二维过渡金属硫化物二次谐波: 材料表征、信号调控及增强

曾周晓松; 王笑; 潘安练

doi:10.7498/aps.69.20200452

摘要

二维过渡金属硫化物(transition metal dichalcogenides, TMDCs)由于可实现从间接带隙到直接带隙半导体的转变, 能带宽度涵盖可见光到红外波段, 及二维限域所带来的优异光电特性, 在集成光子以及光电器件领域受到了广泛的关注. 最近随着二维材料基础非线性光学研究的深入, 二维TMDCs也展现出了在非线性光学器件应用上的巨大潜能. 本综述聚焦于二维层状TMDCs中关于二次谐波的研究工作. 首先简述一些基本的非线性光学定则, 然后讨论二维TMDCs中原子层数、偏振、激子共振、能谷等相关的二次谐波特性. 之后将回顾这些材料二次谐波信号的调制及增强工作, 讨论外加电场、应变、表面等离激元结构、纳米微腔等方法和手段的影响机理. 最后进行总结和对未来本领域工作的展望. 理解二维TMDCs二次谐波的产生机制及材料自身结构与外场调控机理, 将对未来超薄的二维非线性光学器件的发展产生深远的意义.

关键词:

Abstract

Two-dimensionl (2D) layered transition metal dichalcogenides (TMDCs) have received great attention in integrated on-chip photonic and photoelectric applications due to their unique physical properties including indirect-to-direct optical bandgap transition, broad bandgap from visible band to near-infrared band, as well as their excellent optoelectric properties derived from the 2D confinement. Recently, with the in-depth study of their fundament nonlinear optical properties, these 2D layered TMDCs have displayed significant potential applications in nonlinear optical devices. In this review, we focus on recent research progress of second harmonic generation (SHG) studies of TMDCs. Firstly, we briefly introduce the basic theory of nonlinear optics (mainly about SHG). Secondly, the several intrinsic SHG relative properties in TMDCs including layer dependence, polarization dependence, exciton resonance effect, valley selection rule are discussed. Thirdly, the latest SHG modulation and enhancement studies are presented, where the electric field, strain, plasmonic structure and micro-cavity enhancement are covered. Finally, we will summarize and give a perspective of possible research direction in the future. We believe that a more in-depth understanding of the SHG process in 2D layered TMDCs as well as the material structure and modulation effects paves the way for further developing the ultra-thin, multifunctional 2D nonlinear optical devices.

Keywords:

作者及机构信息

1.
湖南大学物理与微电子科学学院, 微纳结构物理与应用技术湖南省重点实验室, 长沙　410082

2.
湖南大学材料科学与工程学院, 化学生物传感与计量学国家重点实验室, 微纳结构物理与应用技术湖南省重点实验室, 长沙　410082

通信作者: 王笑, xiao_wang@hnu.edu.cn ; 潘安练, anlian.pan@hnu.edu.cn

基金项目: 国家自然科学基金(批准号: 51525202, U19A2090, 91850116, 51772084)和湖南省自然科学基金(批准号: 2018RS3051)资助的课题

Authors and contacts

1.
Key Laboratory for Micro-Nano Physics and Technology of Hunan Province, School of Physics and Electronic Science, Hunan University, Changsha 410082, China

2.
Key Laboratory for Micro-Nano Physics and Technology of Hunan Province, State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Materials Science and Engineering, Hunan University, Changsha 410082, China

Corresponding author: Wang Xiao, xiao_wang@hnu.edu.cn ; Pan An-Lian, anlian.pan@hnu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51525202, U19A2090, 91850116, 51772084) and the Hunan Provincial Natural Science Foundation of China (Grant No. 2018RS3051)

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施引文献

图 1 (a) MoS₂原子排列的侧视图(左)和俯视图(右), 其中俯视图中对应扶手椅和Z字形两个晶体取向; (b) 机械剥离方法得到的不同层数MoS₂的光学照片^[16]; (c) 2H相MoS₂二次谐波信号随层数增加呈振荡减小的趋势^[16]; (d)人工折叠的两层MoS₂(左)以及对应的二次谐波成像(右)^[31]; (e) 3R相MoS₂晶体结构及倍频偶极排列^[32]; (f) 3R相MoS₂二次谐波呈平方递增的趋势^[32]

Fig. 1. (a) Side view (left) and top view (right) of MoS₂ atomic structure. The highlighted armchair direction and zigzag direction correspond to the top view. (b) Mechanical exfoliated MoS₂ with different layers^[16]. (c) 2H phase MoS₂ layers show diminishing the oscillation in SHG signal^[16]. (d) Optical image of artificial folded MoS₂(left) and its corresponding SHG image(right)^[31]. (e) Crystal structure of 3R phase MoS₂ and corresponding SH dipole^[32]. (f) 3R phase MoS₂ layers show quadratic enhanced SHG with the increase of layers^[32].

下载: 全尺寸图片幻灯片

图 2 产生高效二次谐波的二维材料　(a)螺旋WS₂的光学照片及图中虚线正方形区域内放大的螺旋WS₂样品中心AFM图片^[39]; (b)螺旋WS₂的二次谐波强度随层数递增^[39]; (c) 金字塔结构的WS₂纳米片结构示意图^[41]; (d)金字塔形的WS₂纳米片边缘形成高效二次谐波^[41]

Fig. 2. CVD grown TMDCs with highly efficient SHG: (a) Optical image (left) and zoom in AFM image (right) of spiral WS₂ flake^[39]; (b) layer dependent SHG of spiral WS₂ flake^[39]; (c) schematic illustration of pyramid-like WS₂ structure^[41]; (d) pyramid-like WS₂ displays high intensity of residual edge SHG signal^[41].

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图 3 二次谐波的偏振特性　(a) 单层MoS₂的二次谐波偏振极化图^[16]; (b)单层MoS₂晶体取向俯视图, 其中x方向代表扶手椅方向, y方向代表Z字形方向, θ角是激发光入射方向与扶手椅方向的夹角^[16]; (c) WS₂/MoS₂横向外延异质结^[44]以及(d) WSe₂/WS₂ AA和AB堆垛结构纵向外延异质结^[45]的二次谐波偏振极化图, 其中插图是异质结的二次谐波成像; (e) 人工堆垛两种二维材料使二次谐波极化方向产生叠加^[46]; (f)—(h)利用二次谐波偏振区分单层MoS₂中不同晶界与畴界^[47]

Fig. 3. Polarization properties of SHG in TMDCs: (a) SHG polarization in monolayer MoS₂ shows six fold rotation symmetry^[16]; (b) top view of MoS₂ crystallographic orientation, where x represents armchair direction, y represents zigzag direction and θ is the angle between input laser and armchair direction ^[16]; SHG polarization in (c) WS₂/MoS₂ laterally epitaxial heterostructure^[44] and (d) WSe₂/WS₂ AA, AB vertical heterostructure^[45], where the insets shows correspongding SHG mapping; (e) superposition of SHG polarization by artificial stacks of two different 2D materials^[46]; (f)−(h) demonstration of distinguishing of different grain boundary in monolayer MoS₂ thin film be SHG polarization^[47].

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图 4 二次谐波的激子共振特性　(a) 原理图解释两个入射光子共振A激子的2p态产生二次谐波^[50]; (b) 4 K下单层WSe₂波长依赖的二次谐波信号^[50]; (c) 单层(深蓝)与三层(绿) MoS₂二阶非线性极化率与吸收光谱作为激发光波长的函数^[16]; (d), (e) 对比螺旋WS₂二次谐波激子共振与吸收光谱说明二次谐波增强在稍高于带隙能量处^[51]; (f) 对比单层硒硫化钼合金二次谐波(散点)与荧光光谱(实线)^[52]; (g), (h) 气象生长单层MoS₂边缘增强效应^[47]

Fig. 4. Exciton resonance properties of SHG in TMDCs: (a) Schematic illustration of SHG when two incident photons are resonant with 2p state of A exciton^[50]; (b) excitation wavelength dependent SHG of monolayer WSe₂ at T = 4 K^[50]; (c) second order nonlinear susceptibility and absorption served as the function of pump laser energy in monolayer (blue) and trilayer (green) MoS₂^[16]; (d), (e) illustration of SHG enhancement in spiral WS₂ flake when the excitation energy slightly above bandgap by comparison of reflective spectrum with SHG spectrum^[51]; (f) SHG spectra (dotted traces) of monolayer alloys and corresponding room-temperature PL spectra (solid traces)^[52]; (g), (h) CVD grown monolayer MoS₂ flakes show edge enhanced SHG^[47].

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图 5 二次谐波的能谷选择特性　(a)单层的WSe₂展现出与激发光相反的圆偏振二次谐波^[59]; (b)二维材料二次谐波能谷光学选择定则^[59]

Fig. 5. SHG valley selection rules: (a) Circular polarization-resolved SHG spectra showing the generation of counter-circular SHG in monolayer WSe₂^[59]; (b) interband valley optical selection rules for SHG in 2D TMDCs^[59].

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图 6 电调控二次谐波　(a) 双层MoS₂微电容器件原理图^[67]; (b) 双层MoS₂的二次谐波作为施加电压以及发射波长的函数^[67]; (c) 双层WSe₂中背栅调控可逆的二次谐波^[66]; (d) 单层WSe₂晶体管的光学图片^[59]; (e) 单层WSe₂二次谐波在共振激发下随选定栅压的变化^[59]; (f) 单层WSe₂二次谐波作为栅压和激发能量函数的强度图^[59]

Fig. 6. Electric field modulated SHG: (a) Schematic illustration of bilayer MoS₂ microcapacitor device^[67]; (b) bilayer MoS₂ SHG intensity as the function of applied voltage and SHG emission energy^[67]; (c) reversible SHG induced by back gate in bilayer WSe₂^[66]; (d) optical image of monolayer WSe₂ transistor^[59]; (e) exciton resonant monolayer WSe₂ SHG spectra at selected gate voltage^[59]; (f) monolayer WSe₂ SHG intensity as the function of applied gate voltage and SHG emission energy^[59].

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图 7 应变调控二次谐波　(a)轴向拉升应变导致MoSe₂二次谐波偏振变化^[26]; (b)通过二次谐波表征MoS₂的全应变场^[75]; (c) TiO₂/MoS₂异质结结区处应变提高MoS₂二次谐波^[77]

Fig. 7. Strain modulated SHG: (a) MoSe₂ SHG polarization changed by uniaxial tensile strain^[26]; (b) uniaxial strain map of MoS₂ monolayer flake^[75]; (c) schematic illustration (up) and SHG mapping (down) of TiO₂/MoS₂ structure^[77].

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图 8 超表面调控二次谐波　(a)控制纳米天线相位梯度导向二次谐波出射方向^[81]; (b) 相位δ_x = δ_y = 0时MoS₂二次谐波出射在0°^[81]; (c) 周期性的矩形金小孔构成的超表面结构^[82]; (d)超表面/WS₂构成的超透镜对二次谐波在传播方向上形成聚焦效果^[82]; (e)金超表面导向二阶谷光子的原理图^[79]; (f)实际的二阶光场变化, 0和1代表强度等级^[79]

Fig. 8. Metasurfaces modulated SHG: (a) Schematic illustration of a MoS₂-gold phased array antenna steering SHG emission^[81]; (b) polar plot of the calculated (line) and measured (points) SH pattern along the intensity maximum when phase delay δ_x = δ_y = 0^[81]; (c) the SEM image of the fabricated gold metasurface with rectangular nanoholes of different orientation^[82]; (d) the experimental results of SHG focusing by using the hybrid metasurfaces^[82]; (e) schematic representations of steering second-harmonic waves on RCP pumping with monolayer WS₂^[79]; (f) evolution of the light field for the case shown in (c), “0” and “1” label the intensity order^[79].

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图 9 表面等离激元提高二维材料二次谐波　(a) NPoM模型中, 纳米腔对入射电场产生限域作用(上), 单个纳米银颗粒对WS₂二次谐波成像的增强(下)^[92]; (b)对比不同结构的表面等离激元阵列/半导体二次谐波, 其中123区域分别代表阵列, 两层WSe₂/阵列, 与两层WSe₂区域^[93]; (c) 银纳米栅表面等离激元结构增强WS₂二次谐波达400倍^[94]; (d) PDMS上表面等离激元阵列对WSe₂二次谐波增强三个量级^[95]

Fig. 9. SHG enhancement by plasmonics: (a) Nano cavity strongly confines incident light field (up), and SHG enhancement by Ag nanoparticle in monolayer WS₂ (down)^[92]; (b) compare of SHG signal in different plasmonic array/semiconductor, where points 1, 2, 3 represent the area of nanorod, nanorod/bilayer WSe₂, and bilayer WSe₂, respectively^[93]; (c) SHG enhancement factor over 400 in monolayer WS₂ reached by Ag nanogroove grating^[94]; (d) SHG enhancement over 3 orders in monolayer WSe₂ by plasmonic structure on PDMS^[95].

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图 10 微腔、光子晶体增强二维材料二次谐波　(a)双共振法帕纳米微腔增强二次谐波^[100]; (b)硅波导增强二硒化钼二次谐波^[105]; (c)连续激光激发硒化镓/硅光子晶体结构二次谐波^[106]

Fig. 10. SHG enhancement by micro cavity and photonic crystal: (a) Enhancement of SHG from monolayer MoS₂ in a doubly resonant on-chip optical cavity^[100]; (b) enhancement of SHG by silicon waveguide^[105]; (c) CW excitation of SHG from GaSe/photonic crystal^[106].

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