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.     

Manifestation of attosecond XUV fields temporal structures in attosecond streaking spectrogram

The features of an attosecond extreme ultraviolet (XUV) field are encoded in the attosecond XUV spectrogram. We investigate the effect of the temporal structures of attosecond XUV fields on the attosecond streaking spectrogram. Factors such as the number of attosecond XUV pulses and the temporal chirp of attosecond XUV pulses are considered. Results indicate that unlike the attosecond streaking spectrogram for an attosecond XUV field with two pulses of a half-cycle separation of streaking field, the spectrogram for the attosecond XUV field with three pulses demonstrates fine spectral fringes in separated traces.     

Intensity dependence of laser-assisted attosecond photoionization spectra

We study experimentally the influence of the intensity of the infrared (IR) probe field on attosecond pulse train (APT) phase measurements performed with the RABITT method (Reconstruction of Attosecond Beating by Interference in Two-Photon Transitions). We find that if a strong IR field is applied, the attosecond pulses will appear to have lower-than-actual chirp rates. We also observe the onset of the streaking regime in the breakdown of the weak-field RABITT conditions. We perform a Fourier-analysis of harmonic and sideband continuum states and show that the mutual phase relation of the harmonics can be extracted from higher Fourier components.     

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.     

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.     

Attosecond streaking of correlated two-electron transitions in helium

We present fully ab initio simulations of attosecond streaking for ionization of helium accompanied by shakeup of the second electron. This process represents a prototypical case for strongly correlated electron dynamics on the attosecond time scale. We show that streaking spectroscopy can provide detailed information on the Eisenbud-Wigner-Smith time delay as well as on the infrared-field dressing of both bound and continuum states. We find a novel contribution to the streaking delay that stems from the interplay of electron-electron and infrared-field interactions in the exit channel. We quantify all the contributions with attosecond precision and provide a benchmark for future experiments.     

Electron vortices in photoionization by a pair of elliptically polarized attosecond pulses

The photoionization by two elliptically polarized, time delayed attosecond pulses is investigated to display a momentum distribution having the helical vortex or ring structures. The results are obtained by the strong field approximation method and analyzed by the pulse decomposition. The ellipticities and time delay of the two attosecond pulses are found to determine the rotational symmetry and the number of vortex arms. For observing these vortex patterns, the energy bandwidth and temporal duration of the attosecond pulses are ideal.     

Delay in atomic photoionization

We analyze the time delay between emission of photoelectrons from the outer valence ns and np subshells in noble gas atoms following absorption of an attosecond extreme ultraviolet pulse. Various processes such as elastic scattering of the photoelectron on the parent ion and many-electron correlation affect the apparent "time zero" when the photoelectron leaves the atom. This qualitatively explains the time delay between photoemission from the 2s and 2p subshells of Ne as determined experimentally by attosecond streaking [Science 328, 1658 (2010)]. However, with our extensive numerical modeling, we were only able to account for less than half of the measured time delay of 21 ± 5 as. We argue that the extreme ultraviolet pulse alone cannot produce such a large time delay and it is the streaking IR field that is most likely responsible for this effect.     

Time resolved Fano resonances

Recent advances in the generation of sub-fs extreme ultraviolet pulses and attosecond metrology have opened up the possibility to trace the time evolution of electronic wave packets inside atoms in pump-probe experiments. We investigate the feasibility of observing the buildup of a Fano resonance in the time domain by attosecond streaking techniques. A time-resolved resonance is initialized by a sub-fs extreme ultraviolet-pump pulse in the presence of a synchronized phase-controlled probe laser pulse. The time evolution of the coherent superposition of resonant state and continuum is mapped onto a modulation of the electron spectrum as a function of the time delay between pump and probe pulse. (super-)Coster-Kronig transitions with lifetimes of approximately 400 asec( are identified as prime candidates.     

Phase-dependent electron-ion recombination in a microwave field

Using picosecond laser photoionization of Li in a microwave field we have observed phase-dependent reccombination of the photoelectrons with their parent Li+ ions. Recombination occurs at phases of the microwave field such that energy is removed from the photoelectron in the first microwave cycle after excitation, and there are two maxima in the recombination in each microwave cycle. These observations are consistent with observations made using an attosecond pulse train phase locked to an infrared pulse and with the "simpleman's" model, modified to account for the fact that the photoelectrons are produced in a Coulomb potential.     

Control mechanism of atomic ionization and high-order harmonic generation assisted by attosecond pulses

Attosecond pulses combined with infrared laser constitute a powerful tool for controlling atomic photoionization and high-order harmonic generation (HHG). We apply the intense-field many-body S-matrix theory to solve such two-pulse excitation problems. The theory can give a clear explanation for the oscillation of ionization probability as a function of time delay between infrared field and attosecond pulses with central frequency lying below ionization threshold at moderate infrared intensities. The HHG assisted by such attosecond pulses is also interpreted. In addition to a known dramatic enhancement of HHG, a harmonic emission from rapid oscillation of bound-state population caused by the counter-rotating wave is presented.     

The accurate FROG characterization of attosecond pulses from streaking measurements

We describe a new attosecond FROG algorithm optimized for the characterization of sub-100 as pulses from streaked electron spectra. We make improvements upon the treatment of the attosecond streaking spectrogram, and show that these are necessary in order to accurately characterize shorter pulses with ever larger bandwidths. We investigate the effects of the approximations that must be made in order to apply the generalized projections scheme. PACS  31.15.xg; 32.90.+a; 33.60.+q     

Attosecond streaking in the low-energy region as a probe of rescattering

The dynamics of low-energy photoelectrons (PEs) ionized by a single attosecond pulse in the presence of an intense infrared (IR) laser field is investigated. Whereas attosecond streaking usually involves momentum shifts of high-energy PEs, when PEs have low initial kinetic energies, the IR field can control the continuum-electron dynamics by inducing PE scattering from the residual ion. A semiclassical model is used to show that particular PE trajectories in the continuum involving electron-ion scattering explain the interference patterns exhibited in the low-energy PE spectrum. We confirm the effects of the trajectories by means of a full quantum simulation.     

基于瞬态光栅频率分辨光学开关装置的阿秒延时相位控制

操控多路激光脉冲之间的相对延时（相对相位）对于亚周期相干合成技术意义重大.当周期量级脉冲之间的相对延时接近数十飞秒时,常见的飞秒脉冲测量手段已无法满足脉冲之间相对相位的精确调控需求.本文基于瞬态光栅频率分辨光学开关装置,精确反演出脉冲之间的相对相位.此方案不仅有助于直接产生亚周期（亚飞秒）脉冲,还可应用于时间隐身学和二维相干光谱学等相关领域.     

Probing single-photon ionization on the attosecond time scale

We study photoionization of argon atoms excited by attosecond pulses using an interferometric measurement technique. We measure the difference in time delays between electrons emitted from the 3s(2) and from the 3p(6) shell, at different excitation energies ranging from 32 to 42 eV. The determination of photoemission time delays requires taking into account the measurement process, involving the interaction with a probing infrared field. This contribution can be estimated using a universal formula and is found to account for a substantial fraction of the measured delay.     

Attosecond angle-resolved photoelectron spectroscopy

We report experiments on the characterization of a train of attosecond pulses obtained by high-harmonic generation, using mixed-color (XUV+IR) atomic two-photon ionization and electron detection on a velocity map imaging detector. We demonstrate that the relative phase of the harmonics is encoded both in the photoelectron yield and the angular distribution as a function of XUV-IR time delay, thus making the technique suitable for the detection of single attosecond pulses. The timing of the attosecond pulse with respect to the field oscillation of the driving laser critically depends on the target gas used to generate the harmonics.     

Attosecond pulse extreme-ultraviolet photoionization in a two-color laser field

Attosecond-pulse extreme-ultraviolet (XUV) photoionization in a two-color laser field is investigated. Attosecond pulse trains with different numbers of pulses are examined, and their strong dependence on photoelectronic spectra is found. Single-color driving-laser-field-assisted attosecond XUV photoionization cannot determine the number of attosecond pulses from the photoelectronic energy spectrum that are detected orthogonally to the beam direction and the electric field vector of the linearly polarized laser field. A two-color-field-assisted XUV photoionization scheme is proposed for directly determining the number of attosecond pulses from a spectrum detected orthogonally.     

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.     

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.     

How accurate is the attosecond streak camera?

An attosecond streak camera holds the promise of time resolving the dynamics of photoionization with a few-attosecond accuracy. But can the attosecond measurement be disentangled from the process it measures? We address this question by deriving simple closed-form analytical expressions for the measurement-related apparent time delays in photoionization, associated with the application of the attosecond streak camera and/or resolution of attosecond beating by interference of two-photon transitions techniques. Our analytical results are accurate on about the 1 asec level and show that both intrinsic and measurement-induced delays depend on the same scattering phase and are, therefore, not independent. We also suggest a procedure for extracting intrinsic time delays from the measurement and a possible resolution of the controversy caused by the experiments of Schultze et al. [Science 328, 1658 (2010)].