Time-resolved photoelectron angular distributions from strong-field ionization of rotating naphthalene molecules

A nanosecond laser pulse confines the spatial orientation of naphthalene in 1D or 3D while a femtosecond kick pulse initiates rotation of the molecular plane around the fixed long axis. Time-dependent photoelectron angular distributions (PADs), resulting from ionization by an intense femtosecond probe pulse, exhibit pronounced changes as the molecular plane rotates. Enhanced 3D alignment, occurring shortly after the kick pulse, provides strongly improved contrast in molecular-frame PADs. Calculations in the strong-field approximation show that the striking structures observed in the PADs originate from nodal planes in occupied valence orbitals.     

Kinetic energy release of diatomic and linear triatomic molecules in intense femtosecond laser fields

The kinetic energy release of fragment ions produced by the interaction of femtosecond laser pulse radiation with diatomic and linear triatomic molecules N_2, CO, CO_2 and CS_2 is investigated. In the case of linear polarization, angles at which the kinetic energy release of ions has the maximum value are different from the alignment of molecules though the kinetic energy release of fragment atomic ions depends on the angle between the laser polarization vector and the detection axis of the time-of-flight. For the diatomic molecules, the critical internuclear distance in multielectron dissociative ionization with a circularly polarized light is larger than that with a linearly polarized light. For linear triatomic molecules, our data indicate that a concerted Coulomb explosion process is a universal phenomenon in the interaction of molecules with intense laser fields, even in the circularly polarized regime. During two C－O (or C－S) bonds breaking simultaneously, the C ion obtained larger energy in circular polarization than that in the linear polarization. Different variations of kinetic energy release between the diatomic and the linear triatomic molecules are discussed.     

椭圆偏振强激光场中准直的乙炔分子的高次谐波发射

We perform an experimental study on high-order harmonic generation (HHG) of aligned acetylene molecules induced by a 35-fs 800-nm strong laser field, by using a home-built HHG spectrometer. It is observed that the molecular HHG probability declines with increasing the laser ellipticity, which is in consistence with the deduction from the well-known tunneling-plus-rescattering scenario. By introducing a weak femtosecond laser pulse to nonadiabatically align the molecules, we investigated the molecular orbital effect on the HHG in both linearly and elliptically polarized driving laser fields. The results show that the harmonic intensity is maximum for the molecular axis aligned perpendicularly to the laser electric field. It indicates that both the highest occupied molecular orbitals (HOMO) and HOMO-1 contribute to the strong-field HHG of acetylene molecules. Our study should pave the way for understanding the interaction of molecules with ultrafast strong laser fields.     

Wavelength femtosecond light pulse generated from filamentation-assisted fourth-order nonlinear process in potassium titanyl phosphate crystal

A femtosecond light pulse at 480 nm in wavelength was generated during filamentation of an intense 808 nm femtosecond laser pulse propagating along the x axis and polarized between the y and z axes of a KTP crystal. It was proven that the parametric amplification process by a fourth-order nonlinear polarization (chi(4)(omega(2),omega,omega,omega,-omega(1)) induces frequency generation at 480 nm, where the pump light comes from the incident laser and the seed light comes from the generated supercontinuum by filamentation. The wavelength of the generated signal could be turned from 460 to 520 nm by adjusting the propagation direction in the crystal.     

不同偏振飞秒激光经块状材料传输后的脉宽压缩

实验研究了线偏振和圆偏振状态下的飞秒强激光脉冲在块状材料中的传输过程。不同偏振的激光脉冲在传输过程中得到了不同程度的光谱展宽,经色散补偿后,脉冲时域宽度均得到了压缩。详细分析了压缩脉冲的脉宽以及啁啾情况与入射激光脉冲能量之间的关系,比较了飞秒激光在线偏振及圆偏振情况下的不同压缩效果。在线偏振入射光情况下得到了最短21fs的压缩脉冲宽度,在圆偏振情况下得到的最短脉冲宽度为22fs。实验结果表明,这种光谱展宽与色散补偿方式对圆偏振光同样适用,而且圆偏振的入射激光将更有利于对更高能量的脉冲进行压缩。在色散补偿量相同的情况下,压缩效果随入射脉冲能量变化的规律符合理论估计。     

Postpulse molecular alignment measured by a weak field polarization technique

We report a direct nonintrusive observation of alignment and planar delocalization of CO2 after an intense linearly polarized femtosecond laser pulse excitation. The effects are measured by a polarization technique involving a perturbative probe that itself does not induce appreciable alignment. We show that this technique allows one to measure a signal proportional to -1/3, with theta the angle between the molecular axis and the laser polarization. Simulations that support this analysis allow one to characterize the experimentally observed alignment and planar delocalization quantitatively.     

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.     

飞秒激光脉冲整形技术及其应用

通过频域上控制飞秒激光脉冲幅度、相位和偏振在时域上可以获得几乎任意形状的飞秒激光脉冲,这种飞秒激光脉冲整形技术可为研究光与原子分子非线性相互作用提供一种全新实验技术手段.本文介绍飞秒激光脉冲整形发展历史、技术方法、控制方式及其相关应用,并展望飞秒激光脉冲整形技术未来的发展方向.     

Microjoule-level all-polarization-maintaining femtosecond fiber source

We report on a high-power, high-energy femtosecond fiber source based on direct amplification of parabolic pulses from an environmentally stable passively mode-locked fiber oscillator in an Yb-doped single-polarization photonic crystal fiber. The special pulse shape allows for the generation of high-quality femtosecond pulses beyond nonlinearity limits. The system delivers a pulse energy of 1.2 microJ (21 W average power) at a repetition rate of 17 MHz and a pulse duration of 240 fs in a linearly polarized beam with diffraction-limited quality.     

Probing molecular dynamics at attosecond resolution with femtosecond laser pulses

The kinetic energy distribution of D+ ions resulting from the interaction of a femtosecond laser pulse with D2 molecules is calculated based on the rescattering model. From analyzing the molecular dynamics, it is shown that the recollision time between the ionized electron and the D+2 ion can be read from the D+ kinetic energy peaks to attosecond accuracy. We further suggest that a more precise reading of the clock can be achieved by using shorter fs laser pulses (about 15 fs).     

Possibilities for controlling attosecond x-ray pulse generation during molecular ionization by femtosecond laser radiation

We discuss the role of different factors (molecular sizes and configuration, orientation of the molecular axis with respect to the electric field of a laser pulse, the type of the molecular orbital, etc.), which characterize molecules and their state, in the formation of the nonlinear response of a molecule ionized by a high-power femtosecond laser pulse. In numerical experiments within the framework of a two-dimensional model for the H ₂ ⁺ molecular ion, we study possibilities for controlling the process of nonlinear frequency conversion of femtosecond optical radiation into X-ray radiation of attosecond duration by means of preliminary vibrational or electronic excitation of molecules. We demonstrate the possibilities of using the attosecond pulse generation as a diagnostic tool for probing vibration-rotational dynamics of molecules.     

Rewritable polarization-encoded multilayer data storage in 2,5-dimethyl-4-(p-nitrophenylazo)anisole doped polymer

We report a rewritable polarization-encoded multilayer data storage method with a polymer film doped with the azo dye DMNPAA (2,5-dimethyl-4-(p-nitrophenylazo)anisole). It is found that under two-photon excitation by a linearly polarized femtosecond laser beam at wavelength 780 nm the optical axis of DMNPAA molecules can be oriented to the perpendicular direction of the beam via a trans-cis-trans isomerization process. As a result, multilayer polarization-encoded optical data storage is demonstrated by recording two letters of a bit spacing of 4 microm in the same region of a given layer. It is shown that erasing and rewriting a particular layer is possible.     

Frequency doubling and Fourier domain shaping the output of a femtosecond optical parametric amplifier: easy access to tuneable femtosecond pulse shapes in the deep ultraviolet

Tuneable, shaped, ultraviolet (UV) femtosecond laser pulses are produced by shaping and frequency doubling the output of a commercial optical parametric amplifier (OPA). A reflective mode, folded, pulse shaping assembly employing a spatial light modulator (SLM) shapes femtosecond pulses in the visible region of the spectrum. The shaped visible light pulses are frequency doubled to generate phase- and amplitude-shaped, ultrashort light pulses in the deep ultraviolet. This approach benefits from a simple experimental setup and the potential for tuning the central frequency of the shaped ultraviolet waveform. A number of pulse shapes have been synthesised and characterised using cross-correlation frequency resolved optical gating (XFROG). This pulse shaping method can be employed for coherent control experiments in the ultraviolet region of the spectrum where many organic molecules have strong absorption bands. D.S.N. Parker and A.D.G. Nunn contributed equally to this work.     

Femtosecond laser control of intramolecular vibrations in a liquid

Optical control of coherent intramolecular oscillations in chloroform CHCl₃ and dimethyl sulfoxide (CH₃)₂SO is attained experimentally under normal conditions by means of femtosecond polarization spectroscopy. Nonresonant excitation of the medium is accomplished by a sequence of two linearly polarized laser pulses. The state of the medium is probed by the third pulse via the optical Kerr effect. We show that control over the vibrational dynamics of molecules on a sub-picosecond scale can be achieved by varying the delay between the excitation pulses and their relative intensity.     

Characterization of elliptically polarized femtosecond pulses by molecular-alignment-based frequency resolved optical gating

We demonstrated that molecular-alignment-based cross-correlation frequency resolved optical gating (M-XFROG) could be used for complete characterization of elliptically polarized femtosecond pulses by measuring the orthogonal linear polarization components and the additional polarization projection at 45 degree of the target pulse. The electric field orientation, polarization ellipticity angles, and phase information of the target pulse were also obtained. The transiently aligned air molecules functioned as a linear optical gating function in the measurement processes. The validity and robustness of M-XFROG were confirmed by the comparison between the retrieved optical gating function and measured molecular alignment signal in air.     

All-optical magnetic recording with circularly polarized light

We experimentally demonstrate that the magnetization can be reversed in a reproducible manner by a single 40 femtosecond circularly polarized laser pulse, without any applied magnetic field. This optically induced ultrafast magnetization reversal previously believed impossible is the combined result of femtosecond laser heating of the magnetic system to just below the Curie point and circularly polarized light simultaneously acting as a magnetic field. The direction of this opto-magnetic switching is determined only by the helicity of light. This finding reveals an ultrafast and efficient pathway for writing magnetic bits at record-breaking speeds.     

Phase dependence of enhanced ionization in asymmetric molecules

We study enhanced ionization (EI) in asymmetric molecules by solving the 3D time-dependent Schr?dinger equation for HeH2+ driven by a few-cycle laser pulse linearly polarized along the molecular axis. We find that EI is much stronger when the laser's carrier-envelope phase is such that the electric field at the peak of the pulse is antiparallel to the permanent dipole of the molecule (PDM). This phase dependence is explained by studying the molecule in the presence of a static electric field. When this field is antiparallel to the PDM, the energy of the dressed ground state moves up (with increasing internuclear distance R) to cross with excited states, leading to a stronger ionization via intermediate state resonances and via tunneling. We predict analytically the laser and molecular parameters at which these crossings are expected to occur in any asymmetric molecule.     

波包动力学-飞秒激光操纵波包过程

本文介绍了波包动力学的基本理论和数值模拟方法,尤其是在飞秒激光与分子相互作用领域中的应用,探讨了飞秒激光引起的波包过程（包括波包的制备、波包的干涉）,以及利用调频脉冲、脉冲串和优化脉冲形状控制波包动力学的方案。     

波包动力学-飞秒激光操纵波包过程

本文介绍了波包动力学的基本理论和数值模拟方法,尤其是在飞秒激光与分子相互作用领域中的应用,探讨了飞秒激光引起的波包过程（包括波包的制备、波包的干涉）,以及利用调频脉冲、脉冲串和优化脉冲形状控制波包动力学的方案。     

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.