Phase-matched high harmonic generation for the study of rotational coherence molecular dynamics

We report the observation of periodic modulations in the high order harmonic radiation from diatomic molecules in a semi-infinitive gas cell when a preceding femtosecond laser beam, which is off-axis to the high-harmonic generation beam, modifies the phase-matching condition through the field-free alignment of the molecules. The observed modulations of the high harmonic radiation versus the time delay between the pulses result from periodic changes in the nonlinear refractive index associated with rotational Raman coherence. This opens up a new potential technique for studying rotational coherence dynamics in the ground states of molecules.     

Nonintrusive measurement of field-free molecular alignment

A technique was provided to nonintrusively quantify the field-free alignment of molecules by measuring the transient birefringence caused by the aligned molecules. Pure heterodyne alignment signals were obtained from the difference of the signals under an external electric field with opposite polarity and equal magnitude. The results demonstrated that the pure heterodyne alignment signal directly reproduced the revival structure of molecular alignment and its Fourier transform spectroscopy represented the actual populations of the different J states in the rotational wave packet.     

Selective alignment of molecular spin isomers

We experimentally demonstrate field-free, spin-selective alignment of ortho- and para molecular spin isomers at room temperature. By means of two nonresonant, strong, properly delayed femtosecond pulses within a four wave mixing arrangement, we observed selective alignment for homonuclear diatomics composed of spin 1/2 (15N) or spin 1 (14N) atoms. The achieved selective control of the isomers' angular distribution and rotational excitation may find applications to analysis, enrichment, and actual physical separation of molecular spin modifications.     

Controlling high harmonic generation with molecular wave packets

We show that, by controlling the alignment of molecules, we can influence the high harmonic generation process. We observed strong intensity modulation and spectral shaping of high harmonics produced with a rotational wave packet in a low-density gas of N2 or O2. In N2, where the highest occupied molecular orbital (HOMO) has sigma(g) symmetry, the maximum signal occurs when the molecules are aligned along the laser polarization while the minimum occurs when it is perpendicular. In O2, where the HOMO has pi(g) symmetry, the harmonics are enhanced when the molecules are aligned around 45 degrees to the laser polarization. The symmetry of the molecular orbital can be read by harmonics. Molecular wave packets offer a means of shaping attosecond pulses.     

Ionization effects on field-free molecular alignment observed with high-order harmonic generation

In this paper, high-order harmonic generation (HHG) is demonstrated to provide a sensitive way for studying the dynamic process in the field-free molecular alignment. The dependence of the harmonic yield and the degree of alignment on the intensity of aligning pulse is observed in impulsively aligned CO₂ molecules. A good agreement is found between the experimental and calculated results. At low pump intensities, the harmonic yield increases monotonously until the ionization induced refractive index gradient and neutral molecule depletion are significant. The results show that the optimum intensity is around 8.95 × 10¹³ W/cm²; this value is related to the molecular ionization potential.     

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.     

Dynamical analysis of the effect of elliptically polarized laser pulses on molecular alignment and orientation

In this Letter, we study the molecular alignment and orientation driven by two elliptically polarized laser pulses.It is shown that the field-free molecular alignment can be achieved in a three-dimensional(3D) case, while the field-free molecular orientation is only along the x and y directions, and that the field-free alignment and orientation along different axes are related to the populations of the rotational states. It is demonstrated that changing the elliptic parameter is efficient for controlling both in-pulse and post-pulse molecular alignment and orientation. The delay time also has an influence on the field-free molecular alignment and orientation.     

Alignment-dependent strong field ionization of molecules

We demonstrate a method to measure strong field laser ionization of aligned molecules. The method employs a macroscopic field-free dynamic alignment, which occurs during revivals of rotational wave packets produced by a femtosecond laser pulse. We investigate the dependence of strong field ionization of N2 on molecular orientation. We determine that N2 molecules are four times more likely to ionize when aligned parallel to the field than when aligned perpendicular to it.     

Modulation of third-harmonic generation conversion in the presence of a rotational wave packet

We report a modulation of third-harmonic generation (THG) owing to a rotational coherence in CO(2). The variation in conversion efficiency is mostly attributed to the dependence of chi(3)(tau) on the molecular alignment. THG via type I processes mainly depends on chi(3)(tau), while type II processes are influenced by the wave packet owing to both chi(3)(tau) and Delta k(tau). Observation of the generated third harmonic also shows significant changes of the polarization state owing to the birefringence induced by the rotational wave packet. Numerical modeling shows good qualitative agreement with the experimental data.     

Field-free three dimensional molecular axis alignment

We investigate strategies for field-free three dimensional molecular axis alignment using strong nonresonant laser fields under experimentally realistic conditions. Using the polarizabilites and rotational constants of an asymmetric top rotor molecule (ethene, C2H4), we consider three different methods for axis alignment of a Boltzmann distribution of rotors at 4 K. Specifically, we compare the use of impulsive kick laser pulses having both linear and elliptical polarization to the use of elliptically polarized switched laser pulses. We show that an enhanced degree of field-free three dimensional alignment of ground vibronic state molecules obtains from the use of two orthogonally polarized, time-separated laser pulses.     

Dynamics of molecular alignment steered by a few-cycle terahertz laser pulse

The field-free alignment of molecule ClCN is investigated by using a terahertz few-cycle pulse (THz FCP) based on the time-dependent density matrix theory. It is shown that a high degree of molecular alignment can be obtained by changing the matching number of the THz FCPs in the adiabatic regime and the non-adiabatic regime. The matching number can affect both the maximum value of the alignment and the time at which it is achieved. It is also found that a higher degree of alignment can be achieved by using the THz FCP at lower intensity and there exists an optimal threshold of molecular alignment with the increase of the field amplitude. Also found is the frequency sensitive region in which the degree of maximum alignment can be enhanced greatly by modulating the center frequencies of different THz FCPs. The investigation demonstrates that comparing with a THz single-cycle pulse, a better result of the field-free alignment can be created by a THz FCP at a constant rotational temperature of molecule.     

Extracting continuum electron dynamics from high harmonic emission from molecules

We show that high harmonic generation is the most sensitive probe of rotational wave packet revivals, revealing very high-order rotational revivals for the first time using any probe. By fitting high-quality experimental data to an exact theory of high harmonic generation from aligned molecules, we can extract the underlying electronic dipole elements for high harmonic emission and uncover that the electron gains angular momentum from the photon field.     

High-order harmonic transient grating spectroscopy in a molecular jet

We study high-order harmonic generation in excited media using a four-wave-mixing-like configuration. We analyze the spatial profile of high harmonics emitted by a grating of rotationally excited molecules as a function of the pump-probe delay. We demonstrate a dramatic improvement in the contrast of the diffracted signal relative to the total high harmonic signal. This allows us to observe subtle effects in the rotational wave packet excitation such as the pump-intensity dependence of the wave packet dynamics. High harmonic transient grating spectroscopy can be extended to all forms of molecular excitation and to weak resonant excitation.     

The study of third harmonic demodulation in phase modulation optical heterodyne technique using optical resonator

With the technique of phase modulation optical heterodyne(PMOH), we detected the beat-frequency signal of the reflected wave from a F-P cavity. The frequency of the beat signal was three times of that of the modulation electric field, when the 3rd harmonic of the modulation electric field was used as the phase reference signal. The line shapes of the signal match those of the theoretical calculations, and the dispersion signal has good frequency-discrimination characteristic.     

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.     

Coherent control of rotational wave-packet dynamics via fractional revivals

We show (i) how the evolution of a wave packet created from an initial thermal ensemble can be controlled by manipulating interferences during the wave packet's fractional revivals and (ii) how the wave-packet evolution can be mapped onto the dynamics of a few-state system, where the number of states is determined by the amount of information one wants to track about the wave packet in the phase space. We illustrate our approach by (i) switching off and on field-free molecular axis alignment induced by a strong laser pulse and (ii) converting alignment into field-free orientation, starting with rotationally cold or hot systems.     

Multiple conversion and optical limiting in a subharmonic-pumped parametric oscillator

We demonstrate that multiple coexisting frequency-conversion processes can occur in an externally resonant second-harmonic generator under suitable conditions. Besides the generation of signal and idler waves by subharmonic-pumped parametric oscillation, sum-frequency mixing among the resonant subharmonic (1064-nm), signal, and idler waves was observed, leading to additional emission wavelengths around the harmonic wavelength (532 nm). The output waves both exhibit high frequency stability, with as long as 4 h of mode-hop-free parametric oscillation, and are continuously tunable over 2 GHz. Near degeneracy the parametric oscillator operates as an optical limiter for the harmonic wave.     

基于群速度失配的超声兰姆波二次谐波的时域测量方法

考虑到发射和接收换能器对超声兰姆波时域二次谐波信号所带来的不可避免的影响,提出一种基于基频与二倍频兰姆波群速度失配的超声兰姆波二次谐波的时域测量方法。当基频与二倍频超声兰姆波的相速度匹配而群速度失配时,在超声兰姆波传播过程中所发生的二次谐波信号,在时域上可与源于斜劈换能器的二次谐波信号相分离。采用仅源自于基频兰姆波的时域二次谐波的积分振幅,定量描述兰姆波二次谐波的发生效率。以铝板中传播的兰姆波为例,给出了时域二次谐波的具体测量过程。本文提出的测量方法放宽了超声兰姆波二次谐波的测量条件,且扣除了换能器对二次谐波信号所带来的影响,所测得的二次谐波信号完全来自于基频兰姆波时域信号的二次谐波发生效应。      

利用锁相环和TV-Rb钟控制飞秒激光脉冲的载波包络相移

为了实现对锁模飞秒钛宝石激光器的相位控制，采用改进的相移测量装置，使载波包络频移信号的信噪比提高到了40 dB以上.在此优化测量结果的基础上，利用电子锁相环技术，通过PZT改变激光器腔内端镜的倾斜将飞秒激光脉冲的载波包络相位锁定到了微波参考源TV-Rb钟10 MHz标准信号上，同时激光脉冲重复频率也采用另一个PZT控制激光腔长锁定到了同一个TV-Rb钟10 MHz信号上.锁定后的结果显示重复频率的锁定达到了TV-Rb钟本身的稳定度，而载波包络相位锁定后比锁定前稳定度提高了三个数量级.     

Molecular recollision interferometry in high harmonic generation

We use extreme-ultraviolet interferometry to measure the phase of high-order harmonic generation from transiently aligned CO(2) molecules. We unambiguously observe a reversal in phase of the high-order harmonic emission for higher harmonic orders with a sufficient degree of alignment. This results from molecular-scale quantum interferences between the molecular electronic wave function and the recolliding electron as it recombines with the molecule, and is consistent with a two-center model. Furthermore, using the combined harmonic intensity and phase information, we extract accurate information on the dispersion relation of the returning electron wave packet as a function of harmonic order. This analysis shows evidence of the effect of the molecular potential on the recolliding electron wave.