoretically validating the complete physical chain: “thermally assisted electrical activation of PNRs→domain structure evolution→polarization enhancement→improved electrocaloric performance.” This work elucidates the microscopic origin of the PNR-tailored electrocaloric enhancement and provides robust experimental and theoretical guidance for designing high-performance, lead-free ferroelectrics for solid-state cooling applications.

     

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