ReX2 (X=S, Se): 二维各向异性材料发展的新机遇

doi:10.15541/jim20180171

摘要/Abstract

摘要：

二维材料因其不同于体相的超薄原子结构、大的比表面积和量子限域效应等受到了人们的广泛关注。二维各向异性材料作为二维材料家族的一员, 其取向依赖的物理和化学性质, 使得对该类材料性能的选择性优化成为可能。过渡金属Re基硫属化合物作为各向异性材料的典型代表, 具有可调的可见光波段吸收带隙, 极弱的层间耦合作用力, 以及各向异性的光学、电学性能, 现已成为电子和光电子领域的研究热点之一。本文主要介绍了ReX₂(X=S, Se)的晶体结构和基本性质, 总结目前该材料体系主流的合成方法, 研究其各向异性物理特性及优化的手段和条件, 并对ReX₂的制备和发展进行了展望。

关键词: 各向异性, ReS₂, ReSe₂, 综述

Abstract:

Two dimensional (2D) materials have attracted wide attention due to their ultrathin atomic structure, large specific surface area and quantum confinement effect which are remarkably different from their bulk counterparts. Anisotropic materials are unique among reported 2D materials. Their orientation-dependent physical and chemical properties make it possible to selectively improve the performance of materials. As representative examples, Re-based transition metal dichalcogenides (Re-TMDs) have tunable bandgaps in visible spectrum, extremely weak interlayer coupling, and anisotropic properties in optics and electronics, which make them attractive in the application areas of electronics and optoelectronics. In this riviev, the unique crystal structures and intrinsic properties of the Re-based TMDs semiconductors are introduced firstly, and then the synthetic method is introduced, followed by discussion on the unique physical characterizations and optimized means. Finally, prospects and suggestions are put forward for the preparation and research of ReX₂.

Key words: anisotropy, ReS₂, ReSe₂, review

中图分类号:

TQ174

王人焱, 甘霖, 翟天佑. ReX₂ (X=S, Se): 二维各向异性材料发展的新机遇[J]. 无机材料学报, 2019, 34(1): 1-16.

WANG Ren-Yan, GAN Lin, ZHAI Tian-You. ReX₂ (X=S, Se): A New Opportunity for Development of Two-dimensional Anisotropic Materials[J]. Journal of Inorganic Materials, 2019, 34(1): 1-16.

图/表 11

图1 (a)ReS2单胞结构图[33]; (b)ReX2晶体结构顶视图; (c) ~(d)1T相结构轨道成键和能级示意图[39,40]; (e)ReSe2块体(上)和单层(下)带隙结构[50]; (f)1层、3层、5层的ReS2能带模拟图[51]

Fig. 1 (a) The model unitcell view of ReS2[33]; (b) Top view of the crystalline structure of distorted-1T phase of monolayer ReX2(Black balls represent Re atoms and yellow balls represent S or Se atoms); (c, d) Schematic images of 1T lattice symmetries and energy levels of d-orbital electrons induced by the crystal field[39,40]; (e) First-principles scalar relativistic projector augmented wave calculations of electronic band structures for bulk (top) and single-layer (down) ReSe2[50]; (f) Band structure of monolayer, trilayer and five-layer ReS2 by ab initio-calculations[51]

表1 ReS2和ReSe2单胞晶格参数[36,37]

Table 1 Original unit-cell lattice parameters of ReS2 and ReSe2[36,37]

Materials	a/nm	b/nm	c/nm	α/(°)	β/(°)	γ/(°)	V/nm³
ReS₂	0.6417	0.6510	0.6461	121.10	88.38	106.47	0.21930
ReSe₂	0.6603	0.6717	0.6718	91.87	104.93	118.95	0.24753

图2 (a)ReS2不同层数的PL光谱; (b)ReS2, MoS2, MoSe2, WS2和WSe2的PL强度和层数依赖关系[50]; (c)ReS2和(d) ReSe2单层到块体厚度的拉曼光谱[58]; (e)ReS2纳米卷自组装机制[59]; (f)单层ReS2纳米墙热弯曲示意图[60]

Fig. 2 PL spectra of ReS2 flakes with different number of layers; (b) Integrated PL intensity as a function of number of layers (normalized to that of monolayer) in ReS2, MoS2, MoSe2, WS2 and WSe2[50]; Raman spectra recorded on (c) N-layer ReS2 and (d) N-layer ReSe2 in the parallel polarization configuration[58]; (e) Schematic for the process of oriented self assembly of ReS2 nanoscrolls[59]; (f) Schematic for the TIB of a single ReS2 nanowall[60]

图3 (a)分离前ReS2纳米片SEM照片(左)和分离后TEM照片(右), 插图：剥离样品水溶液光学照片; (b)HRTEM照片[70]; (c)等密度梯度超速离心分离不同密度梯度ReS2纳米片示意图; (d)AFM照片; (e)ReS2拉曼光谱图[63]

Fig. 3 (a) SEM image of ReS2 powders and TEM image of as-exfoliated ReS2 nanosheets with inset showing photograph of a typical dark-brown exfoliated ReS2 suspension in water; (b) High-resolution STEM image of as-exfoliated ReS2 nanosheets[70]; (c) Schematics for different density gradient ultracentrifugation ReS2 nanosheets through iDGU; (d) Atomic force microscopy image of solution-processed ReS2 following deposition on a Si wafer; (e) Raman spectrum of ReS2 nanosheets[63]

图4 (a)PVD制备ReS2薄膜示意图; (b)ReS2薄膜Raman光谱图; (c)光学照片, 插图：AFM照片和TEM照片[88]; (d)蓝宝石衬底和ReS2薄膜光学照片; (e)SiO2/Si衬底CVD生长ReS2纳米片光学照片[74]

Fig. 4 (a) Schematic diagram of synthesized ReS2 film by PVD; (b) Raman spectrum of ReS2 film ; (c) Optical photograph of grown ReS2 film on the SiO2/Si substrate with inset showing the AFM and TEM images[88]; (d) A picture of bare and as-grown ReS2 bilayer film on sapphire wafer by CVD; (e) Optical microscope image of the ReS2 hexagons[74]

图5 (a)Te辅助CVD合成ReS2示意图; (b)转移至SiO2/Si衬底ReS2光学照片, 插图为AFM照片[77]; (c)夹层限域生长ReSe2表面反应机制示意图; (d)A、B面的ReSe2形貌光学照片[89]

Fig. 5 (a) Schematic for the tellurium-assisted CVD growth approach; (b) Optical image of ReS2 after transferred onto SiO2/Si (300 nm) substrate with inset showing AFM image of ReS2 on mica substrate[77]; (c) Schematic of the CVD growth of ReSe2 in the confined reaction space and the surface reaction during the epitaxial growth of the ReSe2 atomic layer on mica; (d) Optical image of ReSe2 in A and B face[89]

图6 (a)泵浦探测少层ReS2纳米片实验示意图, 插图：剥离ReS2光学照片; (b)角度依赖的少层ReS2纳米片光吸收谱; (c)X1, X2激子角度依赖的光吸收极化图[122]; (d)ReS2 Raman光谱[128]和低频Raman光谱[131]; (e)ReS2 不同旋转角度的Raman光谱; (f)少层ReS2纳米片高分辨TEM照片和对应偏振Raman极化图[130]

Fig. 6 (a) A schematic illustrating the pump-probe experiment of few-layer ReS2 with inset showing optical image of few-layer ReS2; (b) Polarization-dependent absorption spectra of few-layer ReS2; (c) Corresponding spectral weights of Lorentzian contributions of X1 (blue dots) and X2(red dots). Yellow line represents the b-axis[122]; (d) Raman spectrum for bulk ReS2[128] and Low-frequency Raman spectroscopy of few layer ReS2[131]; (e) Unpolarized Raman spectra as a function of sample orientation angle; (f) High-magnification ADF-STEM image and corresponded polarization-and orientation-resolved Raman spectra[130]

表2 633 nm激光激发块体和单层ReS2的18种Raman振动光谱[35]

Table 2 The 18 Raman active frequencies in bulk and monolayer ReS2 under 633 nm solid state laser excitation[35]

Symmetry	Bulk/cm^-1	Monolayer/cm^-1	Origin of phonon mode
Ag	140.3	139.2	Out-of-plane vibrations of Re atoms
Ag	145.9	145.3	Out-of-plane vibrations of Re atoms
Eg	153.1	153.6	In-plane vibrations of Re atoms
Eg	163.6	163.6	In-plane vibrations of Re atoms
Eg	217.2	217.7	In-plane vibrations of Re atoms
Eg	237.1	237.7	In-plane vibrations of Re atoms
Cp	278.3	278.3	In- and out-of-plane vibration of Re and S atoms
Cp	284.2	284.7	In- and out-of-plane vibration of Re and S atoms
Eg	307.8	307.8	In-plane vibrations of S atoms
Eg	311.0	311.0	In-plane vibrations of S atoms
Cp	320.6	320.6	In- and out-of-plane vibration of S atoms
Cp	324.9	324.9	In- and out-of-plane vibration of S atoms
Cp	348.8	348.8	In- and out-of-plane vibration of S atoms
Cp	368.9	369.5	In- and out-of-plane vibration of S atoms
Cp	377.9	377.4	In- and out-of-plane vibration of S atoms
Cp	407.3	408.3	In- and out-of-plane vibration of S atoms
Ag	418.7	419.3	Out-of-plane vibrations of S atoms
Ag	438.0	437.5	Out-of-plane vibrations of S atoms

图7 (a)ReS2晶体管光学照片; (b)对应(a)图ReS2的TEM照片; (c)不同电极的I-V曲线; (d)不同电极之间的ReS2转移特性曲线[137]; (e)各向异性ReS2晶体管转移特性曲线, 插图为器件光学照片和R-Vbg曲线; (f)角度依赖的FET迁移率极化图, 插图：器件光学照片[51]; (g)ReS1.23Se0.77合金各向异性转移特性曲线, 插图为器件光学照片[76]

Fig. 7 (a) Optical microscope image of ReS2 four probe transistor; (b) The magnified ADF images taken from the sample in (a); (c) The direction-dependent I-V characteristics with inset showing nonlinear I-V behavior indicate the Schottky Au/ReS2 contacts; (d) The direction-dependent transfer characteristics[137]; (e) Transfer curves of anisotropic ReS2 FETs along two sides with top inset showing optical image of the devices (Scale bar, 10 μm) and low inset showing the 4-probe resistance of the same devices. (f) Normalized field-effect mobility of a six-layer device with inset showing the optical image of the device[51]; (g) Angle-dependent transfer curves of ReS1.23Se0.77 alloy device with inset showing optical image of ReS2 device[76]

图8 (a)角度依赖的ReS2极化光电流图; (b)极化光电流曲线[112]; (c)偏振光I-t曲线; (d)偏振光电流极化图[76]; (e)ReSe2偏振光电器件示意图; (f)器件SEM照片和不同角度的入射光电流分布图[15]

Fig. 8 (a) The photocurrent of ReS2 change as a function of drain bias under different polarization light illuminations; (b) The change of the photocurrent under different drain biases plotted as a function of polarization angle[112]; (c) Photocurrent response of ReS1.06Se0.94 alloy device under light on and off irradiation, and under light with different polarization direction; (d) Polar plots for the photocurrent with respect to the polarization angle of the incident light[76]; (e) Schematic structure of ReSe2 photodetectors; (f) The SEM image and polarization-dependent photocurrent mapping of the device[15]

图9 (a)剥离层状ReS2光学照片; (b)面外热传导曲线; (c)极化方向的热传导曲线; (d)面内热传导分布图; (e)不同厚度的面内极化热导率[151]

Fig. 9 (a) Optical microscopy image of an exfoliated ReS2 ?ake; (b) Through-plane TDTR data at two modulation frequencies; (c) In-plane TDTR data at f = 1.1 MHz and time delay of -50 ps. The dashed lines are the intensity profile of the laser beam; (d) 2D beam-offset scan of the TDTR signal; (e) In-plane thermal conductivity of exfoliated ReS2 ?akes as a function of thickness[151]

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ReX₂ (X=S, Se): 二维各向异性材料发展的新机遇

ReX₂ (X=S, Se): A New Opportunity for Development of Two-dimensional Anisotropic Materials

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