较高阶非线性抽运-探测过程中的空间效应

在飞秒抽运一探测光谱技术中，空间分辨的探测光信号反映了在不同空间位置的材料的非线性效应。当抽运光强度增大时，探测光信号中会出现明显的高阶特别是五阶非线性效应。利用劈裂算子方法直接解决了一维非线性传播方程的问题。在数值模拟中，研究了在不同抽运强度和位置下的抽运一探测过程中的五阶非线性效应。在足够高的抽运场下，探测信号出现清晰的振荡，显示了三阶和五阶非线性效应之间的干涉。当空间位置离抽运场中心足够远时，五阶比三阶非线性效应的衰减快得多，对其物理机制和趋势进行了定性的讨论。

超短脉冲激光光束被局域体全息光栅衍射的性质分析

利用二维耦合波理论,分析了超短脉冲激光光束被完全重叠型的局域体全息光栅衍射的时空变化性质,给出了衍射和透射脉冲激光光束沿光栅出射边界的强度时空分布。以LiNbO3晶体为例,数值研究了衍射光脉冲强度沿光栅出射边界的分布和脉冲波形的变化及光栅的总衍射效率受光栅二维尺寸、入射角度、光栅折射率调制度及入射脉冲的脉冲时域半峰全宽等条件的影响而变化的情况。与一维体全息光栅对超短脉冲激光光束衍射的性质,及此光栅对连续光衍射的性质作比较,给出了合理选择光栅参量及入射条件以在光栅出射边界上得到总衍射效率较大且分布较均匀的衍

基于多台阶反射光栅的飞秒脉冲压缩装置

反射式光栅对是一种具有负色散性质的器件,可用于飞秒激光脉冲的压缩和展宽,具有无材料色散的优点。给出了一种基于多台阶反射光栅的脉冲压缩装置。该装置为倍密度光栅结构,由两个周期分别为40μm和20μm的四台阶反射式光栅组成。实验得到的衍射效率可以达到70%以上,输入脉冲经过两个光栅的衍射后会按原路返回,从而达到色散补偿的效果。利用此压缩装置,脉冲宽度为66.8 fs的输入脉冲压缩至接近傅里叶变换极限脉冲,即46.6 fs,由此证明只要多台阶光栅效率足够高,此装置就有可能成为不同于棱镜对进行飞秒脉冲腔内和腔外压缩的另一种途径。

On Ultrafast Time-Domain TeraHertz Spectroscopy in the Condensed Phase: Linear Spectroscopic Measurements of Hydrogen-Bond Dynamics of Astrochemical Ice Analogs and Nonlinear TeraHertz Kerr Effect Measurements of Vibrational Quantum Beats

Much of the chemistry that affects life on planet Earth occurs in the condensed phase. The TeraHertz (THz) or far-infrared (far-IR) region of the electromagnetic spectrum (from 0.1 THz to 10 THz, 3 cm^-1 to 300 cm^-1, or 3000 μm to 30 μm) has been shown to provide unique possibilities in the study of condensed-phase processes. The goal of this work is to expand the possibilities available in the THz region and undertake new investigations of fundamental interest to chemistry. Since we are fundamentally interested in condensed-phase processes, this thesis focuses on two areas where THz spectroscopy can provide new understanding: astrochemistry and solvation science. To advance these fields, we had to develop new instrumentation that would enable the experiments necessary to answer new questions in either astrochemistry or solvation science. We first developed a new experimental setup capable of studying astrochemical ice analogs in both the TeraHertz (THz), or far-Infrared (far-IR), region (0.3 - 7.5 THz; 10 - 250 cm^-1) and the mid-IR (400 - 4000 cm^-1). The importance of astrochemical ices lies in their key role in the formation of complex organic molecules, such as amino acids and sugars in space. Thus, the instruments are capable of performing variety of spectroscopic studies that can provide especially relevant laboratory data to support astronomical observations from telescopes such as the Herschel Space Telescope, the Stratospheric Observatory for Infrared Astronomy (SOFIA), and the Atacama Large Millimeter Array (ALMA). The experimental apparatus uses a THz time-domain spectrometer, with a 1750/875 nm plasma source and a GaP detector crystal, to cover the bandwidth mentioned above with ~10 GHz (~0.3 cm^-1) resolution.

Using the above instrumentation, experimental spectra of astrochemical ice analogs of water and carbon dioxide in pure, mixed, and layered ices were collected at different temperatures under high vacuum conditions with the goal of investigating the structure of the ice. We tentatively observe a new feature in both amorphous solid water and crystalline water at 33 cm^-1 (1 THz). In addition, our studies of mixed and layered ices show how it is possible to identify the location of carbon dioxide as it segregates within the ice by observing its effect on the THz spectrum of water ice. The THz spectra of mixed and layered ices are further analyzed by fitting their spectra features to those of pure amorphous solid water and crystalline water ice to quantify the effects of temperature changes on structure. From the results of this work, it appears that THz spectroscopy is potentially well suited to study thermal transformations within the ice.

To advance the study of liquids with THz spectroscopy, we developed a new ultrafast nonlinear THz spectroscopic technique: heterodyne-detected, ultrafast THz Kerr effect (TKE) spectroscopy. We implemented a heterodyne-detection scheme into a TKE spectrometer that uses a stilbazoiumbased THz emitter, 4-N,N-dimethylamino-4-N-methyl-stilbazolium 2,4,6-trimethylbenzenesulfonate (DSTMS), and high numerical aperture optics which generates THz electric field in excess of 300 kV/cm, in the sample. This allows us to report the first measurement of quantum beats at terahertz (THz) frequencies that result from vibrational coherences initiated by the nonlinear, dipolar interaction of a broadband, high-energy, (sub)picosecond THz pulse with the sample. Our instrument improves on both the frequency coverage, and sensitivity previously reported; it also ensures a backgroundless measurement of the THz Kerr effect in pure liquids. For liquid diiodomethane, we observe a quantum beat at 3.66 THz (122 cm^-1), in exact agreement with the fundamental transition frequency of the υ4 vibration of the molecule. This result provides new insight into dipolar vs. Raman selection rules at terahertz frequencies.

To conclude we discuss future directions for the nonlinear THz spectroscopy in the Blake lab. We report the first results from an experiment using a plasma-based THz source for nonlinear spectroscopy that has the potential to enable nonlinear THz spectra with a sub-100 fs temporal resolution, and how the optics involved in the plasma mechanism can enable THz pulse shaping. Finally, we discuss how a single-shot THz detection scheme could improve the acquisition of THz data and how such a scheme could be implemented in the Blake lab. The instruments developed herein will hopefully remain a part of the groups core competencies and serve as building blocks for the next generation of THz instrumentation that pushes the frontiers of both chemistry and the scientific enterprise as a whole.

Analysis of an ultrashort pulsed finite beam diffracted by volume gratings

We obtain analytical solutions of the coupled wave equations that describe the Bragg diffraction of ultrashort pulsed finite beams by a thick planar grating, using two-dimensional coupled wave theory. The diffraction properties for the case of an ultrashort pulsed finite beam with Gaussian profiles in both the time and spatial domains are investigated. The spectral bandwidth of the diffracted beam, the Bragg selectivity bandwidth and the diffraction efficiency of the volume grating are influenced by the geometry parameter and the input bandwidth. Therefore extra attention should be paid to designing optical elements based on volume gratings for use with ultrashort pulsed waves in applications of pulse shaping and processing.

频率分辨光学开关法测量飞秒脉冲

阐述了频率分辨光学开关法测量飞秒脉冲的原理，详细分析了模式尺寸效应和非线性效应对飞秒脉冲测量的影响。构建了一台用于飞秒脉冲测量的二次谐波-频率分辨光学开关装置，利用该装置对谐振腔输出的飞秒脉冲及压缩后的脉冲进行了测量。得到了飞秒脉冲的时间宽度及光谱宽度、电场及其相位在时域和频域的详细信息。谐振腔直接输出脉冲的时间宽度为56 fs，光谱宽度为27 nm，时间带宽积为0.686，算法中的最小误差为0.001792。脉冲压缩后的测量结果为27 fs，光谱宽度为92 nm，时间带宽积为1.27，算法误差为0.00

飞秒脉冲通过散射表面后的时域特性

从理论上和实验上对飞秒激光脉冲通过散射表面后的时域特性进行了研究分析。用频率分辨光学开关法对通过散射表面前后的飞秒脉冲进行了测量和对比。理论分析和实验结果表明, 由于散射表面对飞秒脉冲的散射导致飞秒脉冲的展宽和形状的畸变。输入脉冲在时间相关函数的半峰全宽为64 fs; 透射脉冲在时间相关函数半峰全宽的平均值为117 fs。对透射脉冲场的统计特性进行了讨论, 透射脉冲场实部和虚部的概率函数分布遵从高斯函数分布; 强度的概率分布遵从指数分布规律; 给出了入射飞秒脉冲强度的自相关函数分布和飞秒时域散斑场强度的互相关函数分布的实验结果, 并且对二者的时间相关函数进行了讨论。

超短光脉冲感应级联五阶非线性相移分析

由于群速度失配的影响,飞秒光脉冲在感应到FONPS（级联五阶非线性相移）的同时,将不可避免地发生脉冲畸变.通过理论分析及数值模拟,提出了使级联五阶非线性过程运行在较大相位失配条件下的解决方案,成功地消除了脉冲畸变.并且借助于该过程中倍频效率的提高,有效地补偿由于相位失配量的增大所造成的FONPS的下降,实现飞秒基频光脉冲在感应到大的FONPS的同时无脉冲畸变发生.

基于孔径耦合带状线的激光脉冲整形系统

实现了一种新型的激光脉冲整形系统，该系统使用了一个由孔径耦合带状线（ACSL）电脉冲整形器驱动的电光调制器。一个电脉冲整形器由两条通过其公共接地板上的耦合孔径发生耦合作用的带状传输线所组成的四端口装置。更换具有不同耦合孔径的公共接地板，该电脉冲整形发生器可以具有150ps时间结构的任意整形电脉冲。将任意整形的电脉冲输入到电光调制器上，就可以得到任意整形的激光脉冲。利用该系统，激光脉冲整形系统能够产生具有150ps前后沿，1～3ns脉冲宽度可调、高对比度、光滑过渡以及任意整形的激光脉冲。

高功率激光装置前端系统激光脉冲的时间整形及修正技术

针对激光惯性约束聚变实验研究对高功率激光驱动器前端系统复杂时间形状种子激光脉冲的需求, 应用孔径耦合带状线集成波导整形系统设计了满足需要的前端整形激光脉冲。用一种新方法精确计算了孔径耦合带状线电脉冲整形器的耦合系数和孔径宽度的数值关系, 并针对高衬比度整形激光脉冲的需求, 提出了高衬比度双极型集成波导整形系统方案。由该系统可以得到100 ps脉冲前沿、1～3 ns脉冲宽度可调、高衬比度(大于100∶1)、光滑无纹波调制、可精确满足神光II八路及第九路装置需求的前端整形激光脉冲。

整形激光脉冲与激光探针同步技术

实现了应用于神光Ⅱ装置中的高精度整形激光脉冲与激光探针同步方案。在该方案中,激光探针经硅光导开关进行光电转换之后作为激光脉冲整形单元的触发信号,使激光脉冲整形单元,输出与激光探针同步的整形激光脉冲。为了降低由于触发信号不稳定引起的时间晃动,在光电转换之前放大激光探针,以调整激光脉冲整形单元触发信号的幅度。在神光Ⅱ装置中实现了整形激光脉冲与激光探针小于4.5 ps(均方根)的时间同步精度。

Generation of 1.5-12 ns width-tunable 532 nm pulses by adopting laser-induced plasma shutter technique

The pulse-shaping technique has found widespread applications in nonlinear optics and material processing. Experimental research on laser-induced plasma shutter to control the 532 nm pulse width is conducted. The impacts of the total pulse output energy on pulse compression are investigated, and a useful conclusion can be drawn that there exists an optimal value of pulse energy at which the shortest output pulse of 3.23 ns can be obtained without a device for delay-time. Once the device for delay-time is employed to change the optical differences between two laser paths, the pulse width can be further shortened to 1.51 ns. In short, the 1.5-12 ns width-tunable 532 nm laser pulses have been obtained by adopting the laser-induced plasma shutter technique. (C) 2007 Elsevier GmbH. All rights reserved.

Group delay dispersion measurement of Yb : Gd2SiO5, Yb : GdYSiO5 and Yb : LuYSiO5 crystal with white-light interferometry

We report the measured group delay dispersion (GDD) of new crystals Yb:Gd2SiO5 (Yb:GSO), Yb:GdYSiO5 (Yb:GYSO) and Yb:LuYSiO5 (Yb:LYSO) over wavelengths from 1000nm to 1200nm, with a white-light interferometer. Those GDD data should be useful for the dispersion compensation for femtosecond pulse generation in the lasers with these new crystals as the gain media. (C) 2007 Optical Society of America

飞秒脉冲激光器中色散补偿膜的设计

阐述了用光学薄膜进行色散补偿的基本原理，介绍了设计的基本过程．根据Ti：Sapphire飞秒激光器中腔内色散补偿的要求，设定了色散补偿目标，通过计算机优化，得到了一种40层的Ta2O5／SiO2介质膜系．该膜系能在720～870am范围获得大于99．5％的反射率，在510～550nm获得大于90％的透射率，在740～850nm提供较平滑的-40fs^2的群延迟色散．这样的结果经过7次反射后，可以补偿5-mm Ti：sapphire晶体产生的绝大部分群延迟色散。