DAST/SiO2 multilayer structure for efficient generation of 6 THz quasi-single-cycle electromagnetic pulses

We propose a DAST/SiO(2) multilayer structure for efficient generation of near-single-cycle THz transients with average frequency around 6 THz via collinear optical rectification of 800 nm femtosecond laser pulses. The use of such a composite material allows compensation for the phase mismatch that accompanies THz generation in bulk DAST crystals. The presented calculations indicate a strong increase in the THz generation efficiency in the DAST/SiO(2) structure in comparison to the case of bulk DAST crystal.     

有机电光晶体4-(4-二甲基氨基苯乙烯基)甲基吡啶对甲基苯磺酸盐的太赫兹光谱研究

采用色散校正的密度泛函理论(dispersion-corrected density functional theory,DFT-D2)对有机电光晶体4-(4-二甲基氨基苯乙烯基)甲基吡啶对甲基苯磺酸盐(4-N,N-dimethylamino-4′-N′-methyl-stilbazolium tosylate,DAST)进行结构优化和太赫兹光谱计算,通过逐步提高精度进行几何优化的方法寻找DAST收敛的基态稳定结构,获得与DAST初始结构相一致的基态稳定结构.在此结构的基础上,在0—4 THz范围的太赫兹计算光谱与实验测量结果一致,说明采用DFT-D2进行优化的合理性.重要的是,首次通过计算的太赫兹光谱对DAST在0—4 THz范围的太赫兹吸收峰的振动模式进行了详细归属.结果表明:1.12 THz处的振动是DAST阴阳离子的光学声子模式,1.46 THz和1.54 THz两处的振动主要与磺酸盐有关,而2.63 THz和3.16 THz两处的振动则分别源于阳离子的扭转振动和阴离子的转动.该结果不仅很好地说明了阴阳离子分别在太赫兹响应中的贡献,而且为今后通过取代阴阳离子基团获取具有更高二阶非线性效应的DAST衍生物的新合成提供了重要的参考和指导.本文结果说明密度泛函理论在太赫兹光子学上的重要应用,对探究有机电光晶体的太赫兹响应物理原理、性能控制等具有重要的指导价值.     

基于有机吡啶盐晶体的太赫兹频率上转换探测

利用激光泵浦国产有机吡啶盐4-(4-二甲基氨基苯乙烯基)甲基吡啶对甲基苯磺酸盐(4-N,N-dimethylamino-4′-N′-methyl-stilbazolium tosylate,DAST)晶体,通过非线性频率上转换方法实现了室温运转的高灵敏、快响应、宽频段太赫兹探测.高效生成了近红外上转换光,采集到其脉冲包络和光谱,获得了ns量级的时间分辨率,并换算太赫兹波的频率,实现了对太赫兹信息的全面表征.与商用高莱探测器相比,上转换方法在19 THz频点的探测灵敏度高4个数量级;在可探测频率3.15—29.82 THz范围内,响应度普遍高2—3个数量级.结果表明:室温下的光泵频率上转换探测方法在时间分辨率和响应度方面远优于传统的热探测器,极大地提高了差频有源太赫兹系统的动态范围,使差频源在太赫兹波谱分析和成像等领域具有更大的应用潜力.     

非线性有机材料DAST的研究及应用

随着光通信、光信息处理技术等的快速发展,非线性光学材料越来越受到学术界与工业的关注。与无机非线性光学材料相比,有机非线性光学材料具有响应时间短、易于加工和高非线性系数等优点。其中,4-(4-二甲氨基苯乙烯基)甲基吡啶对甲苯磺酸盐(DAST)是人工设计的一种具有非中心对称性和较强极化率的有机非线性材料。大量理论和实验结果表明,DAST具有高二阶光学非线性系数、高电光系数、大双折射率差和低介电常数等特性,能够产生更快、更强的光学非线性响应,还具有优异的太赫兹波发射及吸收性能,是目前综合性能最优、应用最广、最具研究价值的非线性有机材料。近年光谱研究显示,DAST还表现出各向异性的太赫兹光谱特性。文章系统地总结了DAST晶体在太赫兹波发射、二次谐波产生、电光探测和电光调制等众多领域的国内外研究成果,还概括了我们团队近期在DAST基薄膜、太赫兹光谱、光电特性、超材料等新领域的研究进展。此外,还提出将准相位匹配法用于DAST晶体研究、利用电场或自组装膜诱导生长DAST晶体等新思路。对DAST成果的总结和梳理,将促进非线性DAST有机材料在电光调制器、频率转换器、THz探测器等重要领域的应用与理论研究,使其能够更加广泛地应用在光通信、光信息处理、军事技术等重要领域。     

Widely tunable broadband terahertz radiation generation using a configurationally locked polyene 2-[3-(4-hydroxystyryl)-5,5-dimethylcyclohex-2-enylidene] malononitrile crystal via difference frequency generation

Widely tunable terahertz (THz) waves were successfully generated from 0.5 to 10 THz via difference frequency generation (DFG) in a configurationally locked polyene 2-[3-(4-hydroxystyryl)-5,5-dimethylcyclohex-2-enylidene] malononitrile (OH1) crystal. Potassium titanium oxide phosphate optical parametric oscillator pumped by nanosecond Q-switched Nd:YAG laser was used to generate two waves, which were then used to irradiate OH1 crystal. The maximum energy of the generated THz wave was about 461 pJ/pulse. We investigated the dependency of generated THz energy to the excitation pump power density and OH1 crystal thickness. In addition, we compared the THz energy generated by OH1 crystal to 4-N,N-dimethylamino-4′-N′-methyl-4-stilbazolium tosylate (DAST) crystal using DFG, and we achieved 560 times higher energy using OH1 crystal than DAST crystal at around 1.1 THz.     

Design and analysis of a metallic waveguide with a DAST cap for continuously phase-matched terahertz difference frequency generation

We present a novel source for continuous terahertz (THz) wave generation using an organic ionic salt, 4-dimethylamino-N-methyl-4-stilbazolium-tosylate (DAST). THz waves are generated based on difference frequency generation (DFG) in the device. Phase matching condition and THz generation between 1.3 THz and 2.7 THz, for optical pump around 1.6 μm, are investigated. Our calculations predict that the device produces a relatively high THz output power of 11.07 μW from a 4 cm long waveguide at 2 THz.     

非线性光学晶体4-(4-二甲基氨基苯乙烯基)甲基吡啶对甲基苯磺酸盐的制备与性能研究

采用籽晶法制备了大体积高质量的4-(4-二甲基氨基苯乙烯基)甲基吡啶对甲基苯磺酸盐(DAST)晶体，对制备条件进行了优化，对DAST晶体X射线衍射谱图中的主要峰进行了指标化.另外，还对所制备的DAST晶体的透光性、热稳定性进行了研究， 并对265℃的焙烧产物进行了X射线衍射 (XRD)和傅里叶变换红外光谱(FT-IR)测试，证明了260℃是DAST晶体的熔化相变温度， 说明采用熔融法制备DAST晶体是可行的；同时还对DAST晶体的热失重过程进行了初步探讨. 关键词： 4-(4-二甲基氨基苯乙烯基)甲基吡啶对甲基苯磺酸盐 晶体生长 X射线衍射 热稳定性     

Terahertz generation with tandem seeded optical parametric generators

A simple difference frequency generation (DFG) scheme based on two seeded optical parametric generators is presented as a tunable terahertz (THz) source. Using the nonlinear optical crystal 4-dimethylamino-N-methyl-4-stilbazolium-tosylate (DAST) as the DFG crystal, our system has demonstrated continuous and seamless tunable operation from 1.6 to 4.5 THz. The output bandwidth of the THz source is 2.4 GHz. The utility of the source over this spectral range is demonstrated by measuring a high-resolution transmission spectrum of water vapor in air.     

Generation of widely tunable Fourier-transform-limited terahertz pulses using narrowband near-infrared laser radiation

Widely tunable, Fourier-transform-limited pulses of terahertz (THz) radiation have been generated using (i) crystals of the highly nonlinear organic salt 4-N,N-dimethylamino-4′-N′-methyl stilbazolium tosylate (DAST), (ii) zinc telluride (ZnTe) crystals, (iii) gallium phosphide (GaP) crystals, and (iv) low-temperature-grown gallium arsenide (LTG-GaAs) photomixers with THz spiral antennas. Outputs from two narrowband (Δν < 1 MHz, λ ∼ 800 nm) cw titanium-doped sapphire (Ti:Sa) ring lasers with a well-controlled frequency difference were shaped into pulses using acousto-optic modulators (AOM), coupled into an optical fiber, pulse amplified in Nd:YAG-pumped Ti:Sa crystals and used as optical sources to pump the THz emitters. The THz radiation was detected over a broad frequency range and its bandwidth was determined to be ∼10 MHz. The spectroscopic potential of the THz source is illustrated by the absorption spectrum of a pure rotational transition of OCS.     

Use of the organic crystal DAST for terahertz beam applications

We report the use of the organic crystal DAST as a freely propagating electromagnetic-wave sensor at terahertz (THz) frequency. We also report the result of using a DAST crystal as a mid-IR THz emitter. Compared with the optical rectification from our best ZnTe emitter, that obtained by use of DAST demonstrates a sixfold enhancement of radiation at 7-20 THz.     

Widely tunable terahertz-wave generation using an N-benzyl-2-methyl-4-nitroaniline crystal

Widely tunable terahertz (THz)-wave generation using difference frequency generation (DFG) in an organic N-benzyl-2-methyl-4-nitroaniline (BNA) crystal was demonstrated. To our knowledge, this is the first report of THz-wave generation by BNA DFG. Large, high-quality single crystals of BNA (phi 8 mm x 30 mm) were grown using the vertical Bridgman method. The nonlinear optical (NLO) coefficient d(33) of the BNA crystal is approximately 234 pm/V, which is the largest value reported for any yellow NLO material. The collinear phase-matching condition of the type-0 configuration is satisfied using a 0.7-1 microm band pump wavelength. We generated THz waves using an organic BNA crystal; the generation range is 0.1-15 THz.     

利用国内生长的有机晶体DAST作为THz源的研究

利用时域光谱技术分别测量了通过光整流法在国内新生长的有机晶体DAST和国际常用的高效能THz晶体ZnTe中产生的THz脉冲的时域光谱,也测量和分析了有机晶体DAST在THz波段的色散和吸收特性,并通过热辐射探测计(4.2 K Si-bolometer)测量了THz脉冲的绝对能量。结果表明,国内新生长的有机晶体DAST的确是一种高效率的THz产生晶体,优化生长条件后将可得到更高的产生效率。     

Widely linear and non-phase-matched optical-to-terahertz conversion on GaSe:Te crystals

We demonstrate the widely linear and broadband terahertz (THz) generation on GaSe:Te crystals by femtosecond laser pulses. It was found that the dopant, Te atoms, in GaSe crystals significantly enhances the efficiency of THz generation, and its central frequency can be tuned by varying the crystal thickness through non-phase-matched optical rectification. Moreover, the wide-ranging linearity for the optical-to-THz conversion and central-frequency-tunable THz generation promise for GaSe:Te crystals to be potential materials for high-power (>1.36 μW) THz applications.     

Characteristics of efficient few-cycle terahertz radiation generated in as-grown nonlinear organic single crystals

We investigated efficient terahertz wave generation by optical rectification in as-grown nonlinear organic single crystal HMQ-T (2-(4-hydroxy-3-methoxystyryl)-1-methylquinolinium 4-methylbenzenesulfonate). Optimal thickness of crystals directly available by a slow cooling method in methanol solution enabled us to achieve high-field few-cycle THz waves at 800-nm pumping. With 95-mW pumping at 1-kHz repetition rate, an optical-to-THz conversion efficiency of 2.7 × 10⁻⁴ was achieved and the THz electric field strength, measured by electro-optic sampling, was as high as 110.1 kV/cm. Such an efficient THz source based on as-grown HMQ-T crystals can be used for investigation of various nonlinear phenomena in the THz spectral region.     

Highly efficient terahertz electro-optic sampling by material optimization at 1060 nm

Different electro-optic crystals (CdTe, DAST, GaAs, GaP, and ZnTe) are investigated with respect to their ability as detection crystals for terahertz pulse electro-optic sampling at a wavelength of 1060 nm. Calculations of the detection response are in good qualitative agreement with experimental results. While CdTe shows the strongest signal for applications below 1 THz, GaP exhibits a broadband spectrum. By the choice of an adequate crystal a comparable detection efficiency to electro-optic sampling at a wavelength of 800 nm can be achieved.     

Far-infrared properties of DAST

Using terahertz time-domain spectroscopy, we have measured the index of refraction and the absorption coefficient of the organic ionic salt 4-N, N-dimethylamino-4?-N?-methyl-stilbazolium tosylate (DAST). This promising organic electro-optic material exhibits strong absorption and dispersion for frequencies above 1 THz at both room temperature and 83 K. No reduction in the absorption strength is observed when DAST is cooled, suggesting a single-phonon origin of the resonances. A simple vibration of the anion and cation of the salt is suggested as the origin of the exceptionally strong far-infrared absorption and the high-frequency electro-optic properties of DAST.     

High-performance fiber-laser-based terahertz spectrometer

We have developed a rapid scanning terahertz (THz) spectrometer based on a synchronized two-fiber-laser system. When the system is set to the asynchronous optical sampling mode, THz spectra extending to 3 THz can be acquired within 1 μs at a signal-to-noise ratio of the electric field of better than 20. Signal averaging results in a dynamic range of more than 60 dB, and frequency components of more than 4 THz can be detected. When the lasers are set to the same repetition rate, electronically controlled optical sampling at a rate of 2.5 kHz is demonstrated, making the system versatile for different spectroscopic applications. Finally, we compare the THz emission spectra of a photoconductive switch that is pumped at 780 nm and a nonlinear DAST crystal excited at 1550 nm. We find that the spectral range of the spectrometer is significantly enhanced at higher frequencies, while the dynamic range remains constant.     

Difference-Frequency Generation of THz Radiation via Parametric Three-Wave Interaction in CdTe and ZnTe Crystals

Difference-frequency generation of terahertz (THz) radiation in a collinear single-crystal scheme with distributed feedback implemented by means of parametric interaction of counterpropagating optical waves in a periodically inhomogeneous medium exhibiting quadratic nonlinearity is investigated. Using ZnTe and CdTe crystals optically pumped at λ = 0.77 and 1.06 μm, respectively, as an example, the possibility of obtaining parametric generation of THz radiation with an optical-to-THz conversion efficiency exceeding 10^–3 (with an extremely narrow line of oscillation of less than 4 GHz for ZnTe and less than 9 GHz for CdTe at 1 THz) is demonstrated in the undepleted-pump-intensity approximation. The obtained results can be used for construction of narrow-band lasers in the THz frequency range with an output power (in the quasicw regime of oscillation) of about 10⁵ W/cm².     

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.     

太赫兹波发射晶体的亚波长微棱锥增透结构的设计与实验研究

光学整流方法产生太赫兹(THz)辐射常用的非线性发射晶体在THz波段都具有较高的折射率, 使得很大一部分THz波由于晶体表面的菲涅尔反射而无法有效耦合输出. 本文报道了GaP晶体THz波发射器输出表面上亚波长微棱锥增透结构的设计和实验研究. 利用有效介质模型在理论上验证了亚波长光栅结构的增透效果, 并进一步设计了适用于不同频段的增透结构的参数. 实验中, 通过微机械加工手段在GaP晶体输出端面刻划了多种亚波长微棱锥结构, 验证了其增透效果及参数对增透频带的关系. 理论与实验的符合证明该设计思想也可用于其他THz波发射晶体. 关键词： THz波 光学整流 亚波长微棱锥增透结构 微加工