二维磁性材料及多场调控研究进展

肖寒; 弭孟娟; 王以林

doi:10.7498/aps.70.20202204

摘要

二维磁性材料是二维材料家族的新成员, 其在单原胞层厚度依然保持长程磁序且易受外场调控, 这为二维极限下的磁性以及其他新奇物理效应的研究提供了理想的平台, 又为低功耗自旋电子学/磁存储器件的研制开辟了新的途径, 成为国际上备受关注的前沿热点. 本综述首先系统介绍了近年来发现的各类本征二维磁性材料的晶体结构、磁结构以及磁性能, 并讨论了由磁场、电场、静电掺杂、离子插层、堆叠方式、应变、界面等外场调控二维磁性材料磁性能的研究进展, 最后进行总结并展望了二维磁性材料未来发展的研究方向. 深入理解二维磁性材料磁性的起源和机理、研究其磁性能与微观结构之间的关联, 为寻找具有更高居里温度(奈尔温度)的磁性材料、设计多功能的新概念器件具有重要意义.

关键词:

Abstract

The recently discovered two-dimensional magnetic materials have attracted tremendous attention and become a cutting-edge research topic due to their long-range magnetic ordering at a single-unit-cell thickness, which not only provide an ideal platform for studying the magnetism in the two-dimensional limit and other novel physical effects, but also open up a new way to develop low-power spintronics/magnetic storage devices. In this review, first, we introduce the crystal structures, magnetic structures and magnetic properties of various recently discovered intrinsic two-dimensional magnetic materials. Second, we discuss the research progress of controlling the magnetic properties of two-dimensional magnetic materials by magnetic field, electric field, electrostatic doping, ion intercalation, stacking, strain, interface, etc. Finally, we give a perspective of possible research directions of the two-dimensional magnetic materials. We believe that an in-depth understanding of the origin and mechanism of magnetism of the two-dimensional magnetic materials as well as the study of the relationship between magnetic properties and microstructures are of great significance in exploring a magnetic material with a substantially high Curie temperature (Néel temperature), and designing multifunctional new concept devices.

Keywords:

作者及机构信息

山东大学微电子学院, 济南　250100

通信作者: 王以林, yilinwang@email.sdu.edu.cn

基金项目: 国家自然科学基金重大研究计划(批准号: 92065206)和山东省自然科学基金(批准号: ZR2020MA071)资助的课题

Authors and contacts

School of Microelectronics, Shandong University, Jinan 250100, China

Corresponding author: Wang Yi-Lin, yilinwang@email.sdu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 92065206) and the Natural Science Foundation of Shandong Province, China (Grant No. ZR2020MA071)

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施引文献

图 1 不同FM和AFM自旋磁矩的示意图, 以磁性过渡金属离子为代表进行描述(自旋向上的磁矩为浅灰色, 自旋向下的磁矩为深灰色)　(a) FM耦合; (b)层间A-type AFM耦合^[35]; (c)层内AF-zigzag耦合^[35]; (d)层内AF-stripy耦合^[35]; (e)层内AF-Néel耦合^[35]

Fig. 1. Various types of FM and AFM order in layered magnetic materials, represented by magnetic transition metal ions (light grey and dark grey represent spin up and spin down, respectively). From left to right: (a) FM order; (b) interlayer A-type AFM order^[35]; (c) intralayer AF-zigzag order^[35]; (d) intralayer AF-stripy order^[35]; (e) intralayer AF-Néel order^[35].

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图 2 (a) 单层CrX₃的俯视图(左), Cr³⁺ (紫色)和X^－(金色)组成的八面体笼(右)^[43]; (b) 在低温菱方相的坐标系中CrX₃的磁结构. 目前研究只报道CrCl₃的磁矩在ab平面上, 在这里沿[110]和[$\bar {1}\bar {1}0$]方向画出; 在CrBr₃和CrI₃中, 磁矩沿c轴^[44]

Fig. 2. (a) Top view of a CrX₃ monolayer along with an illustration of the coordination (left), and Cr³⁺ (purple) and X^– (gold) in an octahedral cage (right)^[43]; (b) magnetic structures of CrX₃ in the coordinate system of the low temperature rhombohedral structure. The moments in CrCl₃ are drawn along the [110] and [$\bar {1}\bar {1}0$] directions here, but are only known to be in the ab plane. Moments in ferromagnetic CrBr₃ and CrI₃ are along the c axis^[44].

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图 3 NiI₂单斜晶体结构的俯视图(a)、侧视图(b)和晶胞结构(c)^[29]

Fig. 3. Top view (a), side view(b) and unit cell structure (c) of NiI₂ monoclinic structure^[29].

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图 4 (a) CrTe晶体结构的俯视图(左)和侧视图(右)^[19]; (b) Cr₂Te₃晶体结构的俯视图(左)和侧视图(右)^[57]

Fig. 4. (a) Top view (left) and side view (right) of CrTe crystal structure^[19]; (b) top view (left) and side view (right) of Cr₂Te₃ crystal structure^[57].

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图 5 1T-VSe₂晶体结构的俯视图(左)和侧视图(右) (a = b = 3.35 Å, c = 6.1 Å)^[60]

Fig. 5. Top view (left) and side view (right) of the atomic structure of layered 1T-VSe₂ crystal (a = b = 3.35 Å, c = 6.1 Å)^[60].

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图 6 (a) FePS₃晶体结构的俯视图和侧视图^[30]; (b) FePS₃的原胞结构; (c)—(e)分别为FePS₃, MnPS₃以及NiPS₃的磁结构示意图^[65]

Fig. 6. (a) Top and side views of atomic structure of FePS₃ crystal^[30]; (b) unit-cell structure of FePS₃; (c)−(e) magnetic structures of FePS₃, MnPS₃ and NiPS₃, respectively^[65].

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图 7 (a) CrPS₄的晶体结构和磁结构, 黑色和红色的箭头指向磁矩的方向; (b) CrPS₄单层的ab平面图^[76]

Fig. 7. (a) Crystal structure and magnetic structure of CrPS₄, the black and red arrows point to the directions of magnetic moments; (b) ab plane of CrPS₄ monolayer^[76].

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图 8 Cr₂Ge(Si)₂Te₆晶体结构的俯视图(左)和侧视图(右), 单位原胞用黑线表示^[80]

Fig. 8. Schematic illustration of the crystalline structure of Cr₂Ge(Si)₂Te₆ from the top view (left) and the side view (right), a unit cell is indicated by a black line^[80].

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图 9 (a) 单层Fe₃GeTe₂的晶体结构示意图, 左边为俯视图(沿着[001]), 右边为侧视图(沿着[010])^[38]; (b) Fe_2.76Ge_0.94Te₂的磁结构^[83]

Fig. 9. (a) Atomic structure of monolayer Fe₃GeTe₂. The left panel shows the view along [001], and the right panel shows the view along [010]^[38]. (b) The magnetic structure of Fe_2.76Ge_0.94Te₂^[83].

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图 10 (a) Bi₂Te₃的五原子单元层; (b) MnBi₂Te₄的七原子单元层; (c) MnBi₂Te₄的晶体结构和磁结构; (d) MnBi₄Te₇的晶体结构和磁结构^[89]

Fig. 10. (a) Quintuple layer of Bi₂Te₃; (b) septuple layer of MnBi₂Te₄; (c) crystal structure and magnetic structure of MnBi₂Te₄; (d) crystal structure and magnetic structure of MnBi₄Te₇^[89].

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图 11 (a) 过渡金属卤化物的俯视图; (b) 4个氧和2个卤化物离子配位过渡金属离子形成强扭曲八面体结构图(顶部)和过渡金属卤化物的侧视图(底部)^[91]

Fig. 11. (a) Top view of transition-metal oxyhalides; (b) a strongly distorted octahedron formed by one metal ion coordinated by 4 oxygen and 2 halide ions (top), the side view of transition-metal oxyhalides (bottom)^[91].

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图 12 (a)双层反铁磁CrI₃中MCD信号随磁场的变化^[16]; (b) 在H // (0001) 和H⊥(0001) 方向MnBi₂Te₄依赖磁场的磁化曲线(H_SF为自旋-翻转磁场)^[84]; (c) 双层反铁磁CrI₃的线性磁电效应^[40]: 在一个固定的磁场下磁化的样品的磁化强度的相对和绝对变化(分别为ΔM/M₀和ΔM)随施加电场的变化; (d) H // c方向、不同温度下MnBi₄Te₇等温磁化的磁滞回线, H_f, 一级自旋翻转场^[107]

Fig. 12. (a) MCD signal in AFM bilayer CrI₃ as a function of magnetic field^[16]; (b) field-dependent magnetization curves of MnBi₂Te₄ for H // (0001) and H⊥(0001), where H_SF is spin-flop magnetic field^[84]; (c) linear magnetoelectric effect in AFM bilayer CrI₃^[40]: relative and absolute changes in the sheet magnetization (ΔM/M₀ and ΔM, respectively) as a function of applied electric field measured under a fixed magnetic field; (d) full magnetic hysteresis loop of isothermal magnetization of MnBi₄Te₇ taken at various temperatures for H // c, H_f, first-order spin-flip transition field^[107].

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图 13 (a) 双栅控双层CrI₃器件结构示意图^[39]; (b), (c) 静电掺杂控制单层(b)和双层(c) CrI₃的磁性^[105], 其中(b)是以零栅压下相应值归一化的矫顽场(洋红色)、饱和场(紫色)、居里温度(橙色)与栅压(底轴)及掺杂浓度(顶轴)的关系, 正(负)值分别代表电子(空穴)浓度, (c) 4 K下掺杂浓度-磁场决定的双层CrI₃相图

Fig. 13. (a) Schematic of a dual-gated bilayer CrI₃ device^[39]. (b), (c) Controlling magnetism in monolayer (b) and bilayer CrI₃ (c) by electrostatic doping^[105]: (b) Coercive force (magenta), saturation magnetization (purple) (both at 4 K) and Curie temperature (orange) normalized by their values at zero gate voltage as a function of gate voltage (bottom axis) and induced doping density (top axis) with positive (negative) value for electron (hole) density; (c) doping density-magnetic field phase diagram of bilayer CrI₃ at 4 K.

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图 14 离子插层实验结果　(a), (b) Cr₂Ge₂Te₆有机阳离子插层的实验结果^[112], 其中(a) Cr₂Ge₂Te₆和 (TBA) Cr₂Ge₂Te₆晶体结构示意图; (b) 纯Cr₂Ge₂Te₆和 (TBA) Cr₂Ge₂Te₆在H // ab方向磁化强度随温度(左)及(TBA) Cr₂Ge₂Te₆在H // ab方向磁化强度随磁场(右)的变化; (c), (d) Fe₃GeTe₂锂离子插层的实验结果^[38], 其中(c) Fe₃GeTe₂器件结构示意图, 电解质(LiClO₄溶解在聚氧乙烯中)覆盖Fe₃GeTe₂薄片和侧栅; (d) 3层Fe₃GeTe₂的居里温度随栅极电压的变化

Fig. 14. Experimental results of ion intercalation. (a), (b) Results of the organic cation intercalation for Cr₂Ge₂Te₆^[112]: (a) Schematic diagrams of crystal structures of Cr₂Ge₂Te₆ and (TBA) Cr₂Ge₂Te₆; (b) temperature-dependent magnetization (M-T) of pristine Cr₂Ge₂Te₆ and (TBA) Cr₂Ge₂Te₆ for H//ab (left) and magnetic field-dependent magnetization (M-H) of (TBA) Cr₂Ge₂Te₆ for H//ab (right). (c), (d) Results of the Li⁺ intercalation for Fe₃GeTe₂^[38]: (c) Schematic of the Fe₃GeTe₂ device structure, the electrolyte (LiClO₄ dissolved in polyethylene oxide) covers both Fe₃GeTe₂ flake and side gate; (d) Curie temperature of the tri-layer Fe₃GeTe₂ as a function of the gate voltage.

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图 15 CrI₃压力调控的实验结果^[52]　(a) CrI₃的菱方相和单斜相的俯视图(左)和侧视图(右), 其中绿(紫)色原子分别代表顶层(底层)的Cr原子, 棕色原子代表I原子; (b)高压实验装置示意图; (c)在不同静水压力下, 隧穿电流I_t随磁场的变化关系

Fig. 15. Experimental results of CrI₃ under hydrostatic pressure^[52]: (a) Schematic of rhombohedral stacking and monoclinic stacking with top (left) and side (right) view, the green (purple) atoms represent the Cr atoms in the top (bottom) layer while the brown ones represent the I atoms; (b) schematic of high-pressure experimental set-up; (c) tunneling current, I_t, versus magnetic field, H, at different pressures.

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图 16 CrBr₃自旋极化STM的实验结果^[115], 其中(a), (b)分别为H型堆叠(a)和R型堆叠(b)的单层(1L)和双层(2L)区域的STM图以及高分辨的原子图像; (c) SP-STM测量示意图; (d), (e) 利用Cr针尖测得的H型堆叠(d)和R型堆叠(e)双层CrBr₃的自旋-极化隧穿与磁场的关系, 黑色(红色)曲线对应面外磁场正向(反向)扫描的结果

Fig. 16. Experimental results of spin-polarized STM for CrBr₃^[115]. (a), (b) STM images of H-type stacked (a) and R-type stacked (b) CrBr₃ films with both a monolayer (1L) region and a bilayer (2L) island. Magnified, atomically resolved images of the bilayer island and its extended bottom region of the H-type stacked and R-type stacked CrBr₃ films are resolved. (c) Schematic of SP-STM measurement. (d), (e) Spin-polarized tunneling on the H-type stacked (d) and R-type stacked (e) CrBr₃ bilayer as a function of magnetic field with a Cr tip. The out-of-plane magnetic field was swept upward (black curve) and downward (red curve).

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图 17 Fe₃GeTe₂的应力调控^[120]　(a) 应变实验装置示意图; (b) 1.5 K下矫顽场随应力的变化关系; (c) 剩余反常霍尔电阻$R_{xy}^{\rm r}$(由165 K的值归一化)在不同压力下随温度的变化关系

Fig. 17. Straining regulation of Fe₃GeTe₂^[120]: (a) Schematic diagram of device in the strain experimental set-up; (b) coercive field as a function of strain at 1.5 K; (c) remnant anomalous Hall resistance $R_{xy}^{\rm r}$ normalized by the values at 165 K as a function of temperature with varying strain.

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图 18 (a), (b) FePS₃/Fe₃GeTe₂异质结的实验结果^[121], 其中(a)为FePS₃, Fe₃GeTe₂薄片中的磁序; (b) Fe₃GeTe₂ (红线), FePS₃/Fe₃GeTe₂ (蓝线)的Kerr角度随温度的变化; (c), (d) Bi₂Te₃/Fe₃GeTe₂异质结的实验结果^[122], 其中(c) Bi₂Te₃和Fe₃GeTe₂晶体结构示意图; (d) Bi₂Te₃(8)/Fe₃GeTe₂(4)异质结在不同温度下的反常霍尔电阻, 数字表示样品的厚度; (e), (f) 纯Cr₂Ge₂Te₆ (e)及沉积50 nm NiO后的Cr₂Ge₂Te₆/NiO (f) MOKE信号随温度的变化曲线^[123]

Fig. 18. (a), (b) Experimental results of FePS₃/Fe₃GeTe₂^[121]: (a) Magnetic ordering in vdW Fe₃GeTe₂ and FePS₃ thin flakes; (b) extracted Kerr rotations as a function of the temperature for Fe₃GeTe₂ (red curve) and FePS₃/Fe₃GeTe₂ (blue curve), respectively. (c), (d) Experimental results of Bi₂Te₃/Fe₃GeTe₂^[122]: (c) Schematic structures of Bi₂Te₃ and Fe₃GeTe₂; (d) anomalous Hall resistances of the Bi₂Te₃(8)/Fe₃GeTe₂(4) heterostructure at different temperatures, respectively, the number represents the thickness of the sample. (e), (f) Temperature dependence of MOKE signals of the Cr₂Ge₂Te₆ without (e) and with (f) NiO capping layer^[123].

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表 1 常见的磁性材料及其磁性质

Table 1. A list of typical magnetic materials and their magnetic properties.

材料类别	材料	磁耦合	磁转变温度T_N/T_c	描述模型	带隙/eV	参考文献
过渡金属卤化物	CrCl₃	A-type AFM	1L: 10 K/T_c 2L: 16 K/T_N Bulk: 17 K/T_N	//XY	3.0	[44,46,47]
	CrBr₃	FM	1L: 27 K/T_c 2L: 36 K/T_c Bulk: 37 K/T_c	⊥between Isingand Heisenberg	2.2	[44,45,47]
	CrI₃	A-type AFM/Few L	1L: 45 K/T_c 2L: 45 K/T_N Few L: 46 K/T_N	⊥Ising	1.2	[44,45,47,48]
	CrI₃	FM/Bulk	Bulk: 61 K/T_c	⊥Ising	1.2	[44,45,47,48]
	1T-FeCl₂	A-type AFM/Bulk	Bulk: 24 K/T_N	⊥		[44]
	1T-FeCl₂	FM/1L	1L: 109 K/T_c	⊥Heisenberg	Semimetal	[55]
	1T-FeBr₂	A-type AFM/Bulk	Bulk: 14 K/T_N	⊥		[44]
	1T-FeBr₂	FM/1L	1L: 81 K/T_c	⊥Heisenberg	Semimetal	[55]
	1T-FeI₂	Intralayer AF-stripy/Bulk	Bulk: 9 K/T_N	⊥		[44]
	1T-FeI₂	FM/1L	1L: 42 K/T_c	⊥Heisenberg	Semimetal	[55]
	1T-CoCl₂	AFM/Bulk	Bulk: 25 K/T_N	//		[44]
	1T-CoCl₂	FM/1L	1L: 85 K/T_c	Heisenberg		[55]
	1T-CoBr₂	A-type AFM/Bulk	Bulk: 19 K/T_N	//		[44]
	1T-CoBr₂	FM/1L	1L: 23 K/T_c	Heisenberg		[55]
	1T-CoI₂	AFM	Bulk: 11 K/T_N			[44]
	NiI₂	A-type AFM	2.0 nm: 35 K/T_N Bulk: 75 K/T_N		1.11/1L 1.23/Bulk	[29]
过渡金属硫化物	CrSe^#	FM	Bulk: 280 K/T_c			[21]
	CrTe₂^#	FM	Bulk: 310 K/T_c		0	[97]
	CrTe	FM	11 nm: 140 K/T_c 45 nm: 205 K/T_c	⊥	0	[19]
	Cr₂Te₃	FM	5 nm: 280 K/T_c 40.3 nm: 170 K/T_c	⊥	0	[57]
	FeTe (hexagonal)	FM	4 nm: 170 K/T_c Bulk: 220 K/T_c	Heisenberg		[20]
	${\rm MnSe}_x{}^*$	FM/1L	1L: > 300 K/T_c	⊥	3.39	[61]
	${\rm MnSe}_x{}^*$	AFM/Bulk		⊥	3.39	[61]
	1T-VSe₂^*	FM/1L	1L: > 300 K (470 K)/T_c	//	0	[22,60]
	2H-VSe₂	A-type AFM		//	Semimetal	[98]
	V₅S₈	FM/3.2 nm	3.2 nm: 2 K/T_c	⊥	0	[99]
	V₅S₈	AFM/Bulk	Bulk: 32 K/T_N	⊥	0	[99]
	FeTe (tetragonal)	AFM-Néel	5 nm: 45 K/T_N Bulk: 70 K/T_N	Heisenberg		[20]
	Cr₂S₃	FM	15 nm: 120 K/T_c 45 nm: 300 K/T_c			[59]
	Cr₂O₃^#	AFM	Bulk: 307 K/ T_N	⊥	3.5	[100,101]
过渡金属磷化合物	FePS₃	Intralayer AF-zigzag, interlayer FM	1L: 118 K/T_N Bulk: 118 K/T_N	⊥Ising	1.5	[30,65,72]
	NiPS₃	Intralayer AF-zigzag, interlayer FM	2L: 130 K/T_N Bulk: 150 K/T_N	// XY	1.6	[31,65,67]
	MnPS₃	Intralayer AF-Néel, interlayer FM	Bulk: 78 K/T_N	// Heisenberg	2.4	[65,68,71]
	CoPS₃	Intralayer AF-zigzag, interlayer FM	Bulk: 120 K/T_N	// XY		[66]
	MnPSe₃	Intralayer AF-zigzag, interlayer FM	5L: 70 K/T_N Bulk: 70 K/T_N	// XY	2.3	[32]
	FePSe₃^#	Intralayer AF-zigzag, interlayer FM	Bulk: 119 K/T_N	⊥Ising	1.3	[73,74]
	CrPS₄	A-type AFM	Bulk: 36 K/T_N	⊥	1.3	[75,76,102]
	CrPS₄	FM/1L	1L: 50 K/T_c	⊥	2.28	[77]
过渡金属锗碲化合物	Cr₂Si₂Te₆	FM	1L: 80 K/T_c Bulk: 31 K/T_c	⊥Ising	1.2	[80,81,103]
	Cr₂Ge₂Te₆	FM	2L: 28 K/T_c 3L: 35 K/T_c Bulk: 61 K/T_c	⊥Heisenberg	0.45	[17,80]
	Fe₃GeTe₂	FM	1L (onAl₂O₃): 20 K/T_c 1L (on Au): 130 K/T_c Bulk: 220—230 K/T_c	⊥Ising	0	[38,82]
	Fe₅GeTe₂	FM	12 nm: 270—300 K/T_c Bulk: 310 K/T_c	⊥	0	[26]
过渡金属铋碲化合物	MnBi₂Te₄	A-type AFM	3SL: 18 K/T_N 4SL: 21 K/T_N Bulk: 25 K/T_N	⊥Heisenberg		[84,85]
	MnBi₄Te₇	A-type AFM	Bulk: 13 K/T_N	⊥		[89]
	MnBi₆Te₁₀	A-type AFM	Bulk: 11 K/T_N	⊥		[89]
	VBi₂Te₄	A-type AFM		//		[90,104]
	NiBi₂Te₄	A-type AFM		//		[90]
	EuBi₂Te₄	A-type AFM		//		[90]
过渡金属氧卤化物	FeOCl	AFM	2.0—2.4 nm: 14 K/T_N Bulk: 84—92 K/T_N			[34]
	CrOCl	FM/1L	1L: 160 K/T_c	⊥Ising	2.38	[91]
	CrOCl	AFM	Bulk: 13.5 K/T_N	⊥	2.31	[96]
	CrSBr	FM/1L	1L: 160 K/T_c	// Heisenberg	0.757	[93]
	CrSCl	FM/1L	1L: 150 K/T_c	// Heisenberg	0.856	[93]
	CrSI	FM/1L	1L: 170 K/T_c	// Heisenberg	0.473	[93]
注: 绿色背底表示为实验中发现的铁磁材料, 橙色背底表示为实验中发现的反铁磁材料, 灰色背底表示为理论预测的铁磁或反铁磁材料; 上标^#为体相材料, 其单层磁性在实验中还未发现; 上标为磁性是否为本征磁性尚未确定的磁性材料; ⊥表示易磁化轴垂直于平面(ab), ∥表示易磁化轴平行于平面(ab)*.

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