Ruddlesden-Popper结构杂化非常规铁电体的研究进展

doi:10.15541/jim20240521

无机材料学报 ›› 2025, Vol. 40 ›› Issue (6): 587-608.DOI: 10.15541/jim20240521

Ruddlesden-Popper结构杂化非常规铁电体的研究进展

张碧辉¹^,²^,³(), 刘小强²^,⁴(), 陈湘明²

1.重庆理工大学理学院, 重庆 400054
2.浙江大学材料科学与工程学院, 杭州 310058
3.电子科技大学材料与能源学院, 成都 610054
4.浙江大学台州研究院, 全省先进固态储能技术及应用重点实验室, 台州 318000

收稿日期:2024-12-17 修回日期:2025-02-24 出版日期:2025-06-20 网络出版日期:2025-02-19
通讯作者: 刘小强, 教授. E-mail: xqliu@zju.edu.cn
作者简介:张碧辉(1996-), 女, 讲师. E-mail: zhangbh@cqut.edu.cn
基金资助:
国家自然科学基金(52172131)

Recent Progress of Hybrid Improper Ferroelectrics with Ruddlesden-Popper Structure

ZHANG Bihui¹^,²^,³(), LIU Xiaoqiang²^,⁴(), CHEN Xiangming²

1. College of Science, Chongqing University of Technology, Chongqing 400054, China
2. School of Materials Science and Engineering, Zhejiang University, Hangzhou 310058, China
3. School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 610054, China
4. Zhejiang Key Laboratory of Advanced Solid State Energy Storage Technology and Applications, Taizhou Institute of Zhejiang University, Taizhou 318000, China

Received:2024-12-17 Revised:2025-02-24 Published:2025-06-20 Online:2025-02-19
Contact: LIU Xiaoqiang, professor. E-mail: xqliu@zju.edu.cn
About author:ZHANG Bihui (1996-), female, lecturer. E-mail: zhangbh@cqut.edu.cn
Supported by:
National Natural Science Foundation of China(52172131)

摘要/Abstract

摘要：

杂化非常规铁电性(Hybrid Improper Ferroelectricity, HIF)指的是在含钙钛矿结构单元的化合物中, 通过阴离子八面体面内旋转和面外倾侧耦合而产生的二阶铁电序。HIF有望在强磁电耦合多铁性材料中获得重要应用, 并极大地拓展铁电体物理学的内涵和外延。本文总结了Ruddlesden-Popper(R-P)结构HIF的实验研究进展, 建立了双层R-P结构铁电体的居里温度(T_C)和许容因子(τ)之间的线性关系, 并阐述其HIF物理起源。基于HIF的内禀电控磁性, 在双层R-P铁氧体中观察到室温极性相和弱铁磁相共存, 这一发现具有重要的科学意义。此外, 在A位离子有序三层R-P氧化物中报道的铁电性显著拓宽了HIF的研究广度和深度。尽管R-P结构的HIF的研究已取得显著进展, 但在新材料体系和单相多铁性材料探索方面仍需进一步努力。

关键词: 杂化非常规铁电性, Ruddlesden-Popper结构, 单相多铁性, 综述

Abstract:

Hybrid improper ferroelectricity (HIF) is recognized as a secondary ferroelectric phenomenon induced by coupling of in-plane rotation and out-of-plane tilt of anion octahedra in compounds with the units of perovskite structure. HIF is expected to be applicable in the multiferroic materials with strong magnetoelectric coupling owing to its intrinsic characteristic for electric-field control of magnetism, thereby greatly extending the connotation and denotation of ferroelectric physics. This paper focuses on the experimental progress of HIF materials with Ruddlesden-Popper (R-P) structure. It also establishes the linear relationship between Curie temperature (T_C) and tolerance factor (τ) of double-layered R-P oxides, elucidating the underlying physical mechanisms of HIF. Based on intrinsic electric-field control of magnetism for HIF, the detection of coexistence of polar and weak ferromagnetic phases in ferrites with double-layered R-P structures is of great scientific significance. Additionally, the documented ferroelectricity in the A-site cation-ordered triple-layered R-P oxide has significantly expanded the fields of HIF. Although significant progress has been achieved in understanding HIF in R-P oxides, more efforts should be made to explore more new material systems and single-phase multiferroic materials.

Key words: hybrid improper ferroelectricity, Ruddlesden-Popper structure, single-phase multiferroicity, review

中图分类号:

O482

张碧辉, 刘小强, 陈湘明. Ruddlesden-Popper结构杂化非常规铁电体的研究进展[J]. 无机材料学报, 2025, 40(6): 587-608.

ZHANG Bihui, LIU Xiaoqiang, CHEN Xiangming. Recent Progress of Hybrid Improper Ferroelectrics with Ruddlesden-Popper Structure[J]. Journal of Inorganic Materials, 2025, 40(6): 587-608.

图/表 17

图1 (a)基于R-P结构的HIF的多功能特性总结; (b)基于Web of Science数据库总结的近年发表的R-P氧化物文章数量

Fig. 1 (a) Summary of multifunctional properties in HIF with R-P structure; (b) Number of articles published on R-P oxides in recent years based on the Web of Science database

图2 (a)常规铁电相变和(b)非常规铁电相变的能量变化[23]

Fig. 2 Energetics of a transition from paraelectric to ferroelectric phase for (a) proper and (b) improper ferroelectric system[23] F represents thermodynamic free energy of the system, η represents atomic polarity displacement, and T represents temperature. The black line represents the free energy of T>TC, and the minimum value of the free energy is at η=0, indicating that it is a paraelectric phase. The red line indicates the free energy of T<TC, and the minimum value of the free energy is at η≠0, indicating that it is a ferroelectric phase. The three lines between black and red indicate the transition state between the paraelectric phase and the ferroelectric phase. Colorful figure is available on website.

图3 R-P结构A′2AB2O7从(a)顺电相到(b)铁电相的对称模分解及(c)铁电相中每层沿a轴的反铁畸变位移(X)及总的铁电极化强度(Ptotal)示意图[25]

Fig. 3 Symmetry mode decomposition of the (a) paraelectric to (b) ferroelectric structure in R-P A′2AB2O7, and (c) representation of anti-ferrodistortive displacements (X) at every layer and total ferroelectric polarization (Ptotal) in ferroelectric structure[25]

图4 (a) A3B2O7 R-P型氧化物的铁电a−a−c+结构; (b) A3B2O7的氧八面体倾转的第一性原理振幅和诱导极性模式(按ABO3结构τ递增排列)[26]

Fig. 4 (a) Ferroelectric a−a−c+ structure of A3B2O7 R-P phase; (b) First principles amplitudes of two octahedral rotations and induced polar mode for a suite of A3B2O7 materials, arranged by increasing τ of ABO3 parent[26]

图5 (a, b) (Ca,Sr)3Ti2O7单晶的a0a0c+和a−a−c0两个氧八面体倾转模式的示意图; (c, d) Ca2.46Sr0.54Ti2O7单晶的(c) (001)解理表面照片和(d)室温环形差分干涉衬度照片; (e) Ca3−xSrxTi2O7(x=0, 0.54, 0.85)单晶沿[110]方向的电滞回线; (f) IP-PFM的配置示意图[49]

Fig. 5 (a, b) Schematic diagrams of two octahedral tilt modes of a0a0c+and a−a−c0 of (Ca,Sr)3Ti2O7 single crystal; (c) Photographic and (d) circular differential interference contrast image of a cleaved (001) surface of Ca2.46Sr0.54Ti2O7 single crystal; (e) Ferroelectric hysteresis loops of Ca3−xSrxTi2O7 (x=0, 0.54, 0.85) single crystal along [110] orientation; (f) Schematic picture of IP-PFM measurement[49]

表1 双层R-P结构Ca3Ti2O7基氧化物的铁电性能相关参数[43-44,49,64,70 -73,79 -81]

Table 1 Parameters regarding ferroelectric properties of Ca3Ti2O7-based oxides with double-layered R-P structure[43-44,49,64,70 -73,79 -81]

Compound		τ	P_r/(μC·cm^-2)	E_c/(kV·cm^-1)	T_C/K	Ref.
Ca₃Ti₂O₇	Ceramic	0.8465	0.9	110	1085	[64]
Ca₃Ti₂O₇	Sol-Gel ceramic	0.8465	4.32	108	1046	[80]
Ca₃Ti₂O₇	Two-step ceramic	0.8465	1.32	78	—	[79]
Ca₃Ti₂O₇	Film	0.8465	8	5	—	[81]
Ca₃Ti₂O₇	Single crystal	0.8465	8	150	—	[49]
Ca_2.9Sr_0.1Ti₂O₇	Ceramic	0.8487	0.5	210	1034	[73]
Ca_2.8Sr_0.2Ti₂O₇	Ceramic	0.8508	0.2	190	970	[73]
Ca_2.7Sr_0.3Ti₂O₇	Ceramic	0.8529	0.12	185	940	[73]
Ca_2.6Sr_0.4Ti₂O₇	Ceramic	0.8550	0.1	170	850	[73]
Ca_2.46Sr_0.54Ti₂O₇	Single crystal	0.8580	0.54	150	—	[49]
Ca_2.15Sr_0.85Ti₂O₇	Single crystal	0.8645	0.85	180	—	[49]
Ca₃Ti_1.9Mn_0.1O₇	Ceramic	0.8481	0.6	122	1075	[43]
Ca₃Ti_1.8Mn_0.2O₇	Ceramic	0.8497	0.4	145	1030	[43]
Ca₃Ti_1.7Mn_0.3O₇	Ceramic	0.8513	0.3	150	1000	[43]
Ca₃Ti_1.8Al_0.1Nb_0.1O₇	Ceramic	0.8472	1.24	160	1082	[44]
Ca₃Ti_1.8Al_0.1Nb_0.1O₇	Ceramic	0.8453	0.5	130	1099	[44]
Ca₃Ti_1.9Al_0.1O_6.95	Ceramic	0.8480	0.5	130	973	[44]
Ca_2.9La_0.1Ti_1.9Al_0.1O₇	Ceramic	0.8484	0.39	115	950	[64]
Ca_2.8La_0.2Ti_1.8Al_0.2O₇	Ceramic	0.8503	0.17	117	797	[64]
Ca_2.7La_0.3Ti_1.7Al_0.3O₇	Ceramic	0.8521	0.16	120	645	[64]
Ca_2.85Na_0.15Ti₂O₇	Ceramic	0.8469	0.2	50	—	[71]
Ca_2.99Na_0.01Ti₂O₇	Ceramic	0.8466	0.5	80	—	[72]
Ca_2.9Ru_0.1Ti₂O₇	Ceramic	0.8428	4.4	100	—	[70]

图6 双层R-P结构Ca3Ti2O7基化合物的铁电性能对比[40]

Fig. 6 Comparison of ferroelectric properties for Ca3Ti2O7-based compounds with double-layered R-P structure[40]

图7 (a)室温下利用g=100衍射斑点得到的DF-TEM照片, 红蓝箭头代表沿[100]的铁电极化方向; (b)利用g=220衍射斑点得到的DF-TEM照片; (c) Ca3[Mn0.5(Fe0.5Nb0.5)0.5]2O7陶瓷室温下的PFM测试结果; (d)改变交流电压条件下的一次与二次谐波压电响应图; (e, f)不同直流偏压下的(e)振幅蝴蝶曲线及(f)相位迟滞回线[45]

Fig. 7 (a) DF-TEM image obtained at room temperature (RT) using the g=100 diffraction spot showing the ferroelectric domains, with blue and red arrows indicating directions of ferroelectric polarization along [100]; (b) DF-TEM image obtained at RT using the reflection g=220; (c) PFM measurements for Ca3[Mn0.5(Fe0.5Nb0.5)0.5]2O7 ceramics at RT: mappings of topography, amplitude contrast, phase contrast, and contact resonant frequency; (d) First and second harmonic responses versus AC voltage; (e, f) Local switching spectroscopy for (e) amplitude voltage butterfly loops and (f) phase voltage hysteresis loops under various DC bias[45]

图8 双层R-P结构Sr基氧化物(Sr3Sn2O7单晶[112]、(Sr,Ba)3Sn2O7陶瓷[84]、(Sr,Ca)3Sn2O7陶瓷[85]、(Sr,Ba)3Zr2O7陶瓷[86]、Sr3(Sn,Zr)2O7陶瓷[113])的铁电性能对比

Fig. 8 Comparison of ferroelectric properties for Sr-based oxides with R-P structure (Sr3Sn2O7 single crystal[112], (Sr,Ba)3Sn2O7 ceramics[84], (Sr,Ca)3Sn2O7 ceramics[85], (Sr,Ba)3Zr2O7 ceramics[86], and Sr3(Sn,Zr)2O7 ceramics[113])

图9 (a)根据空间群对称性分析得到Sr3Sn2O7随温度变化的四个相结构[118]; (b)研究建立的Sr3Sn2O7的相图[118]; (c)根据300 K条件下的NPD精修结果计算的晶体结构分层极化(左图), [010]面的晶体结构示意图(右图), 其中Sr、Zr和O原子分别为灰色、蓝色和红色[119]; (d) Sr3Hf2O7中原子和分层极化对宏观极化的贡献, Sr1−O表示钙钛矿层之间的SrO层, Sr2−O表示岩盐层和钙钛矿层之间的SrO层[120]

Fig. 9 (a) Crystal structures of four phases observed experimentally for Sr3Sn2O7, specified by space group symmetry and Glazer tilt notation[118]; (b) Phase diagram of Sr3Sn2O7 established in the present study[118]; (c) Calculated layer-resolved polarization using a point-charge approximation for the crystal structure refined against NPD data at 300 K (left panel), [010] projected crystal structure (right panel) with Sr, Zr, and O atoms in gray, blue, and red, respectively[119]; (d) Atomic contributions and layer-by-layer contributions to polarization in Sr3Hf2O7, in which Sr1-O represents the SrO layer between perovskite layers, and Sr2-O represents the SrO layer between rock-salt and perovskite layers[120]

图10 双层R-P结构的铁电体的TC与τ的关系[40]

Fig. 10 TC of double-layered R-P ferroelectrics against τ of their perovskite unit[40]

图11 Li2Sr(Nb1−xTax)2O7氧化物的介电常数与温度的依赖关系以及铁电相变模型[65]

Fig. 11 Dependence of dielectric constant on temperature and ferroelectric phase transition schematic of Li2Sr(Nb1−xTax)2O7 oxides[65]

图12 (a) La2SrSc2O7陶瓷的晶体结构示意图, 室温下的P−E电滞回线和不同A位离子有序度下的DFT计算能量对比[123]; (b) La2Sr(Sc1−xFex)2O7陶瓷在400 kV/cm电场和2 Hz频率下的P−E曲线[121]; (c) La2Sr(Sc1−xFex)2O7陶瓷在150~600 K温度范围内的介电常数的温度依赖性[121]; (d) La2Sr(Sc1−xFex)2O7(x=0.15)陶瓷直流磁化率的温度依赖性, 插图是Curie−Weiss拟合结果[121]; (e) La2Sr(Sc1−xFex)2O7(x=0.15)在不同温度下磁化的等温磁场依赖性[121]

Fig. 12 (a) Crystal structures, room temperature P-E loops and the A-site cation ordering dependence of DFT calculated energy for La2SrSc2O7 ceramics[123]; (b) P-E loops for La2Sr(Sc1−xFex)2O7 ceramics under a electric field of 400 kV/cm and a frequency of 2 Hz[121] ; (c) Temperature dependence of dielectric constant for La2Sr(Sc1−xFex)2O7 ceramics over the temperature range of 150-600 K during heating and cooling processes[121]; (d) Temperature dependence of DC magnetic susceptibility of La2Sr(Sc1−xFex)2O7 (x=0.15) ceramics, with inset showing Curie-Weiss fitting results[121]; (e) Isothermal field dependence of magnetization of La2Sr(Sc1−xFex)2O7 (x=0.15) ceramics at various temperatures[121]

图13 双层R-P材料(Ca3Ti2O7陶瓷[80]、Sr3Sn2O7陶瓷[84]、Sr3Zr2O7陶瓷[86]、Li2CaTa2O7陶瓷[26]、Li2SrNb2O7陶瓷[130])铁电性能的对比

Fig. 13 Comparison of ferroelectric properties of double-layered R-P materials (Ca3Ti2O7 ceramics[80], Sr3Sn2O7 ceramics[84], Sr3Zr2O7 ceramics[86], Li2CaTa2O7 ceramics[26], and Li2SrNb2O7 ceramics[130]) (a) Tolerance factor; (b) Curie temperature; (c) Remnant polarization; (d) Coercive field

图14 (a) (1−x)(CaySr1−y)1.15Tb1.85Fe2O7-xCa3Ti2O7(0≤x≤0.3, y=0.60)的相图; (b)铁电极化与饱和磁化强度随成分的变化; (c)当温度为60和100 K时, 线性磁电耦合系数随成分的变化[136]

Fig. 14 (a) Phase diagram of (1−x)(CaySr1−y)1.15Tb1.85Fe2O7-xCa3Ti2O7 (0≤x≤0.3, y=0.60); (b) Ferroelectric polarization and saturated magnetic moment versus composition; (c) Linear magnetoelectric susceptibility versus composition at 60 and 100 K[136]

图15 (a)单层R-P结构氧化物的晶体结构[143]; (b) HRTiO4和NaRTiO4的插层结构示意图[139]; (c) AASmTiO4和(d) AAEuTiO4的SHG信号随温度升高的变化曲线, 其中AA为Na(黄色圆圈)和K(紫色圆圈)[141]

Fig. 15 (a) Crystal structure of several oxides with single layer R-P structure[143]; (b) Schematic diagram of the intercalation structure of HRTiO4 and NaRTiO4[139]; (c, d) Temperature dependence of SHG for (c) AASmTiO4 and (d) AAEuTiO4 with AA representing Na (yellow circles) and K (purple circles)[141]

图16 (a) 390 kV/cm条件下采用PUND法测得的Li2La2Ti3O10陶瓷的P−E电滞回线和J−E电流密度曲线[149]; (b)基于DFT计算的三层R-P结构Li2La2Ti3O10的不同对称性相对于0 K时能量最低Pc相的能量[149]; (c) PUND法测得的Li2Nd2Ti3O10陶瓷的室温P−E电滞回线[150]; (d) Li2La2Ti3O10(LLTO)和Li2Nd2Ti3O10(LNTO)陶瓷的氧八面体畸变角度θT和θR[150]; (e)基于Rietveld精修的Li2La2Ti3O10陶瓷晶体结构示意图(绿色、棕色和红色球分别代表Li+、La3+和O2−离子, 而Ti4+离子位于氧八面体的中心)[149]; (f)通过玻恩有效电荷方法计算的Li2La2Ti3O10中每一层对应的极化贡献[149]

Fig. 16 (a) Room temperature P−E loop and J−E curves measured at 390 kV/cm by PUND method[149]; (b) Calculated energies for Li2La2Ti3O10 with different crystal symmetries in the triple-layered R-P structure relative to the lowest energy Pc phase at 0 K[149]; (c) Room temperature P−E loops of Li2Nd2Ti3O10 ceramics measured through PUND method[150]; (d) Rotation (θR) and tilt (θT) angles of Li2La2Ti3O10 (LLTO) and Li2Nd2Ti3O10 (LNTO) ceramics, respectively[150]; (e) Schematic diagrams of crystal structures for Li2La2Ti3O10 ceramics based on the Rietveld refinement (the green, brown, and red balls represent Li+, La3+, and O2− ions, respectively, while Ti4+ cations reside in the oxygen octahedra center)[149]; (f) Layer-by-layer contributions to polarization in Li2La2Ti3O10 calculated by the Born effective charge mode[149]

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Ruddlesden-Popper结构杂化非常规铁电体的研究进展

Recent Progress of Hybrid Improper Ferroelectrics with Ruddlesden-Popper Structure

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