High-order harmonic generation by few-cycle 800 nm laser pulses in neon gas in the presence of a strong terahertz (THz) field is investigated numerically with propagation effects taken into account. Our calculations show that the combination of THz fields with up to 12 fs laser pulses can be an effective gating technique to generate single attosecond pulses. We show that in the presence of the strong THz field only a single attosecond burst can be phase matched, whereas radiation emitted during other half-cycles disappears during propagation. The cutoff is extended and a wide supercontinuum appears in the near-field spectra, extending the available spectral width for isolated attosecond pulse generation from 23 to 93 eV. We demonstrate that phase matching effects are responsible for the generation of isolated attosecond pulses, even in conditions when single atom response yields an attosecond pulse train.
We perform a joint measurement of terahertz waves and high-order harmonics generated from noble atoms driven by a fundamental laser pulse and its second harmonic. By correlating their dependence on the phase-delay of the two pulses, we determine the generation of THz waves in tens of attoseconds precision. Compared with simulations and models, we find that the laser-assisted soft-collision of the electron wave packet with the atomic core plays a key role. It is demonstrated that the rescattering process, being indispensable in HHG processes, dominant THz wave generation as well but in a more e…
High-order harmonic generation from atomic systems is considered in the crossed fields of a relativistically strong infrared laser and a weak attosecond-pulse train of soft x-rays. Due to one-photon ionization by the x-ray pulse, the ionized electron obtains a starting momentum that compensates the relativistic drift which is induced by the laser magnetic field, and allows the electron to efficiently emit harmonic radiation upon recombination with the atomic core in the relativistic regime. In this way, short pulses of coherent hard x-rays of up to 40 keV energy and 10 as duration can be broug…
We study laser-assisted photodetachment time delays by attosecond pulse trains from the closed-shell negative ions F- and Cl-. We investigate the separability of the delay into two contributions: (i) the Wigner-like delay associated with one-photon ionization by the attosecond pulse train and (ii) the delay associated with exchange of an additional laser photon in the presence of the potential of the remaining target. Based on the asymptotic form of the wave packet, the latter term is expected to be negligible because the ion is neutralized leading to a vanishing laser-ion interaction with inc…
The strong coupling between two autoionizing states in helium is studied theoretically with the pump-probe scheme. An isolated 100-as XUV pulse is used to excite helium near the 2s2p(1P) resonance state in the presence of an intense infrared (IR) laser. The laser field introduces strong coupling between 2s2p(1P) and 2p^2(1S) states. The IR also can ionize helium from both autoionizing states. By changing the time delay between the XUV and the IR pulses, we investigated the photoelectron spectra near the two resonances. The results are used to explain the recent experiment by Gilbertson et al. …
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 harm…
We study the temporal aspects of laser-assisted extreme ultraviolet (XUV) photoionization using attosecond pulses of harmonic radiation. The aim of this paper is to establish the general form of the phase of the relevant transition amplitudes and to make the connection with the time-delays that have been recently measured in experiments. We find that the overall phase contains two distinct types of contributions: one is expressed in terms of the phase-shifts of the photoelectron continuum wavefunction while the other is linked to continuum--continuum transitions induced by the infrared (IR) la…
We present the experimental and theoretical details of our recent published letter [Phys. Rev. Lett. 115. 123002] on synchronized high-harmonic and terahertz-wave spectroscopy (HATS) from nonadiabatically aligned nitrogen molecules in dual-color laser fields. Associating the alignment-angle dependent terahertz wave generation with the synchronizing high-harmonic signal, the angular differential photoionization cross section (PICS) for molecules can be reconstructed, and the minima of the angle on PICS show great convergence between the theoretical predictions and the experimental deduced resul…
We apply the convergent close-coupling (CCC) formalism to analyse the processes of laser assisted electron impact ionisation of He, and the attosecond time delay in the photodetachment of the H^{-} ion and the photoionisation of He. Such time dependent atomic collision processes are of considerable interest as experimental measurements on the relevant timescale (attoseconds 10^{-18} s) are now possible utilising ultrafast and intense laser pulses. These processes in particular are furthermore of interest as they are strongly influenced by many-electron correlations. In such cases their theoret…
We present a study of high-order-harmonic generation (HHG) assisted by extreme ultraviolet (XUV) attosecond pulses, which can lead to the excitation of inner-shell electrons and the generation of a second HHG plateau. With the treatment of a one-dimensional model of krypton, based on time-dependent configuration interaction singles (TDCIS) of an effective two-electron system, we show that the XUV-assisted HHG spectrum reveals the duration of the semiclassical electron trajectories. The results are interpreted by the strong-field approximation (SFA) and the importance of the hole transfer durin…
We study the generation of terahertz radiation from atoms and molecules driven by an ultrashort fundamental laser and its second harmonic field by solving time-dependent Schrödinger equation (TDSE). The comparisons between one-, two-, and three- dimensional TDSE numerical simulations show that initial ionized wave-packet and its subsequent acceleration in the laser field and rescattering with long-range Coulomb potential play key roles. We also present the dependence of the optimum phase delay and yield of terahertz radiation on the laser intensity, wavelength, duration, and the ratio of two-c…
Laser assisted photoemission by a chirped subfemtosecond extreme ultraviolet (XUV) pulse is considered within an exactly solvable quantum-mechanical model. Special emphasis is given to the energy dependence of photoexcitation cross-section. The streaked spectra are analyzed within the classical picture of initial time-momentum distribution r_ini(p,t) of photoelectrons mapped to the final energy scale. The actual time-momentum distribution in the absence of the probe laser field is shown to be a poor choice for r_ini, and a more adequate ansatz is suggested. The semiclassical theory offers a si…
A time-resolved spectroscopic protocol exploiting terahertz-assisted photoionization is proposed to reconstruct transient density matrix. Population and coherence elements are effectively mapped onto spectrally separated peaks in photoionization spectra. The beatings of coherence dynamics can be temporally resolved beyond the pulse duration, and the relative phase between involved states is directly readable from the oscillatory spectral distribution. As demonstrated by a photo-excited multilevel open quantum system, the method shows potential applications for sub-femtosecond time-resolved mea…
We present a theoretical study of atomic laser-assisted photoionization emission (LAPE). We consider an atom driven by a linearly polarized XUV laser in two different scenarios: i) a single attosecond pulse (in both the streaking and sideband regimes) and ii) an attosecond pulse train. The process takes place assisted by a linearly polarized infrared (IR) laser field. In all these cases the energy and angle-resolved photoelectron spectrum (PES) is determined by a leading contribution, related to the intracycle factor [Gramajo et al., J. Phys. B 51, 055603 (2018)], complemented by other ones, d…
Brunel harmonics appear in the optical response of an atom in process of laser-induced ionization, when the electron leaves the atom and is accelerated in the strong optical field. In contrast to recollision-based harmonics, the Brunel mechanism does not require the electron returning to the core. Here we show that in the presence of a strong ionizing terahertz (THz) field, even a weak driving field at the optical frequencies allow for generating Brunel harmonics effectively. The strong ionizing THz pump suppresses recollisions, making Brunel dominant in a wide spectral range. High-order Brune…
We study laser-assisted photoionization by attosecond pulses using a time-independent formalism based on diagrammatic many-body perturbation theory. Our aim is to provide an ab inito route to the "delays" for this above-threshold ionization process, which is essential for a quantitative understanding of attosecond metrology. We present correction curves for characterization schemes of attosecond pulses, such as "streaking", that account for the delayed atomic response in ionization from neon and argon. We also verify that photoelectron delays from many-electron atoms can be measured using simi…
Ultrashort electron pulses are crucial for time-resolved electron diffraction and microscopy of fundamental light-matter interaction. In this work, we study experimentally and theoretically the generation and characterization of attosecond electron pulses by optical-field-driven compression and streaking at dielectric or absorbing interaction elements. The achievable acceleration and deflection gradient depends on the laser-electron angle, the laser's electric and magnetic field directions and the foil orientation. Electric and magnetic fields have similar contributions to the final effect and…
We describe in detail how attosecond delays in laser-assisted photoionization can be computed using perturbation theory based on two-photon matrix elements. Special emphasis is laid on above-threshold ionization, where the electron interacts with an infrared field after photoionization by an extreme ultraviolet field. Correlation effects are introduced using diagrammatic many-body theory to the level of the random-phase approximation with exchange (RPAE). Our aim is to provide an ab initio route to correlated multi-photon processes that are required for an accurate description of experiments o…
The magnetic-field effect of the laser pulse is investigated in laser-assisted XUV ionization. By numerically solving the three-dimensional time-dependent Schrödinger equation, we find that the photoelectron momentum distribution is distorted by the magnetic-field effect of the IR streaking field. It results in a transverse-momentum- and time-delay-dependent longitudinal photoelectron momentum shift, which is further analytically confirmed by employing the nondipole corrected strong field approximation. We also demonstrate that the magnetic field does not affect the time shift retrieved from t…
We investigate the angle-resolved photoelectron spectra from laser-assisted photoionization for helium and neon atoms using an \textit{ab initio} method based on time-dependent surface flux and configuration interaction singles. We find that the shape of the distributions can be interpreted using a propensity rule, an intrinsic difference in the absorption and emission processes, as well as interference effects between multiple paths to the final angular momentum state. In neon we find that the difference between absorption and emission is hidden in the first sideband due to the multiple compe…
Photoelectron interferometry with spectrally shaped polychromatic infrared pulses
Lund University（隆德大学）；Sorbonne Université, CNRS, Laboratoire de Chimie Physique-Matière et Rayonnement, LCPMR（索邦大学，法国国家科学研究中心，物理化学物质与辐射实验室）；Institute of Atomic and Molecular Physics, Jilin University（吉林大学原子与分子物理研究所）；Albert-Ludwigs-Universität Freiburg（弗赖堡大学）；EUCOR Centre for Quantum Science and Quantum Computing, Albert-Ludwigs-Universität Freiburg（弗赖堡大学 EUCOR 量子科学与量子计算中心）；University of Gothenburg（哥德堡大学）
Laser-assisted photoemission from a solid is considered within a numerically exactly solvable one-dimensional model of a crystal. The effect of the inelastic scattering and of the finite duration of the pump pulse on the photoelectron dynamics is elucidated. The phenomenological result that the photoexcited wave packet moves with the group velocity dE/dk and traverses on average the distance equal to the mean free path is found to hold for energies far from the spectral gaps of the final state band structure. On the contrary, close to a spectral gap the photoelectron is found to move during th…
We present a new theoretical approach to attosecond laser-assisted photo- and Compton ionization. Attosecond x-ray absorption and scattering are described by $\hat{\mathrsfs{S}}^{(1,2)}$-matrices, which are coherent superpositions of "monochromatic" $\hat{S}^{(1,2)}$-matrices in a laser-modified Furry representation. Besides refining the existing theory of the soft x-ray photoelectron attosecond streak camera and spectral phase interferometry (ASC and ASPI), we formulate a theory of hard x-ray photoelectron and Compton ASC and ASPI. The resulting scheme has a simple structure and leads to clos…
We describe numerically the ionization process induced by linearly and circularly polarized XUV attosecond laser pulses on an aligned atomic target, specifically, the excited state Ne$^*(1s^22s^22p^5[{}^2\text{P}^\text{o}_{1/2}]3s[^1\text{P}^o])$. We compute the excited atomic state by applying the time-dependent restricted-active-space self-consistent field (TD-RASSCF) method to fully account for the electronic correlation. We find that correlation-assisted ionization channels can dominate over channels accessible without correlation. We also observe that the rotation of the photoelectron mom…
The ongoing development of intense high-harmonic generation (HHG) sources has recently enabled highly nonlinear ionization of atoms by the absorption of at least 10 extreme-ultraviolet (XUV) photons within a single atom [Senfftleben \textit{et al.}, arXiv1911.01375]. Here we investigate the role that reshaping of the fundamental, few-cycle, near-infrared (NIR) driving laser within the 30-cm-long HHG Xe medium plays in the generation of the intense HHG pulses. Using an incident NIR intensity that is higher than what is required for phase-matched HHG, signatures of reshaping are found by measuri…
