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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.

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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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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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