Single-Cycle Terahertz Pulse Generation from OH1 Crystal via Cherenkov Phase Matching

OH1 crystal is an organic nonlinear optical crystal with a large nonlinear optical constant. However, it has dispersion of refractive indices in the terahertz (THz) frequency. This limits the frequencies that satisfy the phase matching conditions for THz wave generation. In this study, we addressed the phase matching conditions for THz wave generation by combining an OH1 crystal with prism-coupled Cherenkov phase matching. We observed the generation of single-cycle THz pulses with a spectrum covering a frequency range of 3 THz. These results prove that combining prism-coupled Cherenkov phase matching with nonlinear optical crystals yields a THz wave generation method that is insusceptible to crystal dispersion.     

Monochromatic and Tunable Terahertz Source Based on Nonlinear Optics

Recent progresses made by authors on monochromatic and tunable terahertz （THz） generation based on nonlinear optics are reviewed, including THz parametric oscillation （TPO） and difference frequency generation （DFG）. From the technical point of view, we develop extra- and intra-cavity surface-emitted TPO, as well as DFG with QPM-GaAs crystal. From the point of view of mechanism, Cherenkov phase-matching is comprehensively investigated in both bulk crystal and planar waveguide. A novel scheme for cascading enhanced Cherenkov DFG in waveguide is proposed. From the point of view of material, organic crystal 4-N,N-dimethylamino-4＇-N＇-methyl-stibazolium tosylate （DAST） is utilized as the nonlinear medium.     

Review of a New IR Nonlinear Optical BaGa4Se7 Crystal

A newly grown BaGa4Se7 crystal has been synthesized via the Bridgman-Stockbarger technique. This new crystal has advantages of high nonlinear optics (NLO) coefficients, high laser damage thresholds, and wide transparent regions. The BaGa4Se7 crystal has bright application prospects as a nonlinear gain medium in mid-infrared and terahertz regions. In this paper, the crystalline structure and synthetic method of the BaGa4Se7 crystal are introduced. The refractive indices and absorption coefficients along three dielectric axes between 0.1 THz and 1.0 THz are also obtained. The terahertz difference frequency generation (THz-DFG) characteristics based on the BaGa4Se7 crystal in the frequency range of 0.1 THz to 1.0 THz are analyzed theoretically and the phase-matching conditions are calculated. The application of BaGa4Se7 crystals in terahertz wave generation is also discussed.     

基于双温耦合模型的太赫兹晶体损伤阈值分析

飞秒激光通过非线性光学整流效应产生太赫兹(THz)波时,THz波转换效率会随着飞秒激光功 率的增大而明显提高。然而,飞秒激光功率过高会造成非线性晶体损伤,进而影响THz波的 产生及输出, 因而对飞秒激光作用下非线性晶体的损伤阈值进行研究具有重要意义。本文在经典的双温模 型基础上,引 入电子激发、载流子吸收等电离过程的影响,建立了飞秒激光作用下非线性THz晶体损伤 阈值的预估模 型。采用有限差分法,数值模拟了飞秒激光辐照下THz晶体的温度场变化,并据此对 晶体损伤阈值进行 预估。在此基础上,分析比较了LiNbO₃、ZnTe和ZnSe 3种THz晶体的损伤 阈值随激光脉宽的变化规 律。结果表明,晶体的禁带宽度和比热容越大 ,晶体的损伤 阈值就越大;LiNbO₃晶体因其具有更高的损伤阈值,在产生高功率THz波方面 具有更大的优势。     

产生太赫兹辐射源的Nd:YAG双波长准连续激光器

产生太赫兹波辐射的方法可分为电子学和光子学两大类.在光子学领域,非线性光学差频方法是获取高功率、低成本、便携式、室温运转太赫兹波的主要方法之一.实验研究了激光二极管(LD)端面抽运Nd:YAG1319 nm/1338 nm双波长准连续线偏振运转激光器,理论计算了输出双波长在非线性晶体DAST(4-N,N-dimethylamino-4'-N-'methyl-stilbazolium tosylate)中差频产生太赫兹辐射的平均功率.在重复频率50 kHz时,双波长激光平均输出功率达到2.22 W,斜率效率12.72%,线偏振度0.983,脉冲宽度71.91 ns.M2因子仅为1.165,不稳定性小于0.487%.根据非线性差频理论,计算出可在1 mm厚DAST晶体中获得4.71 mw的3.23 THz高相干性太赫兹波辐射.这两条非常接近的谱线为进一步通过非线性光学差频方法获得高相干性太赫兹波提供了理论基础.     

Kilowatt-peak Terahertz-wave Generation and Sub-femtojoule Terahertz-wave Pulse Detection Based on Nonlinear Optical Wavelength-conversion at Room Temperature

Intense Terahertz (THz)-wave generation and highly sensitive THz-wave detection were obtained by wavelength conversion with nonlinear optical susceptibility χ⁽²⁾ of LiNbO₃ crystals. Maximum peak output of about 50 kW (5 μJ/pulse) was demonstrated in an injection-seeded THz-wave parametric generator pumped by post-amplified emission from a microchip Nd:YAG laser. Using the sub-nanosecond pulse duration of the laser proposed herein provides effective mitigation of stimulated Brillouin scattering in LiNbO₃, producing higher gain for wavelength conversion between near-infrared (near-IR) pump light and THz waves. Monochromatic THz radiation was obtained in the continuous tuning range of 0.7–2.9 THz. Additionally, highly sensitive THz-wave detection was demonstrated based on up-conversion from THz waves to near-IR light as well as efficient THz-wave generation. The signal generated with non-collinear phase-matching condition showed spectroscopic detection on the screen apart from the LiNbO₃ crystal. Highly sensitive detection with minimum energy of about 80 aJ/pulse (0.8 μW at peak) and a large dynamic range of more than 100 dB were achieved in this experiment.     

The Polarization and Efficiency of the Terahertz Pulses Generated by Tilted-Pulse-Front Pumping Scheme

Optical rectification of laser pulses in LiNbO₃ by tilted-pulse-front pumping(TPFP) is a powerful way to generate terahertz(THz) pulses. However, comprehensive theoretical analysis is still lack. In this work, we first established and presented a detailed theoretical model for TPFP scheme, which then was used to analyze the pump beam polarization dependent terahertz pulses generated by this scheme. The terahertz pulses polarization and generation efficiency for various pump beam polarization angle were investigated by using nonlinear susceptibility tensor of LiNbO₃ crystal. The results indicate that one can change the polarization state of the terahertz pulse by changing the pump beam polarization.     

Compact High-Repetition-Rate Monochromatic Terahertz Source Based on Difference Frequency Generation from a Dual-Wavelength Nd:YAG Laser and DAST Crystal

Although high-repetition-rate dual-wavelength Nd:YAG lasers at 1319 and 1338 nm have been realized for quite a long time, we have employed it in generating monochromatic terahertz (THz) wave in this paper for the first time. The dual-wavelength laser was LD-end-pumped and acousto-optically (AO) Q-switched with the output power of watt level operating at different repetition rates from 5.5 to 30 kHz. Using a 0.6-mm-thick organic nonlinear crystal DAST for difference frequency generation (DFG), a compact terahertz source was achieved at 3.28 THz. The maximum average output power was about 0.58 μW obtained at a repetition rate of 5.5 kHz, corresponding to the conversion efficiency of about 6.4?×?10^?7. The output power scaling is still feasible with higher pump power and a longer nonlinear DFG crystal. Owing to the compactness of the dual-wavelength laser and the nonlinear crystal, a palm-top terahertz source is expected for portable applications such as imaging and so on.     

Compact Tunable Narrowband Terahertz-Wave Source Based on Difference Frequency Generation Pumped by Dual Fiber Lasers in MgO:LiNbO<Subscript>3</Subscript>

We demonstrate a high-average-power, single longitudinal-mode, and tunable terahertz (THz)-wave source based on difference frequency generation (DFG) in a MgO:LiNbO₃ (MgO:LN) crystal. The waves for DFG are generated using a pair of Yb-doped pulsed fiber lasers with a master oscillator power fiber amplifier configuration. The average power of the THz-wave output reaches 450 μW at 1.07 THz (280 μm) at a linewidth of 7.2 GHz, and the tunability ranges from 0.35 to 1.07 THz under the pulse repetition frequency of 500 kHz. A short burn-in test of the THz wave is also carried out, and the output power stability is within ± 5% of the averaged power without any active stabilizing technique. The combination of MgO:LN-DFG and stable and robust fiber laser sources is highly promising for the development of high-average-power THz-wave sources, particularly in the high transmission sub-THz region. This approach may enable new applications of THz-wave spectroscopy in imaging and remote sensing.     

Terahertz Imaging System for Medical Applications and Related High Efficiency Terahertz Devices

A terahertz (THz) imaging system and high efficient terahertz sources and detectors for medical applications were developed. A fiber laser based compact time domain terahertz tomography system was developed with a high depth resolution of less than 20 μm. Three-dimensional images of porcine skin were obtained including some physical properties such as applied skin creams. The discrimination between healthy human tissue and tumor tissue has been achieved using reflection spectra. To improve the THz imaging system, a ridge waveguide LiNbO₃ based nonlinear terahertz generator was studied to achieve high output power. A ridge waveguide with 5-7 μm width was designed for high efficiency emission from the LiNbO₃ crystal by the electro-optic Cherenkov effect. Terahertz electronic sources and detectors were also realized for future imaging systems. As electronic source devices, resonant tunneling diode (RTD) oscillators with a patch antenna were fabricated using an InGaAs/InAlAs/AlAs triple barrier structure. On the other side, Schottky barrier diode (SBD) detectors with a log-periodic antenna were fabricated by thin-film technology on a Si substrate. Both devices operate above 1 THz at room temperature. This electronic THz device set could provide a future high performance imaging system.     

Temperature Dependence of Crystal Structure and THz Absorption Spectra of Organic Nonlinear Optical Stilbazolium Material for High-Output THz-Wave Generation

A stilbazolium material comprising 4-dimethylamino-N′-methyl-4′-stilbazolium tosylate (DAST), which has a large nonlinear optical susceptibility, was studied for application in terahertz (THz)-wave generation. The temperature-dependent structure of the DAST crystal was measured by using powder X-ray diffraction from ?100 to 200 °C, indicating a volume expansion of 4.6 %. The lattice constants show anisotropic thermal expansion. Also, the temperature dependence of THz absorption spectra was measured by terahertz time-domain spectroscopy (THz-TDS) in the temperature range varying from ?80 to 88.1 °C. A strong absorption peak was found at around 1 THz, shifting slightly toward a lower frequency with increasing temperature. The temperature dependence of the THz spectra was compared with that of X-ray diffraction. The shifting of THz-vibrational frequencies of the DAST crystal suggests that the change in its lattice structure is temperature dependent.     

飞秒激光作用下光整流晶体的损伤阈值分析

光整流效应是产生太赫兹波的有效途径之一,而产生高功率太赫兹波则需要采用高强度的飞秒激光激励光整流晶体,但激光强度过大会造成晶体损伤,从而严重影响高功率太赫兹波的输出。因此,对光整流晶体的损伤阈值进行研究具有重要的理论意义与实用价值。通过对飞秒激光与非线性光整流晶体材料相互作用物理过程进行分析,建立了飞秒激光作用下光整流晶体损伤阈值的预估模型,比较分析了铌酸锂、碲化锌和硒化锌三种晶体材料的损伤阈值随飞秒激光脉宽的变化规律。结果表明,当飞秒激光的脉宽相对较小时,光致电离在整个作用过程中占主导地位,随着脉宽的增大,雪崩电离逐渐起主要作用;雪崩电离速率和光致电离速率均与晶体的禁带宽度密切有关,光整流晶体材料禁带宽度越大,晶体材料的损伤阈值越高;铌酸锂晶体的损伤阈值明显高于碲化锌和硒化锌晶体,更适合用于高功率太赫兹波的产生。     

Terahertz Phonon Mode Engineering of Highly Efficient Organic Terahertz Generators

For terahertz (THz) wave generators based on organic electrooptic crystals, their intrinsic phonon modes are playing an essential role in THz generation characteristics. Here, this study proposes an effective design strategy for THz phonon mode engineering of organic electrooptic salt crystals for efficient optical‐to‐THz frequency conversion. To reduce phonon‐mode intensity, strongly electronegative trifluoromethyl group acting as strong hydrogen‐bond acceptor is incorporated into molecular anions. New 2‐(4‐hydroxy‐3‐methoxystyryl)‐1‐methylquinolinium 4‐(trifluoromethyl)benzenesulfonate (HMQ‐4TFS) crystals exhibit a relatively small absorption coefficient in the THz spectral range between 0.5 and 4 THz, which is attributed to suppressed molecular vibrations due to strong hydrogen bonds involving the 4TFS anion. In addition, HMQ‐4TFS crystals possess a very large macroscopic optical nonlinearity, comparable (or even higher) to benchmark stilbazolium crystals. Based on the low‐intensity THz phonon modes and the large optical nonlinearity, a 0.37 mm thick HMQ‐4TFS crystal pumped with 150 fs infrared laser pulses facilitates very efficient THz wave generation by optical rectification, delivering 23 times higher peak‐to‐peak THz electric field than the widely used standard inorganic ZnTe crystal (1.0 mm thick) and a broader spectral bandwidth. Therefore, strongly electronegative groups introduced into molecular salt electrooptic crystals provide a very promising design strategy of THz phonon mode engineering for developing intense broadband THz sources.     

基于非线性光学差频及参量效应的太赫兹源

基于非线性光学技术的THz源具有其独特的性能和优点,将基于非线性光学差频原理和光学参量效应,从理论上研究并分析THz波与抽运光、闲频光及相位匹配角之间的关系,得到THz波输出的条件和范围,并设计出宽波段连续可调的THz源。以调QNd∶YAG激光器和光学参量振荡器(OPO)作为抽运源,以GaSe和MgO∶LiNbO3晶体作为差频非线性晶体,根据相位匹配理论及光学参量效应,搭建两套THz波产生系统。其中,基于光学参量效应的THz辐射源有效地产生出THz信号。     

基于CO2激光的AgGaS2差频产生太赫兹波的数值分析

采用中红外CO₂激光差频产生太赫兹波是提高转换效率和输出功率的一种有效方法。根据差频过程中的三波互作用对AgGaS₂晶体进行了理论分析,数值模拟了oeo类和oee类两种匹配条件下差频产生太赫兹波的角度调谐曲线,并计算了光波在晶体中的走离角和允许参量。另外,还考虑了晶体的有效非线性系数和理论功率转换效率。研究结果表明,AgGaS₂晶体适用于中红外CO₂激光差频产生可广泛调谐的太赫兹波。     

ZnTe晶体对太赫兹波的电光响应及极化匹配

给出了ZnTe电光晶体折射率和吸收系数随太赫兹波频率而变化的计算曲线,比较了太赫兹波在ZnTe中传播时的相速度和群速度。通过与太赫兹频率和晶体厚度相关的电光效率响应函数,理论计算了ZnTe电光晶体对太赫兹脉冲的探测电光响应,得到了晶体厚度与探测到的太赫兹频谱宽度的定性关系,从计算结果中找到了ZnTe电光晶体在5.3 THz和6.2 THz等多个频点的探测盲点,这些探测盲点来自于ZnTe电光晶体与相应频点太赫兹波的栅格共振吸收。结合自制的大口径太赫兹光导天线和1 kHz脉冲重复频率的太赫兹时域光谱实验系统,通过差分探测技术,从实验上得到了太赫兹波极化方向与〈110〉型ZnTe晶体晶轴方向的六个最佳匹配角度,给出了太赫兹电场最大值随晶轴与太赫兹波极化方向之间夹角变化的曲线及经验公式,这将有利于在实践中对该现象的深入理解和对探测灵敏度的有效提高。     

Terahertz Generation and Optical Properties of Lithium Ternary Chalcogenide Crystals

We have investigated the generation of THz radiation in lithium ternary compounds LiInSe₂, LiGaSe₂, LiInS₂, LiGaS₂ and characterized these materials by THz time-domain spectroscopy. Using 800 nm femtosecond excitation pulse, all crystals produce THz radiation due to an optical rectification corresponding to the nonlinear optical coefficient d ₃₃. We have measured refractive indices along the x-axis and the z-axis for all crystals in the range 150–700 μm and fitted them by using Sellmeier equation. With respect to the obtained results, velocity-matching between the incident laser pulse and the generated THz wave cannot be achieved at 800 nm, but for shorter wavelengths. Hence, an enhanced THz generation in Lithium ternary compounds may be observed by using a laser emitting below 800 nm.     

GaAs参量振荡产生太赫兹波的腔相位匹配研究

基于腔相位匹配的方法,研究了GaAs微片状晶体构成的光学微腔光参量振荡产生太赫兹波的条件与参数设计.计算了腔相位匹配下GaAs晶体的最优化腔长,通过调节GaAs晶体的温度研究了太赫兹波的输出情况,模拟了不同波长下最低的能量阈值.结果表明,在完全相位匹配很难实现的情况下,采用腔相位匹配能很容易地实现大范围的太赫兹波调谐输出.结果为小型化光学太赫兹源的实验与理论研究提供了参考.     

Characteristics of THz-wave radiation using a monolithic grating coupler on a LiNbO3 crystal

Wide tunable terahertz (THz) wave generation was successfully demonstrated utilizing a grating coupler fabricated on the surface of a LiNbO₃ crystal which was pumped by a Q-switched Nd:YAG laser. In this paper, we report the detailed characteristics of the oscillation and the radiation including tunability, spatial and temporal coherency, directivity, and efficiency. Oscillation using a LiTaO₃ crystal was also performed, in which experimental phasematching condition values agreed well with the calculated one.     

Yellow‐Colored Electro‐Optic Crystals as Intense Terahertz Wave Sources

This study presents newly developed yellow‐colored organic electro‐optic crystals to provide high terahertz (THz) wave generation efficiency. Compared with currently existing red‐ or orange‐colored electro‐optic crystals, which are used for most benchmark organic THz sources, yellow‐colored crystals have additional superior advantages for THz wave generation, e.g., higher transparency in the visible wavelength range with accompanying different phase‐matching possibilities. The new yellow‐colored crystals consist of a highly nonlinear optical 4‐(4‐hydroxystyryl)‐1‐methylpyridinium (OHP) cation, with a relatively short wavelength of maximal absorption at 390 nm in solution, and various halogen‐substituted benzenesulfonate anions, with strong secondary‐bonding ability. OHP 4‐chlorobenzenesulfonate (OHP‐CBS) crystals exhibit large off‐resonant macroscopic optical nonlinearity and high transparency, with a cut‐off wavelength for solid‐state absorption near 490 nm. OHP‐CBS crystals provide excellent THz wave generation characteristics based on optical rectification. A 0.53 mm thick OHP‐CBS crystal delivers ≈27 times higher optical‐to‐THz conversion efficiency and a much broader spectrum bandwidth compared with the standard 1.0 mm thick ZnTe at 1300 nm pumping. Particularly, compared with a benchmark organic quinolinium crystal with a similar thickness of 0.55 mm, OHP‐CBS crystals exhibit 1.7 times higher optical‐to‐THz conversion efficiency, and show a significantly different THz spectral shape.