Electronic excitations and alternation of conjugated polymers

The electronic excitations and fluorescence of conjugated polymers are related to large or small alternation ? of the transfer integrals t(1 ± ?) along the backbone. The fluorescence of polysilanes (PSs) and poly (para-phenylenevinylene (PPV) is linked to large ?, which places the one-photon gap Eg below the lowest two-photon gap Ea and reduces distortions due to electron-phonon (e-p) coupling. In contrast to small ? not, vert, similar 0.1 in ?-conjugated polymers, such as polyacetylene (PA), para-conjugated phenyls lead to an extended ?-system with increased alternation, to states localized on each ring and to charge-transfer excitations between them. Surprisingly good agreement is found between semiempirical parametric method 3 (PM3) bond lengths and exact Pariser-Parr-Pople (PPP) ?-bond orders for trans-stilbene, where the PPV bipolarons are confined to two phenyls. Stilbene spectra are consistent with increased alternation and small e-p distortions.

Second harmonic generation in poled molecularly doped polymer films : Push-pull butadienes in poly(methyl methacrylate) and polystyrene

We report second harmonic generation in a new class of organic materials, namely donor-acceptor substituted all-trans butadienes doped in poly(methyl methacrylate) or polystyrene and oriented by corona poling at elevated temperatures. Second harmonic measurements were made at room temperature. The observed d33 coefficients are greater than those of potassium dihydrogen phosphate or 4-dimethylamino-4'-nitrostilbene doped in similar polymer matrices. Rotational diffusion coefficients estimated from the decay characteristics of the second harmonic intensity in the polymer films indicate that the polymer matrix plays a major role in stabilizing the dopants in a nonlinear optics conducive environment.

Multiphoton absorption in CsLiB6O10 with femtosecond infrared laser pulses

Nonlinear absorption and refraction characteristics of cesium lithium borate (CsLiB6O10) crystal have been studied using Z-scan technique. Ti:sapphire laser with 110 fs pulse width operating at 800 nm wavelength and pulse repetition rate of 1 kHz is used as the source of photons. Intensity of the laser pulse is varied from 0.541 to 1.283 T W/cm2 to estimate the intensity dependence of multiphoton absorption coefficients. Using the theory of multiphoton absorption proposed by Sutherland [ Handbook of Nonlinear Optics, in 2nd ed., edited by D. G. McLean and S. Kirkpatrick, Dekker, New York (2003) ], found that open aperture Z-scan data fit well for the five-photon absorption (5PA) process. 5PA coefficients are obtained by fitting the expressions into the open aperture experimental data for various peak intensities (I00). The nonlinear refractive index n2 estimated from closed aperture Z-scan experiment is 1.075×10−4 cm2/T W at an input peak intensity of 0.723 T W/cm2. The above experiment when repeated with a 532 nm, 6 ns pulsed laser led to an irreversible damage of the sample resulting in an asymmetric open aperture Z-scan profile. This indicates that it is not possible to observe multiphoton absorption in this regime of pulse width using 532 nm laser.

Two mechanisms for population inversion via two-colour coherent excitation in three-level systems

We analyse the physical origin of population inversion via continuous wave two-colour coherent excitation in three-level systems by dressing the inverted transition. Two different mechanisms are identified as being responsible for the population inversion. For V-configured systems and cascade (E) configured systems with inversion on the lower transition, the responsible mechanism is the selective trapping of dressed states, and the population inversion approaches the ideal value of 1. For Lambda-configured systems and Xi-configured systems with inversion on the upper transition, population inversion is based on the selective excitation of dressed states, with the population inversion tending towards 0.5. As the essential difference between these two mechanisms, the selective trapping of dressed states occurs in systems with strong decay into dressed states while the selective excitation appears in systems with strong decay out of dressed states.

Enhancement of four-wave mixing induced by interacting dark resonances

We analyse a four-wave mixing (FWM) scheme in a five-level atomic system in which double-dark resonances are present. It is found that the enhancement of FWM in both electromagnetically induced transparency (EIT) windows can be obtained even without the condition of multiphoton resonance. Moreover, the conversion efficiency of FWM in one EIT window can be much larger than that in the other due to the presence of interacting dark resonances.

Coherent population transfer with chirped few-cycle laser pulses in an excited-doublet four-level system

The behavior of population transfer in an excited-doublet four-level system driven by linear polarized few-cycle ultrashort laser pulses is investigated numerically. It is shown that almost complete population transfer can be achieved even when the adiabatic criterion is not fulfilled. Moreover, the robustness of this scheme in terms of the Rabi frequencies and chirp rates of the pulses is explored.

Incoherent subharmonic light scattering in isotropic media

Incoherent subharmonic light scattering in isotropic media is a new kind of nonlinear light scattering, which involves single input photon and multiple output photons of equal frequency. We investigate theoretically the dependence of the subharmonic scattering intensity on the hyperpolarizability of molecules and the incident intensity using nonlinear optics theory similar to that used for Hyper-Rayleigh scattering and degenerate optical parametric oscillators. It is derived that the subharmonic scattering intensities grow exponentially or superexponentially with the hyperpolarizability of molecules and the incident intensity. (C) 2004 Elsevier B.V. All rights reserved.

超短脉冲照射下氟化锂的烧蚀机理及其超快动力学研究

研究了超短脉冲激光照射下LiF晶体的破坏机理及其超快动力学过程，利用扫描电镜和原子力显微镜等测试手段，观测了飞秒激光照射下LiF晶体的烧蚀形貌。利用烧蚀面积与激光脉冲能量的对数关系确定了LiF晶体的破坏阈值，并利用非线性玻璃棒展宽脉宽，得到了800nm激光作用下LiF破坏阈值对激光脉宽（50～1000fs）的依赖关系；利用抽运一探针超快探测平台，探测了LiF烧蚀过程中反射率的变化。采用雪崩击穿模型，并根据晶体材料反射率与材料的介电常量的依赖关系，通过数值计算，模拟了材料烧蚀阈值与脉宽的依赖关系及材料激发过

Controllable atom localization via double-dark resonances in a tripod system

We propose an atom localization scheme for a tripod-type atom making use of the sharp absorption peak resulting from interacting double-dark resonances. It is demonstrated that the probability of finding the atom at a particular position, as well as the localization precision, can be dramatically enhanced. The probability can be doubled by adjusting the Rabi frequency of the control field to the maximum Rabi frequency of the standing-wave field. Moreover, much better spatial resolution can be achieved for smaller detunings of the control and the standing-wave fields. (c) 2006 Optical Society of America.

脉冲啁啾对于阿秒脉冲的影响

采用单电子近似和软核势模型，通过数值求解一维含时薛定谔方程，理论研究了当脉冲分别带有正、负啁啾的情况下所产生的阿秒脉冲，分析了不同脉冲啁啾特性对阿秒脉冲的强度和宽度的影响，研究结果表明，无论是正啁啾还是负啁啾，随着啁啾量的增加，都将使激光脉冲由产生单个阿秒脉冲趋向于产生阿秒脉冲链，正啁啾和负啁啾对于阿秒脉冲宽度的影响是不同的，负啁啾对于阿秒脉冲宽度影响很小，适当的负啁啾有利于缩小阿秒脉冲的宽度；而正啁啾脉冲产生的阿秒脉冲较无啁啾时展宽，且随着啁啾量的增加，其阿秒脉冲宽度迅速增大。

飞秒强激光经氩气和氩团簇的传播

通过数值求解三维电场传播方程，理论模拟了飞秒强激光脉冲（50fs，10^16w／cm^2）在氩气和中等尺寸氩团簇中的传播效应．结果表明，飞秒强激光脉冲经氩气传播将发生频谱蓝移展宽和光束发散；而经中等尺寸氩团簇传播，则存在一定程度的自聚焦效应．

超短激光脉冲在不同色散参量光子晶体光纤中传输的数值模拟

为了使得数值模拟更为精确, 采用广义非线性薛定谔方程(GNSE)描述超短激光脉冲在光子晶体光纤中的传输演化过程, 并利用二阶分步傅里叶方法通过求解方程, 数值计算了相同脉宽和能量的超短脉冲在不同色散参量的光子晶体光纤中非线性传输和超连续谱的产生。比较了超短脉冲在光纤不同色散区传输时, 高阶色散和非线性效应对超连续谱的产生以及对脉冲波形演化的影响。结果表明, 相对于超短脉冲中心波长位于光子晶体光纤的正常和反常色散区, 可以相应获得短波波段和长波波段的超连续谱输出, 当超短脉冲中心波长位于零色散波长点时, 通