耦合双振子模型手性分子的微观参量对和频过程的影响

用经典理论方法推出了适合于耦合双振子模型的手性分子的超极化率,给出了分子超极化率与分子微观参量的关系式.由微观与宏观极化率的关系,具体讨论了分子微观参量对宏观介质极化与和频过程产生效率的影响,本模型得到的理论结果与已有的实验结果很好地符合. 关键词： 手性分子介质 和频产生 超极化率 二阶极化率     

基于螺旋单电子模型的手性分子的三阶非线性极化率

本文从螺旋手性分子单电子模型出发,推导手性分子的三阶光学非线性,给出螺旋手性分子三阶极化率张量元的解析表达式,并讨论分析了实际的螺旋分子的极化率张量的非零元素.     

基于耦合双振子模型的手性分子的超极化率

本文从手性分子的耦合双振子经典模型出发,推导出手性分子的超极化率.在特定情况下,给出了三阶非线性极化率的表达式.基于该模型讨论了手性介质分子各向同性分布的宏观非线性极化率.     

非对称量子阱中的二阶非线性光学极化率

本文主要研究了一个特殊非对称量子阱中的二阶非线性光学极化率,并且利用量子力学中的密度矩阵算符理论和迭代方法导出了二次谐波极化率的解析表达式.最后,以典型的GaAs/AlGaAs非对称量子阱为例作了数值计算.数值结果表明,较大的二次谐波极化率与系统的非对称性有关,系统的非对称性越大,二次谐波极化率越大.     

有序分子体系的三阶和四阶非线性光谱学的实验可观测量和宏观感应率及微观极化率张量元

对于线性和非线性光谱，有序的分子体系(如分子界面和分子膜)的取向分析可以通过对形式非常简单的广义取向泛函．对于二阶非线性光谱学，即光学二次谐波和和频振动光谱，这一简化描述对于理解分子界面和膜的光谱和取向的细节很有助益．为了将这一简化描述应用于更高阶的相干非线性光谱学，对于具有旋转对称性的界面或膜的三阶和四阶非线性光谱学的实验可观测量和宏观感应率及微观极化率张量元进行了计算并得到了具体表达式．这些通用的表达式将有助于典型的三、四阶非线性光谱学，即光学三次谐波、简并的相干反斯托克斯拉曼光谱、光学四次谐波和简并     

手性分子2, 3-丁二醇的旋光拉曼光谱研究

本文从拉曼峰和旋光拉曼峰出发,通过键极化率和微分键极化率分析研究(2R, 3R)-2, 3-丁二醇. 通过分子C₁和C₂两种点群的优化结构,获得不依赖于这两种结构的结果 和有关这个手性系统物理图像的丰富信息.对分子拉曼键极化率分析,得出在拉曼弛豫过程中, 电荷主要从外围流向骨架结构.对分子微分键极化率的分析,显示在不对称C原子和与其相联系的H原子 两侧化学键, C-O和C-CH₃的微分键极化率的符号正好相反,意味着这个分子具有相当好的手性 不对称性质.对比对称和反对称的键极化率、微分键极化率,本文得到这样的结论: 对于(特别是键伸缩的)键极化率,(大体上是)对称的大于反对称的; 而对于微分键极化率则是反对称的大于对称的. 关键词： 旋光拉曼 键极化率 微分键极化率 2,3-丁二醇     

手性分子反-2,3-环氧丁烷的旋光拉曼光谱研究

本文从拉曼峰强出发,求得了反-2,3-环氧丁烷分子的拉曼键极化率,明确了拉曼激发下电荷的分布的信息.还从旋光拉曼(Raman optical activity,ROA)谱的峰强,求取了该分子的旋光拉曼键极化率.由分子手性中心的C-H产生的偶极矩与拉曼激发过程中,电荷流动产生的跃迁磁偶极矩的耦合,来理解旋光拉曼活性产生的机理.分析表明,旋光拉曼活性分子手性中心的C-H键两侧的旋光拉曼极化率符号相反,显示着手性分子局域的不对称性.还得到了对称和反对称坐标的键极化率和旋光拉曼极化率,并且从对称性的角度,即C2群的不可约表示,讨论了这些极化率的内涵.     

对称陀螺分子转动反对称极化率

使用半经典微扰理论和角动量理论，研究了对称陀螺分子转动磁能级的共振反对称极化率，结果表明磁能级反对称极化率不仅存在而且同对称极化率具有相同的数量级。以NH3为例，计算了这些量。     

对称陀螺分子转动反对称极化率

使用半经典微扰理论和角动量理论,研究了对称陀螺分子转动磁能级的共振反对称极化率,结果表明磁能级反对称极化率不仅存在而且同对称极化率具有相同的数量级.以NH3为例,计算了这些量.     

4-戊基-4'-氰基联苯液晶的分子二阶非线性光学极化率测量方法

在玻璃衬底上制得单层硬脂酸的Langmuir-Blodgett(LB)膜,做为4-戊基-4''-氰基联苯(5CB)液晶的取向层,在取向层上旋涂一层5CB液晶,用透射二次谐波方法测量出5CB液晶分子二阶非线性光学极化率,其值为β=7×10-29esu.对比文献值,测量得到的结果符合较好.     

Nonlinear optical properties of urea

We report measurements on the second and third order nonlinear hyperpolarizabilities of the urea molecule using the techniques of dc field induced second-harmonic generation and four-wave mixing. Single crystals of urea have been grown and found to have high optical damage thresholds from the near ir to the uv region of the spectrum.     

Fabrication of Periodic Waveguides Using Organic Crystals and Fluorinated Polyimides for Quasi-Phase-Matched Second-Harmonic Generation

We have developed a new method to fabricate periodic waveguide structures used for quasi-phase-matched second-harmonic generation, where nonlinear optical organic crystals and fluorinated copolyimides are alternately arranged. Quasi-phase-matched second-harmonic generation from an organic waveguide device has been demonstrated.     

Second-harmonic generation with traveling-wave pulses

We experimentally studied properties of traveling-wave excitation and traveling-wave pulse compression for a Nd : glass laser system with a streak camera. These properties were extended to second-harmonic generation with a type-11 KDP crystal. We found that the second-harmonic pulse generated from the chirped-fundamental pulse also has a good chirp linearity, but the spectral bandwidth and temporal duration were reduced. We demonstrated the effective subpulse suppression in the compressed pulse with the second-harmonic generation. The pulse with tilted wave front, short wavelength and high contrast ratio can be obtained by the second-harmonic generation of traveling-wave pulse.     

Transmission reflection anomaly in second-harmonic generation from a monolayer

We show experimentally that in second-harmonic generation from a monolayer the radiation propagating in transmission and that in reflection can have very different magnitudes. The origin of this difference lies in destructive and constructive interference of the components of the nonlinear polarization that drive the field at the second-harmonic frequency.     

Non-phase-matched enhancement of second-harmonic generation in multilayer nonlinear structures with internal reflections

Traditional notions of second-harmonic generation rely on phase matching or quasi phase matching to achieve good conversion efficiencies. We present an entirely new concept for efficient second-harmonic generation that is based on the interference of counterpropagating waves in multilayer structures. Conversion efficiencies are an order of magnitude larger than with phase-matched second-harmonic generation in similar multilayer structures.     

Efficient second-harmonic generation by scattering from porous gallium phosphide

We experimentally study second-harmonic generation by femtosecond Cr: forsterite-laser radiation scattered on the surface of porous gallium phosphide with characteristic pore sizes and distances between the pores comparable with the second-harmonic wavelength. The intensity of the second-harmonic signal from samples with initial crystallographic surface orientations (110) and (111) is more than an order of magnitude higher than the intensity of the second harmonic generated in reflection from single-crystal gallium phosphide. The efficiency of second-harmonic generation by macroporous gallium phosphide substantially increases as the pump wave-length becomes shorter. The influence of light localization and scattering effects on the enhancement of second-harmonic generation and polarization properties of the second-harmonic is discussed.     

Large second-harmonic generation at 1.55 μmin oxidized AlGaAs waveguides

We report on CW second-harmonic generation in selectively oxidized AlGaAs multilayer waveguides. Frequency doubling of a 1.55 μm pump is observed with 2.8% W(-1) conversion efficiency and a maximum second-harmonic power around 0.3 mW. This is the strongest second-harmonic generation ever reported in semiconductor waveguides and an encouraging result toward integrated spontaneous parametric downconversion in the telecom range.     

Efficiency of the second-harmonic generation with the zeroth-order bessel-profile beams in uniaxial crystals

We study the efficiency of the second-harmonic generation with the zeroth-order Bessel beam (SHGzoBB) in uniaxial crystals. We show that the conversion efficiency is always less than that of the second-harmonic generation with the Gaussian beam (SHGGB). The fundamental reason relies on the fact that the advantage associated with the ??nondiffractive?? nature of the Bessel beam is not sufficient to compensate the disadvantage of its wave-vector distribution. We show that the zeroth-order Bessel beam is not the optimum beam for the second-harmonic generation in uniaxial crystals.     

Backward second-harmonic and third-harmonic generation in a periodically poled potassium titanyl phosphate waveguide

We observed backward second-harmonic and backward third-harmonic generation in a periodically poled KTiOPO(4) waveguide using nanosecond laser pulses. The highest conversion efficiency achieved for the backward second-harmonic generation, occurring at the 25th-order grating, was ~0.6% . The backward third-harmonic generation was the result of mixing the pump beam with the forward or the backward second-harmonic beam. Conversion efficiency of ~0.4% was achieved at a pump wavelength of 1233.7 nm, where the two constituent nonlinear processes are both quasi-phase matched.     

Efficient ultrafast ultraviolet generation based on frequency doubling in short-period periodically-poled KTiOPO4 crystal

We have efficiently generated ultrafast coherent ultraviolet (UV) pulses based on second-harmonic generation in a periodically-poled KTiOPO₄ crystal with the period as short as 2.55 μm. The highest output power is measured to be 20.1 mW at 377.1 nm with the conversion efficiency of 15.6%. Such an output wavelength is probably among the shortest ones generated by forward second-harmonic generation in a periodically-poled KTiOPO₄ crystal.