Ultrafast Plasmon Thermalization in Epitaxial Graphene Probed by Time-Resolved THz Spectroscopy

The control of carrier transport by electrical, chemical, or optical Fermi level tuning is central to graphene electronics. Here, an optical pump—terahertz (THz) probe spectroscopy—is applied to investigate ultrafast sheet conductivity dynamics in various epitaxially grown graphene layers representing a large variety of carbon allotropes, including H₂ intercalated films. The graphene layers display a prominent plasmonic response connected with induced THz transparency spectra on ultrashort timescale. It is generally believed that the plasmonic excitations appear due to wrinkles, and substrate terraces that bring about natural confinement potentials. It is shown that these potentials act within micrometer-sized domains with essentially isotropic character. The measured ultrafast dynamics are entirely controlled by the quasi-Fermi level of laser-excited carriers through their temperature. The photocarriers undergo a disorder-enabled super-collision cooling process with an initial picosecond transfer of the optically deposited heat to the lattice followed by a sub-nanosecond relaxation governed by the lattice cooling. The transient spectra is described by a two-temperature Drude-Lorentz model revealing the ultrafast evolution of the carrier temperature and chemical potential and providing crucial material parameters such as Fermi energy, carrier mobility, carrier confinement length, and disorder mean free path.     

飞秒激光泵浦剥离层石墨烯实现太赫兹波放大的研究

基于光激发石墨烯的瞬态电子-空穴的弛豫/复合过程中,在Dirac点附近形成粒子数反转并产生THz波段负动态电导率的机理,研究剥离层石墨烯在室温条件下实现THz波段电磁波的受激放大。理论推导了剥离层石墨烯动态电导率的表达式,并研究了动态电导率随信号波长、石墨烯层数和泵浦光强度的变化关系,对单层和多层石墨烯结构作了分析比较。分析了与动态电导率有关的增益并进行了数值计算与模拟。研究表明,在室温条件下,剥离层石墨烯可以实现THz波段电磁波的有效放大。     

光抽运石墨烯太赫兹负动态电导率的理论研究

石墨烯特殊的零带隙能带结构和载流子弛豫特性,在研究太赫兹辐射源相干放大领域引起广泛关注。考虑带内和带间跃迁对电导率的贡献,研究了光抽运单层和多层石墨烯中非平衡二维电子-空穴系统的动态电导率特性。结果表明,在足够强的光抽运下,石墨烯中的粒子数反转能够使得动态电导率的实部在太赫兹频段内出现负值,这使基于石墨烯的太赫兹放大或受激辐射源成为可能。同时,通过研究动量弛豫时间、温度、层数、光强对石墨烯的负动态电导率的影响表明,石墨烯多层结构的动态电导率最小值的绝对值更大,作为太赫兹激光器的激活介质更具优势。     

Observation of Amplified Stimulated Terahertz Emission from Optically Pumped Heteroepitaxial Graphene-on-Silicon Materials

We experimentally observed the fast relaxation and relatively slow recombination dynamics of photogenerated electrons/holes in a heteroepitaxial graphene-on-Si material under pumping with a 1550-nm, 80-fs pulsed fiber laser and probing with the corresponding terahertz beam generated by and synchronized with the pumping laser. The time-resolved electric-nearfield intensity originating from the coherent terahertz photon emission is electrooptically sampled in total-reflection geometry. The Fourier spectrum fairly agrees the product of the negative dynamic conductivity and the expected THz photon spectrum reflecting the pumping photon spectrum. This phenomenon is interpreted as an amplified stimulated terahertz emission.     

Progress of Terahertz Devices Based on Graphene

Graphene is a one-atom-thick planar sheet of sp2-hybridized orbital bonded honeycomb carbon crystal. Its gapless and linear energy spectra of electrons and holes lead to the unique carrier transport and optical properties, such as giant carrier mobility and broadband flat optical response. As a novel material, graphene has been regarded to be extremely suitable and competent for the development of terahertz （THz） optical devices. In this paper, the fundamental electronic and optic properties of graphene are described. Based on the energy band structure and light transmittance properties of graphene, many novel graphene based THz devices have been proposed, including modulator, generator, detector, and imaging device. This progress has been reviewed. Future research directions of the graphene devices for THz applications are also proposed.     

High-Contrast Imaging of Graphene via Time-Domain Terahertz Spectroscopy

We demonstrate terahertz (THz) imaging and spectroscopy of single-layer graphene deposited on an intrinsic Si substrate using THz time-domain spectroscopy. A single-cycle THz pulse undergoes multiple internal reflections within the Si substrate, and the THz absorption by the graphene layer accumulates through the multiple interactions with the graphene/Si interface. We exploit the large absorption of the multiply reflected THz pulses to acquire high-contrast THz images of graphene. We obtain local sheet conductivity of the graphene layer analyzing the transmission data with thin-film Fresnel formula based on the Drude model.     

Emission of Terahertz Radiation from Two-Dimensional Electron Systems in Semiconductor Nano- and Hetero-Structures

This paper reviews recent advances in emission of terahertz radiation from two-dimensional (2D) electron systems in semiconductor nano-heterostructures. 2D plasmon resonance is first presented to demonstrate intense broadband terahertz emission from InGaP/InGaAs/GaAs and InAlAs/InGaAs/InP material systems. The device structure is based on a high-electron mobility transistor and incorporates the author??s original interdigitated dual-grating gates. Second topic focuses on graphene, a monolayer carbon-atomic honeycomb lattice crystal, exhibiting unique carrier transport and optical properties owing to massless and gapless energy spectrum. Coherent stimulated terahertz emission from femtosecond infrared-laser pumped epitaxial graphene is experimentally observed, reflecting the occurrence of negative dynamic conductivity and population inversion.     

Active Graphene-Based Terahertz Dual-Band Modulator Implemented in the Presence of External Fields

In this work, we numerically demonstrate a dynamic graphene-based dual-band metamaterial modulator (gDMM) in the presence of an external magnetic field and gate electric field. With the objective of modulating terahertz waves at two separate channels, we utilize the proposed dual-field control method to dynamically modulate the optical conductivity of graphene, and thus the working frequencies of the gDMM. An interpretation for such dependence on the external fields is presented based on a quantum understanding of the energy structure of graphene, and a numerical method based on the finite element method (FEM) is employed to investigate the optical responses of our proposed gDMM. Our results show that, by varying the strength of external fields, one can switch the operation status of the two working channels located at 3.18 THz and 9.04 THz, with modulation depths exceeding 84.4%. Only 30 meV of energy is required for shifting the Fermi level to accomplish the switch, which is extremely low compared with methods in previous works using gate electric control alone. Simultaneous ON/OFF statuses are also realized. Such great tunability and controllability of our proposed gDMM over a wide frequency range may give rise to a new class of dynamic devices for terahertz and microwave applications.     

Silicon Carbide Terahertz Emitting Devices

In recent years, terahertz (THz) sources between 0.1 THz and 10 THz have attracted much attention for imaging and sensing applications. THz emission from radiative transitions in impurity states has been demonstrated in Si and Ge devices by either electrical or optical pumping. Compared to Si as the material for THz emission, the wide-band-gap material SiC exhibits several advantages such as a higher dopant ionization energy, which allows a higher device operating temperature. Combining with its superior material qualities such as high breakdown field and high thermal conductivity, SiC is a promising material for high-temperature and high-power THz emitting devices. This article describes recent progress in using SiC materials to increase the operating temperature and output power of dopant-based THz sources.     

强THz场下GaAs和InSb中瞬态谷间散射和碰撞电离

运用系宗蒙特卡罗法计算了强THz场作用下, n型掺杂的GaAs和InSb中随时间变化的散射机制以及载流子非线性动力学演变, 获取了电子散射至卫星谷并弛豫回原能谷的时间信息, 并追踪描绘了载流子瞬态增加的过程, 结果同时显示了强场作用下谷间散射是GaAs中的主要散射机制, 而碰撞电离则是InSb中的关键因素.此外进一步讨论了这两种机制对于相关物理量: 平均动能、平均速度、材料的电导率的影响, 结果说明这两种机制导致了非线性效应并在两种材料中起到相反的作用, InSb中碰撞电离的响应时间比GaAs中谷间散射的响应时间更长.该研究结果在THz调制领域有一定的指导意义.     

Calculation and Study of Graphene Conductivity Based on Terahertz Spectroscopy

Based on terahertz time-domain spectroscopy system and two-dimensional scanning control system, terahertz transmission and reflection intensity mapping images on a graphene film are obtained, respectively. Then, graphene conductivity mapping images in the frequency range 0.5 to 2.5 THz are acquired according to the calculation formula. The conductivity of graphene at some typical regions is fitted by Drude-Smith formula to quantitatively compare the transmission and reflection measurements. The results show that terahertz reflection spectroscopy has a higher signal-to-noise ratio with less interference of impurities on the back of substrates. The effect of a red laser excitation on the graphene conductivity by terahertz time-domain transmission spectroscopy is also studied. The results show that the graphene conductivity in the excitation region is enhanced while that in the adjacent area is weakened which indicates carriers transport in graphene under laser excitation. This paper can make great contribution to the study on graphene electrical and optical properties in the terahertz regime and help design graphene terahertz devices.     

Terahertz Dynamics of Quantum-Confined Electrons in Carbon Nanomaterials

Low-dimensional carbon nanostructures, such as single-wall carbon nanotubes (SWCNTs) and graphene, offer new opportunities for terahertz science and technology. Being zero-gap systems with a linear, photon-like energy dispersion, metallic SWCNTs and graphene exhibit a variety of extraordinary properties. Their DC and linear electrical properties have been extensively studied in the last decade, but their unusual finite-frequency, nonlinear, and/or non-equilibrium properties are largely unexplored, although they are predicted to be useful for new terahertz device applications. Terahertz dynamic conductivity measurements allow us to probe the dynamics of such photon-like electrons, or massless Dirac fermions. Here, we use terahertz time-domain spectroscopy and Fourier transform infrared spectroscopy to investigate terahertz conductivities of one-dimensional and two-dimensional electrons, respectively, in films of highly aligned SWCNTs and gated large-area graphene. In SWCNTs, we observe extremely anisotropic terahertz conductivities, promising for terahertz polarizer applications. In graphene, we demonstrate that terahertz and infrared properties sensitively change with the Fermi energy, which can be controlled by electrical gating and thermal annealing.     

Lifetime Measurement of Excitons in Si by Terahertz Time-domain Spectroscopy with High Spectral Resolution

We have developed an optical pump and terahertz (THz) probe spectroscopy scheme to study the photoexcited dynamics in solids ranging from sub-microsecond to a millisecond regime. We applied the developed scheme to measure the lifetime of long-lived indirect excitons in Si through the observation of intra-exciton transitions, resolving the fine structure of excitons with high spectral resolution in a spectral range from 0.5 to 7 THz (2 to 29 meV). We also performed the lifetime measurement of the lowest energy spin-forbidden dark excitons under the magnetic field. Through the observation of intra-exciton transitions, otherwise inaccessible spin-forbidden dark excitons were directly probed by the THz time-domain spectroscopy. By comparing with the photoluminescence spectroscopy, we revealed that the lowest energy dark excitons are accumulated in the crystal, whereas the recombination dynamics is governed by the nonradiative decay process.     

基于石墨烯的太赫兹光电功能器件研究进展

作为一种新型光电材料,石墨烯独特的能带结构和电子输运特性,使其与太赫兹科学有着密切的内在关系：石墨烯内部的等离子体振荡频率在太赫兹频段;人为调谐石墨烯的禁带宽度在0~0.3 eV时,正好覆盖太赫兹频段;光电导率的外部可控性等,这些特点使得石墨烯有望成为太赫兹频段新一代高性能设备研制的基础。最近的研究显示,石墨烯在太赫兹波产生、调控、检测等光电功能器件的研制中取得了很好的成果。重点介绍了基于石墨烯的太赫兹光电功能器件,包括太赫兹源器件、可控调控器件及检测器研究的最新进展,并对这一快速发展的研究领域进行了展望。     

THz modulator based on the Drude model

An amplitude modulator for the terahertz (THz) range is designed. The Drude model is adopted, in which the collision damping is independent of the carrier energy. The Si block with 808 nm laser is illustrated, and it will generate the photocarriers. The injected photo-carriers will change the conductivity and dielectric of the sample, which have direct relationship with the absorption coefficient of the THz wave, hence to control the characteristics of the THz wave in the sample. By changing the light intensity, due to the different photon-generated carrier concentrations, the single transmission of the THz wave in the silicon substrate is changed remarkably.     

基于光抽运-太赫兹探测技术的ZnSe纳米薄膜的光致载流子动力学特性

利用光抽运-太赫兹探测技术,研究了ZnSe纳米 薄膜的载流子弛豫过程和太赫兹波段 电导率的时间演化过程。通过监测THz探测脉冲的变化,系统地研究了ZnSe纳米晶在光激发 载流子诱导下的瞬态光电导特性,并用Drude-Smith模型对瞬态电导率进行了拟合。在400 nm 的激光脉冲激励下,太赫兹脉冲的负透过率呈现出超快的上升和双指数衰减现象。时间常数 为5ps的快速衰减过程主要由ZnSe纳米晶界面缺陷处的光载流子后向散射控制,而时间常数 大于1ns的慢衰减过程主要是由载流子从导带到价带的复合引起的。瞬态电导率随时间的演 化表明,ZnSe纳米材料是制备超快THz开关的很好的备选材料。     

二维材料异质结增强的硅基太赫兹光调制器

研究了石墨烯/氮化硼二维异质结增强的硅基太赫兹波光调制器。利用太赫兹波时域谱系统和实验室自主搭建的太赫兹波动态测试系统分别测试了808 nm激光对太赫兹波的静态和动态调制。当照射在太赫兹波调制器上的激光功率从0增加至500 mW时,平均太赫兹波透过率从58%下降到13%,静态调制深度最高达到76%(500 mW)。动态测试获得的最大调制速度为15 kHz (100 mW)。实验结果表明,与单层石墨烯增强的硅基调制器相比,石墨烯/氮化硼异质结可以更大地提高硅对于太赫兹波的调制深度,并提升调制速度。     

InSb光电导太赫兹源材料性质及辐射场研究

为了研究锑化铟(InSb)半导体材料光电导太赫兹辐射过程,用数值计算方法分析材料内载流子迁移率和表面电流,以及不同性质抽运激光器对太赫兹波近场强度的影响,用宏观电磁场理论和微观半导体理论分析材料表面电流,比较了InSb和GaAs材料的太赫兹波功率谱曲线。结果表明,InSb材料载流子弛豫时间越长,载流子迁移率越大;表面电流与载流子寿命和弛豫时间成正比;宏观电磁场理论更适于分析表面电流;抽运激光饱和能量密度越大,太赫兹近场辐射强度越强;抽运激光脉冲宽度越短,太赫兹近场辐射强度越强;InSb光电导辐射太赫兹波功率比GaAs高。该结果为基于InSb光电导太赫兹辐射源的研究奠定了一定的基础。     

Terahertz Photon Mixing Effect in Gapped Graphene

We theoretically calculate the terahertz waves mixing effect in doped graphene with a finite bandgap. The temperature dependence of the nonlinear intraband optical response at bandgap opening of few tens of meV are investigated. When the external electric field is weak, a moderate level of bandgap opening is found to slightly enhance the nonlinear optical response. The optical response is however significantly altered under strong-field condition. The strong-field nonlinear optical conductivity exhibits two distinct response ‘hot spot’: (i) low temperature with large bandgap and (ii) high temperature with small bandgap. The electric field required for the nonlinear response to dominate over the linear response is typically in the order of 10⁴ V/cm. This value increases rapidly by a factor of 10 in large bandgap and high temperature regimes. Our results suggest that photon mixing effect in gapped graphene is strongly gapped dependent and hence the bandgap opening has to be carefully engineered in order to optimize the photon mixing effect in gapped graphene.     

High Mobility 3D Dirac Semimetal (Cd3As2) for Ultrafast Photoactive Terahertz Photonics

The Dirac semimetal cadmium arsenide (Cd₃As₂), a 3D electronic analog of graphene, has sparked renewed research interests for its novel topological phases and excellent optoelectronic properties. The gapless nature of its 3D electronic band facilitates strong optical nonlinearity and supports Dirac plasmons that are of particular interest to realize high-performance electronic and photonic devices at terahertz (1 THz = 4.1 meV) frequencies, where the performance of most dynamic materials are limited by the tradeoff between power-efficiency and switching speed. Here, all-optical, low-power, ultrafast broadband modulation of terahertz waves using an ultrathin film (100 nm, λ/3000) of Cd₃As₂ are experimentally demonstrated through active tailoring of the photoconductivity. The measurements reveal the photosensitive metallic behavior of Cd₃As₂ with high terahertz electron mobility of 7200 cm² (Vs)⁻¹. In addition, optical fluence dependent ultrafast charge carrier relaxation (15.5 ps), terahertz mobility, and long momentum scattering time (157 fs) comparable to superconductors that invoke kinetic inductance at terahertz frequencies are demonstrated. These remarkable properties of 3D Dirac topological semimetal envision a new class of power-efficient, high speed, compact, tunable electronic, and photonic devices.