We investigate the laser-assisted single XUV photon double ionization of ground state helium. By solving full six-dimensional time-dependent schr{ö}dinger equation, we study the correlation and angular distribution. The discussion in joint energy and angular distributions reveals the competition in odd and even parity double ionization processes in the presence of weak laser field. The emission angle between two photoelectrons can be adjusted by the laser parameters. We depicts how the laser field enhance and/or enable the back-to-back and side-by-side emission of double ionization.
We present and discuss a new computationally inexpensive method to study, within the single active electron approximation, the interaction of a complex system with an intense ultrashort laser pulse. As a first application, we consider the one photon single ionisation of the highest occupied molecular orbital of the water molecule by a laser pulse. The ionisation yield is calculated for different orientations of the molecule with respect to the field polarization axis and for different carrier envelope phases of the pulse, and compared against predictions of another single active electron appro…
We report on the observation of time-resolved quantum beats in the helium fluorescence from the transition 1s3p -> 1s2s, where the initial state is excited by XUV free-electron laser radiation. The quantum beats originate from the Zeeman splitting of the magnetic substates due to an external magnetic field. We perform a systematic study of this effect and discuss the possibilities of studying this phenomenon in the XUV and x-ray regime.
Ionization with ultrashort pulses in the extreme ultraviolet (XUV) regime can be used to prepare an ion in a superposition of spin--orbit substates. In this work, we study the coherence properties of such a superposition, created by ionizing xenon atoms using two phase-locked XUV pulses at different frequencies. In general, if the duration of the driving pulse exceeds the quantum beat period, dephasing will occur. If however, the frequency difference of the two pulses matches the spin--orbit splitting, the coherence can be efficiently increased and dephasing does not occur.
It is shown that it is feasible to use ultrashort time delay between two XUV femtosecond pulses in order to control two photon resonant ionization. The proposal is demonstrated on the spectrum of Helium, in terms of nonperturbative solutions of the time dependent Schroedinger equation. Comparison with results from second order time dependent perturbation theory provides additional insight.
We explore the influence of elliptical polarization on the (non)sequential two-photon double ionization of atomic helium with ultrashort extreme ultraviolet (XUV) light fields using time-dependent full ab-initio simulations. The energy and angular distributions of photoelectrons are found to be strongly dependent on the ellipticity. The correlation minimum in the joint angular distribution becomes more prominently visible with increasing ellipticity. In a pump-probe sequence of two subsequent XUV pulses with varying ellipticities, polarization tagging allows to discriminate between sequential …
The collision-ionization mechanism of nonsequential double ionization (NSDI) process in IR+XUV two-color laser fields [\PRA \textbf{93}, 043417 (2016)] has been investigated by us recently. Here we extend this work to study the collision-excitation-ionization (CEI) mechanism of NSDI processes in the two-color laser fields with different laser conditions. It is found that the CEI mechanism makes a dominant contribution to the NSDI as the XUV photon energy is smaller than the ionization threshold of the He$^+$ ion, and the momentum spectrum shows complex interference patterns and symmetrical str…
Recent experimental developments of high-intensity, short-pulse XUV light sources are enhancing our ability to study electron-electron correlations. We perform time-dependent calculations to investigate the so-called "sequential" regime (photon energy above 54.4 eV) in the two-photon double ionization of helium. We show that attosecond pulses allow to induce and probe angular and energy correlations of the emitted electrons. The final momentum distribution reveals regions dominated by the Wannier ridge break-up scenario and by post-collision interaction.
We present a theoretical study of transient absorption and reshaping of extreme ultraviolet (XUV) pulses by helium atoms dressed with a moderately strong infrared (IR) laser field. We formulate the atomic response using both the frequency-dependent absorption cross section and a time-frequency approach based on the time-dependent dipole induced by the light fields. The latter approach can be used in cases when an ultrafast dressing pulse induces transient effects, and/or when the atom exchanges energy with multiple frequency components of the XUV field. We first characterize the dressed atom r…
We consider an electron in an atom driven by an infrared (IR) elliptically polarized laser field after its ionization by an ultrashort extreme ultraviolet (XUV) pulse. We find that, regardless of the atom species and the laser ellipticity, there exists XUV parameters for which the electron returns to its parent ion after ionizing, i.e., undergoes a recollision. This shows that XUV pulses trigger efficiently recollisions in atoms regardless of the ellipticity of the IR field. The XUV parameters for which the electron undergoes a recollision are obtained by studying the location of recolliding p…
Phase-shift differences and amplitude ratios of the outgoing $s$ and $d$ continuum wave packets generated by two-photon ionization of helium atoms are determined from the photoelectron angular distributions obtained using velocity map imaging. Helium atoms are ionized with ultrashort extreme-ultraviolet free-electron laser pulses with a photon energy of 20.3, 21.3, 23.0, and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The measured values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to an excited …
Photoelectron emission from excited states of laser-dressed atomic helium is analyzed with respect to laser intensity-dependent excitation energy shifts and angular distributions. In the two-color XUV (exteme ultra\-violet) -- IR (infrared) measurement, the XUV photon energy is scanned between \SI{20.4}{\electronvolt} and the ionization threshold at \SI{24.6}{\electronvolt}, revealing electric dipole-forbidden transitions for a temporally overlapping IR pulse ($\sim\!\SI{e12}{\watt\per \centi\meter\squared}$). The interpretation of the experimental results is supported by numerically solving t…
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. …
The remarkable precision of frequency comb (FC) lasers is transferred to the extreme ultraviolet (XUV, wavelengths shorter than 100 nm), a frequency region previously not accessable to these devices. A frequency comb at XUV wavelengths near 51 nm is generated by amplification and coherent upconversion of a pair of pulses originating from a near-infrared femtosecond FC laser. The phase coherence of the source in the XUV is demonstrated using Helium atoms as a ruler and phase detector. Signals in the form of stable Ramsey-like fringes with high contrast are observed when the FC laser is scanned …
In anticipation of upcoming two-photon double ionization of atoms and particularly Helium, under strong short wavelength radiation sources (45 eV), we present quantitative signatures of direct two-photon double ejection, in the photoelectron spectrum (PES) and the peak power dependence, that can be employed in the interpretation of related data. We show that the PES provides the cleanest signature of the process. An inflection (knee) in the laser power dependence of double ionization is also discernible, within a window of intensities which depends on the pulse duration and cross sections
We investigate two-photon double ionization of helium by intense ($10^{15} W/cm^2$) ultrashort ($\approx 300$ as) soft X-ray pulses (E = 91.6 eV). The time-dependent two-electron Schrödinger equation is solved using a coupled channel method. We show that for ultrashort pulses the angular distribution of ejected electrons depends on the pulse duration and provides novel insights into the role of electron correlations in the two-electron photoemission process. The angular distribution at energies near the ``independent electron'' peaks is close to dipolar while it acquires in the ``valley'' of c…
Noncollinear wave-mixing spectroscopies with attosecond extreme ultraviolet (XUV) pulses provide unprecedented insight into electronic dynamics. In infrared and visible regimes, heterodyne detection techniques utilize a reference field to amplify wave-mixing signals while simultaneously allowing for phase-sensitive measurements. Here, we implement a self-heterodyned detection scheme in noncollinear wave-mixing measurements with a short attosecond XUV pulse train and two few-cycle near infrared (NIR) pulses. The initial spatiotemporally overlapped XUV and NIR pulses generate a coherence of both…
We study theoretically the photoabsorption spectra of an attosecond XUV pulse by a laserdressed atomic system. A weak XUV excites an autoionizing state which is strongly coupled to another autoionizing state by a laser. The theory was applied to explain two recent experiments [Loh, Greene, and Leone, Chem. Phys. 350, 7 (2008); Wang, Chini, Chen, Zhang, Cheng, He, Cheng, Wu, Thumm, and Chang, Phys. Rev. Lett. 105 143002 (2010)] where the absorption spectra of the XUV lights were measured against the time delay between the laser and the XUV. In another example, we study an attosecond pulse excit…
The operation of a frequency comb at extreme ultraviolet (XUV) wavelengths based on pair-wise amplification and nonlinear upconversion to the 15th harmonic of pulses from a frequency comb laser in the near-infrared range is reported. Following a first account of the experiment [Kandula et al., Phys. Rev. Lett. 105, 063001 (2010)], an extensive review is given of the demonstration that the resulting spectrum at 51 nm is fully phase coherent and can be applied to precision metrology. The pulses are used in a scheme of direct-frequency-comb excitation of helium atoms from the ground state to the …
We report experiments on field-free molecular alignment performed at FLASH, the free electron laser (FEL) in Hamburg. The impulsive alignment induced by a 100 fs near-infrared laser pulse in a rotationally cold CO_2 sample is characterized by ionizing and dissociating the molecules with a time delayed extreme ultra-violet (XUV) FEL pulse. The time-dependent angular distributions of ionic fragments measured by a velocity map imaging spectrometer shows rapid changes associated with the induced rotational dynamics. The experimental results also show hints of a dissociation process that depends no…
Time delays of electrons emitted from an isotropic initial state and leaving behind an isotropic ion are assumed to be angle-independent. Using an interferometric method involving XUV attosecond pulse trains and an IR probe field in combination with a detection scheme, which allows for full 3D momentum resolution, we show that measured time delays between electrons liberated from the $1s^2$ spherically symmetric ground state of helium depend on the emission direction of the electrons relative to the linear polarization axis of the ionizing XUV light. Such time-delay anisotropy, for which we me…
We investigate the absorption line shapes of laser-dressed atoms beyond the single-atom response, by using extreme ultraviolet (XUV) attosecond pulse trains to probe an optically thick helium target under the influence of a strong infrared (IR) field. We study the interplay between the IR-induced phase shift of the microscopic time-dependent dipole moment and the resonant-propagation-induced reshaping of the macroscopic XUV pulse. Our experimental and theoretical results show that as the optical depth increases, this interplay leads initially to a broadening of the IR-modified line shape, and …
We investigate the possibility to monitor the dynamics of autoionizing states in real time and control the yields of different ionization channels in helium by simulating XUV-pump IR-probe experiments focused on the N=2 threshold. The XUV pulse creates a coherent superposition of doubly excited states which is found to decay by ejecting electrons in bursts. Prominent interference fringes in the photoelectron angular distribution of the $2s$ and $2p$ ionization channels are observed, along with sizable out-of-phase quantum beats in the yields of the corresponding parent ions.
We show that time ordering underlying time-dependent quantum dynamics is a physical observable accessible by attosecond streaking. We demonstrate the extraction of time ordering for the prototypical case of time-resolved two-photon double ionization (TPDI) of helium by an attosecond XUV pulse. The Eisenbud-Wigner-Smith time delay for the emission of a two-electron wavepacket and the time interval between subsequent emission events can be unambiguously determined by attosecond streaking. The delay between the two emission events sensitively depends on the energy, pulse duration, and angular dis…
We theoretically examine neon atoms in ultrashort and intense x rays from free electron lasers and compare our results with data from experiments conducted at the Linac Coherent Light Source (LCLS). For this purpose, we treat in detail the electronic structure in all possible nonrelativistic cationic configurations using a relativistic multiconfiguration approach. The interaction with the x rays is described in rate-equation approximation. To understand the mechanisms of the interaction, a path analysis is devised which allows us to investigate what sequences of photoionization and decay proce…
We investigate an angular dependence of the photoemission time delay in helium as measured by the RABBITT (Reconstruction of Attosecond Beating By Interference of Two-photon Transitions) technique. The measured time delay $ τ_a=τ_W+τ_{cc} $ contains two distinct components: the Wigner time delay $τ_W$ and the continuum-continuum CC) correction $τ_{cc}$. In the case of helium with only one $1s\to Ep$ photoemission channel, the Wigner time delay $τ_W$ does not depend on the photoelectron detection angle relative to the polarization vector. However, the CC correction $τ_{cc}$ shows a noticeable a…
Breakdown of sequential tunnel ionization in ultrashort electromagnetic pulses
National Research Nuclear University MEPhI（国立研究核大学）；P.N. Lebedev Physical Institute of the Russian Academy of Sciences（俄罗斯科学院列别捷夫物理研究所）；Prokhorov General Physics Institute of the Russian Academy of Sciences（俄罗斯科学院普罗霍罗夫普通物理研究所）
We investigate theoretically the dissociative ionization of a H2+ molecule using two ultrashort laser (pump-probe) pulses. The pump pulse prepares a dissociating nuclear wave packet on an ungerade surface of H2+. Next, an UV (or XUV) probe pulse ionizes this dissociating state at large (R = 20 - 100 bohr) internuclear distance. We calculate the momenta distributions of protons and photoelectrons which show a (two-slit-like) interference structure. A general, simple interference formula is obtained which depends on the electron and protons momenta, as well as on the pump-probe delay on the puls…
We investigate theoretically electron dynamics under a VUV attosecond pulse train which has a controlled phase delay with respect to an additional strong infrared laser field. Using the strong field approximation and the fact that the attosecond pulse is short compared to the excited electron dynamics, we arrive at a minimal analytical model for the kinetic energy distribution of the electron as well as the photon absorption probability as a function of the phase delay between the fields. We analyze the dynamics in terms of electron wave packet replicas created by the attosecond pulses. The ab…
Measurements of the phase of two-photon matrix elements are presented for resonant and antiresonant two-color ionization of helium. A tunable, narrow-bandwidth, near-infrared (NIR) laser source is used for extreme ultra-violet (XUV) high-harmonic generation (HHG). The 15th harmonic of the laser is used within (1+1') XUV+NIR two-photon ionization, and tuned in and out of resonance with members of the 1s$n$p $^1$P$_1$ ($n=3,4,5$) Rydberg series, covering a broad spectral range with high spectral resolution. The technique allows to observe characteristic rapid changes in the phase of the two-phot…
The evolution of electron wavepackets determines the course of many physical and chemical phenomena and attosecond spectroscopy aims to measure and control such dynamics in real-time. Here, we investigate radial electron wavepacket motion in Helium by using an XUV attosecond pulse train to prepare a coherent superposition of excited states and a delayed femtosecond IR pulse to ionize them. Quantum beat signals observed in the high resolution photoelectron spectrogram allow us to follow the field-free evolution of the bound electron wavepacket and determine the time-dependent ionization dynamic…
We investigate the role of electron correlation in the two-photon double ionization of helium for ultrashort XUV pulses with durations ranging from a hundred attoseconds to a few femtoseconds. We perform time-dependent ab initio calculations for pulses with mean frequencies in the so-called "sequential" regime (photon energy above 54.4 eV). Electron correlation induced by the time correlation between emission events manifests itself in the angular distribution of the ejected electrons, which strongly depends on the energy sharing between them. We show that for ultrashort pulses two-photon doub…
We use R-Matrix with Time-dependence (RMT) theory, with spin-orbit effects included, to study krypton irradiated by two time-delayed XUV ultrashort pulses. The first pulse excites the atom to 4s$^{2}$4p$^{5}$5s. The second pulse then excites 4s4p$^{6}$5s autoionising levels, whose population can be observed through their subsequent decay. By varying the time delay between the two pulses, we are able to control the excitation pathway to the autoionising states. The use of cross-polarised light pulses allows us to isolate the two-photon pathway, with one photon taken from each pulse.
We investigate the photoionization spectrum of helium by attosecond XUV pulses both in the spectral region of doubly excited resonances as well as above the double ionization threshold. In order to probe for convergence, we compare three techniques to extract photoelectron spectra from the wavepacket resulting from the integration of the time-dependent Schroedinger equation in a finite-element discrete variable representation basis. These techniques are: projection on products of hydrogenic bound and continuum states, projection onto multi-channel scattering states computed in a B-spline clos…
We report on the experimental observation of strong-field dressing of an autoionizing two-electron state in helium with intense extreme-ultraviolet laser pulses from a free-electron laser. The asymmetric Fano line shape of this transition is spectrally resolved, and we observe modifications of the resonance asymmetry structure for increasing free-electron-laser pulse energy on the order of few tens of $μ$J. A quantum-mechanical calculation of the time-dependent dipole response of this autoionizing state, driven by classical extreme-ultraviolet (XUV) electric fields, reveals a direct link betwe…
Photoelectron spectroscopy of 3s3p doubly excited helium dressed with strong near-infrared laser fields
Nagoya University（名古屋大学）；RIKEN, SPring-8 Center（理化学研究所 SPring-8 中心）；Fu-Jen Catholic University（辅仁大学）；Japan Synchrotron Radiation Research Institute（日本同步辐射研究机构）；University of Toyama（富山大学）
We investigate numerically with Hylleraas coordinates the frequency dependence of the carrier-envelope phase (CEP) effect on bound-bound transitions of helium induced by an ultrashort laser pulse of few cycles. We find that the CEP effect is very sensitive to the carrier frequency of the laser pulse, occurring regularly even at far-off resonance frequencies. By analyzing a two-level model, we find that the CEP effect can be attributed to the quantum interference between neighboring multi-photon transition pathways, which is made possible by the broadened spectrum of the ultrashort laser pulse.…
We study the photoionization and autoionization of Helium atom subject to ultrashort laser pulses by using a Feshbach formalism in the time domain. We solve the time-dependent Schrödinger equation in terms of a configuration interaction (CI) spectral method, in which the total wavefunction is expanded with configurations defined within bound-like ($\mathcal{Q}$) and scattering-like ($\mathcal{P}$) halfspaces. The method allowsone to provide accurate descriptions of both the atomic structure (energy positions and widths) and the photodynamics. We illustrate our approach by i) calculating the ti…
Compton scattering is one of the fundamental interaction processes of light with matter. Already upon its discovery [1] it was described as a billiard-type collision of a photon kicking a quasi-free electron. With decreasing photon energy, the maximum possible momentum transfer becomes so small that the corresponding energy falls below the binding energy of the electron. Then ionization by Compton scattering becomes an intriguing quantum phenomenon. Here we report a kinematically complete experiment on Compton scattering at helium atoms below that threshold. We determine the momentum correlati…
We study the higher-harmonic generation (HHG) using elliptically polarized two-color driving fields. The HHG via bi-chromatic counter-rotating laser fields is a promising source of circularly polarized ultrashort XUV radiation at the attosecond time scale. The ellipticity or the polarization of the attosecond pulses can be tweaked by modifying the emitted harmonics' ellipticity, which can be controlled by varying the driver fields. We propose a simple setup to control the polarization of the driving fields, which eventually changes the ellipticity of the attosecond pulses. A well-defined scali…
Unraveling and controlling chemical dynamics requires techniques to image structural changes of molecules with femtosecond temporal and picometer spatial resolution. Ultrashort-pulse x-ray free-electron lasers have significantly advanced the field by enabling advanced pump-probe schemes. There is an increasing interest in using table-top photon sources enabled by high-harmonic generation of ultrashort-pulse lasers for such studies. We present a novel high-harmonic source driven by a 100 kHz fiber laser system, which delivers 10$^{11}$ photons/s in a single 1.3 eV bandwidth harmonic at 68.6 eV.…
Multiphoton-ionized electrons are born into a strong light field that will determine their short-term future. By controlling the infrared beam, we enable atoms or molecules to generate extreme ultraviolet (XUV) pulses and synthesize attosecond pulses - the shortest controlled events ever produced. Here we show that a weak obliquely incident beam imposes an optical grating on the fundamental beam, resulting in a spatially modulated attosecond pulse. We observe the modulation on a spectrally resolved near-field XUV image, encoding all information of the spectral phase of the recollision electron…
We investigate the evolution of extreme ultraviolet (XUV) spectral lineshapes in an optically-thick helium gas under near-infrared (IR) perturbation. In our experimental and theoretical work, we systematically vary the IR intensity, time-delay, gas density and IR polarization parameters to study lineshape modifications induced by collective interactions, in a regime beyond the single atom response of a thin, dilute gas. In both experiment and theory, we find that specific features in the frequency-domain absorption profile, and their evolution with propagation distance, can be attributed to th…
We theoretically study the process of photoelectron emission of the Helium atom by a high-intensity short-wavelength laser at a resonance condition of the residual singly charged ion. Photoionization followed by strong resonance coupling in the ion leads to a change in the photoelectron spectrum due to Rabi oscillations in the residual ion. Similarly to resonance fluorescence at high laser intensity, the photoelectron spectrum at high intensities evolves into a multi-peaked structure. The number of peaks in the photoelectron spectrum is related to the number of Rabi cycles following the photoi…
Using the finite-element discrete variable representation of the nonequilibrium Green's function (NEGF) we extend previous work [K.~Balzer et al., Phys. Rev. A \textbf{81}, 022510 (2010)] to nonequilibrium situations and compute---from the two-time Schwinger-Keldysh-Kadanoff-Baym equations---the response of the helium atom and the heteronuclear molecule lithium hydride to laser fields in the uv and xuv regime. In particular, by comparing the one-electron density and the dipole moment to time-dependent Hartree-Fock results on one hand and the full solution of the time-dependent Schrödinger equa…
An autoionizing resonance in molecular N$_2$ is excited by an ultrashort XUV pulse and probed by a subsequent weak IR pulse, which ionizes the contributing Rydberg states. Time- and angular-resolved photoelectron spectra recorded with a velocity map imaging spectrometer reveal two electronic contributions with different angular distributions. One of them has an exponential decay rate of $20\pm5$ fs, while the other one is shorter than 10 fs. This observation is interpreted as a manifestation of interference stabilization involving the two overlapping discrete Rydberg states. A formalism of int…
We present numerical simulations of high-order harmonic generation in helium using a temporally synthesised and spatially non-homogeneous strong laser field. The combination of temporal and spatial laser field synthesis results in a dramatic cut-off extension far beyond the usual semiclassical limit. Our predictions are based on the convergence of three complementary approaches: resolution of the three dimensional Time Dependent Schrödinger Equation, time-frequency analysis of the resulting dipole moment and classical trajectories extraction. Employing a combination of temporally and spatially…
An optical coherent control scheme has been proposed and theoretically investigated where an extreme ultraviolet single attosecond pulse (SAP) propagates through a dense helium gas dressed by a time-delayed femtosecond laser pulse. The laser pulse couples the 2s2p(^1P) and 2s^2(^1S) autoionizing states when the SAP excites the 2s2p state. After going through the gas, the spectral and temporal profiles of the SAP are strongly distorted. A narrowed but enhanced spike in the spectrum shows up for specific intensities and time delays of the laser, which exemplifies the control of a broadband photo…
