超高真空条件下分子束外延生长的单层二维原子晶体材料的研究进展

王兴悦; 张辉; 阮子林; 郝振亮; 杨孝天; 蔡金明; 卢建臣

doi:10.7498/aps.69.20200174

摘要

二维原子晶体材料具有与石墨烯相似的晶格结构和物理性质, 为纳米尺度器件的科学研究提供了广阔的平台. 研究这些二维原子晶体材料, 一方面有望弥补石墨烯零能隙的不足; 另一方面继续发掘它们的特殊性质, 有望拓宽二维原子晶体材料的应用领域. 本文综述了近几年在超高真空条件下利用分子束外延生长技术制备的各种类石墨烯单层二维原子晶体材料, 其中包括单元素二维原子晶体材料(硅烯、锗烯、锡烯、硼烯、铪烯、磷烯、锑烯、铋烯)和双元素二维原子晶体材料(六方氮化硼、过渡金属二硫化物、硒化铜、碲化银等). 通过扫描隧道显微镜、低能电子衍射等实验手段并结合第一性原理计算, 对二维原子晶体材料的原子结构、能带结构、电学特性等方面进行了介绍. 这些二维原子晶体材料所展现出的优异的物理特性, 使其在未来电学器件方面具有广阔的应用前景. 最后总结了单层二维原子晶体材料领域可能面临的问题, 同时对二维原子晶体材料的研究方向进行了展望.

关键词:

二维原子晶体材料 /
扫描隧道显微镜 /
分子束外延 /
晶格结构

Abstract

Two-dimensional atomic crystal materials have similar lattice structures and physical properties to graphene, providing a broad platform for the scientific research of nanoscaled devices. The emergence of two-dimensional materials presents the new hope of science and industry. As is well known, graphene is the most widely studied two-dimensional (2D) material in recent ten years. Its unique atomic structure and electronic band structure make it have novel physical and chemical properties and broad applications in electronic devices, optical devices, biosensors, solar cell, and lithium ion battery. In recent years, graphene-like single-layered 2D materials have attracted much attention. Researches of these 2D atomic crystal materials and their physical properties, on the one hand, are expected to make up for the lack of band gap in graphene, and on the other hand, continue to explore their unique properties, expand the application of 2D atomic crystal materials. Among all the preparation methods of single-layered 2D atomic crystal materials, the molecular beam epitaxy (MBE) is considered to be the most competitive method. The manufacturing process of MBE is usually carried out under ultra-high vacuum condition, which ensures the cleanness of the 2D material surface. At the same time, the solid growth substrate needed for epitaxial growth can be used as a carrier to support and stabilize the growth of 2D materials. In this review, we summarize many single-layered 2D materials prepared by MBE under ultra-high vacuum conditions in recent years, including monatomic 2D atomic crystal materials (silicene, germanene, stanene, hafnene, borophene, phosphorene, bismuthene, antimonene) and binary atomic crystal materials (hexagonal boron nitride, transition metal dichalcogenides, copper selenide, silver telluride). In addition, by scanning tunneling microscopy (STM), low-energy electron diffraction (LEED) and first-principles calculations, we investigate the atomic structures, energy gap modulations, and electrical properties of 2D materials. These 2D atomic crystal materials exhibit the excellent physical properties, which will make them have broad application prospects in future electronic devices. Finally, we summarize the problems faced by the further development of 2D materials and suggest several potential development directions.

Keywords:

two-dimensional atomic crystal materials /
scanning tunneling microscope /
molecular beam epitaxy /
lattice structure

作者及机构信息

王兴悦,
张辉,
阮子林,
郝振亮,
杨孝天,
蔡金明,
卢建臣

昆明理工大学材料科学与工程学院, 昆明　650093

通信作者: 卢建臣, jclu@kust.edu.cn

基金项目: 国家级-国家自然科学基金(61901200)

Authors and contacts

Wang Xing-Yue,
Zhang Hui,
Ruan Zi-Lin,
Hao Zhen-Liang,
Yang Xiao-Tian,
Cai Jin-Ming,
Lu Jian-Chen

Faculty of Materials Science and Engineering, Kunming University of Science and Technology, Kunming 650093, China

Corresponding author: Lu Jian-Chen, jclu@kust.edu.cn

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施引文献

图 1 (a) 自由状态硅烯的结构模型; (b) 自由状态下硅烯的能带结构^{[ 23]}; (c), (d) Ag(111)上硅烯不同相的STM图像^{[ 24]}; (e) Ir(111)上硅烯的STM图像、STM模拟和理论计算结构图^{[ 25]}

Fig. 1. (a) Structure model of free silicene; (b) band structure of silicene in free state^{[ 23]}; (c), (d) the STM images of different phases of silicene on Ag(111)^{[ 24]}; (e) STM image, simulated STM image, theoretical calculation structure of silicene on Ir(111)^{[ 25]}.

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图 2 (a) Pt(111)上锗烯的STM图像; (b)和(c)分别为Pt(111)表面锗烯的结构与电子局域函数; (d) Pt(111)上锗烯的LEED图案^{[ 26]}; (e)不同蜂窝结构下二维Ge的能量与六边形晶格常数的关系; (f), (g) 用力常数和线性响应理论得到的声子色散曲线, 分别用黑色曲线和绿色虚线表示^{[ 27]}

Fig. 2. (a) STM image of germanene on Pt(111); (b) and (c) are the structure and electron localization functions of germanene on Pt(111) surface, respectively; (d) LEED pattern of germanene on Pt(111)^{[ 26]}; (e) energy versus hexagonal lattice constant of 2D Ge is calculated for various honeycomb structures; (f) and (g) phonon dispersion curves obtained by force-constant and linear response theory are presented by black and dashed green curves, respectively^{[ 27]}.

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图 3 (a) 顶层及次顶层Sn原子排布及STM图; (b) Sn原子排布侧视图 (A层为顶层, B层为次顶层)^{[ 32]}; (c) 锡烯薄膜的高分辨STM图像; (d) 蜂窝状锡烯的原子模型示意图; (e) 沿图(c)蓝线的剖面图, 显示相邻的Sn原子在表观高度上是相同的; (f) Cu(111)表面的二维BZs; (g)和(h) Cu(111)表面0.9 ML的锡烯沿着M-Γ-K-M₂ (g)和M-Γ-M′-Γ₂ (h)方向的ARPES能谱^{[ 33]}

Fig. 3. (a) Top view of both the top and bottom Sn atoms and its STM image; (b) side view of Sn atoms arrangement (layer A is the top layer, layer B is the sub top layer)^{[ 32]}; (c) high-resolution STM image of the stanene film; (d) schematic atomic model of the honeycomb stanene; (e) profile along the line in c showing that the adjacent Sn atoms are identical in apparent height; (f) 2D BZs of ultraflat stanene on Cu(111); (g) and (h) ARPES spectra of 0.9 ML stanene on Cu(111) along the M-Γ-K-M₂ (g) and M-Γ-M′-Γ₂ (h) directions^{[ 33]}.

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图 4 (a), (b)二维硼片结构图^{[ 40]}; (c) Ag(111)上硼结构的STM形貌图, 生长期间衬底温度为570 K, 硼岛被标记为S1相; (d) 图4(c)表面经650 K退火后硼片的STM图像, 两种不同的相分别称为S1和S2; (e) S1相的高分辨率STM图像; (f) S2相的高分辨率STM图像; (g) S1相的俯视图和侧视图; (h) S2相的俯视图和侧视图^{[ 41]}

Fig. 4. (a) and (b) are two-dimensional boron sheets structure figures^{[ 40]}; (c) STM topographic image of boron structures on Ag(111), with a substrate temperature of ~570 K during growth; (d) STM image of boron sheets after annealing the surface in Fig.4(c) to 650 K. The two different phases are labelled “S1” and “S2”; (e) high-resolution STM image of S1 phases; (f) high-resolution STM image of S2 phases; (g) top and side views of the S1 model; (h) top and side views of the S2 model^{[ 41]}.

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图 5 (a) Ir(111)表面上铪烯的STM图像及LEED图; (b) Ir(111)上铪烯的原子分辨STM图像; (c) Ir(111)衬底上铪平面的电荷分布图^{[ 43]}

Fig. 5. (a) STM image and LEED image of hafnium on Ir(111); (b) atomic resolution STM images of hafnium on Ir(111); (c) the 2D charge density in the Hf plane on Ir(111) substrate^{[ 43]}.

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图 6 (a) Au(111)单层磷烯的高分辨率STM图像; (b)沿(a)中红线的线轮廓^{[ 47]}; (c) 少层磷烯的俯视图和侧视图; (d) DFT计算得到的单层磷烯的能带结构^{[ 46]}

Fig. 6. (a) High-resolution STM image of single layer phosphorus on Au(111); (b) the line profile along the red line in panel (a)^{[ 47]}; (c) top and side views of few-layer phosphorene; (d) DFT-calculated band structure of phosphorene monolayer^{[ 46]}.

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图 7 (a) 二碲化钯(PdTe₂)晶体上锑烯生长过程示意图; (b) 大面积锑烯岛在PdTe₂上的STM图像; (c) 单层锑烯的原子分辨STM图像; (d) 样品暴露空气前后的XPS测量数据^{[ 53]}; (e) Cu(111)衬底上的翘曲单层锑烯和锑烯纳米岛的结构模型; (f) 图(e)的侧视图; (g) Cu(111)上单层锑烯的大面积STM图像和LEED图; (h) 第一层翘曲层和岛的原子分辨STM图像^{[ 54]}

Fig. 7. (a) Schematic of monolayer antimonene formed on PdTe₂ substrate; (b) STM image of large antimonene island on PdTe₂; (c) atomic resolution STM image of monolayer antimonene; (d) XPS results before and after sample exposure to air^{[ 53]}; (e) the structural model of buck antimonene monolayer and antimonene nanoisland on Cu(111) substrate; (f) side view of panel (e); (g) large-scale STM image and LEED pattern of the antimonene monolayer on Cu(111); (h) atomic resolution STM image of the first buckled layer and island^{[ 54]}.

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图 8 (a) SiC (0001)表面单层铋烯的STM图; (b) 占据态下高分辨STM图; (c) 铋烯在SiC (0001)上的结构模型; (d) 基于模型(c)计算得到的能带图和ARPES测量到的能带结构^{[ 61]}

Fig. 8. (a) STM image of bismuthene on SiC (0001); (b) high resolution STM image for occupied states; (c) bismuthene on SiC(0001) structural model; (d) theoretical band structure and ARPES measurementsts^{[ 61]}.

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图 9 (a) h-BN纳米材料的结构模型; (b) Cu (111)上单层h-BN的STM图像; (c) 室温下单层h-BN/Cu (111)的对比LEED图^{[ 70]}; (d) 利用BN粒子、纳米管和纳米片制备聚合物复合材料的热导率^{[ 71]}

Fig. 9. (a) Structural model of h-BN nanomaterials; (b) STM image of single layer h-BN on Cu (111); (c) contrast-inverted LEED pattern of a single layer h-BN/Cu (111) recorded at room temperature^{[ 70]}; (d) thermal conductivity of polymeric composites using BN particles, nanotubes and nanosheets^{[ 71]}.

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图 10 (a) Au(111)表面MoS₂单层岛的大规模STM图像; (b) 单个六边形MoS₂岛横跨单个Au(111)台阶的STM图像^{[ 75]}; (c) MoS₂从块体到单层能带带隙的转变^{[ 76]}; (d) 单层MoS₂光电晶体管原理图^{[ 77]}

Fig. 10. (a) Large-scale STM image of MoS₂ single-layer islands on the Au(111) surface; (b) STM image of a single MoS₂ island with a hexagon shape crossing a single Au(111) step^{[ 75]}; (c) bandgap transition of MoS₂^{[ 76]} from bulk to monolayer; (d) schematic of monolayer MoS₂ photodetector^{[ 77]}.

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图 11 (a) 单层MoSe₂的结构示意图^{[ 80]}; (b) DFT优化得到的Au(111)表面单层MoSe₂原子结构; (c) 单层MoSe₂的原子分辨图像; (d) 基于(b)中优化结构的STM模拟图; (e) Au(111)上单层MoSe₂岛的STM图像^{[ 83]}; (f) 图(e)中蓝色虚线标示的MoSe₂岛的高度轮廓图

Fig. 11. (a) Structural model of monolayer MoSe₂^{[ 80]}; (b) DFT optimized monolayer MoSe₂ atomic model on Au(111) surface; (c) atomic resolution STM image of monolayer MoSe₂; (d) theoretical simulated STM image based on the calculated structure in (b); (e) STM image of singlelayer MoSe₂ islands on Au(111) substrate^{[ 83]}; (f) height profile of MoSe₂ islands marked by a dashed blue line in (e).

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图 12 (a) 利用直接硒化的Pt(111)表面生长单层PtSe₂的示意图; (b) Pt(111)表面形成PtSe₂薄膜的LEED图; (c) 具有摩尔条纹PtSe₂薄膜的大面积STM图; (d) 单层PtSe₂的原子分辨STM图^{[ 88]}

Fig. 12. (a) Schematic of the fabrication of PtSe₂ thin films by a single step of direct selenization of a Pt(111) substrate; (b) LEED pattern of a PtSe₂ film formed on the Pt(111) substrate; (c) large-scale STM image shows the Moiré pattern of PtSe₂ thin film on Pt(111); (d) atomic resolution STM image of single layer PtSe₂^{[ 88]}.

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图 13 (a) NiSe₂薄膜的生长过程示意图; (b) 层状NiSe₂材料具有T和H两种构型^{[ 92]}; (c) 大面积NiSe₂的STM图像和(d)摩尔结构STM图像^{[ 93]}

Fig. 13. (a) Schematic of the fabrication process of NiSe₂ thin films; (b) NiSe₂ layer has two configurations of T and H^{[ 92]}; large-scale STM image (c) and Moiré pattern (d) of the 2D NiSe₂ film^{[ 93]}.

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图 14 (a) 单层WSe₂晶体结构示意图^{[ 98]}; (b) WSe₂薄膜的原子分辨STM图像(75 nm × 75 nm); (c) 单层WSe₂的理论能带结构^{[ 100]}; (d) WSe₂/石墨烯异质结构光致发光图谱^{[ 101]}; (e) 单层WSe₂ 1H相和1T' 相的原子结构; (f) 对应的具有高对称点标记的二维布里渊区; (g) 沿ΓY方向的ARPES图谱^{[ 102]}

Fig. 14. (a) Schematic of the crystal structure of monolayer WSe₂^{[ 98]}; (b) atomic resolution STM image(75 nm × 75 nm) of WSe₂ film; (c) theoretical band structures of monolayer WSe₂^{[ 100]}; (d) photoluminescence of WSe₂/Graphene heterostructure^{[ 101]}; (e) atomic structure of single layer 1H and 1T' WSe₂; (f) corresponding 2D Brillouin zones with high symmetry points labeled; (g) ARPES map along ΓY^{[ 102]}.

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图 15 (a) 在HOPG衬底上形成的单层VSe₂; (b) HOPG上VSe₂的结构模型; (c) 在VSe₂岛上与衬底上测量得到的dI/dV 谱; (d), (e) 图(c)中标记的两个峰的高斯分布, 峰值位置分别为–0.28 V和0.23 V^{[ 107]}; (f) 一维图案的单层VSe₂的AFM图像、原子分辨STM图像、模拟STM图像与结构模型^{[ 108]}

Fig. 15. (a) Monolayer VSe₂ formed on HOPG substrate; (b) schematic of the fabrication process; (c) dI/dV spectra measured on the VSe₂ island and the substrate; (d), (e) Gaussian-fitting of the two peaks marked in (c), the peak positions are –0.28 V and 0.23 V, respectively^{[ 107]}; (f) AFM attractive-force image, atomic resolution STM image, simulated STM image, and structural model of 1D-patterned ML VSe₂ match each other^{[ 108]}.

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图 16 (a) 单层CuSe二维材料的大面积、高质量STM图像; (b) 两种取向相反的三角形孔洞和边界处平行四边形孔洞; (c) 单个三角形孔洞的高分辨图像; (d)和(e) CuSe表面Fe原子选择性吸附的STM图像^{[ 110]}

Fig. 16. (a) Large area and high quality STM image of single layer CuSe; (b) two kinds of triangle holes with opposite orientation and parallelogram holes at boundary; (c) a high resolution STM image of single triangle hole; (d) and (e) STM image of Fe atoms selective adsorption on CuSe surface^{[ 110]}.

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图 17 (a) 具有一维摩尔条纹结构单层CuSe的高分辨STM图像; (b) 自由单层CuSe的原子结构模型图; (c), (d) 单层CuSe的能带结构^{[ 113]}

Fig. 17. (a) High resolution STM image of monolayer CuSe with 1 D moiré pattern; (b) atomic structure model of free monolayer CuSe; (c), (d) band structure of monolayer CuSe^{[ 113]}.

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图 18 (a) Ag(111)衬底上大面积单层AgTe的STM图像; (b) Ag(111)衬底上单层AgTe的LEED图; 具有较高Te覆盖的(c)大面积STM图像和(d)原子分辨的STM图像, 显示了AgTe的六角形图案结构^{[ 116]}

Fig. 18. (a) STM image of large-scale AgTe monolayer on Ag(111) substrate; (b) LEED pattern of monolayer AgTe on Ag(111); (c) large-scale and (d) atomic resolution STM images of the AgTe on Ag(111) with higher Te coverage, showing the patterned hexagonal structure of AgTe^{[ 116]}.

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图 19 (a) Au(111)衬底上二维TiTe₂层的STM图像; (b) 模拟STM图像, 显示了$ \left( {\sqrt 3 \times 5} \right)$ (红色矩形)和$ \left( {\sqrt 3 \times \sqrt 7 } \right)$(黑色平行四边形)超结构^[120]; (c) 以石墨烯为中间层, 基于SiC(0001)衬底的PdSe₂岛的STM图像^{[ 122]}; (d) Bi₂Te₃薄膜的STM图(500 nm × 500 nm); (e) 拓扑绝缘体Bi₂Te₃的结构模型^{[ 127]}

Fig. 19. (a) STM image of 2D TiTe₂ layer on Au(111) substrate; (b) simulated STM image, showing both $ \left( {\sqrt 3 \times 5} \right)$ and $ \left( {\sqrt 3 \times \sqrt 7 } \right)$ (black parallelogram) superstructures^[120]; (c) STM image of PdSe₂ islands on graphene on SiC(0001)^{[ 122]}; (d) STM image (500 nm × 500 nm) of Bi₂Te₃ thin film; (e) structure model of the Bi₂Te₃ topological insulator^{[ 127]}.

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表 1 分子束外延方法制备的单元素二维材料的生长衬底、表征方法、平面构型、物理性能和潜在应用的总结

Table 1. Summary of growth substrate, characterization methods, configurations, physical properties, and potential appli-cations of monatomic two-dimensional materials grown by MBE.

单层二维原子晶体材料	生长衬底	表征方法	平面构型	物理性能和潜在应用	文献
硅烯	Ir(111)	STM, LEED	翘曲	自由状态下能隙为1.55 meV;	[ 24]
	Ag(111)	STM	翘曲	Ag(111)上硅烯载流子迁移率为100 cm²·V^–1·s^–1;	[ 25, 128 -132]
	Ag(110)	STM	翘曲	Ag(111)上硅烯载流子迁移率为100 cm²·V^–1·s^–1;	[ 131]
	Ru(0001)	STM, LEED	翘曲	量子自旋霍尔效应; 场效应晶体管;	[ 132]
	ZrB₂	STM, ARUPS	翘曲	谷电子学器件;	[ 133]
	Pb(111)	STM	翘曲	铁磁性	[ 134]
锗烯	Pt(111)	STM, LEED	翘曲	载流子迁移率高达 6.54 × 10⁵ cm²·V^–1·s^–1;	[ 26]
	Au(111)	STM, LEED	翘曲	能隙23.9 meV;	[ 135]
	Al(111)	STM, LEED, XPD	翘曲	量子自旋霍尔效应;	[ 136]
	Ag(111)	STM, LEED, ARPES	翘曲	高温超导体; 自旋极化电输运;	[ 137]
	Cu(111)	STM	平坦	负热膨胀系数; 热电材料	[ 138]
锡烯	Bi₂Te₃	STM, RHEED, ARPES	翘曲	热导率11.6 W·m^–1·K^–1; 巨磁阻效应;	[ 32]
	Cu(111)	STM, ARPES	平坦	自旋轨道耦合诱导带隙约0.3 eV;	[ 33]
	Sb(111)	STM	翘曲	拓扑超导体; 近室温量子霍尔效应	[ 139]
硼烯	Ag(111)	STM, XPS	翘曲	超导温度: 10—24 K; 超高储氢能力; 杨氏模量可达398 GPa·nm	[ 41, 140]
铪烯	Ir(111)	STM, LEED	平坦	强自旋轨道耦合作用; 磁矩为1.46 μ_B	[ 43]
磷烯	Au(111)	STM, XPS	翘曲	能隙2.0 eV; 光探测器; 太阳能电池;	[ 45, 47]
	Cu_xO	STM, XPS	平坦	电子迁移率高达1000 cm²·V^–1·s^–1.	[ 141]
锑烯	PdTe₂	STM, LEED, XPS	翘曲	能隙可达2.28 eV; 光电子器件;	[ 53]
	Cu(111)	STM, LEED, XPS	翘曲	拓扑绝缘体; 金属氧化物半导体场效应晶体管	[ 54]
铋烯	SiC	STM, ARPES	平坦	热电材料, 热电优值高达2.4	[ 61]

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表 2 分子束外延方法制备的双元素二维材料的生长衬底、表征方法、平面构型、物理性能和潜在应用的总结

Table 2. Summary of growth substrate, characterization methods, configurations, physical properties and potential applications of binary two-dimensional materials grown by MBE.

单层二维原子晶体材料	生长衬底	表征方法	平面构型	物理性能和潜在应用	文献
六方氮化硼	Ir(111)	STM, LEED, XPS	平面蜂窝状结构	能隙为6 eV的绝缘体;	[ 67]
	Ni(111)	STM, XPD		高功率电子学器件; 低摩擦材料;	[ 68]
	Rh(111)	STM, LEED		高功率电子学器件; 低摩擦材料;	[ 69, 142]
	Cu(111)	STM, LEED, AFM		场效应晶体管的介电层; 深紫外探测器件; 抗氧化涂层	[ 70, 143]
二硫化钼	Au(111)	STM, XPS	2H	载流子迁移率可达200 cm²·V^–1·s^–1; 电流开/ 关比为1 × 10⁸; 能隙1.8 eV	[ 75, 144]
	SrTiO₃	STM, SEM, Raman PL	2H	载流子迁移率可达200 cm²·V^–1·s^–1; 电流开/ 关比为1 × 10⁸; 能隙1.8 eV	[ 145]
二硒化钼	Au(111)	STM, LEED, ARPES	2H	直接带隙约1.5 eV; 激子束缚能0.55 eV, 光电子学器件	[ 82, 83]
	双层石墨烯	STM, LEED, Raman	2H	直接带隙约1.5 eV; 激子束缚能0.55 eV, 光电子学器件	[ 80]
二硒化铂	Pt(111)	STM, LEED, XPS, ARPES	1T	能隙2 eV; 螺旋状自旋结构; 自旋动量锁定; 自旋电子学器件; 气体传感器	[ 88]
		STM, LEED, XPS, ARPES		能隙2 eV; 螺旋状自旋结构; 自旋动量锁定; 自旋电子学器件; 气体传感器	[ 146, 147]
二硒化镍	Ni(111)	STM, LEED, XPS	1T	NiSe₂/Li电池可逆放电容量为351.4 mA·h·g^–1	[ 91, 93]
二硒化钨	石墨烯	STM, RHEED, ARPES	2H + 1T'	双激子态; 谷霍尔效应; 谷赝自旋	[ 102]
二硒化钒	HOPG	STM, AFM, XPS	1T	室温下二维铁磁性; 超高导电性、电荷密度波	[ 107, 108]
硒化铜	Cu(111)	STM, LEED, STEM	平面蜂窝状结构一维摩尔条纹结构	周期孔洞结构用于选择性吸附;	[ 110]
	Cu(111)	STM, LEED, ARPES	平面蜂窝状结构一维摩尔条纹结构	节线型狄拉克费米子能带结构; 拓扑非平庸的量子自旋霍尔态	[ 113]
碲化银	Ag(111)	STM, LEED	平面蜂窝状结构	节线型狄拉克费米子能带结构; 拓扑非平庸的量子自旋霍尔态	[ 116, 117]

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超高真空条件下分子束外延生长的单层二维原子晶体材料的研究进展