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二维磁性过渡金属卤化物的分子束外延制备及物性调控

李培根 张济海 陶野 钟定永

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二维磁性过渡金属卤化物的分子束外延制备及物性调控

李培根, 张济海, 陶野, 钟定永

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
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  • 二维磁性材料的自发磁化可以维持到单层极限下, 为在二维尺度理解和调控磁相关性质提供了一个理想的平台, 也使其在光电子学和自旋电子学等领域具有重要的应用前景. 晶体结构为层状堆叠的过渡金属卤化物具有部分填充的d轨道和较弱的范德瓦耳斯层间相互作用等特性, 是合适的二维磁性候选材料. 结合分子束外延 (MBE)技术, 不仅可以精准调控二维磁性材料生长达到单层极限, 而且可以结合扫描隧道显微术等先进实验技术开展原子尺度上的物性表征和调控. 本文详细介绍了多种二维磁性过渡金属卤化物的晶体结构和磁结构, 并展示了近几年来通过MBE技术生长的二维磁性过渡金属卤化物以及相应的电学和磁学性质. 随后, 讨论了基于MBE方法对二维磁性过渡金属卤化物的物性进行调控的方法, 包括调控层间堆垛、缺陷工程以及构筑异质结. 最后, 总结并展望了二维磁性过渡金属卤化物研究领域在未来的发展机会与挑战.
    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.
      通信作者: 钟定永, dyzhong@mail.sysu.edu.cn
    • 基金项目: 国家自然科学基金(批准号: 11974431, 92165204, 11832019)和广东省基础与应用基础研究基金(批准号: 2021B0301030002)资助的课题.
      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

    Fig. 1.  Schematic of molecular beam epitaxy.

    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)

    Fig. 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.

    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]

    Fig. 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 Vs = 1 V; (g), (h) experimental and simulated STM images at Vs = –1 V[79].

    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]

    Fig. 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 Vs = 1.4 V[20].

    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]

    Fig. 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].

    图 6  (a) α-RuCl3β-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]

    Fig. 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].

    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]

    Fig. 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].

    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]

    Fig. 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].

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

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

    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[93]

    Fig. 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].

    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]

    Fig. 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 Vs = 1.5 V[20].

    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]

    Fig. 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].

    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]

    Fig. 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].

    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
    VCl23.58120°-AFM/bulkTN = 36 K/bulk//Insulator[3638, 46]
    120°-AFM/1L
    VBr23.76120°-AFM/bulkTN = 30 K/bulk//Insulator[3638, 46]
    120°-AFM/1L
    VI24.04AFM /bulkTN = 16 K/bulk//Insulator[3638, 46]
    120°-AFM/1L
    CrCl23.55AFM/1L[36, 38]
    CrBr23.74AFM/1L[36, 38]
    CrI${}_2^* $a1 = 3.88, a2 = 4.23,
    a3 = 4.18
    FM/1LMott insulator[35]
    MnCl23.64AFM/bulkTN = 2 K/bulk//Insulator[36, 38, 47]
    120°-AFM/1L
    MnBr23.80AFM/bulkTN = 2 K/bulk//Insulator[36, 38, 48]
    120°-AFM/1L
    MnI${}_2^* $4.06HM/bulkTN = 3.4 K/bulk//Insulator[36, 38, 49]
    120°-AFM/1L
    FeCl${}_2^* $3.43AFM/bulkTN = 24 K/bulkHM[37, 38, 50]
    FM/1LTC = 109 K/1L
    FeBr23.63AFM/bulkTN = 14 K/bulkHM[37, 38, 50]
    FM/1LTC = 81 K/1L
    FeI23.91AFM/bulkTN = 9 K/bulkHM[37, 38, 51]
    FM/1LTC = 42 K/1L
    CoCl23.42AFM/bulkTN = 25 K/bulk//Insulator[37, 38, 52]
    FM/1LTC = 85 K/1L
    CoBr23.62AFM/bulkTN = 18 K/bulk//Insulator[37, 38, 50]
    FM/1LTC = 23 K/1L
    CoI23.80HM/bulkTN = 11 K/bulkInsulator[42, 53]
    HM
    NiCl23.50AFM/bulkTN = 52 K/bulk//Insulator[38, 39, 54]
    FM/1LTC = 118 K/1L
    NiBr${}_2^* $3.80HM/bulkTN = 23 K/bulk//Ferroelectric insulator[40, 55]
    Noncollinear/1LTC = 28 K/1L
    NiI23.88HM/bulkTN = 60 K/bulkFerroelectric semiconductor[41]
    HM/1LTN = 21 K/1L
    VCl36.28AFM/bulkTN = 20 K/bulkDHM[56, 57]
    FM/1LTC = 80 K/1L
    VBr36.37AFM/bulkTN = 27 K/bulk//Semiconductor[58, 59]
    FM/1LTC = 20 K/1L
    VI36.83FM/ interlayerTc = 50 K/bulkMott insulator[30, 60]
    FM/ intralayerTC = 60 K/1L
    CrCl${}_3^* $6.01AFM/ interlayerTN = 17 K/bulk//Semiconductor[22, 61]
    FM/ intralayerTC = 13 K/1L
    CrBr${}_3^* $6.30FM/ interlayerTc = 37 K/bulkSemiconductor[20, 62]
    FM/ intralayerTC = 34 K/1L
    CrI${}_3^* $6.95FM/ intralayerTc = 61 K/bulkSemiconductor[16, 63]
    AFM/ few LTC = 45 K/1L
    MnCl36.21FM/1L//DHM[64]
    MnBr36.58FM/1L//DHM[64]
    MnI37.08FM/1L//DHM[64]
    FeCl36.22HM/bulkTN = 15 K/bulkSemiconductor[65, 66]
    FM/1L
    FeBr36.61AFM/bulkTN = 16 K/bulkSemiconductor[65, 67]
    FM
    FeI37.12FM/1LSemiconductor[65]
    NiCl35.94FM/1LTC = 497 K/1LDHM[68]
    NiBr36.31FM/1LTC = 595 K/1L//DHM[68]
    NiI36.82FM/1LTC = 682 K/1LDHM[68]
    α-RuCl${}_3^* $6.19AFM QSL/bulkTN = 7 K/bulkMott insulator[44, 45, 69]
    AFM QSL/1L
    RuBr36.25FM/1LTI[70]
    RuI37.10FM/1 LTC = 360 K/1LTI[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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  • 收稿日期:  2022-04-17
  • 修回日期:  2022-05-18
  • 上网日期:  2022-06-14
  • 刊出日期:  2022-06-20

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