Competing Octahedral Modes in the Hybrid Improper Ruddlesden–Popper Ferroelectric Ln2SrSc2O7

IF 7.2 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Chemistry of Materials Pub Date : 2025-05-22 DOI:10.1021/acs.chemmater.5c00325

Yu Lu Wei, Zhe Guo, Zheng Duan Zhang, Jiamin Lin, Diming Xu, Yuhui Huang, Xue-Zeng Lu, Xiao Qiang Liu, Xiang Ming Chen

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Abstract

The ferroelectric polarization in hybrid improper ferroelectrics (HIFs) is induced by the combination of oxygen octahedral in-plane rotation (OOR) and out-of-plane tilting (OOT) in perovskite-like structures. Specifically, the widely reported A2₁am phase is established by the one-component order parameters (OPs) of the OOR and the OOT in the double-layered Ruddlesden–Popper compounds. In the present work, an unexpected polar P2₁am phase is identified in Ln₂SrSc₂O₇ (Ln = Pr, Nd, Sm) ceramics, showing a one-component OP of the OOT and a two-component OP of the OOR and thus leading to the coexistence of the polar and antipolar distortions within the phase. The room-temperature ferroelectricity is approved by the well-defined ferroelectric polarization–electric field hysteresis loops. In situ diffraction analysis reveals a phase transition to the nonpolar Amam phase at high temperatures. The magnitude of ferroelectric polarization is significantly influenced by the degree of A-site cation disorder and the tolerance factor, while the Curie temperature exhibits a linear increase with a decreasing tolerance factor, independent of the degree of A-site cation disorder. This work emphasizes the critical role of complicated oxygen octahedral distortions and offers a strategic pathway for the rational design of advanced HIF materials.

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杂化不当Ruddlesden-Popper铁电材料Ln2SrSc2O7的竞争八面体模式

杂化不当铁电体（hif）中的铁电极化是由类钙钛矿结构中氧八面体的面内旋转（OOR）和面外倾斜（OOT）共同引起的。具体来说，广泛报道的A21am相是由双层Ruddlesden-Popper化合物中OOR和OOT的单组分序参数（OPs）建立的。在本研究中，在Ln2SrSc2O7 （Ln = Pr, Nd, Sm）陶瓷中发现了一个意想不到的极性P21am相，显示出OOT的单组分OP和OOR的双组分OP，从而导致相内极性和反极性扭曲共存。明确定义的铁电极化-电场磁滞回线证实了室温铁电性。原位衍射分析显示在高温下相变为非极性Amam相。铁电极化强度受a位阳离子无序度和容差因子的显著影响，居里温度随容差因子的减小呈线性增加，与a位阳离子无序度无关。这项工作强调了复杂氧八面体畸变的关键作用，为先进HIF材料的合理设计提供了战略途径。

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来源期刊

Chemistry of Materials 工程技术-材料科学：综合

CiteScore

14.10

自引率

5.80%

发文量

929

审稿时长

1.5 months

期刊介绍： The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.