Toward generation of μJ range sub-ps THz pulses by optical rectification

Recently the possibility of scaling up the energy of sub-ps THz pulses generated in lithium-niobate by tilted pulse front excitation was demonstrated. Using 500 μJ energy pump pulses at 780 nm center wavelength, we achieved THz pulses with energy up to 240 nJ. In this article, results of calculations using a simple model predict the possibility of increasing the THz pulse energy above 1 μJ and the quantum efficiency up to 50% by decreasing the temperature. The dependence of the THz pulse energy and the maximum achievable electric field on the crystal length and the pump pulse duration is also presented. According to the calculations, generation of the maximum THz energy needs a specific pump pulse duration, because of increasing dispersion and absorption with increasing frequency. Not only longer, but also shorter pulses lead to a degradation of the THz energy. Results of calculations for GaSe, GaP and ZnTe are also presented. PACS 07.57.Hm; 42.65.Ky; 42.79.Nv     

FOX-7转晶行为的太赫兹光谱及理论计算研究

1, 1 -二氨基- 2, 2 -二硝基乙烯(FOX-7)是一款新型高能钝感炸药, 为了研究温度变化对其分子结构特性的影响, 利用太赫兹时域光谱技术对持续升温(298K→393 K)过程中FOX-7 在0.2—2.5 THz 频率范围内的吸收光谱进行了在线探测, 结果发现随着样品温度的升高, FOX-7 的吸收谱带发生变化, 于384 K 时出现一个新的吸收特征峰, 且该吸收峰的峰强逐渐升高. 基于密度泛函理论(DFT), 对样品在298 K 和393 K 温度下的晶体结构进行了小于2.5 THz 范围内吸收频谱的模拟计算, 完成了对FOX-7 两种晶型实验吸收特征峰的指认. 分析表明FOX-7 的分子结构会受温度的影响而发生改变, 互为异构晶型的基团表现出的振动模式不同, 温度384 K 时FOX-7 开始发生α→β 晶型转变, 且该晶型转变过程是可逆的, 新出现的1.12 THz 特征峰在393 K 时的振动是由—NO₂ 和—NH₂ 的摆动及各自的扭动所致.     

低温液态水的太赫兹吸收特性研究

太赫兹波的光子能量只有毫电子伏特,远低于各种化学键的键能,因此不会和生物组织发生有害的电离反应;另一方面,由于大部分生物分子转动和振动所具有的特征能量都在太赫兹范围内,所以利用太赫兹波可以对生物分子进行识别。水是生物环境中最重要的液体,生物分子与液态水之间的相互作用决定了其生物活性,因此研究液态水的太赫兹特性就显得十分重要。水作为极性液体,其中的偶极分子-偶极分子间的相互作用和极性分子间的氢键会对太赫兹波产生较大的吸收作用,这就使利用太赫兹技术研究液体环境下的生物分子动力学特性变得相当困难。微流控技术通过改变微流控芯片中液体通道的深度来控制液体样品的厚度,以减少太赫兹波与液体样品的作用距离,从而使水对太赫兹波的吸收大幅减小。利用对太赫兹波的透过率高达95%的Zeonor 1420R材料和双面胶制作了可重复性使用的夹心式微流控芯片,芯片上液体通道的长度、宽度、深度分别为2 cm,5 mm和50 μm。另外,设计制作了一个制冷系统,由制冷片、散热模块、温度传感器、保温箱和温度控制器构成,该制冷系统可以对保温箱的内部环境制冷并在一定程度上保持恒温。在实验过程中,将注满水的微流控芯片置于保温箱中,利用制冷系统对微流控芯片中的水进行制冷处理,从8～-3 ℃每隔1 ℃进行一次太赫兹透射测量,通过对实验数据的分析,发现随着温度降低,水的太赫兹透过率不断增大,说明水对太赫兹波的吸收随着温度的降低而降低。此结果为将来在不同低温环境下利用微流控技术研究液体样品的太赫兹吸收特性打下了基础,为太赫兹在生物领域的应用与发展提供了技术支持。     

Interaction of argon clusters with intense VUV-laser radiation: the role of electronic structure in the energy-deposition process

The response of Ar clusters to intense vacuum-ultraviolet pulses is investigated with photoion spec-troscopy. By varying the laser wavelength, the initial excitation was either tuned to absorption bands of surface or bulk atoms of clusters. Multiple ionization is observed, which leads to Coulomb explosion. The efficiency of resonant 2-photon ionization for initial bulk and surface excitation is compared with that of the nonresonant process at different laser intensities. The specific electronic structure of clusters plays almost no role in the explosion dynamics at a peak intensity larger than 1.8 x 10(12) W/cm(2). The inner ionization of atoms for resonant and nonresonant excitation is then saturated and the energy deposition is mainly controlled by the plasma heating rate. Molecular dynamics simulations indicate that standard collisional heating cannot fully account for the strong energy absorption.     

电场诱导水的太赫兹透射特性研究

许多生物分子自身的转动、振动或分子团的整体振动模式都位于太赫兹波段内,因此可以利用太赫兹光谱技术对生物分子进行检测。同时又由于太赫兹波的光子能量仅为毫电子伏量级,不会对分子的内部结构造成破坏,所以太赫兹时域光谱技术在生物检测方面具有良好的应用前景。众所周知,绝大多数的生物分子只有在液体条件下才能发挥其生物活性,所以研究液体环境下生物分子之间的相互作用就非常必要。然而水分子的转动模式、振动模式以及和氢键有关的能量均处于太赫兹波段,从而对其产生强烈的吸收;另外,水分子为极性分子,而极性分子对太赫兹波有强烈的共振吸收,这就使利用太赫兹技术对生物分子活性进行动态表征产生了困难。因此在研究溶液中的生物分子与太赫兹波的相互作用时,最大限度地减小水分子对太赫兹波的吸收就成为近年来的研究热点。目前,减少水对太赫兹波吸收的主要方法有：在溶液样品中加入抑制氢键缔合的离子来减小水对太赫兹的吸收;通过改变溶液的温度来调节水对太赫兹的吸收;利用微流控芯片技术,通过减小被测样品与太赫兹波的作用距离来减小水对太赫兹波的吸收。另外,激光的激励、电场或磁场的处理,也能改变水对太赫兹波的吸收,将盛有去离子水的微流控芯片放于电场中,研究经电场处理不同时间的去离子水对太赫兹吸收强度的影响。结果发现,太赫兹波的透射强度随着去离子水在电场当中静置时间的增加而增强,当在电场中静置60 min时,太赫兹的频谱强度达到最大,与空气的频谱强度接近。由此可以推断外加电场使水分子的偶极矩发生了变化,从而对整体水分子的振动和转动产生了影响,并且改变了水中的氢键结构,导致了太赫兹透射光谱强度的增强。     

Thermal Analysis of Gold Nanorods Heated with Femtosecond Laser Pulses

We present an axisymmetric computational model to study the heating processes of gold nanoparticles, specifically nanorods, in aqueous medium by femtosecond laser pulses. We use a two-temperature model for the particle, a heat diffusion equation for the surrounding water to describe the heat transfer processes occurring in the system, and a thermal interface conductance to describe the coupling efficiency at the particle/water interface. We investigate the characteristic time scales of various fundamental processes, including lattice heating and thermal equilibration at the particle/surroundings interface, the effects of multiple laser pulses, and the influence of nanorod orientation relative to the beam polarization on energy absorption. Our results indicate that the thermal equilibration at the particle/water interface takes approximately 500 ps, while the electron-lattice coupling is achieved at approximately 50 ps when a 48×14 nm gold nanorod is heated to a maximum temperature of 1270 K with the application of a laser pulse having 4.70 J/m(2) average fluence. Irradiation by multiple pulses arriving at 12.5 ns time intervals (80 MHz repetition rate) causes a temperature increase of no more than 3 degrees during the first few pulses with no substantial changes during the subsequent pulses. We also analyze the degree of the nanorods' heating as a function of their orientation with respect to the polarization of the incident light. Lastly, it is shown that the temperature change of a nanorod can be modeled using its volume equivalent sphere for femtosecond laser heating within 5-15% accuracy.     

THz generation via optical rectification with ultrashort laser pulse focused to a line

We report on efficient THz pulse generation via optical rectification with femtosecond laser pulses focused to a line by a cylindrical lens. This configuration provides phase-matched conditions in the superluminal regime. 35 pJ THz pulses have been generated with this technique in a stoichiometric LiNbO₃ crystal pumped by 2 μJ femtosecond laser pulses at room temperature. An unusual superquadratic rise of the THz pulse energy with the laser pulse energy has been observed at high laser energies. This extraordinary energy dependence of the THz generation efficiency is explained by self-focusing of the laser beam in the crystal. Z-scan measurements and comparison of the THz pulse spectra created with laser pulses having different energies confirm this interpretation.     

Study of terahertz pulses at an edge

The propagation behaviour of terahertz （THz） pulses at an edge is characterized. The phenomenon that the amplitude oscillates periodically in the frequency spectrum is similar to Young＇s interference, if the absorption effect is neglected. The oscillation cycle is shorter for a thicker sample. THz pulses at an edge are analyzed by the broadband Huygens-Fresnel diffraction integral. The experimental results are in agreement with the simulation results approximately. The simulation errors are also analyzed.     

飞秒超强激光驱动太赫兹辐射特性的实验研究

强太赫兹源是太赫兹科学技术发展的关键,其中大能量强场太赫兹脉冲源在超快物态调控、新型电子加速器等领域具有重要的应用前景.超快超强激光与等离子体相互作用是近年来发展起来的一种新型的强场太赫兹辐射产生途径.本文报道了利用超强飞秒激光脉冲与金属薄膜靶作用产生太赫兹辐射的实验结果,研究了激光能量和离焦量对靶后太赫兹辐射能量的影响,并通过监测激光背向散射光谱,定性揭示了其变化规律与不同光强下的电子加热机制的相关性.实验表征了太赫兹辐射的频谱、偏振及聚焦光斑情况.测量结果表明,实验产生了脉冲能量达458μJ、聚焦场强高达GV/m量级的超宽带太赫兹辐射,为开展极端太赫兹脉冲与物质相互作用研究提供了一种新的强场太赫兹光源.     

Compact and high-power broadband terahertz source based on femtosecond photonic crystal fiber amplifier

We present a review of the development of a compact and high-power broadband terahertz (THz) source optically excited by a femtosecond photonic crystal fiber (PCF) amplifier.The large mode area of the PCF and the stretcher-free configuration make the pump source compact and very efficient.Broadband THz pulses of 150 μW extending from 0.1 to 3.5 THz are generated from a 3-mm-thick GaP crystal through optical rectification of 12-W pump pulses with duration of 66 fs and a repetition rate of 52 MHz.A strong saturation effect is observed,which is attributed to pump pulse absorption;a Z-scan measurement shows that three-photon absorption dominates the nonlinear absorption when the crystal is pumped by femtosecond pulses at 1 040 nm.A further scale-up of the THz source power is expected to find important applications in THz nonlinear optics and nonlinear THz spectroscopy.     

Experimental study on terahertz radiation

In this letter, we describe a coherent subpicosecond terahertz (THz) spectroscopy system based on nonresonant optical rectification for the generation of THz radiation. We studied the two-photon absorption (TPA) of ZnTe induced by femtosecond laser pulses via THz generation, and its influence on the generation of THz radiation. Experimental results demonstrated that the intensity of pump beam against TPA must be traded off to get an optimum generation of THz radiation. As an example, we measured absorption spectrum of water vapor by time-domain spectroscopy (TDS) in the frequency range from 0.5 to 2.5 THzwith a high overall accuracy.     

The dependence on optical energy of terahertz emission from air plasma induced by two-color femtosecond laser-pulses

The generation of terahertz （THz） emission from air plasma induced by two-color femtosecond laser pulses is studied on the basis of a transient photocurrent model. While the gas is ionized by the two-color femtosecond laser-pulses com- posed of the fundamental and its second harmonic, a non-vanishing directional photoelectron current emerges, radiating a THz electromagnetic pulse. The gas ionization processes at three different laser-pulse energies are simulated, and the corresponding THz waveforms and spectra are plotted. The results demonstrate that, by keeping the laser-pulse width and the relative phase between two pulses invariant when the laser energy is at a moderate value, the emitted THz fields are significantly enhanced with a near-linear dependence on the optical energy.     

Generation and detection of ultrashort pulses of electromagnetic field in the terahertz range and their application for spectroscopy

We present experimental results on generation of pulsed terahertz radiation in a ZnTe crystal using nonlinear optical rectification of high-power femtosecond laser pulses. The use of terahertz pulses for spectroscopy is tested in the rotational lines of absorption of water vapors in the atmosphere. Panoramic spectra of absorption of a number of solvents and protein solutions are measured in the range from 0.2 to 2 THz.     

基于微流控技术的水的太赫兹吸收特性研究

很多生物大分子的特征振动模式和转动模式都位于太赫兹波段范围内,且太赫兹波的低电子能特性使其在实验过程中不会对待测样品造成破坏,所以可以采用太赫兹技术来鉴别生物样品。在许多研究中,生物样品都是溶液状态,溶液中水和其他分子之间的相互作用涉及很多生物现象,所以研究水的太赫兹特性就显得至关重要。众所周知,水分子是十分常见的极性分子,分子间氢键会与太赫兹波发生强烈的相互作用,从而使得水对太赫兹波有很强的吸收作用,导致利用太赫兹技术研究水溶液中生物样品的动态特性变得相当困难。为了解决这一难题,可以引入微流控技术。微流控技术以能精确操控微尺度流体而著称,其沟道深度可以达到50μm甚至更小。由于微流控技术减小了太赫兹波在流体中的传播距离,从而极大地减小了水对太赫兹波的吸收。本研究采用对太赫兹波具有高透过率的Zeonor 1420R材料制成了夹心式微流控芯片,芯片上微沟道的长度、宽度和深度分别为3 cm, 4 mm和50μm,太赫兹探测区的直径为3 mm。在制作微流控芯片时,利用厚度为50μm的强黏性双面胶代替传统夹心式微流控芯片中的聚二甲基硅氧烷(PDMS)薄膜,使微流控芯片在加热过程中不再有漏液现象...     

温度对PEEK太赫兹光谱特性影响研究

聚醚醚酮(PEEK)由于其耐热、耐腐蚀、耐辐照、抗疲劳、电绝缘性等优良性能,在许多领域可以代替金属、陶瓷等传统材料而得到广泛应用。特别是随着5G技术的发展和应用,PEEK已经成为5G热门材料。在PEEK材料实际应用中,温度的影响是一个非常重要和关键的因素。主要研究了PEEK太赫兹光谱以及温度对PEEK太赫兹光谱特性的影响。通过利用太赫兹透射光谱技术,同时结合控温装置,在温度从25～300℃均匀上升过程中,每间隔5℃测试得到PEEK片状样品的太赫兹时域光谱数据,利用光学参数提取算法可以得到PEEK的吸收系数、介电常数等光学参数,进一步得到特定频率下光学常数随温度的变化趋势,从而对材料进行表征和分析。在0.5～4 THz有效光谱范围内,实验结果表明,在常温(25℃)下,PEEK在3.5 THz具有一个明显的特征吸收峰。在25～300℃这个温度范围内,在1 THz频率下,PEEK的吸收系数、介电常数相对于室温分别有4.38%和5.0%的波动,同时PEEK在常温下在1 THz的介电损耗正切值为2.5×10^-3,相比于PMMA和PE等高分子材料,PEEK的介电损耗正切值要低...     

吡虫啉的太赫兹(THz)光谱研究

由超短激光脉冲产生的脉冲波是具有较宽频带的电磁辐射,属于远红外波段,该波段电磁波与物质的相互作用是个崭新的研究领域。文章利用太赫兹时域光谱技术测量了室温下吡虫啉在0.2～2.0 THz范围内的吸收谱和折射率谱。结果表明吡虫啉在此波段有明显的特征吸收峰且吸收系数随频率的增加而增大,折射率也随频率的增加而有所增大,其平均折射率为1.65。实验研究的同时,运用半经验理论计算了吡虫啉分子的结构及其在太赫兹波段的振动频率,并根据计算结果对实验数据进行了解析。计算结果与实验光谱吻合得很好,实验光谱的特征吸收峰是由分子的集体振动及扭转形成, 不同的吸收峰位对应分子不同的振转模式。实验和理论研究的对比表明：分子的远红外吸收特征对于分子的结构和空间排列非常敏感,THz-TDS是研究生物分子集体振动模式和构象结构的好方法。     

木糖醇和D-木糖的太赫兹光谱检测与分析

甜味剂是一种非常重要的食品添加剂,在食品工业中的应用十分广泛,甜味剂的鉴别和检测是一个非常重要的研究课题。太赫兹电磁辐射具有许多独特的性质,太赫兹时域光谱(THz-TDS)技术已发展成为一种重要的无损检测方法。文章利用太赫兹时域光谱技术,对木糖醇和D-木糖进行了光谱测量,结果表明在0.3～2.6THz波段内,木糖醇在1.62,1.87和2.51THz三个频率位置处出现吸收峰,而D-木糖的吸收峰位于1.67,1.96和2.46THz。应用密度泛函理论,对两种样品的单分子结构进行几何优化和频率计算,并据此对实验测量的吸收峰进行了指认,说明部分吸收峰源于单分子的振动模式,另一部分源于分子间相互作用的振动模式。     

时空非均匀等离子体鞘套中太赫兹波的传播特性

高超声速飞行器再入地面的过程中,其周围等离子体的电子密度是非均匀且随时间变化的.对于不同的再入高度,飞行器周围的温度和压强也会发生改变.因此,研究电磁波在时空非均匀等离子体鞘套中的传播特性意义重大.首先建立了时变非均匀的等离子体鞘套模型,然后通过经验公式得到温度、压强与碰撞频率三者的关系.采用时域有限差分方法计算了太赫兹波段中不同电子密度弛豫时间、温度、压强时的反射系数、透射系数和吸收率.研究结果表明:在太赫兹波段中,电子密度的弛豫时间越长,温度越高,压强越大,电磁波越容易穿透等离子体;弛豫时间越短,温度越低,压强越小,等离子体对电磁波吸收率的变化越明显.这些结果为解决"黑障"问题提供了理论依据.     

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.     

A multi-band and polarization-independent perfect absorber based on Dirac semimetals circles and semi-ellipses array

We design a four-band terahertz metamaterial absorber that relied on the block Dirac semi-metal(BDS). It is composed of a Dirac material layer, a gold reflecting layer, and a photonic crystal slab(PCS) medium layer. This structure achieved perfect absorption of over 97% at 4.06 THz, 6.15 THz, and 8.16 THz. The high absorption can be explained by the localized surface plasmon resonance(LSPR). And this conclusion can be proved by the detailed design of the surface structure. Moreover, the resonant frequency of the device can be dynamically tuned by changing the Fermi energy of the BDS. Due to the advantages such as high absorption, adjustable resonance, and anti-interference of incident angle and polarization mode, the Dirac semi-metal perfect absorber(DSPA) has great potential value in fields such as biochemical sensing, information communication, and nondestructive detection.