简并四波混频的速率方程理论

本文采用量子态跃迁速率公式及能量和动量守恒定律,对简并四波混频进行了理论处理,推导出光子密度运动方程并得到精确解。对饱和现象(泵浦抽空)、非线性反射率随探测波的变化以及参量振荡等给出了令人满意的定量描述。得到了比以往的经典理论更完善的结果。 关键词：     

O (3P) + H2 → OH+H反应的立体动力学研究

用BMS1势能面[Brandão 等, J.Chem.Phys. 121, 8861 (2004)],选取碰撞能为34.6kcal/mol,用准经典轨线方法研究了O ( ) + 反应的立体动力学性质。计算并讨论了k与j'的夹角的分布关系P ( )以及描述k-k'- j'三者关系的二面角分布。（k为反应物速度方向,k'为产物的速度方向,j'为产物的角动量方向） 的峰值在90°附近并且关于90°呈对称性分布,这表明产物角动量的方向与初速度的方向垂直。二面角分布P( )关于散射平面呈反对称性分布,这一结果表明产物的角动量具有强烈的极化效应。另外,我们还研究了振动激发对产物角动量的影响,结果表明产物的矢量性质对反应物的初始振动态非常敏感。     

Entangled femtosecond free induction signals in a cadmium sulfide crystal at room temperature

Entangled free induction decay (EFID) femtosecond signals are experimentally observed for the first time at a wavelength of 790 nm in a cadmium sulfide (CdS) crystal in the two-photon absorption (TPA) regime upon excitation by two crossed (angle, 60°) laser beams. The sample emitted two EFID signals simultaneously in opposite directions. The signals were diffracted by nonequilibrium electric polarization gratings induced by two laser beams in accordance with the laws of energy and momentum conservation. The possibility of exciting EFID signals in the three-photon absorption regime is discussed.     

Doppler-free spectroscopy of neon atoms dressed by optical photons in nearly-degenerate four-wave mixing

We have investigated nearly degenerate four-wave mixing in neon on the 607 nm line. We have considered the case where one pump beam saturates the medium while the two other incident beams have a much weaker intensity. The frequency of the most intense pump beam is equal to the frequency of the probe beam. When the frequency of the second pump beam is scanned, narrow resonances are observed. These resonances correspond to transitions between the energy levels of the atom dressed by the photons of the intense pump beam.     

Low‐noise,vibrational phase‐sensitive chemical imaging by balanced detection RIKE

We perform a back‐to‐back comparison between two nonlinear vibrational imaging techniques: stimulated Raman scattering (SRS) and balanced detection Raman‐induced Kerr effect (BD‐RIKE). Using a compact fiber‐based laser system for generation of pump and Stokes signals, we image polymer beads as well as human hepatocytes under the same experimental conditions. We show that BD‐RIKE, despite the slightly lower signal levels, consistently offers an improved signal‐to‐noise ratio with respect to SRS, resulting in significantly higher image quality. Importantly, we observe that such quality is not affected by the static birefringence of the sample, which makes BD‐RIKE a robust and attractive alternative to SRS. We also highlight a unique advantage of the technique, which is its capability to easily access both the real and imaginary parts of the nonlinear susceptibility, thus allowing for vibrational phase imaging. The phase information can be readily obtained from BD‐RIKE with minimal experimental effort and provides an additional chemical selectivity channel for coherent Raman microscopy. Copyright © 2014 John Wiley & Sons, Ltd.     

O(3P)+H2→OH+H反应的立体动力学研究

利用BMS1势能面[Brandao等,J.Chem.Phys.121,8861(2004)],选取碰撞能为34.6 kcal/mol,用准经典轨线方法研究了O(3P)+H2反应的立体动力学性质.计算并讨论了k与j'的夹角的分布关系P(θr)以及描述k-k'-j'三者关系的二面角分布P((ρ)r).(k)为反应物速度方向,k'为产物的速度方向,j'为产物的角动量方向)P(θr)的峰值在90°附近并且关于90°呈对称性分布,这表明产物角动量的方向与初速度的方向垂直.二面角分布P((ρ)r)关于散射平面呈反对称性分布,这一结果表明产物的角动量具有强烈的极化效应.另外,我们还研究了振动激发对产物角动量的影响,结果表明产物的矢量性质对反应物的初始振动态非常敏感.     

Phase‐shaping strategies for coherent anti‐Stokes Raman scattering

The identification of large molecules in complex environments requires probing of multiple vibrational resonances rather than a single resonance. Phase‐shaping the excitation pulses allows the coherent mixing of several resonances so that the presence of molecules can be inferred directly from the integrated output pulse energy. This avoids the need for the collection of spectra or multiple measurements. This article describes a particular implementation for coherent anti‐Stokes Raman scattering microscopy that uses a broadband pump and probe field in combination with a narrowband Stokes field. We numerically study the possibilities of optimizing selectivity, specificity, and sensitivity by precalculating pulse shapes using an evolutionary algorithm. Copyright © 2011 John Wiley & Sons, Ltd.     

三维自散焦介质中光束聚焦的最佳参量选择

对三维自散焦介质中由交叉相位调制效应诱导的光束聚焦过程进行了系统研究,讨论了抽运光振幅、抽运光-信号光初始偏移和抽运光-信号光波长比三个参量对信号光聚焦过程的影响。根据自散焦介质中强抽运光诱导弱信号光聚焦满足抽运光与探测光模型,对传输方程进行了优化,大大减少了数值模拟运算时间。数值方法采用分布傅里叶方法。数值模拟结果表明：抽运光越强、抽运光-信号光波长比越大,信号光聚焦程度越大;抽运光-信号光初始偏移存在一个最佳值,使得光束聚焦达到最佳效果。通过参量最佳值的选择,可提高光束聚焦的效率。     

Phase sensitive parametric amplification of optical vortex beams

Optical vortex beams with different topological charges are amplified in a travelling wave phase sensitive parametric interaction. Amplified beams observed either in the near field or in the far field domains exhibit patterns that depend on the relative phase between the pump and the vortex beams. Experimental results are compatible with the conservation of orbital angular momentum of the input beam whatever phase matching conditions.     

Cherenkov phase-matching in Raman-seeded four-wave mixing by a femtosecond Bessel beam

It is demonstrated experimentally that the angle vs. wavelength dependence of the emission generated by multi-step four-wave mixing process seeded by stimulated Raman scattering in water under femtosecond Bessel beam excitation is determined by the longitudinal phase-matching from IR to near UV. It is shown that if on-axis phase velocity of the pump Bessel beam is equal to the phase velocity of the Stokes axial wave, then, similar to Cherenkov radiation, all the other anti-Stokes beams too acquire that axial velocity.     

Comparison of three kinds of polarized Bessel vortex beams propagating through uniaxial anisotropic media

A comparison of differently polarized Bessel vortex beams propagating through a uniaxial anisotropic slab is discussed in terms of the vector wave function expansions.The magnitude profiles of electric field components, the transformation of polarization modes, and the distributions of orbital angular momentum(OAM) states of the reflected and transmitted beams for different incident angles are numerically simulated.The results indicate that the magnitude profiles of electric field components for different polarization modes are distinct from each other and have a great dependence on the incident angle,thus the transformation of polarization modes which reflects the change of energy can be affected largely.As compared to the x and circular polarization incidences, the reflected and transmitted beams for the radial polarization incidence suffer the fewest transformation of polarization modes, showing a better energy invariance.The distributions of OAM states of the reflected and transmitted beams for different polarization modes are diverse as well, and the derived OAM states of the transmitted beam for radial polarization present a focusing effect, concentrating on the state between two predominant OAM states.     

Observation of saturation of energy transfer between copropagating beams in a flowing plasma

Experiments demonstrate energy and power transfer between copropagating, same frequency, beams crossing at a small angle in a plasma with a Mach 1 flow. The process is interpreted as amplification of the low intensity probe beam by the stimulated scatter of the high intensity pump beam. The observed probe amplification increases slowly with pump intensity and decreases with probe intensity, indicative of saturation limiting the energy and power transfer due to ion-wave nonlinearities and localized pump depletion. The results are consistent with numerical modeling including ion-wave nonlinearities.     

基于“泵浦-探测”效应的等离子体通道中三次谐波增强与光谱分析

利用“泵浦-探测”非共线双等离子体通道方法实现三次谐波增强。泵浦光与探测光间的耦合作用能有效改善探测光光丝中的饱和效应,克服光强钳制对谐波强度增加的限制。实验中将两束能量分别为4.4和10.2 mJ、中心波长均为810 nm、脉宽均为60 fs的超短脉冲在空气中非共线聚焦,能各自形成光丝且产生微弱三次谐波。当强光在时域上超前于弱光时,强光会预先成丝形成等离子体通道,对后续弱光产生调制,使探测光产生的三次谐波强度明显增强。实验发现270 nm谐波能量增加的显著区域内频谱宽度出现振荡变化,当两光以27.3 mrad小角度相交于几何焦点前约15 mm,且探测光滞后约55 fs时,获得的能量增长倍率达到近70倍,对应谱宽约为5 nm。     

Generation of multi-color stimulated raman emission from two-color linearly or circularly polarized pump beams

A laser beam at two different frequencies separated by 587 cm^–1 is focused into pressurized hydrogen (rotational transition energy, 587 cm^–1) to generate multi-color stimulated Raman emission. The polarization state and the pulse energy are measured for each generated emission line using linearly and circularly polarized pump beams. The effect of the polarization is discussed by using a parameter characterizing the polarizability of hydrogen and a conservation rule for the angular momentum in four-wave mixing. Many rotational lines are generated with linearly polarized pump beams through a four-wave mixing process. This is in striking contrast to the results obtained by using a single-color circularly polarized pump beam which generates only one rotational line through a conventional stimulated Raman process.     

Wave-particle interactions in marginally unstable plasma as a means of energy transfer between energetic particle populations

Energy exchange between waves and resonant (usually energetic) particles is an essential feature of wave-particle interactions in plasma. If the resonant interaction in a magnetized unstable plasma involves two or more cyclotron resonances, the wave excitation can, at the same time, mediate the energy transfer between different populations of energetic particles. This effect, which is particularly pronounced in a marginally unstable plasma, is discussed by example of whistler-electron interactions in connection with particle energization in the Earth?s radiation belts. The process under discussion is similar, although not identical, to alpha channeling known in the physics of tokamak plasma.     

Elementary relaxation processes investigated by femtosecond photoelectron spectroscopy of two‐dimensional materials

Elementary scattering processes in solid matter occur on ultrafast timescales and photoelectron spectroscopy in the time domain represents an excellent tool for their analysis. Conventional photoemission accesses binding energies of electronic states and their momentum dispersion. The use of femtosecond laser pulses in pump‐probe experiments allows obtaining direct insights to the energy and momentum dependence of ultrafast dynamics. This article introduces the elementary interaction processes and emphasizes recent work performed in this rapidly developing field. Decay processes in the low excitation limit are addressed, where electrons decay according to their interaction with carriers in equilibrium. Here, hot electron relaxation in epitaxial metallic film is reviewed. In the limit of an intense optical excitation, scattering of the excited electrons among each other establishes a non‐equilibrium state. Results on charge‐density wave materials and the effect of coherent nuclear motion on the electronic structure, which can break low symmetry ground states, are discussed. Figure reprinted with permission from [71].     

用双光源相位共轭型非相干光时间延迟简并四波混频测量超快速过程

本文提出用双光源相位共轭型非相干光时间延迟简并四波混频测量失相时间和布居弛豫时间的理论,并对其应用进行了讨论.     

Pump-probe spectroscopy of atoms cooled in a 3D lin lin optical lattice

We describe the pump-probe spectroscopy of atoms cooled in a 3D lin⊥lin optical lattice. Our pump-probe configuration consists of two laser fields detuned with respect to the lattice fields. This scheme allows to clearly identify in the probe transmission spectrum the Brillouin and Raman resonances, by studying their positions as functions of the angle between the pump and probe beams. We describe these resonances in detail, and compare the experimental results to the theoretical predictions. Our conclusions are supported by transport-spectroscopy measurements, which allow to distinguish between contributions to the light scattering from propagating and non-propagating atoms. Received 8 April 2002 / Received in final form 9 September 2002 Published online 12 November 2002     

Quantum interference spectroscopy of rubidium-helium exciplexes formed on helium nanodroplets

Femtosecond multiphoton pump-probe photoionization is applied to helium nanodroplets doped with rubidium (Rb). The yield of Rb+ ions features pronounced quantum interference (QI) fringes demonstrating the coherence of a superposition of electronic states on a time scale of tens of picoseconds. Furthermore, we observe QI in the yield of formed RbHe exciplex molecules. The quantum interferogram allows us to determine the vibrational structure of these unstable molecules. From a sliced Fourier analysis one cannot only extract the population dynamics of vibrational states but also follow their energetic evolution during the RbHe formation.