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 correlated emission a significant quadrupolar component within a few hundred attoseconds.
We present fully ab initio simulations of attosecond streaking for ionization of helium accompanied by shake-up of the second electron. This process represents a prototypical case for strongly correlated electron dynamics on the attosecond timescale. 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 qua…
We illustrate how attosecond light pulses can be used to directly mapping out the time-dependence of the correlated motion of two excited atomic electrons, discuss how the two-electron correlations manifest themselves in realistic attosecond measurements, and propose the following for experimental exploration: (a) The single ionization signals which directly reveal bending-vibrational motion of the correlated electron pair, (b) and also its rotational motion. (c) The double ionization signals which directly reveal the two-electron density in momentum space. To facilitate the description of the…
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…
Based on numerical solutions of the time-dependent Schrödinger equation for either one or two active electrons, we propose a method for observing instantaneous level shifts in an oscillating strong infrared (IR) field in time, using a single tunable attosecond pulse to probe excited states of the perturbed atom. The ionization probability in the combined fields depends on both, the frequency of the attosecond pulse and the time delay between both pulses, since the IR field shifts excited energy levels into and out of resonance with the attosecond probe pulse. We show that this method (i) allow…
Strong-field manipulation of autoionizing states is a crucial aspect of electronic quantum control. Recent measurements of the attosecond transient absorption spectrum of helium dressed by a few-cycle visible pulse [Ott et al., arXiv:1205.0519[physics.atom-ph] ] provide evidence of novel ultrafast resonant phenomena, namely, two-photon Rabi oscillations between doubly-excited states and the inversion of Fano profiles. Here we present the results of accurate \emph{ab-initio} calculations that agree with these observations and in addition predict that (i) inversion of Fano profiles is actually p…
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 show that electrons recolliding with the ionic core upon tunnel ionization of noble gas atoms driven by a strong circularly polarized laser field in combination with a counter-rotating second harmonic are spin polarized and that their degree of polarization depends strongly on the recollision time. Spin polarization arises as a consequence of (1) entanglement between the recolliding electron and the ion, and (2) sensitivity of ionization to the sense of electron rotation in the initial state. We demonstrate that one can engineer the degree of spin polarization as a function of time by tunin…
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 study resonant two-photon ionization of helium atoms via the $1s3p$, $1s4p$ and $1s5p^1$P$_1$ states using the 15$^\mathrm{th}$ harmonic of a titanium-sapphire laser for the excitation and a weak fraction of the laser field for the ionization. The phase of the photoelectron wavepackets is measured by an attosecond interferometric technique, using the 17$^\mathrm{th}$ harmonic. We perform experiments with angular resolution using a velocity map imaging spectrometer and with high energy resolution using a magnetic bottle electron spectrometer. Our results are compared to calculations using th…
We present the first demonstration of two-photon double ionization of neon using an intense extreme ultraviolet (XUV) attosecond pulse train (APT) in a photon energy regime where both direct and sequential mechanisms are allowed. For an APT generated through high-order harmonic generation (HHG) in argon we achieve a total pulse energy close to 1 $μ$J, a central energy of 35 eV and a total bandwidth of $\sim30$ eV. The APT is focused by broadband optics in a neon gas target to an intensity of $3\cdot10^{12} $W$\cdot$cm$^{-2}$. By tuning the photon energy across the threshold for the sequential …
The evolution of electron wavepackets determines the course of many physical and chemical phenomena and attosecond spectroscopy aims to measure and control such dynamics in real-time. Here, we investigate radial electron wavepacket motion in Helium by using an XUV attosecond pulse train to prepare a coherent superposition of excited states and a delayed femtosecond IR pulse to ionize them. Quantum beat signals observed in the high resolution photoelectron spectrogram allow us to follow the field-free evolution of the bound electron wavepacket and determine the time-dependent ionization dynamic…
Intense attosecond magnetic field pulses are predicted to be produced by intense few cycle circularly polarized UV pulses. Numerical solutions of the time dependent Schrödinger equation for H$_2^+$ are used to study the dynamical process. Spiralling attosecond circular electron wave packets are created with nanometer molecular dimensions, thus generating magnetic fields of several tens of Teslas ($10^5$ Gauss). Simulations show that the induced magnetic field is critically dependent on the pulse wavelength $λ$ and pulse duration $nτ$ ($n$ number of cycle) as predicted by a classical model. For…
Quantum-mechanical investigation is presented to study single attosecond pulse generation by gating high-order harmonic emission from H$_2^+$ molecule in intense laser pulses with time-dependent ellipticity. The high-order harmonic generation from H$_2^+$ molecule in superposition of a left and a right-hand circularly polarized Gaussian pulse is studied and the effect of time duration and carrier-envelope phase of laser field on single attosecond pulse generation is investigated. Using laser field formed by combination of a left and a right-hand elliptically polarized Gaussian pulse, the effec…
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 calculate the transient absorption of an isolated attosecond pulse by helium atoms subject to a delayed infrared (\ir) laser pulse. With the central frequency of the broad attosecond spectrum near the ionization threshold, the absorption spectrum is strongly modulated at the sub-\ir-cycle level. Given that the absorption spectrum results from a time-integrated measurement, we investigate the extent to which the delay-dependence of the absorption yields information about the attosecond dynamics of the atom-field energy exchange. We find two configurations in which this is possible. The first…
We show that the correlation dynamics in coherently excited doubly excited resonances of helium can be followed in real time by two-photon interferometry. This approach promises to map the evolution of the two-electron wave packet onto experimentally easily accessible non-coincident single electron spectra. We analyze the interferometric signal in terms of a semi-analytical model which is validated by a numerical solution of the time-dependent two-electron Schrödinger equation in its full dimensionality.
Using extreme-ultraviolet attosecond-pulse-trains, we investigate the photoionization dynamics of a Helium atom in the presence of moderately-strong (~10^12 W/cm^2) femtosecond laser pulses. The electronic structure of a laser-dressed atom is traced in real-time through precision measurements of ion-yields and photo-electron angular distributions. Quantum interferences between photo-excitation paths are interpreted using the Floquet formalism. As the laser pulse intensity ramps on femtosecond timescales, we observe transitions between ionization channels mediated by different atomic resonances…
We report theoretical calculations of high-order harmonic generation (HHG) of Xe with the inclusion of multi-electron effects and macroscopic propagation of the fundamental and harmonic fields in an ionizing medium. By using the time-frequency analysis we show that the reshaping of the fundamental laser field is responsible for the continuum structure in the HHG spectra. We further suggest a method for obtaining an isolated attosecond pulse (IAP) by using a filter centered on axis to select the harmonics in the far field with different divergence. We also discuss the carrier-envelope-phase dep…
The ionization of atoms with sequences of attosecond pulses gives rise to excited ionic states that are entangled with the emitted photoelectron. Still, the ionic ensemble preserves some coherence that can be controlled through the laser parameters. In helium, control of the $2s/2p$ He$^+$ coherence is mediated by the autoionizing states below the $N=2$ threshold [Phys. Rev. Res. {\bf 3}, 023233 (2021)]. In the present work we study the role of the resonances both below and above the $N=3$ threshold on the coherence of the $N=3$ He$^+$ ion, in the attosecond pump-probe ionization of the helium…
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 …
In this work we demonstrate the generation of two intense, ultrafast laser pulses that allow a controlled interferometric measurement of higher harmonic generation pulses with 12.8 attoseconds in resolution (half the atomic unit of time) and a precision as low as 680 zeptoseconds ($10^{-21}$ seconds). We create two replicas of a driving femtosecond pulse which share the same optical path except at the focus where they converge to two foci. An attosecond pulse train emerges from each focus through the process of HHG. The two attosecond pulse trains from each focus interfere in the far field pro…
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…
Nonsequential multiple ionization of atoms in intense laser fields is initiated by a recollision between an electron, freed by tunneling, and its parent ion. Following recollision, the initial electron shares its energy with several bound electrons. We use a classical model based on rapid electron thermalization to interpret recent experiments. For neon, good agreement with the available data is obtained with an upper bound of 460 attoseconds for the thermalization time.
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…
Attosecond pulses can ionize atoms in a coherent process. Since the emerging fragments are entangled, however, each preserves only a fraction of the initial coherence, thus limiting the chance of guiding the ion subsequent evolution. In this work, we use \emph{ab initio} simulations of pump-probe ionization of helium above the $2s/2p$ threshold to demonstrate how this loss of coherence can be controlled. Thanks to the participation of $2\ell n\ell'$ states, coherence between the ionic $2s$ and $2p$ states, which are degenerate in the non-relativistic limit, results in a stationary, delay-depen…
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 present experimental results showing the appearance of a near-continuum in the high-order harmonic generation (HHG) spectra of atomic and molecular species as the driving laser intensity of an infrared pulse increases. Detailed macroscopic simulations reveal that these near-continuum spectra are capable of producing IAPs in the far field if a proper spatial filter is applied. Further, our simulations show that the near-continuum spectra and the IAPs are a product of strong temporal and spatial reshaping (blue shift and defocusing) of the driving field. This offers a possibility of producing…
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.
In the present work we report on the current progress of the recently constructed GW attosecond extreme ultraviolet (XUV) source developed at the Institute of Electronic Structure and Laser of the Foundation for Research and Technology-Hellas (I.E.S.L-FO.R.T.H.). By the implementation of a compact-collinear polarization gating arrangement, the generation of a broadband, coherent XUV quasi-continuum produced by the interaction of a many-cycle infrared field with a gas phase medium is achieved. The spectral width of the XUV emission generated in Xenon, is spanning in the range of 17-32 eV and ca…
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 describe a numerical method that simulates the interaction of the helium atom with sequences of femtosecond and attosecond light pulses. The method, which is based on the close-coupling expansion of the electronic configuration space in a B-spline bipolar spherical harmonic basis, can accurately reproduce the excitation and single ionization of the atom, within the electrostatic approximation. The time dependent Schrödinger equation is integrated with a sequence of second-order split-exponential unitary propagators. The asymptotic channel-, energy- and angularly-resolved photoelectron distr…
Attosecond pulses can be used to initiate and control electron dynamics on a sub-femtosecond time scale. The first step in this process occurs when an atom absorbs an ultraviolet photon leading to the formation of an attosecond electron wave packet (EWP). Until now, attosecond pulses have been used to create free EWPs in the continuum, where they quickly disperse. In this paper we use a train of attosecond pulses, synchronized to an infrared (IR) laser field, to create a series of EWPs that are below the ionization threshold in helium. We show that the ionization probability then becomes a fun…
We investigate the response of two three-body Coulomb systems when driven by attosecond half-cycle pulses: The hydrogen molecular ion and the helium atom. Using very short half-cycle pulses (HCPs) which effectively deliver ``kicks'' to the electrons, we first study how a carefully chosen sequence of HCPs can be used to control to which of one of the two fixed atomic centers the electron gets re-attached. Moving from one electron in two atomic centers to two electrons in one atomic center we then study the double ionization from the ground state of He by a sequence of attosecond time-scale HCPs…
In our model the electron dynamics are described by a two-state approximation. This might appear a rough approximation since it neglects coupling through excited electronic states and ionization channels. However at high intensity (laser fields equivalent to the Coulomb force) and long wavelength (photon energy much lower than the ionization potential) the dissociation process occurs by adiabatic polarization involving the lowest electronic states. For the experiment in question, with intensities above 10x14 W cm-2 and photon energies of 1.5eV, such an approach is well justified. More contenti…
A novel and universal interference structure is found in the photoelectron momentum distribution of atoms in intense infrared laser field. Theoretical analysis shows that this structure can be attributed to a new form of Coulomb-field-driven backward-scattering of photoelectrons in the direction perpendicular to the laser field, in contrast to the conventional rescattering along the laser polarization direction. This transverse backward-scattering process is closely related to a family of photoelectrons initially ionized within a time interval of less than 200 attosecond around the crest of th…
Imaging in real time the complete dynamics of a process as fundamental as photoemission has long been out of reach due to the difficulty of combining attosecond temporal resolution with fine spectral and angular resolutions. Here, we achieve full decoding of the intricate angle-dependent dynamics of a photoemission process in helium, spectrally and anisotropically structured by twophoton transitions through intermediate bound states. Using spectrally- and angularly-resolved attosecond electron interferometry, we characterize the complex-valued transition probability amplitude towards the photo…
Attosecond photoionisation time delays reveal information about the potential energy landscape an outgoing electron wavepacket probes upon ionisation. In this study we experimentally quantify, for the first time, the dependence of the time delay on the angular momentum of the liberated photoelectrons. For this purpose, electron quantum-path interference spectra have been resolved in energy and angle using a two-color attosecond pump-probe photoionisation experiment in helium. A fitting procedure of the angle-dependent interference pattern allows us to disentangle the relative phase of all four…
At the core of attosecond science lies the ability to generate laser pulses of sub-femtosecond duration. In tabletop devices the process relies on high-harmonic generation, where a major challenge is to obtain high yields and high cutoff energies required for the generation of attosecond pulses. We develop a computational method that can simultaneously resolve these issues by optimizing the driving pulses using quantum optimal control theory. Our target functional, an integral over the harmonic yield over a desired energy range, leads to a remarkable cutoff extension and yield enhancement for …
We calculate the atomic structure of hydrogen and helium, atoms and molecules in an intense magnetic field, analytically and numerically with a judiciously chosen basis.
We present a theoretical study of the photoelectron attosecond beating at the basis of RABBIT (Reconstruction of Attosecond Beating By Interference of Two-photon transitions) in the presence of autoionizing states. We show that, as a harmonic traverses a resonance, its sidebands exhibit a peaked phase shift as well as a modulation of the beating frequency itself. Furthermore, the beating between two resonant paths persists even when the pump and the probe pulses do not overlap, thus providing a sensitive non-holographic interferometric means to reconstruct coherent metastable wave packets. We …
Ionization by relativistically intense short laser pulses is studied in the framework of strong-field quantum electrodynamics. Distinctive patterns are found in the energy probability distributions of photoelectrons. Except of the already observed patterns, which were studied in Phys. Rev. A {\bf 94}, 013402 (2016), we discover an additional interference-free smooth supercontinuum in the high-energy portion of the spectrum, reaching tens of kiloelectronovolts. As we show, the latter is sensitive to the driving field intensity and it can be detected in a narrow polar-angular window. Once these …
The complex Kohn variational method is extended to compute light-driven electronic transitions between continuum wavefunctions in atomic and molecular systems. This development enables the study of multiphoton processes in the perturbative regime for arbitrary light polarization. As a proof of principle, we apply the method to compute the photoelectron spectrum arising from the pump-probe two-photon ionization of helium induced by a sequence of extreme ultraviolet and infrared-light pulses. We compare several two-photon ionization pump-probe spectra, resonant with the (2s2p)1P1o Feshbach reson…
Double photoelectron emission from He atoms by intense laser pulses with a wave length of $394.5\,nm$ is computed for intensities $3.5 - 9.2\times 10^{14}W/cm^2$. Joint momentum distributions confirm the characteristics seen in classical trajectory calculations. The pronounced transition from back-to-back to side-by-side emission with increasing intensity, the $He^{++}/He^+$ ratios, and a modulation of joint energy spectra agree well with a recent experiment [Henrichs et al., PRA 98, 43405 (2018)], if one admits an increase of experimental intensities by a factor $\sim 2$. We find that Freeman…
Amplitude and phase of wavepackets encode the dynamics of quantum systems. However, the rapidity of electron dynamics on the attosecond timescale has precluded their complete measurement in the time domain. Here, we demonstrate that spectrally-resolved electron interferometry reveals the amplitude and phase of a photoelectron wavepacket created through a Fano autoionizing resonance in helium. Replicas obtained by two-photon transitions interfere with reference wavepackets formed through smooth continua, allowing the full temporal reconstruction, purely from experimental data, of the resonant w…
We propose a theoretical approach for the interpretation of pump-probe measurements where an attosecond pulse is absorbed in the presence of an intense laser pulse. This approach is based on abstractly defined dressed bound states, which capture the essential aspects of the interaction with the laser pulse and facilitate a perturbative description of transitions induced by the attosecond pulse. Necessary properties of dressed bound states are defined and various choices are discussed and compared to accurate numerical solutions of the time-dependent Schroedinger equation.
The possibility of achieving highly selective excitation of low metastable states of hydrogen and helium atoms by using short laser pulses with reasonable parameters is demonstrated theoretically. Interactions of atoms with the laser field are studied by solving the close-coupling equations without discretization. The parameters of laser pulses are calculated using different kinds of optimization procedures. For the excitation durations of hundreds of femtoseconds direct optimization of the parameters of one and two laser pulses with Gaussian envelopes is used to introduce a number of simple s…
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…
With the classical three-dimensional ensemble model, we have investigated the microscopic recollision dynamics in nonsequential double ionization of helium by 800 nm laser pulses at 2.0 PW/cm^2. We demonstrate that the asymmetric energy sharing between the two electrons at recollision plays a decisive role in forming the experimentally observed V-shaped structure in the correlated longitudinal electron momentum spectrum at the high laser intensity [Phys. Rev. Lett. 99, 263003 (2007)]. This asymmetric energy sharing recollision leaves footprints on the transverse electron momentum spectra, whic…
Attosecond pulses, produced through high-order harmonic generation in gases, have been successfully used for observing ultrafast, sub-femtosecond electron dynamics in atoms, molecules and solid state systems. Today's typical attosecond sources, however, are often impaired by their low repetition rate and the resulting insufficient statistics, especially when the number of detectable events per shot is limited. This is the case for experiments where several reaction products must be detected in coincidence, and for surface science applications where space-charge effects compromise spectral and …
