氢负离子在梯度电场中光剥离的波包动力学研究

利用含时微扰论和闭合轨道理论相结合的方法, 给出了氢负离子在梯度电场中自关联函数的计算公式, 并且对体系的自关联函数进行了计算和分析. 重点探讨了激光脉冲的宽度、梯度电场中背景电场强度及电场梯度对氢负离子体系的自关联函数的影响. 研究结果表明, 当激光脉冲的脉冲宽度较短, 远小于剥离电子的闭合轨道的周期时, 量子波包的回归现象显著, 自关联函数中会出现一系列比较明显的回归峰, 这是由于沿闭合轨道返回的电子波包和出射的电子波包之间产生干涉形成的. 但是随着激光脉冲宽度的增加, 量子波包的回归现象减弱. 当脉冲宽度和闭合轨道的周期相差不是很大时, 自关联函数中的回归峰逐渐变宽, 振荡渐趋平缓, 相邻的峰之间发生相互干涉, 从而导致对应关系消失. 除此之外, 我们还发现梯度电场中背景电场强度和电场梯度对体系的自关联函数也会发生显著的影响. 随着背景电场强度和电场梯度的增加, 剥离电子的闭合轨道的周期变短, 自关联函数中回归峰的个数逐渐增加, 量子回归现象增强. 因此, 我们可以通过改变脉冲的宽度、外加电场强度的大小对氢负离子发生光剥离的自关联函数进行调控. 我们的结果对于实验研究原子或离子体系在外场中的波包动力学性质可以提供一定的参考价值.     

Electric field controlled, pulsed autoionization in two electron wave packets

In this paper, control of the evolution of a two electron wave packet through the application of a static electric field is demonstrated. Specifically, application of a small electric field is used to produce pulsed autoionization events, the timing of which can be controlled on a picosecond time scale. The technique is demonstrated by exciting calcium atoms using a short-pulsed laser to the 4p(3/2)19d doubly excited state, which is energy degenerate with the 4p(1/2)nk stark states. Evolution of the resultant wave packet is monitored through the application of a second short laser pulse, which stimulates the atoms to emit a photon producing singly excited Rydberg states which are detected using field ionization.     

Semiclassical calculation of ionisation rate for Rydberg helium atoms in an electric field

The ionisation of Rydberg helium atoms in an electric field above the classical ionisation threshold has been examined using the semiclassical method, with particular emphasis on discussing the influence of the core scattering on the escape dynamics of electrons. The results show that the Rydberg helium atoms ionise by emitting a train of electron pulses. Unlike the case of the ionisation of Rydberg hydrogen atom in parallel electric and magnetic fields, where the pulses of the electron are caused by the external magnetic field, the pulse trains for Rydberg helium atoms are created through core scattering. Each peak in the ionisation rate corresponds to the contribution of one core-scattered combination trajectory. This fact further illustrates that the ionic core scattering leads to the chaotic property of the Rydberg helium atom in external fields. Our studies provide a simple explanation for the escape dynamics in the ionisation of nonhydrogenic atoms in external fields.     

First-principles electron dynamics control simulation of diamond under femtosecond laser pulse train irradiation

A real-time and real-space time-dependent density functional is applied to simulate the nonlinear electron-photon interactions during shaped femtosecond laser pulse train ablation of diamond. Effects of the key pulse train parameters such as the pulse separation, spatial/temporal pulse energy distribution and pulse number per train on the electron excitation and energy absorption are discussed. The calculations show that photon-electron interactions and transient localized electron dynamics can be controlled including photon absorption, electron excitation, electron density, and free electron distribution by the ultrafast laser pulse train.     

Controlling the angular momentum composition of a Rydberg electron wave packet

Sequences of phase-locked laser pulses have been employed to control the orbital angular momentum character of an electron wave packet, which is initially created from a superposition of s and d Rydberg series. By an intelligent choice of phase, which depends on the excitation energy and the quantum defects, we are able to selectively pump down either all or a fraction of one or other angular momentum component, and by employing multichannel quantum-defect theory we are able to analyze the quantum-state distribution in detail.     

H-在金属面附近光剥离的波包动力学研究

利用波包演化和自关联函数方法对H^-在金属面附近光剥离的波包动力学进行了研究.结果表明,金属面附近光剥离电子的波包演化和回归结构与H^-到金属面的距离、激光脉冲的脉冲宽度和初始动量都有一定的关系.因此,可以通过改变离子表面距离和激光脉冲的参数对光剥离电子的动力学性质进行调控研究.除此之外,光剥离电子的镜像态寿命对波包的演化和自关联函数也会产生一定的影响:考虑镜像态寿命的影响时,随着时间的演化,波包概率密度的振幅逐渐减小,波包整体上有明显的衰减,寿命对波包演化过程中的干涉有削弱的作用;通过对电子波包的自关联函数研究,发现无限长寿命的电子波包有很好的量子回归现象,而当考虑寿命因素后光剥离电子波包随着时间的演化会发生周期性的坍塌和扩散,经过一段时间后,该回归现象消失.本文的理论研究可以为表面附近电子波包动力学的实验研究提供一定的参考价值. 关键词： 波包 演化和回归 自关联函数 金属面     

Quantum state reconstruction of a rotational wave packet created by a nonresonant intense femtosecond laser field

We have experimentally determined the amplitudes and phases of a rotational wave packet in an adiabatically cooled benzene molecule, created by a nonresonant intense femtosecond laser field. In this wave-packet reconstruction, the initial wave packet is further interfered by a replica of the first laser pulse, and the resultant modulation in population is observed in a state-resolved manner. Though several states with different nuclear-spin modifications are populated in the initial condition, a single wave packet created from one of them (with J=0) is specifically reconstructed. Phase shifts characteristic of stepwise Raman excitation beyond the perturbative regime are experimentally identified.     

Extracting the phase distribution of the electron wave packet ionized by an elliptically polarized laser pulse

We use an interferometic scheme to extract the phase distribution of the electron wave packet from above-threshold ionization in elliptically polarized laser fields. In this scheme, an electron wave packet released from a circularly polarized laser pulse acts as a reference wave and interferes with the electron wave packet ionized by a time-delayed counter-rotating elliptically polarized laser field. The generated vortex-shaped interference pattern in the photoelectron momentum distribution enables us to extract the phase distribution of the electron wave packet in the elliptically polarized laser pulse with high precision. By artificially screening the ionic potential at different ranges when solving the time-dependent Schördinger equation, we find that the angle-dependent phase distribution of the electron wave packet in the elliptically polarized laser field shows an obvious angular shift as compared to the strong-field approximation, whose value is the same as the attoclock shift. We also show that the amplitude of the angle-dependent phase distribution is sensitive to the ellipticity of the laser pulse, providing an alternative way to precisely calibrate the laser ellipticity in the attoclock measurement.     

Observation of inner electron ionization from radial rydberg wave packets in two-electron atoms

We have observed multiphoton ionization of the 5s core electron from a 5snd radial Rydberg wave packet of Sr atoms using a short optical pulse. When the outer nd electron is at its outer turning point the inner 5s electron is removed from the atom, and the outer electron is left in a Sr+ Rydberg state, but when the outer electron is at the inner turning point this does not occur. Analysis of the final Sr+ Rydberg states shows that the two electrons interact as the inner electron leaves, so that the outer electron is not simply projected onto the Sr+ Rydberg states.     

Excitation of Rydberg states of atoms and diatomic molecules by short laser impulses

Excitation of multilevel Rydberg states (atoms and diatomic molecules) is studied under an intense time-periodic perturbation that is instantaneously turned on and off. For a one-quantum excitation from a lower lying state, general expressions for the Laplace images of the population amplitudes of Rydberg states are obtained with regard to their decay characteristics. It is shown that the problem considered is reduced to the determination of the positions and widths of the energy levels of a quantum system in the field of monochromatic laser radiation of the same frequency and intensity as that in a pulse mode. To determine these quantities, an integral formulation is proposed for the eigenvalue problem for energies that is relatively simply solved with regard to the effect of the ionic core and its complex vibration-rotation structure on diatomic molecules. The specific features of the excitation of Rydberg states and the behavior of Rydberg wave packets are studied depending on the intensity and duration of laser radiation. A quantum phenomenon of rotational orientation of electron-excited diatomic molecules is considered.     

磁场中氢里德堡波包的自动关联函数

本文采用激光短脉冲激发磁场中氢原子,研究氢里德堡波包在磁场中随时间的演化.结果证实氢里德堡波包在磁场中的运动也与闭合轨道密切相关.讨论了脉冲宽度τ对自动关联函数的影响以及不同初始态下的自动关联函数.     

Mapping attosecond electron wave packet motion

Attosecond pulses are produced when an intense infrared laser pulse induces a dipole interaction between a sublaser cycle recollision electron wave packet and the remaining coherently related bound-state population. By solving the time-dependent Schr?dinger equation we show that, if the recollision electron is extracted from one or more electronic states that contribute to the bound-state wave packet, then the spectrum of the attosecond pulse is modulated depending on the relative motion of the continuum and bound wave packets. When the internal electron and recollision electron wave packet counterpropagate, the radiation intensity is lower. We show that we can fully characterize the attosecond bound-state wave packet dynamics. We demonstrate that electron motion from a two-level molecule with an energy difference of 14 eV, corresponding to a period of 290 asec, can be resolved.     

高次谐波产生阿秒极紫外和X光脉冲研究新进展

 近年来在可见光谱范围内已经把激光脉冲压缩到接近一个光学周期(2～3 fs)的物理极限,几fs的时间分辨精度可以描述分子化学反应过程,但是要探测远小于可见光周期的电子跃迁过程则需要阿秒(as)量级的光脉冲。利用脉冲间具有相同载波包络相位的阿秒脉冲序列能把可见光波段的光学频率梳向极紫外波段扩展;利用电子和离子碰撞复合过程短于一个光周期这个时间窗,通过测量激光场椭圆极化率对电子轨迹的微扰实现了as精度的分辨率;通过测量碰撞复合过程中的高能电子的辐射谱可以重构阿秒X光脉冲以及探测强场下束缚态和连续态电子动力学。     

Clocking femtosecond X rays

Linear-accelerator-based sources will revolutionize ultrafast x-ray science due to their unprecedented brightness and short pulse duration. However, time-resolved studies at the resolution of the x-ray pulse duration are hampered by the inability to precisely synchronize an external laser to the accelerator. At the Sub-Picosecond Pulse Source at the Stanford Linear-Accelerator Center we solved this problem by measuring the arrival time of each high energy electron bunch with electro-optic sampling. This measurement indirectly determined the arrival time of each x-ray pulse relative to an external pump laser pulse with a time resolution of better than 60 fs rms.     

Interference effects in the theory of multiphoton laser-simulated bremsstrahlung for electron wave packets that are broad in their momentum representation

The interference peculiarities of absorption and emission of external laser field quanta by a spatially narrow electron wave packet during its scattering at a potential center are considered. The angular and energy distributions for an electron due to scattering in a laser field are obtained and analyzed within the framework of the perturbation theory based on interaction with the potential center. A new mechanism of effective heating of plasma produced in a cluster under the effect of intense external laser field is found. Drastic changes in angular distribution due to the interference of incident and scattered parts of an electron wave packet are revealed.     

Multiphoton stimulated bremsstrahlung for broad (in the momentum representation) electron wave packets in an ultrashort laser pulse field

We consider features of absorption and emission of external laser field quanta by a broad (in the momentum representation) electron wave packet during its scattering from a potential center. Various scattering modes for the electron wave packet in a high-intensity laser field are analyzed using perturbation theory of potential energy. It is found that the absorption of laser field energy by an electron is substantially more effective as compared to the case of a plane wave. The important role of a number of interference effects associated with the large width of the initial electron momentum distribution is demonstrated.     

Experimental observation of revival structures in picosecond laser-induced alignment of I2

We report the experimental observation of revival structures in the alignment of a ground-state rotational wave packet following nonresonant excitation of I2 molecules by an intense picosecond laser pulse. The revivals appear at characteristic time delays following the excitation by the pump laser pulse, and show a significant narrowing of the angular distribution during a few picoseconds. The interaction with the pump laser also leads to a steady-state alignment of the molecule, due to rotational pumping.     

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.     

Demonstration of turnstiles as a chaotic ionization mechanism in Rydberg atoms

We present an experimental and theoretical study of the chaotic ionization of quasi-one-dimensional potassium Rydberg wave packets via a classical phase-space turnstile mechanism. Turnstiles form a general transport mechanism for numerous chaotic systems, and this study explicitly illuminates their relevance to atomic ionization. We create time-dependent Rydberg wave packets, subject them to alternating applied electric-field pulses, and measure the electron survival probability. Ionization depends not only on the initial electron energy, but also on the classical phase-space position of the electron with respect to the turnstile--that part of the electron packet inside the turnstile ionizes after the applied ionization sequence, while that part outside the turnstile does not. The survival data thus encode information on the shape and location of the turnstile, in good agreement with theoretical predictions.     

Coherent electron scattering captured by an attosecond quantum stroboscope

We demonstrate a quantum stroboscope based on a sequence of identical attosecond pulses that are used to release electrons into a strong infrared (IR) laser field exactly once per laser cycle. The resulting electron momentum distributions are recorded as a function of time delay between the IR laser and the attosecond pulse train using a velocity map imaging spectrometer. Because our train of attosecond pulses creates a train of identical electron wave packets, a single ionization event can be studied stroboscopically. This technique has enabled us to image the coherent electron scattering that takes place when the IR field is sufficiently strong to reverse the initial direction of the electron motion causing it to rescatter from its parent ion.