Growth of two-dimensional single crystal materials controlled by atomic steps

Chang Chao; Kou Jin-Zong; Xu Xiao-Zhi

doi:10.7498/aps.72.20230887

Abstract

Since the successful mechanical exfoliation of graphene in 2004, two-dimensional materials have aroused extensive research and fast developed in various fields such as electronics, optoelectronics and energy, owing to their unique structural and physicochemical properties. In terms of synthesis methods, researchers have made further advancements in the atomic step method, building upon traditional techniques such as mechanical exfoliation, liquid-phase exfoliation, vapor-phase deposition, wet chemical synthesis, and nanomaterial self-assembly. These efforts aim to achieve high-quality large-scale two-dimensional single crystal materials. In this article, the representative research on the growth of two-dimensional single crystal materials controlled by atomic steps in recent years is reviewed in detail. To begin with, the research background is briefly introduced, then the main synthesis methods of two-dimensional single crystal materials are discussed and the challenges and reasons for the difficulty in epitaxially preparing non-centrosymmetric materials are analyzed. Subsequently, the growth mechanisms and recent advances in the preparation of two-dimensional single crystal materials assisted by atomic steps are presented. The theoretical basis and universality of atomic step-controlled nucleation in two-dimensional single crystal material are analyzed. Furthermore, the challenges and future directions for achieving large-scale, directionally controllable two-dimensional single crystal materials are predicted. Finally, potential applications of the step method in the future scalable chip device fabrication are systematically discussed.

Keywords:

two-dimensional single crystal materials /
atomic steps /
non-centrosymmetry /
epitaxial growth

Authors and contacts

1.
Guangdong Provincial Key Laboratory of Quantum Engineering and Quantum Materials, School of Physics, South China Normal University, Guangzhou 510006, China
2.
Guangdong-Hong Kong Joint Laboratory of Quantum Matter, Frontier Research Institutefor Physics, South China Normal University, Guangzhou 510006, China

Corresponding author: Kou Jin-Zong, jinzongkou@scnu.edu.cn ; Xu Xiao-Zhi, xiaozhixu@scnu.edu.cn

Funds: Project supported by the Guangdong Basic and Applied Basic Research Foundation (Grant Nos. 2020B1515020043, 2019A1515110302) and the National Natural Science Foundation of China (Grant No. 52102043).

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Cited By

图 1 (a)单核生长和(b)外延生长原理示意图

Figure 1. Schematic diagrams of (a) single nuclei growth and (b) epitaxial growth.

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图 2 (a)中心对称和(b)非中心对称二维材料的原子结构示意图. 图(a)中灰色圆球对应同种元素原子; 图(b)中橙色圆球和蓝色圆球分别对应2种元素原子. 中心对称的结构翻转180°后可以复原, 非中心对称的结构翻转180°后无法复原

Figure 2. Schematic diagrams of atomic structure of (a) centrosymmetric and (b) non-centrosymmetric 2D materials. Gray balls in Fig. (a) correspond to the same kind of atoms, orange and blue balls in Fig. (b) correspond to two kinds of atoms, respectively. A centrosymmetric structure can be restored after being turned over 180°, and a non-centrosymmetric structure cannot be restored after being turned over 180°.

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图 3 在Cu (a) (112), (b) (113), (c) (133)和(d) (223)晶面上制备的单向排列石墨烯SEM图^[138]

Figure 3. SEM images of unidirectionally aligned graphene domains on (a) (112), (b) (113), (c) (133) and (d) (223) facets of Cu^[138].

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图 4 (a) Ge (110)面单向排列石墨烯SEM图^[142]; (b)单晶单层石墨烯的HRTEM图^[142]; (c)石墨烯种子沿Ge (110)面的[$ \overline 1 10 $]方向单向排列的AFM图^[127]; (d), (e)石墨烯成核与台阶边缘对接的单向排列示意图^[127]

Figure 4. (a) SEM image of unidirectional graphene grown on Ge (110) surface^[142]; (b) HRTEM image of single crystal monolayer graphene^[142]; (c) AFM image of graphene seeds aligned along [$ \overline 1 10 $] direction of Ge (110) surface^[127]; (d), (e) schematic illustration of graphene nucleation docking with the step edge for unidirectional alignment^[127].

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图 5 (a) Cu (110)面单向排列的hBN SEM图; (b) hBN晶畴拼接处的TEM图, 插图为低倍TEM图; (c), (d) H₂在1000 ℃下经30 min刻蚀Cu(110)和Cu(111)上hBN的SEM图; (e) hBN晶格之字形边缘与Cu(110)表面的Cu$ \langle {211} \rangle $方向台阶结合原子示意图; (f)不同hBN边缘与Cu (110)表面的Cu $ \langle {211} \rangle $方向台阶形成能^[158]

Figure 5. (a) SEM image of as-grown unidirectionally aligned hBN domains on Cu (110) substrate; (b) TEM images of neighboring merged hBN domains, inset shows the same image at a lower magnification; (c), (d) SEM images of hBN film as-grown on Cu(110) and Cu(111) surfaces after H₂ etching at 1, 000 ℃ for 30 min; (e) atomic configuration of a zigzag edge of hBN lattice attaching to the Cu$ \left\langle {211} \right\rangle $ atomic step edge on the vicinal Cu (110) surface; (f) formation energies of various hBN edges attached to a Cu $\langle {211}\rangle $ step edge of vicinal Cu(110) substrate^[158].

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图 6 (a), (b)制备单晶Au (111)的示意图及CVD法在其表面生长MoS₂的SEM图^[169]; (c)—(e) Au (607) , Au (2 1 11) 面的MoS₂ SEM以及拉曼图^[170]; (f), (h)MoS₂形态变化示意图; (g), (i)不同S/Mo比例下制备的2D MoS₂三角形、1D MoS₂纳米带SEM图^[171]

Figure 6. (a), (b) Schematic illustration of processes of single crystal Au(111) formation and SEM image of MoS₂ grown on its surface by CVD method^[169]; (c)–(e) SEM images and Raman spectra of MoS₂ on Au (607), Au (2 1 11)facets^[170]; (f), (h) schematic illustration of the morphological evolution of MoS₂; (g), (i) SEM images of 2D monolayer MoS₂ triangles and 1D MoS₂ nanoribbons at different S/Mo ratios^[171].

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图 7 (a) O₂刻蚀WS₂薄膜后的SEM图; (b)对齐WS₂岛拼接区域STEM图; (c) WS₂晶格STEM图; (d) 2 inch单层WS₂薄膜光学图; (e) a-Al₂O₃独立WS₂晶畴光学图; (f), (g)WS₂晶畴AFM图, 台阶方向$\langle 1\bar 1 01 \rangle$^[174]

Figure 7. (a) SEM image of WS₂ films after O₂ etching; (b) STEM image of merged area of aligned WS₂ islands; (c) STEM image of WS₂ lattice; (d) photograph of 2 inch WS₂ monolayer thin film; (e) optical image of individual WS₂ islands on a-Al₂O₃; (f), (g) AFM image of a WS₂ island, the direction of the steps is $ \langle1\bar 1 01 \rangle$^[174].

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图 8 不同成核位置导致不同生长结果的原理示意图　(a)同时在台阶边缘和台阶平面处成核会导致正反取向;　(b)只在台阶边缘处成核会导致单一取向

Figure 8. Schematic diagrams of different growth results at different nucleation positions: (a) Positive and negative orientation when nucleation occur on both step edges and terrace; (b) single orientation when nucleation only occurs on step edges.

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图 9 (a)退火前c-Al₂O₃表面; (b)退火中c-Al₂O₃表面; (c)长时间退火后c-Al₂O₃表面; (d)MoS₂边缘同氧空位缺陷台阶与无氧空位平行台阶结合能; (e)反平行MoS₂晶畴跨不同台阶(Ⅰ, Ⅱ和Ⅲ)能量; (f)3种台阶边缘处MoS₂边缘^[180]

Figure 9. (a) Original c-Al₂O₃ surface before annealing; (b) original c-Al₂O₃ surface during annealing; (c) original c-Al₂O₃ surface after a long annealing time; (d) binding energy of a MoS₂ grain on a straight parallel step with O vacancy and on a defective step without O vacancy; (e) energy difference between antiparallel MoS₂ grains that cross different types of step edges (Ⅰ, Ⅱ and Ⅲ); (f) MoS₂ grain on three types of step edges^[180].

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图 10 (a), (b)穿过c-Al₂O₃台阶边缘的2个反平行WS₂晶粒示意图; (c) 2个反平行WS₂晶粒之间的能量差; (d), (e)穿过a-Al₂O₃台阶边缘的2个反平行WS₂(MoS₂)晶粒示意图; (f) 2个反平行WS₂(MoS₂)晶粒之间的能量差, 沿着不同方向的台阶都是为了打破反平行线^[180]

Figure 10. (a), (b) Schematic diagrams of two antiparallel WS₂ grains that across a step edge of c-Al₂O₃; (c) energy difference between two antiparallel WS₂ grains; (d), (e) schematic diagrams of two antiparallel WS₂ (MoS₂) grains that across a step edge of a-Al₂O₃; (f) energy difference between two antiparallel WS₂ (MoS₂) grains. Steps along different directions all work for breaking of antiparallel alignments^[180].

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表 1 二维材料的应用领域及其挑战

Table 1. Applications and future challenges of two-dimensional materials.

领域	应用方向	优势	挑战
电子	晶体管、传感器、存储设备、互连、柔性电子产品、透明导电薄膜	高载流子迁移率、可调带隙、优异的机械和化学稳定性	可扩展性、可重复性、接口工程、设备集成、环境稳定性
光电子	LEDs、太阳能电池、光电探测、光调制器、吸收器	高载流子迁移率、可调带隙、优异的光吸收和发射	可重复性、环境稳定性、界面能源、设备集成、成本
催化	水分解、CO₂还原、析氢反应、氧化还原反应	高比表面积、可调电子和化学性能、催化活性	可扩展性、反应稳定性、优异的选择性、成本
储能	电池、超级电容器、燃料电池、电催化、储氢	高表面积、可调的电子和化学性能、优异的电化学性能	可扩展性、反应稳定性、选择性、成本、毒性
传感器	气体、生物、应变传感器	灵敏度高、选择性好、电子和化学性能可调、稳定性好	可扩展性、环境稳定性、选择性、设备集成
生物医学	药物输送、生物传感、组织工程、生物成像	生物相容性、高表面积、可调的电子和化学性质、稳定性	选择性、可扩展性、毒性、生物环境稳定性、监管批准
环境	水处理、空气净化、能量收集	高表面积、电子和化学性能可调、优异的光催化和电催化	可扩展性、环境稳定性、选择性、成本

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表 2 衬底台阶调控TMDs生长^[180]

Table 2. Controversial growth behaviours of TMDs on substrates with steps^[180].

Substrate	TMDs	Alignment/%	Symmetry breaking	Ref.
a-Al₂O₃	WS₂	99	√	[174]
a-Al₂O₃	MoS₂	86	√	[181]
c-Al₂O₃	MoS₂	99	√	[16]
c-Al₂O₃	WS₂	>90	√	[182]
c-Al₂O₃	WSe₂	92	√	[105]
Au(533)	WS₂	>90	√	[183]
Au(111)	MoS₂	99	√	[184]
Au(111)	MoS₂	98	√	[169]
β-Ga₂O₃	MoS₂	>90	√	[172]
c-Al₂O₃	MoS₂	50	×	[177]
c-Al₂O₃	MoS₂	50	×	[178]
c-Al₂O₃	MoS₂	60	×	[173]
c-Al₂O₃	MoS₂	50	×	[185]
c-Al₂O₃	MoS₂	56	×	[176]
Au(111)	MoS₂	50	×	[186]
Au(111)	MoS₂	50	×	[187]
Ag(111)	MoS₂	50	×	[188]

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表 3 衬底台阶调控hBN生长^[180]

Table 3. Controversial growth behaviours of hBN on substrates with steps^[180].

Substrate	Alignment/%	Symmetry breaking	Ref.
Cu (110)	99	√	[158]
Cu (111)	99	√	[130]
Cu (102) Cu (103)	97	√	[122]
Cu (110)	50	×	[189]
Cu (110) Cu (111)	21 54	×	[75]
Cu (111)	50	×	[190]
Ni (111)	50	×	[113]
Ni (111)	54	×	[191]
Ge (110)	52	×	[179]

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