Attosecond spectroscopy for filming the ultrafast movies of atoms,molecules and solids

Three decades ago, a highly nonlinear nonpertubative phenomenon, now well-known as the high harmonic generation (HHG), was discovered when intense laser irradiates gaseous atoms. As the HHG produces broadband coherent radiation, it becomes the most promising source to obtain attosecond pulses. The door to the attosecond science was opened ever since. In this review, we will revisit the incredible adventure to the attoworld. Firstly, the progress of attosecond pulse generation is outlined. Then, we introduce the efforts on imaging the structures or filming the ultrafast dynamics of nuclei and electrons with unprecedented attosecond temporal and Angstrom spatial resolutions, utilizing the obtained attosecond pulses as well as the high harmonic spectrum itself.     

Characterization of attosecond XUV pulses from photoelectron spectra of atoms

A method to characterize attosecond extreme ultra violet (XUV) pulses from photoelectron spectra of atoms is presented. A pump pulse prepares a coherent superposition of two atomic bound states, from which photoionization takes place after variable time delays by the attosecond XUV pulse. Information on the spectral phase of the attosecond XUV pulse is extracted from the analysis of photoelectron spectra as a function of photoelectron energy and time delay. Together with information on the spectral intensity obtained from a separate optical measurement, a temporal shape of the attosecond XUV pulse can be precisely reconstructed. After the theoretical formulation of the problem, we present numerical examples for H atom and show that, depending on the choice of energy separation of two bound states, a different accuracy is reached to characterize attosecond XUV pulses.     

Attosecond temporal gating with elliptically polarized light

Temporal gating allows high accuracy time-resolved measurements of a broad range of ultrafast processes. By manipulating the interaction between an atom and an intense laser field, we extend gating into the nonlinear medium in which attosecond optical and electron pulses are generated. Our gate is an amplitude gate induced by ellipticity of the fundamental pulse. The gate modulates the spectrum of the high harmonic emission and we use the measured modulation to characterize the sub-laser-cycle dynamics of the recollision electron wave packet.     

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。     

Unraveling the solid-liquid-vapor phase transition dynamics at the atomic level with ultrafast x-ray absorption near-edge spectroscopy

X-ray absorption near-edge spectroscopy (XANES) is a powerful probe of electronic and atomic structures in various media, ranging from molecules to condensed matter. We show how ultrafast time resolution opens new possibilities to investigate highly nonequilibrium states of matter including phase transitions. Based on a tabletop laser-plasma ultrafast x-ray source, we have performed a time-resolved (～3 ps) XANES experiment that reveals the evolution of an aluminum foil at the atomic level, when undergoing ultrafast laser heating and ablation. X-ray absorption spectra highlight an ultrafast transition from the crystalline solid to the disordered liquid followed by a progressive transition of the delocalized valence electronic structure (metal) down to localized atomic orbitals (nonmetal-vapor), as the average distance between atoms increases.     

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.     

Atomic and molecular dynamics triggered by ultrashort light pulses on the atto- to picosecond time scale

Time-resolved investigations of ultrafast electronic and molecular dynamics were not possible until recently. The typical time scale of these processes is in the picosecond to attosecond realm. The tremendous technological progress in recent years made it possible to generate ultrashort pulses, which can be used to trigger, to watch, and to control atomic and molecular motion. This tutorial focuses on experimental and theoretical advances which are used to study the dynamics of electrons and molecules in the presence of ultrashort pulses. In the first part, the rotational dynamics of molecules, which happens on picosecond and femtosecond time scales, is reviewed. Well-aligned molecules are particularly suitable for angle-dependent investigations like x-ray diffraction or strong-field ionization experiments. In the second part, the ionization dynamics of atoms is studied. The characteristic time scale lies, here, in the attosecond to few-femtosecond regime. Although a one-particle picture has been successfully applied to many processes, many-body effects do constantly occur. After a broad overview of the main mechanisms and the most common tools in attosecond physics, examples of many-body dynamics in the attosecond world (e.g., in high-harmonic generation and attosecond transient absorption spectroscopy) are discussed.     

Frequency-resolved optical gating of isolated attosecond pulses in the extreme ultraviolet

The pulse shape and phase of isolated attosecond extreme ultraviolet (XUV) pulses with a duration of 860 asec have been determined simultaneously by using frequency-resolved optical gating based on two-photon above-threshold ionization with 28-eV photons in He. From the detailed characterization, we succeeded in shaping isolated XUV pulses on an attosecond time scale by precise dispersion control with Ar gas density or by changing the driving pulse width. These results offer a novel way to excite and observe an electron motion in atoms and molecules.     

Direct XUV probing of attosecond electron recollision

We demonstrate that the recolliding electron wave packet, fundamental to many strong field phenomena, can be directly imaged with sub-A spatial and attosecond temporal resolution using attosecond extreme ultraviolet (XUV) pulses. When the recolliding electron revisits the parent ion, it can absorb an XUV photon yielding high energy electron and thereby providing a measurement of the electron energy at the moment of recollision. The full temporal evolution of the recollision wave packet can be reconstructed by measuring the photoelectron spectra for different time delays between the driving laser and the attosecond XUV probe. The strength of the photoelectron signal can be used to characterize the spatial distribution of the electron density in the longitudinal direction. Elliptical polarization can be used to characterize the electron probability in transversal direction.     

利用阿秒激光追踪和控制原子分子内部电子的运动(英文)

随着强激光技术的快速发展,在物质与激光相互作用下,实验上发现了很多新奇的物理现象。这些现象成功地被各种理论模型和数值模拟所解释和证明。一种很重要的现象就是所谓的高次谐波产生:在原子和分子与强激光相互作用时,能够放出能量为基频光子能量几倍到几百倍的大能量光子。在实验上,人们已经可以通过合成截止频率附近的几个谐波来产生脉冲长度在阿秒量级的激光脉冲(1阿秒=10~(-18)s)。阿秒脉冲的获得开启了超快科学一个全新的领域:人们可以在电子运动的自然时间尺度上去探测和操控原子分子内部电子的运动,这是继飞秒科学后人们操控微观世界物质运动的又一大飞跃。在本文中,我们就最近几年我们在理论上所开展的阿秒物理做一个简单的综述,重点强调利用阿秒光去控制电子的电离动力学以及探测分子内部电子运动。     

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...     

利用阿秒激光追踪和控制原子分子内部电子的运动

随着强激光技术的快速发展, 在物质与激光相互作用下,实验上发现了很多新奇的物理现象。这些现象成功地被各种理论模型和数值模拟所解释和证明。一种很重要的现象就是所谓的高次谐波产生：在原子和分子与强激光相互作用时, 能够放出能量为基频光子能量几倍到几百倍的大能量光子。在实验上, 人们已经可以通过合成截止频率附近的几个谐波来产生脉冲长度在阿秒量级的激光脉冲（1阿秒=10-18秒）。阿秒脉冲的获得开启了超快科学一个全新的领域：人们可以在电子运动的自然时间尺度上去探测和操控原子分子内部电子的运动,这是继飞秒科学后人们操控微观世界物质运动的又一大飞跃。在本文中,我们就最近几年我们在理论上所开展的阿秒物理做一个简单的综述,重点强调利用阿秒光去控制电子的电离动力学以及探测分子内部电子运动.     

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.     

红外激光场中共振结构原子对极紫外光脉冲的压缩效应

通过数值求解一维原子的含时薛定谔方程, 研究了具有共振结构的原子在双色场(红外激光(IR)+极紫外光(XUV)) 驱动下发射高次谐波的特征. 研究结果表明, 具有共振结构的原子所发射的高次谐波与无共振结构原子(简称为一般原子)发射的高次谐波有明显不同, 共振结构的原子除了在某一能量附近(原子的共振能量+电离能)高次谐波的强度有很大提高外, 它还对XUV光的响应较一般原子表现得更为敏感, 即使XUV光的强度较弱, 也能够明显提高XUV光脉冲中心频率附近的谐波强度, 更重要的是通过调节双色场的时间延迟, 能使输入的XUV光的脉宽得到明显的压缩, 通过时间-频率分析给出了发生这种现象的原因. 由此提出了通过滤波-连续反馈的方式可使XUV光的脉冲从200 as压缩至120 as左右.     

Subfemtosecond K-shell excitation with a few-cycle infrared laser field

Subfemtosecond bursts of extreme ultraviolet radiation, facilitated by a process known as high-order harmonic generation, are a key ingredient for attosecond metrology, providing a tool to precisely initiate and probe ultrafast dynamics in the microcosms of atoms, molecules, and solids. These ultrashort pulses are always, and as a by-product of the way they are generated, accompanied by laser-induced recollisions of electrons with their parent ions. By using a few-cycle infrared (λ(0)=2.1 μm) driving laser, we were able to directly excite high-energy (～870 eV) inner-shell electrons through laser-induced electron recollision, opening the door to time-resolved studies of core-level and concomitant multielectron dynamics.     

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.     

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.     

超快激光的新前沿—阿秒科学

超短脉冲激光正在进行着从飞秒（1fs=10^-15s)向阿秒（1attosecond=10^-18s)的跨越,这一跨越对于激光原理和激光应用来说都有很重要的意义,文章通过阿秒脉冲与飞秒脉冲比较来介绍超快激光的新前沿－阿秒科学,包括阿秒科学的诞生,现状以及由于阿秒脉冲的产生而出现的阿秒科学的概况 。     

Attosecond physics with neutrons and electrons: Ultrafast entanglement and decoherence phenomena involving protons in condensed matter and molecules

Nuclei and electrons in condensed matter and/or molecules are usually entangled, due to the prevailing electromagnetic interactions. Usually, the “environment” of a microscopic scattering system (e.g., a proton) causes an ultrafast decoherence, thus making atomic and/or nuclear entanglement effects not directly accessible to experiments. However, neutron Compton scattering (NCS) and electron Compton scattering represent ultrafast techniques operating in the sub-femtosecond timescale, thus opening a way for investigation of such dehoherence and short-lived entanglement phenomena of atoms in molecules and condensed matter. The experimental context of NCS and a new striking scattering effect from protons (H-atoms) in several condensed systems and molecules are described. In short, one observes an “anomalous” decrease of scattering intensity from protons, which seem to become partially “invisible” to the neutrons. The experiments apply large energy (several electronvolts) and momentum (10–200 Å^?1 transfers, and the collisional (or scattering) time between the neutron and a struck proton is only 100–1000 attoseconds long. Similar results are also obtained with electron-atom Compton scattering at large momentum transfers. As an example, we present new NCS experimental results from a single crystal, which also provide new physical insights into the attosecond quantum dynamics of protons in molecules and condensed matter. Theoretical discussions and models are presented which show that the effect under consideration is caused by the non-unitary time evolution (due to decoherence) of open quantum systems during the ultrashort, but finite, time-window of the neutron-proton scattering process. The conceptual connection with the well known Quantum Zeno Effect is pointed out. The experimental results, together with their qualitative interpretation “from first principles,” show that epithermal neutrons being available at spallation sources, and electron spectrometers providing large momentum transfers, may represent novel tools for investigation of thus far unknown physical and chemical attosecond phenomena.