太赫兹量子级联激光器材料生长及表征

采用气态源分子束外延方法生长了束缚态到连续态跃迁太赫兹量子级联激光器（terahertz quantum-cascade laser,简称THz QCL）有源区结构,并且采用电化学CV仪、霍尔测试仪以及高分辨X射线衍射对材料的质量进行表征,得出THz QCL有源区具有很高的晶体质量.另外,采用蒙特卡罗方法模拟了共振声子THz QCL器件的I-V曲线,分析了在不同偏压下子能级的对齐状况和电子的输运特征. 关键词： 太赫兹 量子级联激光器 分子束外延 X射线衍射     

Dynamics of molecular alignment steered by a few-cycle terahertz laser pulse

The field-free alignment of molecule ClCN is investigated by using a terahertz few-cycle pulse (THz FCP) based on the time-dependent density matrix theory. It is shown that a high degree of molecular alignment can be obtained by changing the matching number of the THz FCPs in the adiabatic regime and the non-adiabatic regime. The matching number can affect both the maximum value of the alignment and the time at which it is achieved. It is also found that a higher degree of alignment can be achieved by using the THz FCP at lower intensity and there exists an optimal threshold of molecular alignment with the increase of the field amplitude. Also found is the frequency sensitive region in which the degree of maximum alignment can be enhanced greatly by modulating the center frequencies of different THz FCPs. The investigation demonstrates that comparing with a THz single-cycle pulse, a better result of the field-free alignment can be created by a THz FCP at a constant rotational temperature of molecule.     

All-optical ultrafast polarization switching of terahertz radiation by impulsive molecular alignment

We experimentally demonstrate ultrafast polarization switching of terahertz (THz) radiation generated by dual-color driving pulses composed of orthogonally polarized fundamental and second-harmonic waves, which can be controlled by field-free molecular alignment in air by modulating the relative phase between the two field components as a transient dynamic wave plate. By fine-tuning the time delay to properly match the molecular alignment revivals, a significant polarization modulation of the THz radiation is observed and both linearly and elliptically polarized THz radiations can be obtained.     

Influence factor analysis of field-free molecular orientation

The effects of the characteristics of molecules and external fields on field-free molecular orientation are investigated through the comparison of HBr with LiH driven by the combination of a two-color laser pulse and a time-delayed THz laser pulse. It is shown that the dipole interaction has greater influence on field-free orientation than the hyperpolarizability interaction. In addition to the temperature dependence of orientation degree, the effects of the amplitudes of the two-color laser pulse and THz laser pulse, rising time, and THz laser frequency on molecular orientation are also discussed.     

Dynamical analysis of the effect of elliptically polarized laser pulses on molecular alignment and orientation

In this Letter, we study the molecular alignment and orientation driven by two elliptically polarized laser pulses.It is shown that the field-free molecular alignment can be achieved in a three-dimensional(3D) case, while the field-free molecular orientation is only along the x and y directions, and that the field-free alignment and orientation along different axes are related to the populations of the rotational states. It is demonstrated that changing the elliptic parameter is efficient for controlling both in-pulse and post-pulse molecular alignment and orientation. The delay time also has an influence on the field-free molecular alignment and orientation.     

基于IrMn/Fe/Pt交换偏置结构的无场自旋太赫兹源

与目前商用的太赫兹源相比,自旋太赫兹源具有超宽频谱、固态稳定以及成本低廉等优点,这使其成为下一代太赫兹源的主要研究焦点.但使用自旋太赫兹源时,通常需要外加磁场使铁磁层的磁化强度饱和,才能产生太赫兹波,这制约了其应用前景.基于此,本文制备了一种基于Ir Mn/Fe/Pt交换偏置结构的自旋太赫兹波发生器,通过Ir Mn/Fe中的交换偏置场和Fe/Pt中的超快自旋流注入与逆自旋霍尔效应相结合,在无外加磁场下产生了强度可观的太赫兹波.在Ir Mn和Fe的界面中插入超薄的Cu,可以使Fe在厚度很薄时零场下实现饱和磁化,并且其正向饱和场最高可达–10 m T,从而进一步提升无场下的太赫兹发射效率.零场下出射的太赫兹波的动态范围超过60 d B,达到可实用化的水平.通过旋转样品,发现产生的太赫兹波的偏振方向也会随之旋转,并且始终沿着面内垂直于交换偏置场的方向.此外,在此交换偏置结构的基础上,引入了一层自由的铁磁金属层Fe,设计了一种以Ir Mn/Fe/Pt/Fe为核心结构的自旋阀太赫兹源,发现产生的太赫兹强度在两层铁磁层反平行排列时比平行排列以及不引入自由铁磁金属层时均大约提升了40%.结果表明,基...     

Effect of mutual configuration between molecular orientation and atomic orientation in the oriented Ar (3P2)+oriented CF3H reaction

The steric effect in the dissociative energy transfer reaction of Ar (3P2,MJ=2)+CF3H has been observed as a function of the mutual configurations between the molecular orientation and the atomic orientation in the collision frame. The reactivity is significantly changed depending on the mutual configuration between the molecular orientation and the atomic orientation. Especially, the molecular alignment dependence is dramatically changed depending on the configuration of the atomic alignment.     

2.9THz束缚态向连续态跃迁量子级联激光器研制

采用气源分子束外延技术生长了GaAs/AlGaAs束缚态向连续 态跃迁的太赫兹量子级联激光器材料, 基于半绝缘等离子体波导工艺制作了太赫兹量子级联激光器. 测量了激光器的发射光谱和功率-电流-电压关系曲线, 研究了器件的激光特性. 器件激射频率约2.95 THz, 脉冲模式下, 最高工作温度为67 K. 连续波模式下, 阈值电流密度最低为230 A/cm², 最大光输出功率1.2 mW, 最高工作温度为30 K. 关键词： 太赫兹 量子级联激光器 分子束外延 波导     

Water vapor: An extraordinary terahertz wave source under optical excitation

In modern terahertz (THz) sensing and imaging spectroscopy, water is considered a nemesis to be avoided due to strong absorption in the THz frequency range. Here we report the first experimental demonstration and theoretical implications of using femtosecond laser pulses to generate intense broadband THz emission from water vapor. When we focused an intense laser pulse in water vapor contained in a gas cell or injected from a gas jet nozzle, an extraordinarily strong THz field from optically excited water vapor is observed. Water vapor has more than 50% greater THz generation efficiency than dry nitrogen. It had previously been assumed that the nonlinear generation of THz waves in this manner primarily involves a free-electron plasma, but we show that the molecular structure plays an essential role in the process. In particular, we found that THz wave generation from H₂O vapor is significantly stronger than that from D₂O vapor. Vibronic activities of water cluster ions, occurring naturally in water vapor, may possibly contribute to the observed isotope effect along with rovibrational contributions from the predominant monomers.     

Study of the rates of collisional decay of population, orientation, and alignment by stimulated photon echo in a molecular gas

A stimulated photon echo technique with specially selected linear polarizations of the coherent resonant driver pulses is used to study depolarizing collisions in the molecular gas SF₆ and in mixtures of it with buffer He and Xe. The collisional decay rates of the population, orientation, and alignment in an ensemble of gas particles are determined for the first time in a single experiment. These relaxation rates are measured as a function of the longitudinal translational velocities of the resonant particles. To within the experimental accuracy, no significant dependence of the collisional decay rates on the translational velocities of the particles was observed. This result confirms the conventional theoretical approach to depolarizing collisions. In pure SF₆ the decay rates for the orientation and alignment were lower than the relaxation constant for collisions involving a change in the longitudinal velocity (elastic collisions) that is known from experimental observations of the ordinary photon echo. This means that only some of the elastic collisions participate in destroying the multipole moments of the levels. Evidence is found that the relaxation of the multipole moments created by polarized radiation in a resonant medium of molecular SF₆ gas depends on j, the total angular momentum of the level. Zh. éksp. Teor. Fiz. 113, 826–833 (March 1998)     

Terahertz Quantum Cascade Laser at 3.39THz

We demonstrate the growth of terahertz quantum cascade laser （THz QCL） by gas source molecular beam epitaxy. X-ray diffraction and cross-sectional transmission electron microscopic measurements show the high crystalline quality of the THz QCL active region, From the cross-sectional transmission electron microscopy image, sharp interfaces are observed and the deduced cascade period thickness is consistent with the result of x-ray diffraction. The test device is lasing at 3.39THz and operating up to lOOK in pulsed mode. At IOK, the maximum output power is greater than 1 mW with a threshold current density of 738 A/cm^2.     

Manipulating Nonlinear Photocurrent from Interlayer Coupling in Bilayer Metamaterials for Polarized Terahertz Generation

Polarized terahertz (THz) wave generation is of great significance for chiral and anisotropic sensing applications. However, how to manipulate amplitude, polarization, and ellipticity of the THz generation is still a fundamental challenge. Herein, polarized THz wave generation is achieved from a bilayer metamaterial consisting of T-shaped structure (TSS) and split resonator rings (SRRs) by combining Maxwell and hydrodynamic equations. The elliptically polarized THz wave can be synthetized directly from horizontally and vertically polarized THz components due to the orthogonal nonlinear photocurrents along the arm-directions of TSS and SRRs, respectively. Besides, the ellipticity and the orientation angle of the THz polarization ellipse can be modulated by the twist angle between the SRRs and TSS layers. The maximum ellipticity can reach 0.34 while the orientation angle is tunable from −0.45 to 0.48π by tuning the twist angle. This work proposes an interlayer coupling method for the polarized THz sources based on metamaterials in potential circular dichroism and chiral sensing applications.     

THz radiation generation via the interaction of two‐colour ultra‐short laser pulses with SO2 and NH3 gases

In this work, using a two‐dimensional particle‐in‐cell Monte Carlo collision computation method, terahertz (THz) radiation generation via the interaction of two‐colour, ultra‐short, high‐power laser pulses with the polyatomic molecular gases sulphur dioxide (SO₂) and ammonia (NH₃) is examined. The influence of SO₂ and NH₃ pressures and two‐colour laser pulse parameters, i.e., pulse shape, pulse duration, and beam waist, on the THz radiation generation is studied. It is shown that the THz signal generation from SO₂ and NH₃ increases with the background gas pressure. It is seen that the THz emission intensity for both gases at higher laser pulse durations is higher. Moreover, for these polyatomic gases, the plasma current density increases with increase in the laser pulse beam waist. A more powerful THz radiation intensity with a larger time to peak of the plasma current density is observed for SO₂ compared to NH₃. In addition, many THz signals with small intensities are observed for both polyatomic gases. It is seen that for both SO₂ and NH₃ the generated THz spectral intensity is higher at higher gas pressures.     

太赫兹电磁波大气吸收衰减逐线积分计算

大气对太赫兹辐射传输存在一定的非协作性,即存在吸收衰减。为了实现太赫兹辐射的有效应用必须细致地了解太赫兹辐射大气传输的窗口位置、宽度及大气透过率。选取了处理大气非均匀路径、吸收带重叠等大气辐射传输问题的最精确方法逐线积分法,发展计算程序,并基于HITRAN分子谱线数据,对水汽、氧气、臭氧、氮气、二氧化碳等单组分气体分子对太赫兹辐射传输的吸收衰减情况进行了计算与分析,并给出了在太赫兹电磁波大气传输衰减中占主要因素的水汽和氧气的衰减峰位置。     

Study on orientation mechanisms of poly(vinylidenefluoride-trifluoroethylene) molecules aligned by atomic force microscopy

We have developed a molecular orientation control technique for polymers utilizing contact-mode atomic force microscopy (AFM). In this paper, we studied the molecular alignment mechanism of this technique by applying it to poly(vinylidenefluoride-trifluoroethylene) (P(VDF-TrFE)). The resultant alignment and formed crystal size were strongly dependent on the temperature during the modification. They also depended on the scan line spacing of the modification. These results made the alignment mechanism clear. The obtained molecular alignment was stable against the heat treatment even at the temperatures just below T_m.     

Improvement and analysis of computational methods for prediction of residual dipolar couplings

We describe a new, computationally efficient method for computing the molecular alignment tensor based on the molecular shape. The increase in speed is achieved by re-expressing the problem as one of numerical integration, rather than a simple uniform sampling (as in the PALES method), and by using a convex hull rather than a detailed representation of the surface of a molecule. This method is applicable to bicelles, PEG/hexanol, and other alignment media that can be modeled by steric restrictions introduced by a planar barrier. This method is used to further explore and compare various representations of protein shape by an equivalent ellipsoid. We also examine the accuracy of the alignment tensor and residual dipolar couplings (RDC) prediction using various ab initio methods. We separately quantify the inaccuracy in RDC prediction caused by the inaccuracy in the orientation and in the magnitude of the alignment tensor, concluding that orientation accuracy is much more important in accurate prediction of RDCs.     

Terahertz-wave generation with periodically inverted gallium arsenide

We overview methods of THz-wave generation using frequency down-conversion in GaAs with periodically-inverted crystalline orientation. First, we compare different nonlinear-optical materials suitable for THz generation, analyze THz generation process in quasi-phase-matched crystals and consider theoretical limits of optical-to-THz conversion. Then, we review single-pass optical rectification experiments with femtosecond pump pulses, performed in periodically-inverted GaAs, where monochromatic THz output tunable in the range 0.9–3.0 THz was produced. Finally, we describe a novel approach to create a compact highly efficient tunable (0.5–3.5 THz) room temperature monochromatic THz source, based on the concept of intracavity THz generation via resonantly-enhanced difference frequency mixing. This approach allowed generating of 1 mW of average THz power, potentially scalable to 10–100 mW.     

Polarization state of high-order harmonic emission from aligned molecules

High harmonic emission in isotropic gases is polarized in the same direction as the incident laser polarization. Laser-induced molecular alignment allows us to break the symmetry of the gas medium. By using aligned molecules in high harmonic generation experiments, we show that the polarization of the extreme ultraviolet emission depends strongly on the molecular alignment and the orbital structure. Polarization measurements give insight into the molecular orbital symmetry. Furthermore, molecular alignment will allow us to produce attosecond pulses with time-dependent polarization.     

Self‐assembly and structure formation in liquid crystalline phthalocyanine thin films studied by Raman spectroscopy and AFM

This work presents an investigation of films prepared by doctor blade casting, the formation of self‐assembled microstructures of a liquid crystalline phthalocyanine with highly oriented molecules. Raman Spectroscopy in combination with atomic force microscopy is applied to study the structures within the films. By keeping the substrate at room temperature or at 353 K during coating, different geometric structures namely rods and islands form. Rod‐like structures are growing in coating direction, whereas directional growth of the islands is not observed. The distribution of the rod lengths varies widely, whereas the width appears more uniform. Annealing of the samples shows a different behavior of the two textures. Islands tend to melt, and rods smooth their structural form, which is extracted from Raman imaging in combination with atomic force microscopy. Additionally, Raman imaging gives insight into laterally different relative crystallinity. These observations are discussed in the context of the molecular orientation as probed by polarized Raman spectroscopy. These polarized Raman spectra indicate azimuthal alignment of the molecules within the rods (edge on alignment). This alignment occurs along and also perpendicular to the growth direction. In contrast to the alignment in the rods, the molecules inside the islands occurring at higher temperature do not show preferential molecular orientation. After annealing, no preferential molecular orientation is observed in rods because of the loss of anisotropy, too. Copyright © 2012 John Wiley & Sons, Ltd.     

基于THz光谱技术的1,3-二硝基苯挥发气体检测方法研究

针对工业生产过程中1,3-二硝基苯挥发气体突发性泄露等情况的发生,设计了一种基于太赫兹(THz)特征光谱吸收技术的检测方法,该方法可通过1,3-二硝基苯在THz波段的特征波长对痕量剧毒有害气体进行检测。系统设计了双气室结构,为THz波提供差分数据,一组为标准空气,另一组为待测样气。由1,3-二硝基苯在THz波段的四个主吸收带0.635,0.912,1.095和1.435THz可根据对应吸收带吸收系数的比例关系得到对应波长上的吸收幅值,最终反演气体浓度。经过对两种传统检测方法的实验分析和对THz吸收检测方法的仿真研究可知,色谱法检测速度无法实现实时检测,红外吸收法对环境湿度要求很高,需经干燥处理,而THz吸收法对环境湿度要求较低,且具备实时性,更适合于实际应用。