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利用飞秒激光脉冲激发铁磁/非磁异质结构有望实现高效太赫兹辐射, 从而打破制约太赫兹技术快速发展的瓶颈. 拓扑绝缘体是一种新型二维材料, 其自旋霍尔角远大于重金属材料, 可以与铁磁层结合构成自旋太赫兹发射器. 为了研究拓扑绝缘体/非磁异质结中的太赫兹产生和调控机理, 本综述从飞秒激光激发的超快光电流响应入手, 结合拓扑绝缘体的晶体结构与电子结构, 分析了拓扑绝缘体薄膜中的太赫兹发射机理, 揭示了不同非线性效应产生的超快光电流随外界条件的依赖关系, 证实了使用多种手段调控拓扑绝缘体出射非线性太赫兹辐射的可能性; 以铁磁/重金属异质结为例, 探究了自旋太赫兹发射器的优势与调控方法. 结合这两种发射机理, 通过非线性太赫兹与自旋太赫兹的合成作用, 可以实现在拓扑绝缘体/铁磁异质结中偏振可调谐的太赫兹发射.Ferromagnet/nonmagnet (FM/NM) heterostructure under the excitation of femtosecond laser has proved to be a potential candidate for high-efficiency terahertz (THz) emission. Topological insulator (TI) is a novel two-dimensional (2D) material with a strong spin-orbital coupling, which endows this material with an extremely large spin-Hall angle. Thus, TI appears to be an attractive alternative to achieving higher-performance spintronic THz emitter when integrated with ferromagnetic material. In this paper, we discuss the ultrafast photocurrent response mechanism in TI film on the basis of the analysis of its crystal and band structures. The discussion of the mechanism reveals a relationship between THz radiation and external conditions, such as crystal orientation, polarized direction and chirality of the laser. Furthermore, we review the spintronic THz emission and manipulation in FM/NM heterostructure. The disclosed relationship between THz radiation and magnetization directions enables an effective control of the THz polarization by optimizing the system, such as by applying twisted magnetic field or fabricating cascade emitters. After integration, the FM/TI heterostructure presents a high efficiency and easy operation in THz radiation. This high-performance topological spintronic THz emitter presents a potential for the achievement of arbitrary polarization-shaping terahertz radiation.
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图 1 Bi2Se3的晶体结构 (a) 三维晶体结构,
$ {{t}}_{{1, 2}, 3} $ 代表晶胞的基矢, 红色框标注的是Bi2Se3的QL层; (b) Bi2Se3的布里渊区; (c) 在xy平面内, 三角形的晶格结构有A, B, C三种可能的结构[38]Fig. 1. The crystal structure of Bi2Se3: (a) 3D schematic of the structure, where
$ {{t}}_{{1, 2}, 3} $ present the primitive lattice vector; (b) Brillioun zone of Bi2Se3; (c) the xy-plane triangle lattice has three possible positions A, B and C[38].图 3 线偏振激光激发下拓扑绝缘体中的超快光电流效应 (a) 分离出的非线性效应产生的太赫兹电场随方位角的变化; (b) 不同效应产生的太赫兹分量在合成太赫兹辐射中的占比[49]
Fig. 3. Separation of the photo-currents in topological insulator excited by linear femtosecond laser pulse: (a) The derived terahertz signals due to nonlinear currents as a function of azimuthal angle; (b) the extracted terahertz electric field generated by different effects[49].
图 4 (a), (b) 样品方位角
$ \phi =30^ \circ $ , 在左旋和右旋圆极化光激发下, 时域和频域下Bi2Se3产生的太赫兹信号; (c) 太赫兹幅值随激光偏振态的变化关系, 其中蓝色曲线代表时域信号, 黄色曲线代表频域信号[48]Fig. 4. (a), (b) THz signals emitted from Bi2Se3 in time and frequency domains under illumination of left- and right- handed circularly polarized light where the azimuth
$ \phi =30^ \circ $ ; (c) THz-wave amplitudes as a function of the polarity of pump laser in time (blue curves) and frequency domains (yellow curves)[48].图 5 (a) Seifert等[74]使用的YIG/Pt异质结构; (b) 在YIG/Pt中插入1.9 nm的铜, 由于自旋注入被阻隔, 太赫兹信号减弱[74]; (c) Wu等[82]使用的W/Co异质结构; (d) W/Co异质结构的太赫兹发射强度接近于500 μm的ZnTe晶体[82]
Fig. 5. (a) The YIG/Pt heterostructure used by Seifert. et al.[74]; (b) after 1.9 nm Cu insertion, the THz field intensity deteriorates because the spin injection is impaired[74]; (c) the Co/W heterostructure used by Wu et al.[82]; (d) the THz waves emitted from Co/W have a peak intensity exceeding that of ZnTe crystals[82].
图 6 (a) 在异质结上施加手性相反的螺旋外磁场可以改变出射太赫兹波的手性; (b) 图(a)的利萨如曲线, 其中
$ {\sigma }^{+} $ 与$ {\sigma }^{-} $ 分别代表左旋与右旋极化的太赫兹信号[85]; (c), (d) Chen等[22]设计的级联太赫兹发射器, 两级发射器铁磁层的磁化方向与入射光方向两两正交, 通过控制出射太赫兹的相位差和振幅, 可以在时域获得合成的圆偏振信号; (e), (f) Wang等[21]使用的双抽运自旋太赫兹发射器, 通过改变脉冲时延可以调控出射太赫兹的时域信号Fig. 6. (a) Manipulation of the terahertz chirality by changing the twisted magnetic field distribution; (b) the Lissajous curves of the THz signals of (a), where
$ {\sigma }^{+} $ and$ {\sigma }^{-} $ present the signals with left-hand and right-hand polarity[85]; (c), (d) the cascade spintronic terahertz emitter designed by Chen et al.[22], a circularly polarized terahertz waves could be obtained by controlling the phase difference between two stage terahertz and their amplitude; (e), (f) dual-pulses induced terahertz emitter reported by Wang et al.[21], the frequency could be manipulated by changing the delay time between two pump laser pulses.图 8 (a) Bi2Se3/Co异质结构示意图; (b) 用飞秒激光分别激发Bi2Se3/Co, Co, Bi2Se3产生的太赫兹信号; (c) 改变入射方向与面内磁场方向后, 异质结发射的太赫兹极性反转[68]
Fig. 8. (a) The schematic diagram of the Bi2Se3/Co heterostructure; (b) THz waveforms generated from Bi2Se3/Co, Co and Bi2Se3; (c) THz waveforms emitted from the heterostructure measured with front and back sample excitation and reversed magnetic field[68].
图 9 (a) Pan等人制备的顶电极器件, 其中Al2O3作为介电层, ITO作为电极材料; (b) (BixSb1–x)2Se3薄膜的光电流与纵向电阻随电压的变化情况[98]
Fig. 9. (a) The Schematic diagram of the top-gate device prepared by Pan et al, where the Al2O3 is dielectric layer while the ITO serves as top gate material; (b) the gate-dependent longitudinal resistance and nonlinear current in (BixSb1–x)2Se3 film[98].
表 1 拓扑绝缘体中的超快光电流与晶体取向ϕ, 入射角θ, 激光偏振态的依赖关系[56]
Table 1. The details of the dependences of CPGE, LPGE, PDE, and OR on
$ \phi $ ,$ \theta $ , and$ \alpha $ [56].非线性效应 晶体方向$ \phi $ 入射角($ \theta \to -\theta $) 1/4波片转角$ \alpha $ CPGE 来源于表面态 极性反转 2$ \alpha $-周期 与$ \phi $无关 $ \mathrm{s}\mathrm{i}\mathrm{n}\left(2\alpha \right) $ LPGE 来源于表面态 极性反转 4$ \alpha $-周期 $ \phi $依赖 $ \mathrm{s}\mathrm{i}\mathrm{n}\left(4\alpha \right) $ PDE $ \phi $依赖 极性反转 4$ \alpha $-周期 $\cos4\alpha$ OR $ \phi $依赖 极性不反转 4$ \alpha $-周期 $ \mathrm{c}\mathrm{o}\mathrm{s}\left(4\alpha \right) $ 表 2 拓扑绝缘体与几种重金属材料的自旋霍尔角[35]
Table 2. Spin Hall angles of several topological insulators and common heavy metals[35]
Material $ {\theta }_{\mathrm{S}\mathrm{H}} $ Ta 0.15 W 0.40 Pt 0.08 Bi2Se3 2.00—3.50 BixSe1–x 18.80 BixSb1–x 52.00 -
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