Monitoring and controlling the electron dynamics in helium with isolated attosecond pulses

Helium atoms in the presence of extreme ultraviolet light pulses can lose electrons through direct photoionization or through two-electron excitation followed by autoionization. Here we demonstrate that, by combining attosecond extreme ultraviolet pulses with near infrared femtosecond lasers, electron dynamics in helium autoionization can be not only monitored but also controlled. Furthermore, the interference between the two ionization channels was modified by the intense near infrared laser pulse. To the best of our knowledge, this is the first time that double excitation and autoionization were studied experimentally by using isolated attosecond pulses.     

Ionization of atoms by chirped attosecond pulses

We investigate the ionization dynamics of atoms by chirped attosecond pulses using the strong field approximation method. The pulse parameters are carefully chosen in the regime where the strong field approximation method is valid. We analyse the effects of the chirp of attosecond pulses on the energy distributions and the corresponding left-right asymmetry of the ionized electrons. For a single chirped attosecond pulse, the ionized electrons can be redistributed and the left-right asymmetry shows oscillations because of the introduction of the chirp. For time-delayed double attosecond pulses at different intensities with the weaker one chirped, exchanging the order of the two pulses shows a relative shift of the energy spectra, which can be explained by the different effective time delays of different frequency components because of the chirp.     

Generation of XUV attosecond pulses in the process of atomic ionization by few-cycle laser radiation

Ionization of a model two-electron atom in the presence of a strong field of ultrashort laser pulses is investigated using the numerical integration of the nonstationary Schrödinger equation, which describes the dynamics of a quantum system in the presence of an electromagnetic wave. The features of two-electron ionization in the presence of one-and two-cycle pulses are analyzed. The suppression of double ionization in the presence of ultrashort laser pulses related to a finite-time interelectron energy exchange upon the laser action is demonstrated. The features of the generation of high-order harmonics and single XUV attosecond pulses are studied for the atomic ionization by few-cycle laser pulses. The parameters of the laser pulse are optimized for the effective generation of a single XUV attosecond pulse.     

脉冲啁啾对于阿秒脉冲的影响

采用单电子近似和软核势模型, 通过数值求解一维含时薛定谔方程, 理论研究了当脉冲分别带有正、负啁啾的情况下所产生的阿秒脉冲.分析了不同脉冲啁啾特性对阿秒脉冲的强度和宽度的影响. 研究结果表明, 无论是正啁啾还是负啁啾, 随着啁啾量的增加, 都将使激光脉冲由产生单个阿秒脉冲趋向于产生阿秒脉冲链. 正啁啾和负啁啾对于阿秒脉冲宽度的影响是不同的, 负啁啾对于阿秒脉冲宽度影响很小, 适当的负啁啾有利于缩小阿秒脉冲的宽度; 而正啁啾脉冲产生的阿秒脉冲较无啁啾时展宽, 且随着啁啾量的增加, 其阿秒脉冲宽度迅速增大.     

Modification of laser-induced state in atomic attosecond transient absorption by the XUV pulse pair

Attosecond transient absorption(ATA) has been developed as an all-optical technique for probing electron dynamics in matter.Here we present a scheme that can modify the laserinduced state and the corresponding ATA spectrum via excitation by a pair of XUV attosecond pulses and by a time-delayed mid-infrared(MIR) laser probe.Different from the scheme of the electronic excitation by a single XUV attosecond pulse,the application of a pair of XUV pulses provides extra degrees of freedom,such as the t...     

周期量级激光脉冲的Thomson散射

用经典辐射理论对线偏振周期量级激光脉冲的线性Thomson散射进行分析，从理论上得到它可产生亚阿秒脉冲的结论. 计算显示，在电子相对论因子为50、激光脉冲中心波长为1μm、归一化光场强度为0.01的情况下，用包含1.5个光周期的激光脉冲，可获得0.2as(半高全宽)的散射脉冲输出. 还对光场载波包络初相φ_ce和电子进入光场的初相φ_in对散射脉冲的影响作了分析讨论，结果表明，在适当的φ_ce和φ_in条件下，能实现单个阿秒脉冲输出，并可对脉冲宽度和频率进行调谐. 关键词： 线性Thomson散射 周期量级激光脉冲 载波包络初相 阿秒脉冲     

Chirped attosecond photoelectron spectroscopy

We study analytically the photoionization of a coherent superposition of electronic states and show that chirped pulses can measure attosecond time scale electron dynamics just as effectively as transform-limited attosecond pulses of the same bandwidth. The chirped pulse with a frequency-dependent phase creates the interfering photoelectron amplitudes that measure the electron dynamics. We show that at a given pump-probe time delay the differential asymmetry oscillates as a function of photoelectron energy. Our results suggest that the important parameter for attosecond science is not the pulse duration, but the bandwidth of phased radiation.     

啁啾激光与半周期脉冲形成的组合场驱动原子产生单个阿秒脉冲

提出了由波长为800 nm、脉冲宽度为5 fs的啁啾激光与半周期脉冲形成组合场,并利用这种组合场驱动一维模型氦原子获得单个阿秒脉冲. 通过数值求解一维氦原子的含时薛定谔方程,发现氦原子在组合场驱动下高次谐波谱的截止位置可以扩展到I_p+21.6U_p. 对第二平台区域不同范围内高次谐波的叠加都能得到单个阿秒脉冲,最短可达37 as,特别是对平台区域的前端进行叠加不仅能够得到较短的单个阿秒脉冲,而且与截止位置附近高次谐波构造的阿秒脉冲相比,强度提高了3个数量级. 关键词： 啁啾激光场 半周期脉冲 高次谐波 阿秒脉冲     

Selective excitation,coherent control,and attosecond spectrochronography of electron subshells in atomic systems

Optical field waveforms with an ultrabroad spectrum and a tailored phase are shown to enable selective excitation, coherent control, and attosecond spectrochronography of electron subshells in many-electron atomic systems. Analysis of the evolution of the density matrix of electron subshells in an atomic system driven by an ultrashort light pulse shows that the interference of different quantum pathways of electron dynamics plays a key role in the buildup of the nonlinear-optical response of such a system. Our analysis suggests a method whereby the attosecond dynamics of individual electron subshells in atoms can be coherently controlled with ultrashort laser pulses.     

强激光等离子体相互作用驱动高次谐波与阿秒辐射研究进展

对超快过程的探测和控制决定了人类在微观层面认识和改造物质世界的能力.阿秒光源可完成对组成物质的电子运动及其关联效应进行超高时空分辨的探测和操控,为人类认识微观世界提供了全新手段,被认为是激光科学史上最重要的里程碑之一.世界主要科技强国都将阿秒科学列为未来10年重要的科技发展方向.利用强激光与物质相互作用产生高次谐波是突破飞秒极限实现高亮度阿秒脉冲辐射的重要方案之一,成为了近年来激光等离子体领域的研究热点.本文聚焦强激光与等离子体相互作用中的高次谐波和阿秒脉冲辐射,主要介绍其产生机制、研究进展和前沿应用,并对未来的发展趋势和创新突破进行展望.     

Use of electron correlation to make attosecond measurements without attosecond pulses

We describe how correlations between electrons can be used to trace the dynamics of correlated two-electron ionization with attosecond precision, without using attosecond pulses. The approach is illustrated using the example of Auger or Coster-Kronig decay triggered by photoionization with an extreme ultraviolet pulse. It requires correlated measurements of angle-resolved energy spectra of both the photo- and Auger electrons in the presence of a laser pulse. To reconstruct the dynamics, we use not only classical time and energy correlation, but also entanglement between the two electrons.     

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.     

Excitation dynamics of Rydberg states in C<Subscript>60</Subscript>

The electron and nuclear dynamics of C₆₀ fullerenes irradiated with femtosecond laser pulses are investigated with photoelectron and photoion spectroscopy. The focus of this work is the detailed exploration of the population mechanism of Rydberg levels within the excitation process of neutral C₆₀. The effect of excitation wavelength, intensity, chirp, and polarization on the kinetic energy distribution of photoelectrons in single-pulse experiments gives first insight into the underlying processes. In combination with time-resolved two-color pump-probe spectroscopy depending on either pump, or probe pulse intensity, a more complete picture of the interaction can be drawn. The results point towards a very interesting but nevertheless complex behavior including four steps: (i) non-adiabatic multielectron excitation of the HOMO (h_u) → LUMO+1 (t_1g) transition; (ii) thermalization within the hot electron cloud on a time scale below 100 fs, followed by a coupling of energy to vibrational modes of the molecule via doorway state(s); (iii) population of electronically excited Rydberg states by multiphoton absorption, and (iv) single photon ionization from the excited Rydberg states. This excitation process results in a characteristic sequence of photoelectron lines in the photoemission spectra. The comparison of the experimental results with recent theoretical work gives convincing evidence that non-adiabatic multielectron dynamics (NMED) plays a key role for the understanding of the response of C₆₀ to short-pulse laser radiation.     

Peculiarities of the ionization of many-electron systems and generation of attosecond pulses in ultrashort laser fields

The ionization of a model two-electron atom in the field of a strong ultrashort laser pulse is studied by numerical integration of the nonstationary Schrödinger equation describing the dynamics of a quantum system in the field of an electromagnetic wave. Pecularities of the two-electron ionization are analyzed for pulses whose duration amounts to one to two periods of oscillation of the electric field of the wave at different frequencies of the incident radiation. For extremely short pulses, the double ionization is found to be suppressed. This effect is caused by the finiteness of the interelectron energy exchange time during the laser action. Peculiarities of the generation of high-order harmonics and single XUV attosecond pulses upon ionization of atoms by laser pulses, whose duration is within one to two optical cycles, are investigated.     

Amplitude and phase reconstruction of electron wave packets for probing ultrafast photoionization dynamics

Ultrafast atomic processes, such as excitation and ionization occurring on the femtosecond or shorter time scale, were explored by employing attosecond high-harmonic pulses. With the absorption of a suitable high-harmonic photon a He atom was ionized, or resonantly excited with further ionization by absorbing a number of infrared photons. The electron wave packets liberated by the two processes generated an interference containing the information on ultrafast atomic dynamics. The attosecond electron wave packet, including the phase, from the ground state was reconstructed first and, subsequently, that from the 1s3p state was retrieved by applying the holographic technique to the photoelectron spectra comprising the interference between the two ionization paths. The reconstructed electron wave packet revealed details of the ultrafast photoionization dynamics, such as the instantaneous two-photon ionization rate.     

Attosecond resolved charging of ions in a rare-gas cluster

A scheme to probe dissipative multielectron motion in time is introduced. In this context attosecond probing enables one to obtain information which is lost at later times and cannot be retrieved by conventional methods in the energy domain due to the incoherent nature of the dynamics. As a specific example we will trace the transient charging of ions in a rare-gas cluster during a strong femtosecond vacuum-ultraviolet pulse by means of delayed attosecond pulses.     

Coherent Control of High Harmonic Generation Driven by Metal Nanotip Photoemission

Steering ultrafast electron dynamics with well-controlled laser fields is very important for generation of intense supercontinuum radiation. It can be achieved through coherent control of the symmetry of the interaction between strong-field laser fields and a metal nanotip. We employ a scheme of two-color laser pulses combined with a weak static field to realize the control of a single quantum path to generate high harmonic generation from a single solid-state nanoemitter. Moreover, a smooth and ultrabroad supercontinuum in the extreme ultraviolet region is obtained, which can produce a single attosecond pulse. Our findings are beneficial for efficient generation of isolated sub-100 as XUV pulses from solid-state sources.     

采用双脉冲驱动产生高次谐波阿秒脉冲

提出了采用双脉冲机理来产生阿秒脉冲的方法.研究发现采用双脉冲不仅可以产生单个的阿秒脉冲，从而突破目前产生阿秒脉冲的驱动源（几个飞秒的超短激光脉冲）的能量限制，而且在相同的峰值强度下，双脉冲能够产生强度更高的阿秒脉冲. 关键词： 阿秒脉冲 双脉冲机理 高次谐波     

高次谐波辐射发射特性研究

报告由不同脉冲宽度(半高宽,FWHM)和不同载波-包络相位(CEP,Φ)的激光产生的高次谐波辐射能量输出时间特性即发射特性的研究结果. 计算表明,由宽度为几个周期的激光产生的高次谐波辐射的截止能量明显低于由无限长脉冲宽度激光产生的截止能量ω_max=3.17U_p+I_p(其中ω_max为光子角频率,U_p和I_p分别为激光有质动力势和原子的电离能). 例如,由两周期(FWHM),Φ＝15°的激光产生的高次谐波辐射的截止能量为ω_max=2.90U_p+I_p,此时发射特性单脉冲(即分布单脉冲)具有最大的能量带宽0.86U_p. 脉冲中心位置的载波相位和时间宽度分别为0.94rad(弧度)和1.29rad. 而该激光脉冲在Φ＝-75°时能产生截止能量为ω_max=2.70U_p+I_p,最大能量带宽为0.70U_p的双分布脉冲,其中心位置分别为-0.58rad和2.43rad,宽度分别为1.22rad和1.33rad. 随着激光脉冲宽度的增加,分布单脉冲的能量带宽比时间宽度下降得更快. 对于一定宽度的激光脉冲,所产生的分布单脉冲的能量带宽和时间宽度的CEP依赖性显示出180°的周期结构. 利用这个有趣的特点,在实验上可以通过调节CEP来选择分布脉冲的能量参数,也可用来定位和控制阿秒脉冲的时间参数. 理论分析指出,只要选择合适的阿秒X射线能量带宽,CEP不稳定性对于光电子谱和测量结果的影响将大为降低,甚至在最大程度上消除这种影响. 这些研究结果不仅有助于在物理上深入了解高次谐波辐射的动力学过程,而且对于进一步在实验上优化和选择阿秒单脉冲和双脉冲具有重要的参考和指导意义. 关键词： 高次谐波产生 鞍点方法 谐波发射特性 分布脉冲     

不同激光等离子体条件下的阿秒光脉冲产生

通过一维粒子模拟研究了利用相对论少周期强激光与固体密度等离子体表面相互作用实现单个孤立阿秒光脉冲产生的参数条件。主要研究描述相互作用的多维参数,如激光强度、入射角和等离子体标尺长度等,对相对论高次谐波能量转换效率和孤立阿秒光脉冲分离度的影响。研究发现,虽然激光等离子体参数对阿秒光脉冲产生的影响是复杂的,但是存在着能够实现大能量孤立阿秒光脉冲的最佳等离子体标尺长度和最佳入射角。当其他相互作用条件确定时,使用中等强度的相对论强激光可以在较宽的参数范围内实现孤立的阿秒光脉冲。大角度入射时,孤立阿秒光脉冲的分离度较高,能够实现孤立阿秒光脉冲的相互作用参数范围也较宽。