Selective excitation and suppression of coherent anti-Stokes Raman scattering by shaping femtosecond pulses

Femtosecond coherent anti-Stokes Raman scattering (CARS) suffers from poor selectivity between neighbouring Raman levels due to the large bandwidth of the femtosecond pulses. This paper provides a new method to realize the selective excitation and suppression of femtosecond CARS by manipulating both the probe and pump (or Stokes) spectra. These theoretical results indicate that the CARS signals between neighbouring Raman levels are differentiated from their indistinguishable femtosecond CARS spectra by tailoring the probe spectrum, and then their selective excitation and suppression can be realized by supplementally manipulating the pump (or Stokes) spectrum with the $\pi $ spectral phase step.     

氦同位素与氢分子碰撞的振转激发分波截面研究

用密耦近似方法和Tang-Toennies势模型计算了E=0·7eV时,氦原子的四种同位素3He,4He,9He,10He与氢分子H2碰撞体系的振转激发分波截面.通过分析各碰撞体系分波截面的差异,探讨了He(3He,4He,9He,10He)-H2碰撞体系的弹性碰撞、纯转动激发和振转激发情况下,其分波截面随量子数和体系约化质量的变化规律.     

Active manipulation of the selective alignment by two laser pulses

This paper solves numerically the full time-dependent Schrdinger equation based on the rigid rotor model, and proposes a novel strategy to determine the optimal time delay of the two laser pulses to manipulate the molecular selective alignment. The results illustrate that the molecular alignment generated by the first pulse can be suppressed or enhanced selectively, the relative populations of even and odd rotational states in the final rotational wave packet can be manipulated selectively by precisely inserting the peak of the second laser pulse at the time when the slope for the alignment parameter by the first laser locates a local maximum for the even rotational states and a local minimum for the odds, and vice versa. The selective alignment can be further optimised by selecting the intensity ratio of the two laser pulses on the condition that the total laser intensity and pulse duration are kept constant.     

Nonlinear phase adjustment of selective excitation pulses

A continuous transformation of an RF waveform with a modified Korteweg-de Vries equation or generalization can be used to adjust the phase behavior of a selective excitation pulse while preserving the magnitude behavior of the spin response. This transformation has applications in removing or adding to the nonlinear phase properties of a selected region.     

Theoretical study of the influence of intense femtosecond laser field on the evolution of the wave packet and the population of NaRb molecule

Employing the two-state model and the time-dependent wave packet method, we have investigated the influences of the parameters of the intense femtosecond laser field on the evolution of the wave packet, as well as the population of ground and double-minimum electronic states of the NaRb molecule. For the different laser wavelengths, the evolution of the wave packet of 6{ }^1\Sigma ^ + state with time and internuclear distance is different, and the different laser intensity brings different influences on the population of the electronic states of the NaRb molecule. One can control the evolutions of wave packet and the population in each state by varying the laser parameters appropriately, which will be a benefit for the light manipulation of atomic and molecular processes.     

矩形弹子球中的量子波包分析(英文)

利用波包分析量子力学体系的动力学行为在研究经典和量子的对应关系方面越来越成为一个非常重要的方法.利用高斯波包分析方法,我们计算了矩形弹子球体系的自关联函数,自关联函数的峰和经典周期轨道的周期符合的很好,这表明经典周期轨道的周期可以通过含时的量子波包方法产生.我们还讨论了矩形弹子球的波包回归和波包的部分回归,计算结果表明在每一个回归时间,波包出现精确的回归.对于动量为零的波包,初始位置在弹子球内部的特殊对称点处,出现一些时间比较短的附加的回归.     

Non-thermal rotational and vibrational excitation of CN produced in the flash photolysis of thiazole

In the flash photolysis of thiazole at low pressure without any diluent, the 0–0, 1–1 and 0–1 bands of the CN violet system were observed in absorption; the 0–0 band at 3883·4 Å showed a high rotational excitation corresponding to a temperature of ?2000 K. The addition of argon makes the NCS bands appear with good intensity and at the same time relaxes the CN rotationally and vibrationally. These observations suggest that highly excited NCS is initially formed in the photodecomposition of thiazole which acted as a precursor to the rotationally and vibrationally excited CN radical. This paper deals with studies on the effect of argon on the relative intensities of CN and NCS and on the non-thermal rotational and vibrational intensity distribution of the CN violet system. The mechanism of formation of rotationally unrelaxed CN in the flash photolysis of thiazole has been proposed.     

飞秒激光脉宽对非绝热耦合分子波包运动的影响研究

利用含时波包法研究了强飞秒泵浦-探测激光场中激光脉宽对非绝热耦合NaI分子波包运动的影响.发现波包的振荡周期随脉宽增长而增大,而振荡幅度随脉宽增长而减小.非绝热效应引起的波包在交叉区域的分裂情况影响各态布居.脉宽增长,NaI分子的激发概率增大,而解离概率减小.研究表明调节激光场脉宽可实现对波包运动的控制从而控制态布居的选择性分布.研究结果可以为实验上实现分子的光控制以及量子调控过程提供一定的参考.     

Li2分子含时波包动力学的理论研究

利用含时量子波包方法计算得到了Li2分子的光电子能谱,并运用波包动力学理论对含有不同参量的光电子能谱现象给出了合理的解释。通过分析文中的直观图像,研究了波包的动力学过程。结果表明,泵浦-探测脉冲的延迟时间对光电子能谱的形状有重要的影响;在较短延迟时间下,能谱独特的四峰现象是由光诱导势的产生引起的。     

Li2分子含时波包动力学的理论研究

利用含时量子波包方法计算得到了Li2分子的光电子能谱,并运用波包动力学理论对含有不同参量的光电子能谱现象给出了合理的解释.通过分析文中的直观图像,研究了波包的动力学过程.结果表明,泵浦-探测脉冲的延迟时间对光电子能谱的形状有重要的影响;在较短延迟时间下,能谱独特的四峰现象是由光诱导势的产生引起的.     

Investigation of plumes produced by material ablation with two time-delayed femtosecond laser pulses

We experimentally investigated and herewith reported the results of laser ablation of copper and gold with two time-delayed femtosecond laser pulses at 800 nm in vacuum. The ablation plume dynamic was monitored by fast plume imaging and time- and space-resolved optical emission spectroscopy. Optical microscopy was used to follow the ablation depth as a function of the delay between the two laser pulses. Nanoparticles deposition on mica substrates was analysed by atomic force microscopy.We estimate roughly the plume's atomization degree - that is the mass fraction of atomized material over the total ablated mass - from the relative intensities of radiation emitted from atoms and nanoparticles. It is shown that the atomization degree depends critically on the time delay between both laser pulses and on the characteristic time of electron-lattice relaxation. The increase of the atomization degree is accompanied by the decrease of the ablation depth. Atomic force microscopy measurements confirm the partial atomization of nanoparticles, as the analyses of particle deposition on mica substrates show a large decrease of the number of nanoparticles for large delay between the two pulses.     

High-resolution rotational spectroscopy of iminosilylene,HNSi

By means of Fourier transform microwave spectroscopy of a supersonic beam, the fundamental rotational transition of isotopic and vibrationally excited iminosilylene, HNSi, has been detected. In addition to seven isotopic species, vibrational satellite transitions from more than 30 vibrationally excited states, including the three fundamental modes, have been detected. Those from ν₂ are particularly intense, enabling detection of transitions from as high as (0,22⁰,0) (i.e. ～10,000 cm^?1 above ground). At high spectral resolution, well-resolved nitrogen quadrupole structure has been observed in nearly every transition. Excitation of ν₁ or ν₃ changes eQq(N) little, but eQq(N) systematically decreases with increasing excitation of the ν₂ bend, from a value of 0.376(5) MHz for (0,0⁰,0) to ?2.257(5) MHz for (0,20⁰,0). With the large amount of new data in hand, it has also been possible to determine the leading vibration–rotation constants (α_i and γ_i) for ν₂ or ν₃ to high precision, and derive a revised semi-empirical equilibrium structure for this fundamental triatomic molecule. Various electronic and molecular properties of iminosilylene have been calculated at the coupled cluster level of theory, and these generally agree well with experiment and previous calculations. An unsuccessful search for HSiN, a highly polar isomer calculated to lie nearly 3 eV above HNSi, is also reported.     

两束重合脉冲控制下的振转态布居转移

利用两束频率比为1:3的重合脉冲控制分子振转态布居转移. 计算结果表明, 初始态|0,0>到目标态|3,1>的跃迁概率接近100%. 两束脉冲的相位可以控制跃迁概率. 当φ ₁ =1.68 π 时, 两束脉冲相互增强, 跃迁概率增加. 当φ ₁ =0.64π 时, 两束脉冲相互抵消, 跃迁概率降低. 第二束脉冲的场强对布居转移过程具有较大影响.     

Analytical efficiency of the molecular rotational quantum echo

The sensitivity of the delay time of the molecular rotational quantum echo to change in the rotational constants of molecules was investigated with a model of the rotational quantum echo considered as an optically induced quantum synchronization of the Fourier rotational modes of an asymmetric molecular top. The J-echo and the K-echo were investigated for the A- and C-configurations of rotation of a top molecule. The contour maps of the dependence of the sensitivity of the delay time of these types of echo to changes in the rotational constants on the parameters of the molecular tops have been obtained for all the rotational constants. They show that the delay time of the rotational quantum echo is greatly dependent on the configuration of rotation of the top molecule and on the rotational constants. It is shown that the optical probing of the rotational quantum echo can also be performed by the optical rotation of the investigated molecule, and in this case the rotational force is dependent on the intramolecular orientation of the magnetic dipole moment. It was determined that a high sensitivity of the delay time of the echo to changes in the rotational constants can be responsible for the broadening of the echo pulse and even for its disappearance. Institute of Molecular and Atomic Physics, National Academy of Sciences of Belarus, 70 F. Skorina Ave., Minsk, 220072, Belarus; e-mail: lssm@imaph.bas-net.by. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 66, No. 6, pp. 758–764, November–December, 1999.     

两种扩展Harper模型的波包动力学

本文通过二次矩M₂(t)和概率分布W_n(t)数值地研究了两种扩展Harper模型的波包动力学,得到了这两种模型中各个相、各条临界线以及三相点的波包扩散情况.对于第一种扩展Harper模型,发现两个金属相中波包是弹道扩散的,在绝缘体相中波包不扩散,而在三相点以及各条临界线上波包是反常扩散的.同时,发现金属相—金属相转变的临界线上的波包动力学行为与金属相—绝缘体相转变的临界线上的相同,但三相点的动力学行为与各临 关键词： 金属绝缘体转变 扩展Harper模型 波包动力学     

Coherent excitation of molecular vibrational modes by high-power ultrashort infrared laser pulses

Coherent dynamics of multiphoton excitation of molecular vibrational modes by subpicosecond IR laser pulses differs greatly from that of picosecond pulse excitation. The resonance response of a molecule is primarily determined by the power broadening rather than the laser carrier frequency. Selective excitation of high vibrational levels is possible with the use of subpicosecond pulses.     

Effect of melting on the excitation of surface acoustic wave pulses by UV nanosecond laser pulses in silicon

The influence of melting on the excitation of Surface Acoustic Wave (SAW) pulses in silicon is studied both theoretically and experimentally. The developed theory of Rayleigh-type SAW laser-induced thermoelastic excitation in a structure composed of a liquid layer on a solid substrate predicts that the SAW is predominantly generated in the solid phase due to the absence of shear rigidity in a liquid. The characteristic changes in the SAW pulse shape as well as the saturation and even the decrease of the SAW pulse amplitude observed above the melting threshold are explained theoretically to be a result of the decrease of the heat flux into the solid phase as well as due to the decrease of the volume of the solid phase caused by melting. Although the heat flux into the solid phase is decreased both as a consequence of the reflectivity increase and the additional energy losses (latent heat of melting) at the phase transition, it is demonstrated that the influence of reflectivity changes on the SAW pulse is negligible in comparison with the effect of melt-front motion. For laser pulses of 7 ns duration at 355 nm, the threshold value of laser fluence for meltingF _m=0.23±0.04 J/cm² and for the ablationF _a=1.3±0.2 J/cm² were determined experimentally as the points of characteristic changes in the observed SAW pulses.     

Optical control of the rotational angular momentum of a molecular Rydberg wave packet

An intuitive scheme for controlling the rotational quantum state of a Rydberg molecule is demonstrated experimentally. We determine the accumulated phase difference between the various components of a molecular electron wave packet, and then employ a sequence of phase-locked optical pulses to selectively enhance or depopulate specific rotational states. The angular momentum composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multipulse response of the time-dependent Rydberg populations.