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     

手性薄膜表面二次谐波圆二向色性的研究

给出了螺旋型手性分子薄膜表面反射方向的圆二向色性的谐波强度表示式,分析了谐波的强度与手性分子的取向,分子的螺距和半径等结构参数的关系,给出了数值模拟结果,发现在入射光强一定的情况下,谐波强度在螺距和半径的取值范围内分别存在着最大值,以及螺距与半径之间满足的关系式随分子取向角的变化而不同。     

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.     

用激活性非线性介质Nd：MgO：LiNbO3产生二次谐波

以Nd:MgO:LiNbO_3同时兼作激活介质和非线性光学材料,研究自倍频激光器。用小型氙灯泵浦,在室温下获得二次谐波激光(0.547μm) 阈值小于4.8'J,最大输出400μJ/shot,工作温度范围大于20℃～45℃,无光损伤。     

手性分子介质非线性光学研究新进展

文章介绍了近年来手性分子介质及材料的非线性光学性质的研究状况，综述了手性分子非线性微观模型的使用情况，给出了一些典型的二阶、三阶非线性光学实验结果，用这些微观模型可以正确地分析这些结果．同时指出了未来研究的趋势，及研究成果可能应用的领域．     

气液界面超分子手性分布的原位二次谐波研究

界面超分子手性因其在材料、催化、生物等领域的应用前景得到了人们的广泛关注。卟啉(porphyrin)衍生物因具有强的π-π堆垛能力、生物兼容性和出色的电子性能,常用于构建界面超分子结构。卟啉衍生物的表面超分子手性研究多数在固体基底上进行。利用二次谐波线二色谱方法分析卟啉衍生物在空气/水界面形成的超分子结构,通过界面层不同位置处产生的S偏振二次谐波强度随入射基频光偏振态的变化研究界面超分子结构的手性分布。实验表明,卟啉衍生物TPPS吸附在两亲分子CTAB在空气/水界面上形成的单层后会形成超分子结构,该结构具有手性,且手性的二维分布是非均匀的。     

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.     

中心对称萘酞菁分子二次谐波产生的实验研究

研究了三种萘酞菁化合物LB膜的制备,并通过二次谐波产生的方法研究了单个对称取代的萘酞菁化合物及双(四叔丁基萘酞菁)铒的二阶非线性光学特性,并对它们的产生机理进行了简单的讨论.单个对称取代的萘酞菁化合物,它们的二次谐波产生机制为磁偶极子耦合机制,双(四叔丁基萘酞菁)铒的二阶非线性光学特性起源于电四极子模型,且它的二阶非线性极化率χ(2)(或超极化率β)大于单个萘酞菁化合物.     

金属-真空表面的二次谐波理论

对于金属表面上的二次谐波产生,现有理论(流体动力学和密度泛函理论)的计算结果与实验数据相差一个数量级。本文利用相关基函数理论计算了Al,Mg和Ag表面上的二次谐波,由于该方法较好地考虑了电子关联,因而明显地改进了理论结果。关键词：     

等离子体钢丝二次谐波辐射的线性转换理论

本文对激光等离子体细丝的线性转换理论作了研究.通过对激光等离子体二次谐波的能量通量的计算发现,二次谐波的平面波理论关于在垂直密度梯度方向没有二次谐波辐射的结论与实验结果不符.在此基础上,我们提出了等离子体细丝的二次谱波线性转换理论,在垂直密度梯度方向有较强的二次谐波发射,这与实验结果较为一致.     

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.     

不同表压下芪盐单层LB膜二次谐波的研究

在不同表压下制备芪盐的单层LB薄膜,测量LB膜的二次谐波信号.在低表压得到增强的二次谐波信号.对比芪盐的透射光谱,认为在LB膜中,芪盐以固相态存在,低表压时的固相态聚集体的吸收峰351nm使四阶非线性极化率x(4)(-2ω;ω,ω,ω,-ω)产生共振增强,四阶光学非线性现象对二次谐波信号产生影响.     

Molecular QED of coherent and incoherent sum-frequency and second-harmonic generation in chiral liquids in the presence of a static electric field

Coherent second-order nonlinear optical processes are symmetry forbidden in centrosymmetric environments in the electric-dipole approximation. In liquids that contain chiral molecules, however, and which therefore lack mirror image symmetry, coherent sum-frequency generation is possible, whereas second-harmonic generation remains forbidden. Here we apply the theory of molecular quantum electrodynamics to the calculation of the matrix element, transition rate, and integrated signal intensity for sum-frequency and second-harmonic generation taking place in a chiral liquid in the presence and absence of a static electric field, to examine which coherent and incoherent processes exist in the electric-dipole approximation in liquids. Third- and fourth-order time-dependent perturbation theory is employed in combination with single-sided Feynman diagrams to evaluate two contributions arising from static field-free and field-induced processes. It is found that, in addition to the coherent term, an incoherent process exists for sum-frequency generation in liquids. Surprisingly, in the case of dc-field-induced second-harmonic generation, the incoherent contribution is found to always vanish for isotropic chiral liquids even though hyper-Rayleigh second-harmonic generation and electric-field-induced second-harmonic generation are both independently symmetry allowed in any liquid.     

Generalized Approximation of Strong Interaction of Waves in the Theory of High-Power Radiation Frequency Doubling

The approximation of strong interaction of waves is developed to analyze the generation of the second harmonic under the conditions of self-action. Based on this method, an approximate expression is obtained for the generation efficiency of the second harmonic with allowance for the effect of higher nonlinearities, depletion of pumping radiation, and linear phase detuning. The effect of phase detuning and change in the spatial distribution of the amplitude of the fundamental radiation on the efficiency of second-harmonic generation has been analyzed. Good agreement of the results of the developed approximate method with experimental data and numerical calculations is shown. The optimum conditions of the second-harmonic generation in a wide range of the laser system radiation intensities are determined.     

不同表压下芪盐LB膜二阶光学非线性的研究

研究了芪盐在不同表压下制备的ＬＢ膜的二阶光学非线性。测量得到在低表压增强的二次谐波信号。对比芪盐的π－Ａ曲线和透射光谱，认为在ＬＢ膜中芪盐以固相态存在，低表压时的固相态聚集体的吸收峰３５１ｎｍ使四阶非线性极化率Ｘ＾（４）（－２ω：ω，ω，ω，－ω）产生共振强，四阶光学非线性现象对二次谐波信号产生影响。     

Anisotropy of second-order nonlinear optical susceptibilities of arsenic triiodide-sulfur addition complex: AsI3 · 3S8

We report the anisotropic linear and second-order nonlinear optical (NLO) properties of arsenic triiodide-octa-sulfur (1:3) adduct, AsI₃ · 3S₈, which spontaneously crystallizes in the trigonal rhombohedral non-centrosymmetric space group R3m. The trigonal symmetry of the AsI₃ · 3S₈ molecule coincides with the crystal symmetry. The crystals are optically uniaxial with n_o/n_e of about 1.2 and show dichroism at the UV-visible wavelengths. Second harmonic generation (SHG) tensor elements were determined from Maker fringes measured with an Nd:YAG laser (∼10 ns pulse, 1064 nm). The coefficient d_222,eff = 32.0 pm/V for the light polarized parallel to the layers of iodine and sulfur atoms in the AsI₃ · 3S₈ crystal ab plane is markedly larger than d₃₃₃ = 11.6 pm/V for the polarization of light parallel to the crystal c axis. The anisotropy parameter, defined as the d_222,eff/d₃₃₃ ratio, is about 2.7 for the AsI₃ · 3S₈ crystal, smaller than that for the isomorphous CHI₃ · 3S₈ crystal (7.3) but larger than for the SbI₃ · 3S₈ crystal (0.7). Highly anisotropic components of the first hyperpolarizability tensor of an AsI₃ · 3S₈ molecule, β, were derived from the quadratic nonlinear susceptibility tensor of the crystal.