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。     

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.     

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.     

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.     

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。     

Difference-frequency terahertz-wave generation from 4-dimethylamino-N-methyl-4-stilbazolium-tosylate by use of an electronically tuned Ti:sapphire laser

Among nonlinear materials, the organic ionic salt crystal 4-dimethylamino- N -methyl-4-stilbazolium-tosylate (DAST) is known for its large nonlinearity. We generated a coherent terahertz (THz) wave, using DAST, from the difference frequency between two oscillating wavelengths of an electronically tuned Ti:sapphire laser. In LiNbO(3), LiTaO(3), KTiOPO(4), and GaP crystals, THz-wave generation was not observed under the same experimental conditions. This result proves the high efficiency of DAST crystals for generation of difference-frequency THz waves.     

GaP波导型发射器产生频率可调谐太赫兹脉冲

报道了利用脉宽可调的光子晶体光纤飞秒激光放大器抽运矩形波导结构的GaP晶体太赫兹(THz) 发射器产生频率可调谐的超快THz脉冲.非线性晶体中光整流过程产生的THz辐射频率随抽运光脉冲宽度而 变化. GaP波导THz发射器可通过波导的几何尺寸来控制色散,以达到增加有效作用长度和提高输出功率的目的. 不同横截面尺寸的波导型发射器的THz辐射峰值频率随相位匹配条件的改变而改变,加以脉宽调节技术, 可以在大频谱范围获得频谱精细可调的THz脉冲.实验中在1 mm×0.7 mm的波导型THz发射器中获得了 频率可调谐的THz脉冲.提出实现THz辐射频率大范围调谐的GaP波导型阵列发射器的实施方案.     

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.     

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.     

〈331〉晶向ZnTe单晶的太赫兹辐射-探测性能理论研究

根据光整流效应辐射太赫兹理论,计算了〈331〉晶向ZnTe单晶的太赫兹辐射性能.通过与〈110〉、〈111〉晶向对比,当晶体方位角为0°或180°时,利用〈331〉晶向ZnTe单晶辐射太赫兹信号可以与〈111〉晶向相当,强于〈110〉晶向.利用电光取样原理,计算了〈331〉晶向ZnTe单晶的太赫兹探测性能,通过理论计算为〈331〉晶向ZnTe 晶体有效辐射太赫兹波提供理论依据.     

Performance of combined 〈1 0 0〉-〈1 1 0〉 ZnTe crystals in an amplified THz time-domain spectrometer

In this work we report on the performance of combined index-matched ZnTe 〈1 1 0〉-〈1 0 0〉 THz emitters and detectors for reduction of etalon effects in a nonlinear crystal-based THz time-domain spectrometer, driven by an amplified femtosecond laser. We demonstrate that the application of a combined electrooptic detector crystal reduces the strength of the first etalon and the average spectral dynamic range oscillations by a factor of two. We also show that even in a simple emitter configuration the emitter-related etalon is significantly reduced due to the transient dielectric effects of carriers created by two-photon absorption in the emitter.     

Terahertz time-domain spectrometer with module heads coupled to photonic crystal fiber

We constructed optical-fiber-based THz time-domain spectrometers (THz TDSs) with standard single-mode fibers (SSMFs) and large-mode-area photonic crystal fibers (LMA PCFs) and compared those to THz waves and spectra. The optical fibers are used for guiding optical pulses from ultra-fast lasers to a THz emitter and detector. The LMA-PCF-based THz TDS exhibits increased bandwidth from 1 to 2 THz and increased field amplitude by a factor of four compared with the SSMF-based THz TDS under the relatively higher excitation power of ultra-fast lasers. This improvement results from LMA PCFs that are suitable for high-power transmission without introducing nonlinear effects. We also fabricated compact THz emitter and detector module heads, which are connected with LMA PCFs. The LMA-PCF-based THz TDS had THz radiation power and bandwidth comparable with those obtained by a conventional THz TDS with a free-space optical arrangement. PACS 42.72.Ai; 42.65.-k; 42.81.DP     

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.     

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.     

Simultaneous all-solid-state multi-wavelength lasers --- a promising pump source for generating highly coherent terahertz waves

A diode-end-pumped Nd:YAG dual-wavelength laser operating at 1319 and 1338 nm is demonstrated. The maximum average output power of the quasi-continuous wave linearly polarized dual-wavelength laser is obtained to be 2.1 W at a repetition rate of 50 kHz with an output power instability of less than 0.38% and beam quality factor M² of 1.45. Using the two lines, the highly coherent and narrow linewidth terahertz radiation of 3.23 THz can be generated in an organic 4-N, N-dimethylamino--methyl-stilbazolium tosylate (DAST) crystal. Meanwhile, the multi-wavelength red laser at 659.5, 664 and 669 nm is generated by frequency doubling and sum frequency processes in a lithium triborate (LBO) crystal. The average red laser output power is enhanced up to 1.625 W at a repetition rate of 15 kHz with an output power instability of better than 0.53% and beam quality factor M² of 6.05. Using the three lines, it is possible to generate the multi-wavelength THz radiation of 3.3, 3.43 and 6.73 THz in an appropriate difference frequency crystal.     

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.     

Effects of Pumping Sizes on THz Radiation Based on Ultrashort Light Pulse Optical Rectification for High Spatial Resolution T-Ray Imaging

We present our experimental studies on the effects of the pumping sizes on THz radiation based on ultrashort light pulse optical rectification for high spatial resolution T-Ray imaging. Our experiments show that high spatial resolution T-ray imaging requires both thin THz emitter and sample, and rigorous tolerance of the gap between the sample and the emitter, as well as small pumping size which usually much smaller compared with THz wavelength. Such a small pumping size results in dramatic decrease of the THz wave power, which originates from strong diffraction of THz wave, the depolarization of the focused tightly pumping beam, the spatial filtering of the emitter exit-surface, and the strong phase-mismatching between the pumping and the high spatial Fourier components of the THz signal, rather than two-photon absorption.     

ZnTe晶体中光学整流产生的THz辐射及其电光探测研究

借助抽运-探测技术研究了ZnTe晶体中光学整流产生的太赫兹(THz)辐射，利用ZnTe晶体的线性电光效应探测THz辐射场分布，观察到了较窄(约为0.2 ps)的THz场分布及相应较宽(响应超过4 THz，半峰宽约为2.4 THz)的THz频谱，并运用琼斯矩阵对实验结果进行了理论拟合. 研究了飞秒激光脉冲波长(750—850 nm)、脉冲宽度(56—225 fs)和晶体旋转与THz辐射产生的关系. 同时改变探测光偏振方向进行偏振调制，并从理论上分析了偏振调制对THz辐射探测的影响. 关键词： THz辐射 光学整流 电光探测 ZnTe     

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.     

铁磁异质结构中的超快自旋流调制实现相干太赫兹辐射

利用飞秒激光脉冲在生长于二氧化硅衬底上的W/CoFeB/Pt和Ta/CoFeB/Pt两类铁磁/非磁性金属异质结构中实现高效、宽带的相干THz脉冲辐射.实验中, THz脉冲的相位随外加磁场的反转而反转,表明THz辐射与样品的磁有序密切相关.为了考察三层膜结构THz辐射的物理机制,分别研究了构成三层膜结构的双层异质结构(包括CoFeB/W, CoFeB/Pt和CoFeB/Ta)的THz辐射.实验结果都与逆自旋霍尔效应相符合, W/CoFeB/Pt和Ta/CoFeB/Pt三层膜结构所辐射的THz强度优于同等激发功率下的ZnTe (厚度0.5 mm)晶体.此外,还研究了两款异质结构和ZnTe的THz辐射强度与激发光脉冲能量密度的关系,发现Ta/CoFeB/Pt的饱和能量密度略大于W/CoFeB/Pt的饱和能量密度,表明自旋电子在Ta/CoFeB/Pt中的界面积累效应相对较小.