Mn-atomic-layered antiphase boundary enhanced ferroelectricity in KNN-based lead-free films

Liqiang Xu, Zhengyang Kong, Beibei Zhu, Xu Wang, Kun Han, Pingfan Chen, Chao Li, Wenbin Wu, Fang-Zhou Yao (), Ke Wang, Zhen Huang () and Feng Chen ()
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Liqiang Xu: Anhui University
Zhengyang Kong: Anhui University
Beibei Zhu: Anhui University
Xu Wang: Anhui University
Kun Han: Anhui University
Pingfan Chen: Anhui University
Chao Li: Xi’an Jiaotong University
Wenbin Wu: Anhui University
Fang-Zhou Yao: Wuzhen Laboratory
Ke Wang: Wuzhen Laboratory
Zhen Huang: Anhui University
Feng Chen: Chinese Academy of Sciences

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract One preferred lead-free ferroelectric, (K,Na)NbO3, offers prominent features of environmentally benign and excellent piezoelectricity, but suffers from poor ferroelectricity. Mn-doping has improved its electrical properties, yet its site occupancy remained unclear. In this study, Mn-atomic-layered antiphase boundaries were created in (K,Na)NbO3-based films, revealing Mn occupying the A-site position. These boundaries stabilized ferroelectricity in these (K,Na)NbO3-based films with a large twice remnant polarization (~72.5 μC/cm2) across a wide frequency range (20 Hz−10 kHz). High-resolution imaging shows densely arranged antiphase boundaries are grown along three crystal axes. These boundaries are Mn-atomic-enriched at a nanoscale width of a single unit cell, equilibrating the interfacial charges and clamp the interfacial strain, resulting in the highly squared hysteresis loops and high Curie temperature of ~400 °C in the films. Our results may provide a paradigm for designing high-performance lead-free ferroelectric films, unleashing their application potential for expelling lead-containing counterparts.

Date: 2025
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DOI: 10.1038/s41467-025-61170-w

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