Two-dimensional magnetic transition metal halides: molecular beam epitaxy growth and physical property modulation

Li Pei-Gen; Zhang Ji-Hai; Tao Ye; Zhong Ding-Yong

doi:10.7498/aps.71.20220727

Abstract

The spontaneous magnetization of two-dimensional (2D) magnetic materials can be maintained down to the monolayer limit, providing an ideal platform for understanding and manipulating magnetic-related properties on a 2D scale, and making it important for potential applications in optoelectronics and spintronics. Transition metal halides (TMHs) are suitable 2D magnetic candidates due to partially filled d orbitals and weak interlayer van der Waals interactions. As a sophisticated thin film growth technique, molecular beam epitaxy (MBE) can precisely tune the growth of 2D magnetic materials reaching the monolayer limit. Moreover, combining with the advanced experimental techniques such as scanning tunneling microscopy, the physical properties of 2D magnetic materials can be characterized and manipulated on an atomic scale. Herein, we introduce the crystalline and magnetic structures of 2D magnetic TMHs, and show the 2D magnetic TMHs grown by MBE and their electronic and magnetic characterizations. Then, the MBE-based methods for tuning the physical property of 2D magnetic TMHs, including tuning interlayer stacking, defect engineering, and constructing heterostructures, are discussed. Finally, the future development opportunities and challenges in the field of the research of 2D magnetic TMHs are summarized and prospected.

Keywords:

Authors and contacts

1.
School of Physics, Sun Yat-sen University, Guangzhou 510275, China
2.
State Key Laboratory for Optoelectronic Materials and Technologies, Sun Yat-sen University, Guangzhou 510275, China

Corresponding author: Zhong Ding-Yong, dyzhong@mail.sysu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 11974431, 92165204, 11832019) and the Guangdong Major Project of Basic and Applied Basic Research, China (Grant No. 2021B0301030002).

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图 1 分子束外延设备示意图

Figure 1. Schematic of molecular beam epitaxy.

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图 2 (a) 单层MX₂俯视图, 过渡金属M²⁺离子与6个X^–离子配位形成三角晶格 (绿色三角形) 排列的边共享八面体 (灰色); (b) 单层MX₃俯视图, 过渡金属M³⁺离子与6个X^–离子配位形成六角蜂窝晶格 (绿色六边形) 排列的边共享八面体 (灰色)

Figure 2. (a) Monolayer MX₂ top view, transition metal M²⁺ ions are coordinated to six X^– ions forming edge-sharing octahedra (grey) arranged in triangular lattice (green triangle); (b) monolayer MX₃ top view, transition metal M³⁺ ions are coordinated to six X^– ions forming edge-sharing octahedra (grey) arranged in hexagonal honeycomb (green hexagon) lattice.

DownLoad: Full-Size Img PowerPoint

图 3 (a) 单层CrI₃生长在Au(111) 表面; (b) 单层CrI₃生长在HOPG表面; (c), (d) 单层CrI₃原子分辨STM图; (e), (f) 单层CrI₃在偏压为1 V时的STM图和模拟图; (g), (h) 单层CrI₃在偏压为–1 V时的STM图和模拟图^[79]

Figure 3. (a) Monolayer CrI₃ grown on Au(111) surface; (b) monolayer CrI₃ grown on HOPG surface; (c), (d) atomic-resolved STM image of monolayer CrI₃; (e), (f) experimental and simulated STM images at V_s = 1 V; (g), (h) experimental and simulated STM images at V_s = –1 V^[79].

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图 4 (a) 单层和双层CrBr₃生长在HOPG表面上; (b) 单层CrBr₃的原子分辨STM图; (c) 单层CrBr₃的dI/dV谱; (d) 单层CrBr₃的自旋极化隧穿谱; (e) 在偏压1.4 V处, 单层CrBr₃在不同磁场下的dI/dV信号^[20]

Figure 4. (a) Growth of monolayer and bilayer CrBr₃ on HOPG surfaces; (b) atomic-resolved STM image of monolayer CrBr₃; (c) dI/dV spectra of monolayer CrBr₃; (d) spin-polarized tunneling spectra of monolayer CrBr₃; (e) dI/dV signals of monolayer CrBr₃ under different magnetic fields at V_s = 1.4 V^[20].

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图 5 (a) 单层CrCl₃生长在双层石墨烯的SiC表面上; (b) 不同温度下的单层CrCl₃随外磁场变化的XMCD信号; (c) 掠入射和垂直入射的XMCD信号; (d), (e) 不同温度下, 在零磁场下的XMCD值^[22]

Figure 5. Monolayer CrCl₃ grown on bilayer graphene/SiC surface; (b) XMCD signals of monolayer CrCl₃ with external magnetic field at different temperatures; (c) XMCD signals for grazing and normal incidence; (d), (e) XMCD values at zero magnetic field as a function of temperature^[22].

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图 6 (a) α-RuCl₃和β-RuCl₃在HOPG表面大范围STM图; (b) α-RuCl₃的高分辨STM图; (c) 单层α-RuCl₃的扫描隧道谱; (d) DFT计算得到的各分态密度; (e), (f) 不同偏压下的恒流模式STM图^[69]

Figure 6. (a) Large scale STM image of monolayer α-RuCl₃ and β-RuCl₃ grown on HOPG surface; (b) high-resolution STM image of monolayer α-RuCl₃; (c), (d) dI/dV spectra and DFT results of monolayer α-RuCl₃; (e), (f) bias-dependent STM images in the constant-current mode ^[69].

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图 7 (a) 具有Jahn-Teller效应的单层CrI₂的俯视图和侧视图^[35]; (b) 单层CrI₂在SiC的双层石墨表面^[35]; (c) 单层CrI₂在Au(111) 表面^[79]

Figure 7. (a) Monolayer CrI₂ crystal structure with Jahn-Teller effect in top and side views^[35]; (b) monolayer CrI₂ on bilayer graphene/SiC surface^[35]; (c) monolayer CrI₂ on Au(111) surface^[79].

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图 8 (a) 单层FeCl₂生长在Au(111) 表面上^[101]; (b) 单层FeCl₂生长在HOPG表面上^[101]; (c) 单层FeCl₂在HOPG表面的各种moiré云纹结构^[101]; (d) 单层和双层FeCl₂在HOPG表面的I-V曲线^[102]; (e) moiré转角与FeCl₂岛高的关系图^[102]

Figure 8. (a) Monolayer FeCl₂ growth on Au(111) surface^[101]; (b) monolayer FeCl₂ growth on HOPG surface^[101]; (c) various moiré structure of monolayer FeCl₂ on HOPG surface^[101]; (d) I-V curves of monolayer and bilayer FeCl₂ on HOPG surface^[102]; (e) correlation between moiré rotation angle and FeCl₂ island height^[102].

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图 9 (a) NiBr₂和NiBr_x薄膜生长在Au(111) 表面; (b), (c) 单层NiBr₂和NiBr_x的原子分辨STM图; (d) 单层NiBr_x和NiBr₂薄膜上的掠入射和垂直入射的MXCD信号^[40]

Figure 9. NiBr₂ and NiBr_x films grown on Au(111) surface; (b), (c) atomic-resolved STM images of single-layer NiBr₂ and NiBr_x; (d) XMCD signals on single-layer NiBr_x and NiBr₂ for grazing and normal incidence^[40].

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图 10 (a) 单层MnI₂生长在双层石墨烯/SiC表面; (b) 单层MnI₂的原子分辨STM图; (c) 单层MnI₂的dI/dV谱^[93]

Figure 10. (a) Monolayer MnI₂ growth on bilayer graphene/SiC surface; (b) atomic-resolved STM image of monolayer MnI₂; (c) dI/dV spectra of monolayer MnI₂^[93].

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图 11 (a) H型堆垛方式的双层CrBr₃形貌图; (b) R型堆垛方式的双层CrBr₃形貌图; (c), (d) H型堆垛 (c) 和R型堆垛 (d) 的双层CrBr₃在偏压为1.5 V时微分电导信号随外磁场变化关系, 针尖选用Cr针尖 ^[20]

Figure 11. (a) H-type stacked bilayer CrBr₃; (b) R-type stacked bilayer CrBr₃; (c), (d) differential conductance signals as a function of external magnetic field for H-type stacked (c) and R-type stacked (d) bilayer CrBr₃ with a Cr tip at V_s = 1.5 V^[20].

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图 12 (a) 原始 (左) 和单个碘空位 (右) 的单层CrI₃磁交换作用^[119]; (b) CrI₃里不同的本征缺陷对局域磁性耦合影响的理论计算结果^[120]; (c) 单层CrI₃中不同点缺陷附近Cr—Cr键长与磁耦合的关系^[120]; (d) 单层FeCl₂中的本征缺陷^[101]; (e) 单层CrI₃中的本征缺陷STM图和模拟图^[130]

Figure 12. (a) Magnetic exchange interaction of pristine (left) and single iodine vacancy (right) of monolayer CrI₃^[119]; (b) theoretical calculations of the effect of local magnetic coupling by different intrinsic defects in CrI₃^[120]; (c) relationship between Cr—Cr bond length and magnetic coupling near different point defects in monolayer CrI₃^[120]; (d) intrinsic defects in monolayer FeCl₂^[101]; (e) experimental and simulated STM images of intrinsic defects in monolayer CrI₃^[130].

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图 13 (a) Majorana零能模出现在CrBr₃/NbSe₂异质结中CrBr₃岛的边缘^[146]; (b) moiré增强的拓扑超导^[147]; (c) 磁涡旋结构在CrBr₃/NbSe₂异质结中^[148]

Figure 13. (a) Majorana zero mode appears at the edge of the CrBr₃ island on the CrBr₃/NbSe₂ system^[146]; (b) moiré-enabled topological superconductivity^[147]; (c) the magnetic vortex in CrBr₃/NbSe₂ heterostructure^[148].

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表 1 二维磁性过渡金属卤化物

Table 1. Two-dimensional magnetic transition metal halides.

材料	面内晶格常数/Å	磁耦合	转变温度	磁易轴	单层电学性质	参考文献
VCl₂	3.58	120°-AFM/bulk	T_N = 36 K/bulk	//	Insulator	[36–38, 46]
VCl₂	3.58	120°-AFM/1L		//	Insulator	[36–38, 46]
VBr₂	3.76	120°-AFM/bulk	T_N = 30 K/bulk	//	Insulator	[36–38, 46]
VBr₂	3.76	120°-AFM/1L		//	Insulator	[36–38, 46]
VI₂	4.04	AFM /bulk	T_N = 16 K/bulk	//	Insulator	[36–38, 46]
VI₂	4.04	120°-AFM/1L		//	Insulator	[36–38, 46]
CrCl₂	3.55	AFM/1L		⊥		[36, 38]
CrBr₂	3.74	AFM/1L		⊥		[36, 38]
CrI${}_2^* $	a₁ = 3.88, a₂ = 4.23, a₃ = 4.18	FM/1L		⊥	Mott insulator	[35]
MnCl₂	3.64	AFM/bulk	T_N = 2 K/bulk	//	Insulator	[36, 38, 47]
MnCl₂	3.64	120°-AFM/1L		//	Insulator	[36, 38, 47]
MnBr₂	3.80	AFM/bulk	T_N = 2 K/bulk	//	Insulator	[36, 38, 48]
MnBr₂	3.80	120°-AFM/1L		//	Insulator	[36, 38, 48]
MnI${}_2^* $	4.06	HM/bulk	T_N = 3.4 K/bulk	//	Insulator	[36, 38, 49]
MnI${}_2^* $	4.06	120°-AFM/1L		//	Insulator	[36, 38, 49]
FeCl${}_2^* $	3.43	AFM/bulk	T_N = 24 K/bulk	⊥	HM	[37, 38, 50]
FeCl${}_2^* $	3.43	FM/1L	T_C = 109 K/1L	⊥	HM	[37, 38, 50]
FeBr₂	3.63	AFM/bulk	T_N = 14 K/bulk	⊥	HM	[37, 38, 50]
FeBr₂	3.63	FM/1L	T_C = 81 K/1L	⊥	HM	[37, 38, 50]
FeI₂	3.91	AFM/bulk	T_N = 9 K/bulk	⊥	HM	[37, 38, 51]
FeI₂	3.91	FM/1L	T_C = 42 K/1L	⊥	HM	[37, 38, 51]
CoCl₂	3.42	AFM/bulk	T_N = 25 K/bulk	//	Insulator	[37, 38, 52]
CoCl₂	3.42	FM/1L	T_C = 85 K/1L	//	Insulator	[37, 38, 52]
CoBr₂	3.62	AFM/bulk	T_N = 18 K/bulk	//	Insulator	[37, 38, 50]
CoBr₂	3.62	FM/1L	T_C = 23 K/1L	//	Insulator	[37, 38, 50]
CoI₂	3.80	HM/bulk	T_N = 11 K/bulk		Insulator	[42, 53]
CoI₂	3.80	HM			Insulator	[42, 53]
NiCl₂	3.50	AFM/bulk	T_N = 52 K/bulk	//	Insulator	[38, 39, 54]
NiCl₂	3.50	FM/1L	T_C = 118 K/1L	//	Insulator	[38, 39, 54]
NiBr${}_2^* $	3.80	HM/bulk	T_N = 23 K/bulk	//	Ferroelectric insulator	[40, 55]
NiBr${}_2^* $	3.80	Noncollinear/1L	T_C = 28 K/1L	//	Ferroelectric insulator	[40, 55]
NiI₂	3.88	HM/bulk	T_N = 60 K/bulk		Ferroelectric semiconductor	[41]
NiI₂	3.88	HM/1L	T_N = 21 K/1L		Ferroelectric semiconductor	[41]
VCl₃	6.28	AFM/bulk	T_N = 20 K/bulk	⊥	DHM	[56, 57]
VCl₃	6.28	FM/1L	T_C = 80 K/1L	⊥	DHM	[56, 57]
VBr₃	6.37	AFM/bulk	T_N = 27 K/bulk	//	Semiconductor	[58, 59]
VBr₃	6.37	FM/1L	T_C = 20 K/1L	//	Semiconductor	[58, 59]
VI₃	6.83	FM/ interlayer	Tc = 50 K/bulk	⊥	Mott insulator	[30, 60]
VI₃	6.83	FM/ intralayer	T_C = 60 K/1L	⊥	Mott insulator	[30, 60]
CrCl${}_3^* $	6.01	AFM/ interlayer	T_N = 17 K/bulk	//	Semiconductor	[22, 61]
CrCl${}_3^* $	6.01	FM/ intralayer	T_C = 13 K/1L	//	Semiconductor	[22, 61]
CrBr${}_3^* $	6.30	FM/ interlayer	Tc = 37 K/bulk	⊥	Semiconductor	[20, 62]
CrBr${}_3^* $	6.30	FM/ intralayer	T_C = 34 K/1L	⊥	Semiconductor	[20, 62]
CrI${}_3^* $	6.95	FM/ intralayer	Tc = 61 K/bulk	⊥	Semiconductor	[16, 63]
CrI${}_3^* $	6.95	AFM/ few L	T_C = 45 K/1L	⊥	Semiconductor	[16, 63]
MnCl₃	6.21	FM/1L		//	DHM	[64]
MnBr₃	6.58	FM/1L		//	DHM	[64]
MnI₃	7.08	FM/1L		//	DHM	[64]
FeCl₃	6.22	HM/bulk	T_N = 15 K/bulk	⊥	Semiconductor	[65, 66]
FeCl₃	6.22	FM/1L		⊥	Semiconductor	[65, 66]
FeBr₃	6.61	AFM/bulk	T_N = 16 K/bulk	⊥	Semiconductor	[65, 67]
FeBr₃	6.61	FM		⊥	Semiconductor	[65, 67]
FeI₃	7.12	FM/1L		⊥	Semiconductor	[65]
NiCl₃	5.94	FM/1L	T_C = 497 K/1L	⊥	DHM	[68]
NiBr₃	6.31	FM/1L	T_C = 595 K/1L	//	DHM	[68]
NiI₃	6.82	FM/1L	T_C = 682 K/1L	⊥	DHM	[68]
α-RuCl${}_3^* $	6.19	AFM QSL/bulk	T_N = 7 K/bulk		Mott insulator	[44, 45, 69]
α-RuCl${}_3^* $	6.19	AFM QSL/1L			Mott insulator	[44, 45, 69]
RuBr₃	6.25	FM/1L		⊥	TI	[70]
RuI₃	7.10	FM/1 L	T_C = 360 K/1L	⊥	TI	[70]
注: FM, AFM, HM, QSL分别表示铁磁态、反铁磁态、螺旋磁态、量子自旋液体态. 在表格中, 灰色填充表示理论计算预测的二维磁性过渡金属卤化物; 黄色填充表示已合成的二维磁性过渡金属卤化物, 但是还缺乏磁性表征; 绿色填充表示已证实的二维磁性过渡金属卤化物. *表示已实现MBE制备的过渡金属卤化物. //和⊥分别表示平面内、平面外磁易轴. HM, DHM和TI分别表示磁性半金属、狄拉克半金属和拓扑绝缘体.

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