<p>Magnetic ordering of perovskite ferroelectric oxides is crucial for enhancing their stability and minimizing energy losses in magnetoelectric devices. However, inducing a transition from a magnetically disordered state to an ordered one remains a formidable challenge. Here, we propose a chemical sulfurization method that significantly enhances the magnetic ordering of multiferroic super-tetragonal phase BiFeO<sub>3</sub> thin film. The out-of-plane and in-plane magnetization significantly increases after sulfurization, accompanied by a rotation of the magnetic easy axis. X-ray absorption spectroscopy and spherical aberration transmission electron microscopy reveal the reconfiguration of local electronic hybridization states, restructuring Fe–O hybridization from pyramid-like FeO<sub>5</sub> to octahedral FeO<sub>6</sub> geometries. This transformation is considered the root cause of the observed magnetic transition in the films. This sulfur-induced strategy for electronic hybridization reconfiguration is expected to break new ground, offering innovative methodologies for modulating perovskite oxides, two-dimensional ferroelectric films, and other ferromagnetic functional thin films.</p>

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Anionic Strategy-Modulated Magnetic Ordering in Super-elongated Multiferroic Epitaxial Films

  • Guoqiang Xi,
  • Yue-Wen Fang,
  • Dongxing Zheng,
  • Shuai Xu,
  • Hangren Li,
  • Jie Tu,
  • Fangyuan Zhu,
  • Xudong Liu,
  • Xiuqiao Liu,
  • Qianqian Yang,
  • Jiushe He,
  • Junwei Zhang,
  • Wugang Liao,
  • Jiesu Wang,
  • Shiyao Wu,
  • Xixiang Zhang,
  • Kuijuan Jin,
  • Jianjun Tian,
  • Linxing Zhang,
  • Xianran Xing

摘要

Magnetic ordering of perovskite ferroelectric oxides is crucial for enhancing their stability and minimizing energy losses in magnetoelectric devices. However, inducing a transition from a magnetically disordered state to an ordered one remains a formidable challenge. Here, we propose a chemical sulfurization method that significantly enhances the magnetic ordering of multiferroic super-tetragonal phase BiFeO3 thin film. The out-of-plane and in-plane magnetization significantly increases after sulfurization, accompanied by a rotation of the magnetic easy axis. X-ray absorption spectroscopy and spherical aberration transmission electron microscopy reveal the reconfiguration of local electronic hybridization states, restructuring Fe–O hybridization from pyramid-like FeO5 to octahedral FeO6 geometries. This transformation is considered the root cause of the observed magnetic transition in the films. This sulfur-induced strategy for electronic hybridization reconfiguration is expected to break new ground, offering innovative methodologies for modulating perovskite oxides, two-dimensional ferroelectric films, and other ferromagnetic functional thin films.