二维范德瓦尔斯异质结构的制备与物性研究

吴燕飞; 朱梦媛; 赵瑞杰; 刘心洁; 赵云驰; 魏红祥; 张静言; 郑新奇; 申见昕; 黄河; 王守国

doi:10.7498/aps.71.20212033

摘要

二维范德瓦尔斯材料(可简称二维材料)已发展成为备受瞩目的材料大家族, 而由其衍生的二维范德瓦尔斯异质结构的集成、性能及应用是现今凝聚态物理和材料科学领域的研究热点之一. 二维范德瓦尔斯异质结构为探索丰富多彩的物理效应和新奇的物理现象, 以及构建新型的自旋电子学器件提供了灵活而广阔的平台. 本文从二维材料的转移技术着手, 介绍二维范德瓦尔斯异质结构的构筑、性能及应用. 首先, 依据湿法转移和干法转移的分类, 详细介绍二维范德瓦尔斯异质结构的制备技术, 内容包括转移技术的通用设备、常用转移方法的具体操作步骤、三维操纵二维材料的方法、异质界面清洁. 随后介绍二维范德瓦尔斯异质结构的性能和应用, 重点介绍二维磁性范德瓦尔斯异质结构, 并列举在二维范德瓦尔斯磁隧道结和摩尔超晶格领域的应用. 因此, 二维材料转移技术的发展和优化将进一步助力二维范德瓦尔斯异质结构在基础科学研究和实际应用上取得突破性的成果.

关键词:

Abstract

Two-dimensional van der Waals materials (2D materials for short) have developed into a novel material family that has attracted much attention, and thus the integration, performance and application of 2D van der Waals heterostructures has been one of the research hotspots in the field of condensed matter physics and materials science. The 2D van der Waals heterostructures provide a flexible and extensive platform for exploring diverse physical effects and novel physical phenomena, as well as for constructing novel spintronic devices. In this topical review article, starting with the transfer technology of 2D materials, we will introduce the construction, performance and application of 2D van der Waals heterostructures. Firstly, the preparation technology of 2D van der Waals heterostructures in detail will be presented according to the two classifications of wet transfer and dry transfer, including general equipment for transfer technology, the detailed steps of widely used transfer methods, a three-dimensional manipulating method for 2D materials, and hetero-interface cleaning methods. Then, we will introduce the performance and application of 2D van der Waals heterostructures, with a focus on 2D magnetic van der Waals heterostructures and their applications in the field of 2D van der Waals magnetic tunnel junctions and moiré superlattices. The development and optimization of 2D materials transfer technology will boost 2D van der Waals heterostructures to achieve breakthrough results in fundamental science research and practical application.

Keywords:

作者及机构信息

1.
北京科技大学材料科学与工程学院材料物理与化学系, 北京　100083

2.
中国科学院物理研究所/北京凝聚态物理国家研究中心, 北京　100190

通信作者: 王守国, sgwang@ustb.edu.cn

基金项目: 国家自然科学基金(批准号: 51625101, 51971026, 52071026, 52130103, 12174426)和中央高校基本科研业务费(批准号: 06500140, FRF-MP-20-05)资助的课题.

Authors and contacts

1.
Department of Materials Physics and Chemistry, School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China

2.
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

Corresponding author: Wang Shou-Guo, sgwang@ustb.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51625101, 51971026, 52071026, 52130103, 12174426) and the Fundamental Research Fund for the Central Universities, China (Grant Nos. 06500140, FRF-MP-20-05).

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施引文献

图 1 干法转移所用的设备示意图

Fig. 1. Schematic diagram of the experimental setup for dry transfer.

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图 2 PMMA为转移介质的基体刻蚀法

Fig. 2. Substrate etching method with PMMA as transfer medium.

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图 3 PMMA/牺牲层或者PMMA支持层的转移法^[51]

Fig. 3. PMMA/sacrificial layer or PMMA supporting layer method^[51].

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图 4 液体楔入的转移法

Fig. 4. Liquid wedging method.

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图 5 基于PDMS的全干性转移法^[44]

Fig. 5. PDMS-based fully dry transfer method^[44].

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图 6 基于PDMS/PC的转移方法

Fig. 6. PDMS/PC-based transfer method.

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图 7 基于PDMS/PPC的转移方法

Fig. 7. PDMS/PPC-based transfer method.

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图 8 热塑性牺牲层的转移法^[49]

Fig. 8. Thermoplastic sacrificial layer transfer method^[49].

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图 9 使用MDP实现二维材料的三维操纵^[81]

Fig. 9. 3D manipulation of 2D materials using MDP^[81].

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图 10 三种典型的二维磁性材料及其特性 (a)、(b)为CrI₃的晶体结构及磁学特性^[95]: (a) CrI₃的晶体结构; (b) 一层、两层、三层的CrI₃在15 K下的磁光克尔(magneto-optical Kerr effect, MOKE)信号随着磁场的变化情况; (c)—(e)为CGT的晶体结构及特性^[96]: (c) CGT的晶体结构; (d)不同层数的CGT的光学图片; (e)不同温度下(d)中CGT的MOKE信号; (f)—(h)^[91]、(i)—(k)^[92]均为FGT的晶体结构及特性: (f) FGT的晶体结构; (g) FGT的纵向电阻随着温度的变化关系, 左上角是霍尔器件的光学图片; (h) FGT的霍尔电阻随着温度的变化关系; (i) FGT的T_C随着厚度的变化关系; (j)被固体电解质LiClO₄覆盖的FGT的纵向电导率随着栅压的变化关系, 器件结构如(j)中插图所示; (k)不同温度下(j)中器件在V_g = 2.1 V时霍尔电压随着磁场的变化关系

Fig. 10. Three typical two-dimensional magnetic materials and their properties. (a) and (b) show the structure and magnetic properties of CrI₃^[95]: (a) Crystal structure of CrI₃; (b) magnetic field dependence of the MOKE signal in monolayer, bilayer and trilayer CrI₃ at 15 K. (c), (d) and (e) show the structure and properties of CGT^[96]: (c) crystal structure of CGT; (d) optical images of CGT with different layers; (e) temperature dependence of the MOKE signal of CGT in (d); (f)–(h)^[91] and (i)–(l)^[92] all show the structure and properties of FGT: (f) crystal structure of FGT; (g) temperature dependence of the longitudinal resistance of FGT device. The upper-left inset shows an optical image of the Hall bar device; (h) temperature dependence of the Hall resistance of FGT device; (i) thickness dependence of the T_C of FGT; (j) conductance as a function of gate voltage V_g measured in a trilayer FGT device covered by solid electrolyte LiClO₄ and the inset shows the structure of the device; (k) Hall resistance of a four-layer FGT flake under a gate voltage of V_g = 2.1 V at different temperatures.

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图 11 基于PDMS全干性转移法制备的二维磁性范德瓦尔斯异质结构　(a)—(d)为FPS/FGT和FPS/FGT/FPS异质结构^[97]: (a) FPS/FGT异质结构的光学图片; (b) FPS/FGT异质结构的原子力显微镜图; (c)—(d) 两种异质结构与单一FGT的Kerr信号随着温度的变化关系, 结果显示异质结构的形成可以有效提升T_C; (e)—(h)为CrBr₃/石墨烯的异质结构^[98]: (e) CrBr₃/石墨烯异质结构的光学图片; (f) 非局域测量技术探测塞曼自旋霍尔效应的示意图; (g)异质结构中石墨烯的非局域电阻在不同磁场下随栅压的变化情况; (h)非局域电阻随温度的变化情况. (i)—(l)为CGT/WS₂异质结^[99]: (i) CGT/WS₂异质结构的光学图片; (j)单层的WS₂和不同CGT/WS₂异质结构的光致发光光谱; (k) 开尔文探针显微镜的示意图; (l) 室温下利用开尔文探针显微镜测量的CGT、WS₂和异质结构的表面能或功函数

Fig. 11. Two-dimensional magnetic van der Waals heterostructures fabricated by all dry transfer method based on PDMS: (a)–(d) FPS/FGT and FPS/FGT/FPS heterostructures^[97]: (a) Optical image of FPS/FGT heterostructure; (b) Atomic force microscopy image of the FPS/FGT heterostructure in (a); (c) and (d) temperature dependence of the Kerr signal between two kinds of heterostructures and individual FGT, and it shows effective enhancement of T_C because of the fabrication of heterostructures; (e)–(h) CrBr₃/graphene heterostructure^[98]: (e) optical image of CrBr₃/graphene heterostructure; (f) diagram of non-local measurements for probing Zeeman spin Hall effect; (g) the non-local resistance R_nl as a function of the back gate V_g acquired under different external field; (h) temperature dependence of the non-local resistance R_nl; (i)–(l) CGT/WS₂ heterostructure^[99]: (i)optical image of CGT/WS₂ heterostructure; (j) Photoluminescence spectra (PL spectra) of individual WS₂ and different CGT/WS₂ heterostructures; (k) schematic diagram of Kelvin probe force microscopy; (l) measured surface potential or work function of CGT, WS₂, and the heterostructure at room temperature.

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图 12 范德瓦尔斯作用力拾取的转移法制备的二维磁性范德瓦尔斯异质结构　(a)—(d)为WSe₂/CrI₃异质结构^[100]: (a) 1L WSe₂/3L CrI₃的结构示意图; (b)在温度15 K和零磁场下的偏振分辨光致发光光谱; (c)、(d)分别为1 L WSe₂/2 L CrI₃的结构示意图以及左、右偏振光激发下的光致发光强度随着磁场的变化情况; (e)、(f)亦为WSe₂/CrI₃异质结^[101]: (e) WSe₂/CrI₃异质结构的光学图片以及虚线框内的光致发光光谱强度分布; (f)通过不同强度的圆偏振光调控的光致发光光谱; (g)—(j)为CrCl₃/双层石墨烯的异质结构^[102]: (g)器件示意图; (h)一个真实器件的光学图片; (i) 在垂直磁场B_⊥= –14 T下双层石墨烯的量子霍尔效应; (j)无外磁场和外加垂直磁场下非局域磁阻测量结果

Fig. 12. Two-dimensional magnetic van der Waals heterostructures fabricated by van der Waals pick-up method. (a)–(d) WSe₂/CrI₃ heterostructure^[100]: (a) Schematic of a monolayer WSe₂ and trilayer CrI₃ heterostructure; (b) polarization-resolved photoluminescence of a WSe₂/trilayer CrI₃ heterostructure at 15 K and zero magnetic field; (c) schematic of a monolayer WSe₂ and bilayer CrI₃ heterostructure; (d) photoluminescence intensity plot of σ⁺ (left) and σ^– (right) polarized excitation and detection as a function of magnetic field and photoenergy; (e) and (f) WSe₂/CrI₃ heterostructure^[101]: (e) optical image of WSe₂/CrI₃ heterostructure and PL intensity in boxed region; (f) circularly polarized PL spectra at selected excitation powers; (g)–(j) CrCl₃/BLG heterostructure^[102]: (g) schematic of device; (h) optical image of an actual device; (i) quantum Hall effect at perpendicular magnetic field B_⊥= –14 T, showing typical quantum Hall plateaus of BLG; (j) magneto-transport nonlocal measurement results at zero and perpendicular magnetic fields.

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图 13 二维范德瓦尔斯磁隧道结　(a)—(c) 层状反铁磁CrI₃的自旋过滤效应^[119]: (a) 双层CrI₃在无磁场、垂直磁场和平面磁场下的磁化状态, 其中在无磁场下能抑制隧穿电流; (b)石墨烯/CrI₃/石墨烯的自旋过滤磁隧道结(sf-MTJs)的示意图, 顶层的BN作为保护层以提高器件的稳定性; (c)不同磁场条件下sf-MTJ 的隧穿电流, 其中势垒层为双层CrI₃; (d), (e)一个4层CrI₃的隧道结^[121]: (d)一个4层 CrI₃ 隧道结的光学图像, 虚线显示隧道结区域; (e)在500 μV 交流激励下, 通过一个双层CrI₃隧穿层的电导随垂直外加磁场的变化; (f), (g) FGT/hBN/ FGT隧道结^[124]: (f)范德瓦尔斯异质结构示意图; (g)在温度T = 4.2 K下隧穿电阻随磁场(平行于FGT c-轴方向)的变化, 在B ≈ ± 0.7 T出现电阻急剧地跳跃, 隧穿磁阻变化达到~160 %; (h), (i) FGT/graphite/FGT异质结构的磁阻效应^[126]: (h) 一个FGT/graphite/FGT的光学和AFM图像; (i)一个典型的GMR效应的输运现象示意图; (j), (k) CrTe₂/石墨烯/CrTe₂磁隧道结^[127]: (j) 1T-CrTe₂/三层石墨烯/1T-CrTe₂ vdW MTJ的结构图; (k)两种vdW MTJ的隧穿磁阻率, 分别以未掺杂和掺杂的石墨烯作为势垒层, 隧穿磁阻率随着B掺杂的石墨烯(Gr–B)层数增加而增大

Fig. 13. 2D van der Waals magnetic tunnel junctions. (a)–(c) Spin-filter effects in layered-antiferromagnetic CrI₃^[119]: (a) Schematic of magnetic states in bilayer CrI₃. (Left) Layered-antiferromagnetic state suppresses the tunneling current at zero magnetic field; (b) schematic of graphene/CrI₃/graphene sf-MTJ, with bilayer CrI₃ as the spin-filter tunnel barrier; (c) tunneling current of a bilayer CrI₃ sf-MTJ at selected magnetic fields; (d)–(e) a tetralayer CrI₃ tunnel junction device^[121]: (d) optical micrograph of a tetralayer CrI₃ tunnel junction device. The dashed line encloses the tunnel junction area; (e) conductance through a bilayer CrI₃ tunnel barrier as a function of an out-of-plane applied magnetic field with 500 μV AC excitation; (f), (g) FGT/hBN/ FGT MTJs^[124]: (f) schematic representation of the van der Waals heterostructure; (g) Tunneling resistance measured at T = 4.2 K with B applied parallel to the FGT c-axis. Very sharp resistance jumps are observed for B ≈ ± 0.7 T, showing the variation in TMR is ~160 %; (h), (i) the MR effect in FGT/graphite/FGT heterostructures^[126]: (h) optical and AFM images of an FGT/graphite/FGT heterostructure; (i) Schematic diagram for the transport behavior of a typical GMR effect; (j), (k) CrTe₂/graphene/CrTe₂ MTJs^[127]: (j) structure of 1T-CrTe₂/Graphene(3 ML)/1T-CrTe₂ vdW MTJ; (k) TMR ratios of two vdW MTJs with graphene and doped graphene as barrier, showing TMR ratios increase with layer numbers of B-doped graphene.

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图 14 转角双层石墨烯的电子结构和非常规超导 (a)双层扭转石墨烯中的摩尔图形和(b)两层的两个 K (K' ) 波矢量之间的差异构成的迷你布里渊区^[130]; (c)在魔角(θ = 1.08°)时出现的扁平带(蓝色)的电子结构, 和(d)在低温(T = 0.3 K)下测得的电导, 其中狄拉克点位于载流子n = 0位置, 较浅的阴影区指示n = ± n_s = ± 2.7 × 10¹² cm^–2附近的超晶格能隙, 较暗的阴影区指示在± n_s/2附近的半填充态; (e)双层扭转石墨烯的器件和四端法测量示意图, 及(f)观测到的非常规超导^[131]

Fig. 14. Electronic structure and unconventional superconductivity of twisted bilayer graphene (TBG). (a) The moiré pattern in TBG; (b) the mini Brillouin zone (MBZ) is constructed from the difference between the two K (K′ ) wave vectors from the two layers^[130]; (c) electronic band dispersion with a flat band of b); (d) measured conductance G of magic-angle TBG device with θ = 1.08° and T = 0.3 K. Dirac point is located at n = 0. The lighter shaded regions are superlattice gaps at carrier density n = ± n_s = ± 2.7 × 10¹² cm^–2. The darker shaded regions denote half-filling states at ± n_s/2; (e) schematic of a typical twisted bilayer graphene device and four-probe measurement scheme and (f) unconventional superconductivity of a magic-angle (θ = 1.08°) twisted graphene moiré superlattice^[131].

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图 15 二维磁性材料的摩尔超晶格及拓扑磁结构　(a)为CrI₃/CrGeTe₃异质结构形成摩尔超晶格的示意图^[137]; (b)—(e)^[138]: (b)二维铁磁材料堆叠在具有磁各向异性的奈尔型反铁磁基底上的示意图; (c)单层二维铁磁性材料(灰色)和层状反铁磁基底(绿色)间由于晶格错配或扭转形成的摩尔超晶格; (d)层间磁耦合强度随摩尔超晶格周期的变化; (e)斯格明子形成的示意图; (f)—(h)范德瓦尔斯作用力拾取的转移法制备的WTe₂/Fe₃GeTe₂异质结构^[139]: (f)异质结构的光学图片; (g)霍尔电阻随着磁场的变化情况, 在发生磁化翻转的地方出现尖峰, 表明存在拓扑霍尔效应; (h)样品在180 K和外加510 Oe的磁场下, WTe₂/40L Fe₃GeTe₂的样品在不同偏转角度下利用洛伦兹透射电镜观测到的斯格明子

Fig. 15. Moiré superlattice and topological magnetic structure in two-dimensional magnetic materials. (a) Schematic diagram of the proposed Moiré pattern in CrI₃/CrGeTe₃ heterostructure^[137]; (b)–(e)^[138]: (b) an ferromagnetic (FM) monolayer on a layered antiferromagmetic (AFM) substrate with lateral Neél order and perpendicular anisotropy; (c) The moiré pattern between the FM monolayer (gray) and AFM substrate (green) arises from the lattice mismatch and/or twisting; (d) phase diagram as a function of moiré period A and the magnitude of interlayer magnetic coupling; (e) schematic diagram of the formation of skyrmion. (f)–(h) WTe₂/Fe₃GeTe₂ heterostructure^[139]: (f) optical image of WTe₂/Fe₃GeTe₂ heterostructure; (g) magnetic field dependence of Hall resistivity, showing a peak and dip near the transition edge before the magnetization saturates, which is a sign of the topological Hall effect; (h) Lorentz transmission electron microscopy observation of skyrmion lattice from under focus to over focus on WTe₂/40L Fe₃GeTe₂ samples at 180 K with a field of 510 Oe.

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二维范德瓦尔斯异质结构的制备与物性研究