Control of femtosecond filamentation by field-free revivals of molecular alignment

We show that the filamentation dynamics of a femtosecond laser probe pulse can be readily controlled by properly matching it to the quantum revivals of pre-aligned molecules prepared through impulsive rotational Raman excitation with an advancing ultrashort pump pulse. Several features of the filamentation process including supercontinuum generation, the length of the plasma channel generated in the wake of the filament, the associated secondary radiations and the multiple filamentation pattern are all easily modified by tuning the cross phase modulation induced by the field-free revivals of molecular alignment, through the delay between the pump and the probe pulses. We show that molecular alignment can also be used to generate conical waves with extremely short intensity spike called shocked X-waves and to further tune the frequency of a few-cycle laser pulse in the wake of a self-guided intense filament.     

基于旋转相干光谱的整形飞秒激光转动动力学调控

我们实验上发展了基于飞秒激光旋转相干光谱的整形飞秒激光转动动力学调控方法,通过脉冲整形技术调控激发脉冲的光谱相位,从而实现对飞秒激光作用下转动态相干激发过程中复原信号及转动布居数的调控. 研究了飞秒激光旋转相干光谱对激光频谱相位的响应机制,突出了飞秒激光频谱相位在气相分子转动态相干激发中的重要作用. 为飞秒激光作用下生物大分子和团簇鉴别及结构探测研究提供了新的参考.     

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.     

Laser-induced Alignment and Coulomb Explosion of CO2

实验研究了CO₂分子在飞秒强激光脉冲作用下的动力学过程,包括分子取向,隧穿电离和库仑爆炸,激光强度从1×10¹³W/cm²变化到6×10¹⁴W/cm². 当激光强度小于分子的电离阈值时,CO₂分子的非绝热转动激发形成一个相干转动波包,波包演化导致分子沿激光电场方向取向. 激光脉冲结束后,分子取向可以周期性地再现,利用另一束激光可以对取向结构进一步进行修饰. 当激光强度大于分子     

Effects of aligning pulse duration on the degree and the slope of nitrogen field-free alignment

Through theoretical analysis,we show how aligning pulse durations affect the degree and the time-rate slope of nitrogen field-free alignment at a fixed pulse intensity.It is found that both the degree and the slope first increase,then saturate,and finally decrease with the increasing pump duration.The optimal durations for the maximum degree and the maximum slope of the alignment are found to be different.Additionally,they are found to mainly depend on the molecular rotational period,and are affected by the temperature and the aligning pump intensities.The mechanism of molecular alignment is also discussed.     

Synthesis of periodic femtosecond pulse trains in the ultraviolet by phase-locked Raman sideband generation

We demonstrate a new technique for femtosecond-pulse generation that employs ultrafast modulation of a laser field phase by impulsively excited molecular rotational or vibrational motion with subsequent temporal compression. An ultrashort pump pulse at 800 nm performs impulsive excitation of a molecular gas in a hollow waveguide, and a weak delayed probe pulse at 400 nm is scattered on the temporal oscillations of its dielectric index. The resultant sinusoidal phase modulation of the probe pulse permits probe pulse temporal compression by use of both positively and negatively dispersive elements. The potential of this new method is demonstrated by the generation of a periodic train of 5.8-fs pulses at 400 nm with positive group-delay dispersion compensation.     

Field-free molecular alignment and its application

Field-free molecular alignment can be achieved by nonadiabatic rotational excitation of molecules with strong femtosecond laser pulses. We experimentally and theoretically demonstrate that the degree of alignment can be improved with multi-pulse excitation. An approach is proposed to tune the frequency of few-cycle pulses using field-free alignment of molecules.     

Selective Alignment of D2 Induced by Two Ultrashort Laser Pulses

通过求解D₂分子在飞秒激光场中的含时薛定谔方程,研究了室温下D₂分子在超快飞秒激光驱动下的的转动波包动力学. 选择用第一束超短飞秒脉冲与温度为300 K的D₂分子系综相互作用产生一个相干转动波包,用第二束超短飞秒脉冲在波包的1/4和3/4恢复周期选择操纵D₂分子取向. 研究结果表明,通过选择两束超短飞秒脉冲的延迟时间,可以有效控制D₂分子转动波包中奇偶态的相对布居,从而选择性的控制D₂分子取向.     

Selective excitation of the molecular rotational wave packet by two time-delayed laser pulses

In this paper, we investigate the control of the molecular wave packet of a linear molecule by two femtosecond laser pulses. It is shown that the odd and the even rotational wave packets created by a single laser pulse can be selectively excited by accurately controlling the time delay of another laser pulse. By inserting the peak of the second laser pulse at the position of maximum or minimum value around quarter or three quarter rotational period of the slope curve with odd (or even) rotational wave packet contribution that is created by the first laser pulse, the odd rotational wave packet can be enhanced (or suppressed) while the even rotational wave packet is suppressed (or enhanced). As a result, the molecular alignments around quarter and three quarter rotational periods can be obtained. Moreover, it is also shown that by inserting the second laser pulse around the quarter or three quarter rotational periods, the changes in the maximum degree of the molecular alignment for the odd and the even rotational wave packet contributions are consistent with their corresponding slope curves at these positions.     

Effect of tunneling ionization on dynamic alignment and post-ionization alignment of nitrogen molecules irradiated by different laser intensities

The dynamic alignment and post-ionization alignment of nitrogen molecules are investigated while considering the effect of tunneling ionization. The effects of tunneling ionization on the angular distribution are calculated when the molecules are irradiated by different laser intensities. The results show that laser intensity directly affects the time and extent of dynamic alignment. Furthermore, the extent of post-ionization alignment is not only determined by laser intensity but also affected by the final extent of dynamic alignment. The post-ionization alignment will dominate during the process of molecular (or molecular ion) rotational alignment for femtosecond laser pulse. The time of tunneling ionization is a significant factor to the final ensemble angular distribution of molecular ions when laser intensity is low.     

Measurement of laser-induced alignment of molecules by cross defocusing

The field-free alignment of CO2 produced in response to the excitation of a molecule by a high-intensity femtosecond pump pulse is measured with a simple coronography-like technique. The technique is based on the defocusing of a time-delayed probe pulse produced by the spatial distribution of aligned molecules. In the intensity regime explored here, the technique is shown to give valuable information about dynamic alignment. With the help of simulations, the degree of alignment is extracted from the data.     

Field-free molecular orientation induced by combined femtosecond single- and dual-color laser pulses：The role of delay time and quantum interference

The coherent control of field-free molecular orientation of CO with combined femtosecond single- and dual-color laser pulses has been theoretically studied. The effect of the delay time between the femtosecond single- and dual-color laser pulses is discussed, and the physical mechanism of the enhancement of molecular orientation with pre-alignment of the molecule is investigated. It is found that the basic mechanism is based on the creation of a rotational wave packet by the femtosecond single-color laser pulse. Furthermore, we investigate the interference between multiple rotational excitation pathways following pre-alignment with femtosecond single-color laser pulse. It is shown that such interference can lead to an enhancement of the orientation of CO molecule by a factor of 1.6.     

Conservation of molecular alignment for cyclic rotational wave packets in periodic pulse trains

The existence of states for which molecular alignment can be maintained for long periods of time is shown. These states, consisting of coherent superpositions of rotational states, are found among cyclic states of the generalized Floquet operator corresponding to a molecule in a short nonresonant laser pulse. For a single pulse alignment can be maintained, in some cases, for more than 40 times the pulse duration. Because of the special properties of these coherent states, arbitrarily long alignment can be achieved by using well-timed pulse trains.     

Tunable light source for coherent anti-Stokes Raman scattering microspectroscopy based on the soliton self-frequency shift

We present a photonic crystal fiber (PCF)-based light source for generating tunable excitation pulses (pump and Stokes) that are applicable to coherent anti-Stokes Raman scattering (CARS) microspectroscopy. The laser employed is an unamplified Ti:sapphire femtosecond laser oscillator. The CARS pump pulse is generated by spectral compression of a laser pulse in a PCF. The Stokes pulse is generated by redshifting a laser pulse in a PCF through the soliton self-frequency shift. This setup allows for probing up to 4000 cm(-1) with a spectral resolution of approximately 25 cm(-1). We characterize the stability and robustness of CARS microspectroscopy employing this light source.     

Role of highest occupied molecular orbitals in molecular field-free alignment by a femtosecond pulse

This paper studies the molecular rotational excitation and field-free spatial alignment in a nonresonant intense laser field numerically and analytically by using the time-dependent Schr?dinger equation. The broad rotational wave packets excited by the femtosecond pulse are defined in conjugate angle space, and their coefficients are obtained by solving a set of coupled linear equations. Both single molecule orientation angles and an ensemble of O₂ and CO molecule angular distributions are calculated in detail. The numerical results show that, for single molecule highest occupied molecular orbital (HOMO) symmetry σ tends to have a molecular orientation along the laser polarization direction and the permanent dipole moment diminishes the mean of the orientation angles; for an ensemble of molecules, angular distributions provide more complex and additional information at times where there are no revivals in the single molecule plot. In particular, at the revival peak instant, with the increase of temperature of the molecular ensemble, the anisotropic angular distributions with respect to the laser polarization direction of the π _g orbital gradually transform to the symmetrical distributions regarding the laser polarization vector and for two HOMO configurations angular distributions of all directions are confined within a smaller angle when the temperature of the molecular ensemble is higher.     

Efficient rotational Raman conversion of XeCl laser radiation in H2

2 is investigated with a XeCl laser. It is shown that energy conversion to rotational Stokes radiation can be efficiently obtained by properly choosing the focusing geometry of pump radiation and the pressure of the Raman medium even at moderate pulse energies. Energy conversion to the first rotational Stokes at 313.8 nm with efficiencies as high as 38% is obtained with a circularly polarised XeCl pump beam of 10-mJ energy focused in 30 bar of H₂. The spectral and optical characteristics of the pump and the rotational Stokes radiation are analysed. Received: 29 May 1996/Revised version: 7 March 1997     

Control of molecular rotation with a chiral train of ultrashort pulses

Trains of ultrashort laser pulses separated by the time of rotational revival (typically, tens of picoseconds) have been exploited for creating ensembles of aligned molecules. In this work we introduce a chiral pulse train--a sequence of linearly polarized pulses with the polarization direction rotating from pulse to pulse by a controllable angle. The chirality of such a train, expressed through the period and direction of its polarization rotation, is used as a new control parameter for achieving selectivity and directionality of laser-induced rotational excitation. The method employs chiral trains with a large number of pulses separated on the time scale much shorter than the rotational revival (a few hundred femtosecond), enabling the use of conventional pulse shapers.     

Collisionally pumped hybrid soft X-ray laser in Ne-like sulphur

We describe an experiment demonstrating XUV amplification following collisional excitation in a capillary discharge plasma irradiated by a picosecond IR laser pulse. Guiding and temporally resolved transmission of the pump laser beam are also demonstrated and analysed. The short pump laser pulse heated rapidly the electrons producing amplification in the 3p¹S₀–3s¹P₁ transition of Ne-like sulphur at 60.84 nm. The estimated gain–length product was equal to 6.8, while the beam divergence reached 2.5 mrad for 30 mm capillary. This new, hybridly pumped collisional soft X-ray laser with the transient gain offers a new way towards efficient table-top XUV sources.     

Numerical simulation of a CW-pumped Cr:YAG passively Q-switched Yb:YAG pulsed laser

A general model of a CW-pumped passively Q-switched laser is presented which considers the pump power and excitation state of the absorber. The recovery time of the absorber is affected by the Q-switched laser pulse length and repetition rate, which results in changes of the output power, peak power and pulse duration of a CW-pumped passively Q-switched solid-state laser. At low pump power, the final inversion population density alters slowly by a small amount and the effect of the absorber's finite recovery time on laser output energy can be ignored. At high pump power, the final inversion population density increases quickly with pump power increase and the output energy decreases greatly. Simulation results of a CW-pumped, Cr:YAG Q-switched, Yb:YAG laser are reported. The numerical simulation results agree with the theoretical analytical analysis.     

Experimental Investigation on Selective Excitation of Two-Pulse Coherent Anti-Stokes Raman Scattering

Selective excitation of coherent anti-Stokes Raman scattering from the benzene solution is achieved by adaptive pulse shaping based on genetic algorithm, and second harmonic generation frequency-resolved optical gating （SHG-FROG） technique is adopted to characterize the original and optimal laser pulses. The mechanism for two-pulse coherent mode-selective excitation of Raman scattering is experimentally investigated by modulating the pump pulse in the frequency domain, and it is indicated that two-pulse coherent mode-selective excitation of Raman scattering mainly depends on the effective frequency components of the pump pulse related to specific vibrational mode. The experimental results suggest that two-pulse CARS has good signal-to-background ratio and high sensitivity, and it has attractive potential applications in the complicated molecular system.