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<p>The mixed tetrahedral–octahedral (MTO) architecture, a characteristic structural motif of brownmillerite and spinel oxides, underpins the multiferroic behaviour and magnetoelectric coupling exhibited by these oxides. Yet, this structural motif remains unexplored in two-dimensional hybrid organic–inorganic perovskites (HOIPs) that typically adopt the octahedral framework. Here we demonstrate that incorporating sterically demanding organic ligands into copper halide HOIPs stabilizes the MTO phase over the Ruddlesden–Popper phase during single-crystal growth. This approach yields a family of MTO perovskites exhibiting structural asymmetry and diverse magnetic orderings. Interestingly, (4,4-difluoropiperidinium)<sub>2</sub>CuBr<sub>4</sub> displays concurrent ferroelectricity and intralayer antiferromagnetism. By monitoring strain-mediated phase evolution, we examine the reversible transition between the MTO and Ruddlesden–Popper phases. Our work broadens the structural diversity of 2D HOIP beyond conventional octahedral frameworks, establishing a framework for exploring emergent multiferroicity and magnetoelectric phenomena.</p><p></p>

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Two-dimensional mixed tetrahedral–octahedral hybrid perovskites with coexisting ferroelectricity and intralayer antiferromagnetism

  • 期刊论文

  • 发表日期：

    2025年11月20日

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  • Ming Wang,
  • Shurong Yuan,
  • Dequan Jiang,
  • Walter P. D. Wong,
  • Hwa Seob Choi,
  • Hengxing Yang,
  • Chuanqi Zhang,
  • Xiaotao Zhang,
  • Yonggang Wang,
  • Wenping Hu,
  • Kian Ping Loh

摘要

The mixed tetrahedral–octahedral (MTO) architecture, a characteristic structural motif of brownmillerite and spinel oxides, underpins the multiferroic behaviour and magnetoelectric coupling exhibited by these oxides. Yet, this structural motif remains unexplored in two-dimensional hybrid organic–inorganic perovskites (HOIPs) that typically adopt the octahedral framework. Here we demonstrate that incorporating sterically demanding organic ligands into copper halide HOIPs stabilizes the MTO phase over the Ruddlesden–Popper phase during single-crystal growth. This approach yields a family of MTO perovskites exhibiting structural asymmetry and diverse magnetic orderings. Interestingly, (4,4-difluoropiperidinium)2CuBr4 displays concurrent ferroelectricity and intralayer antiferromagnetism. By monitoring strain-mediated phase evolution, we examine the reversible transition between the MTO and Ruddlesden–Popper phases. Our work broadens the structural diversity of 2D HOIP beyond conventional octahedral frameworks, establishing a framework for exploring emergent multiferroicity and magnetoelectric phenomena.