Using a three-dimensional quasiclassical technique we explore the double ionization pathways of a diatomic molecule driven by an intense infrared (800nm) ultrashort laser pulse. For intensities corresponding to the tunneling regime, we find that the three main ionization mechanisms have distinct traces when considering the sum of the momenta parallel to the laser field as a function of the inter-electronic angle of escape. In addition, we find that the previously observed "finger-like" structure in the correlated momenta of the strongly driven He is also present for strongly driven diatomic molecules. We show that it is mainly due to the strong interaction, backscattering, the recolliding electron undergoes from the remaining core.
We investigate electron correlation effects in internuclear-distance-dependent enhanced ionization of $\mathrm{H}_2$, $\mathrm{LiH}$, and $\mathrm{HF}$ molecules by intense near-infrared laser pulses using a 3D description of the systems with the time-dependent generalized-active-space configuration-interaction method. This method systematically incorporates electron-electron correlation of the quantum many-electron system under consideration. Our correlated description of diatomic molecules shows that enhanced ionization occurs at certain critical internuclear separations and electron correla…
Diatomic molecules (e.g., O$_2$) in intense laser field exhibit a peculiar suppressed ionization behavior compared to their companion atoms. Several physical models have been proposed to account for this suppression while no consensus has been achieved. In this letter, we aim to clarify the underlying mechanisms behind this molecular ionization suppression. Experimental data recorded at midinfrared laser wavelength and its comparison with that at near-infrared wavelength revealed a peculiar wavelength and intensity dependence of the suppressed ionization of O$_2$ with respect to its companion …
The direct above-threshold ionization (ATI) of diatomic molecules in linearly-polarized infrared and extreme ultraviolet (IR+XUV) laser fields is investigated by the frequency-domain theory based on the nonperturbative quantum electrodynamics. The destructive interference fringes on the angle-resolved ATI spectra, which are closely related to the molecular structure, can be well fitted by a simple predictive formula for any alignment of the molecular axis. By comparing the direct ATI spectra for monochromatic and two-color laser fields, we found that the XUV laser field can both raise the ioni…
A model based on the strong-field and Born-Oppenheimer approximations qualitatively describes the distribution over vibrational states formed in a diatomic molecular ion following ionization of the neutral molecule by intense laser pulses. Good agreement is found with a recent experiment [X. Urbain et al., Phys. Rev. Lett. 92, 163004 (2004)]. In particular, the observed deviation from a Franck-Condon-like distribution is reproduced. Additionally, we demonstrate control of the vibrational distribution by a variation of the peak intensity or a change of frequency of the laser pulse.
We calculate angle-resolved above-threshold ionization spectra for diatomic molecules in linearly polarized laser fields, employing the strong-field approximation. The interference structure resulting from the individual contributions of the different scattering scenarios is discussed in detail, with respect to the dependence on the internuclear distance and molecular orientation. We show that, in general, the contributions from the processes in which the electron is freed at one center and rescatters off the other obscure the interference maxima and minima obtained from single-center processe…
We address the influence of the orbital symmetry and of the molecular alignment with respect to the laser-field polarization on laser-induced nonsequential double ionization of diatomic molecules, in the length and velocity gauges. We work within the strong-field approximation and assume that the second electron is dislodged by electron-impact ionization, and also consider the classical limit of this model. We show that the electron-momentum distributions exhibit interference maxima and minima due to the electron emission at spatially separated centers. The interference patterns survive the in…
We present a detailed comparison of strong-field ionization of diatomic molecules and their companion atoms with nearly equal ionization potentials. We perform calculations in the length and velocity gauge formulations of the molecular strong-field approximation and with the molecular tunneling theory, and in both cases we consider effects of nuclear motion. A comparison of our results with experimental data shows that the length gauge strong-field approximation gives the most reliable predictions.
We investigated electron emissions in strong field enhanced ionization of asymmetric diatomic molecules by quantum calculations. It is demonstrated that the widely-used intuitive physical pic- ture, i.e., electron wave packet direct ionization from the up-field site (DIU), is incomplete. Besides DIU, we find another two new ionization channels, the field-induced excitation with subsequent ionization from the down-field site (ESID), and the up-field site (ESIU). The contributions from these channels depend on the molecular asymmetry and internuclear distance. Our work provides a more comprehens…
We investigate laser-induced nonsequential double ionization from aligned diatomic molecules, using the strong-field approximation in its length and velocity gauge formulations. Throughout, we consider that the first electron dislodges the second by electron-impact ionization. Employing modified saddle-point equations, we single out the contributions of different scattering scenarios to the maxima and minima observed in the differential electron momentum distributions. We show that the quantum interference between the electron orbits starting and ending at a specific center $C_{j}$%, and those…
Strong field photoemission and electron recollision provide a viable route to extract electronic and nuclear dynamics from molecular targets with attosecond temporal resolution. However, since an {\em ab-initio} treatment of even the simplest diatomic systems is beyond today's capabilities approximate qualitative descriptions are warranted. In this paper, we develop such a theoretical approach to model the photoelectrons resulting from intense laser-molecule interaction. We present a general theory for symmetric diatomic molecules in the single active electron approximation that, amongst other…
We address the influence of the molecular orbital geometry and of the molecular alignment with respect to the laser-field polarization on laser-induced nonsequential double ionization of diatomic molecules for different molecular species, namely $\mathrm{N}_2$ and $\mathrm{Li}_2$. We focus on the recollision excitation with subsequent tunneling ionization (RESI) mechanism, in which the first electron, upon return, promotes the second electron to an excited state, from where it subsequently tunnels. We show that the electron-momentum distributions exhibit interference maxima and minima due to t…
The single ionization of noble gas atoms by the combined action of XUV attopulses and an infrared laser field is theoretically investigated by means of a non-perturbative model that under certain approximations gives closed-form expressions for the angular distributions of photoelectrons. Interestingly, our model allow us to interpret the angular distributions as two-center interferences where the separation between the centers is governed by the infrared laser field. Angular distributions are compared to the available experimental data showing a good agreement. Finally, we deduce the conditio…
In this work we report ab initio calculations for the $H_2^+$ molecule interacting with ultrashort intense laser pulses. We analyse several observables that can, in principle, be available experimentally, in order to get a deeper understanding of the strong field molecular dynamics. In particular, we will focus our attention to the interplay between electronic and nuclear dynamics and how the two motions are correlated. We have extended the Resolvent Technique to molecules and we have extracted the correlated energy spectra in different regimes of ionization: from the perturbative regime to th…
We report on the fragmentation dynamics of triply charged, diatomic, molecular ions of NO and CO. Dissociative fragmentation after multiple ionization of NO and CO is studied under the impact of 200 keV proton beam using recoil-ion momentum spectrometer. Kinetic Energy Release distributions (KERDs) for various fragmentation channels were obtained. We have also calculated the potential energy curves (PECs) for ground and several excited states of NO^{3+} and CO^{3+} molecular ion. The obtained KERDs are discussed in the background of the calculated PECs as well as the simple Coulomb excitation …
The energies at geometries close to the equilibrium for the e$^+$BeO and e$^+$LiF ground states were computed by means of diffusion Monte Carlo simulations. These results allow us to predict the equilibrium geometries and the vibrational frequencies for these exotic systems,and to discuss their stability with respect to the various dissociation channels. Since the adiabatic positron affinities were found to be smaller than the dissociation energies for both complexes, we propose these two molecules as possible candidates in the challenge to produce and detect stable positron-molecule systems.
Long-range metastable molecules consisting of two cesium atoms in high Rydberg states have been observed in an ultracold gas. A sequential three-photon two-color photoassociation scheme was employed to form these molecules in states which correlate to $np(n+1)s$ dissociation asymptotes. Spectral signatures of bound molecular states are clearly resolved at the positions of avoided crossings between long-range van der Waals potential curves. The experimental results are in agreement with simulations based on a detailed model of the long-range multipole-multipole interactions of Rydberg-atom pair…
We present an implementation of a time-dependent multiconfiguration self-consistent-field (TD-MCSCF) method [R. Anzaki et al., Phys. Chem. Chem. Phys. 19, 22008 (2017)] with the full configuration interaction expansion for coupled electron-nuclear dynamics in diatomic molecules subject to a strong laser field. In this method, the total wave function is expressed as a superposition of different configurations constructed from time-dependent electronic Slater determinants and time-dependent orthonormal nuclear basis functions. The primitive basis functions of nuclei and electrons are strictly in…
We explore the dependence of the double ionization of the He atom on the frequency of a strong laser field while keeping the ponderomotive energy constant. As we increase the frequency we find that the remarkable "finger-like" structure for high momenta recently found for $ω=0.055$ a.u. \cite{Staudte, Rudenko} persists for higher frequencies. At the same time, at $ω=0.187$ a.u. a new X-shape structure emerges for small momenta that prevails in the correlated momenta distribution. The role of this structure as a signature of the frequency dependence of non-sequential double ionization is discus…
Utilizing a benchmark measurement of laser-induced ionization of an H$_2^+$ molecular ion beam target at infrared wavelength around 2 $μ$m, we show that the characteristic two-peak structure predicted for laser-induced enhanced ionization of H$_2^+$ and diatomic molecules in general, is a phenomenon which is confined to a small laser parameter space --- a Goldilocks Zone. Further, we control the effect experimentally and measure its imprint on the electron momentum. We replicate the behavior with simulations, which reproduce the measured kinetic-energy release as well as the correlated-electro…
A possible route to extract electronic and nuclear dynamics from molecular targets with attosecond temporal and nanometer spatial resolution is to employ recolliding electrons as `probes'. The recollision process in molecules is, however, very challenging to treat using {\it ab initio} approaches. Even for the simplest diatomic systems, such as H$_2$, today's computational capabilities are not enough to give a complete description of the electron and nuclear dynamics initiated by a strong laser field. As a consequence, approximate qualitative descriptions are called to play an important role. …
The capability of generating two intense, femtosecond x-ray pulses with controlled time delay opens the possibility of performing time-resolved experiments for x-ray induced phenomena. We have applied this capability to study the photoinduced dynamics in diatomic molecules. In molecules composed of low-Z elements, \textit{K}-shell ionization creates a core-hole state in which the main decay mode is an Auger process involving two electrons in the valence shell. After Auger decay, the nuclear wavepackets of the transient two-valence-hole states continue evolving on the femtosecond timescale, lea…
A simple, analytical, nonrelativistic ionization rate formula for atoms and positive ions in intense ultraviolet and x-ray electromagnetic fields is derived. The rate is valid at arbitrary values of the Keldysh parameter and confirmed by results from ab initio numerical solutions of the single active electron, time-dependent Schroedinger equation. The proposed rate is particularly relevant for experiments employing the new free electron laser (FEL) sources under construction worldwide.
Quasi-static models of barrier suppression have played a major role in our understanding of the ionization of atoms and molecules in strong laser fields. Despite their success, in the case of diatomic molecules these studies have so far been restricted to fields aligned with the molecular axis. In this paper we investigate the locations and heights of the potential barriers in the hydrogen molecular ion in an electric field of arbitrary orientation. We find that the barriers undergo bifurcations as the external field strength and direction are varied. This phenomenon represents an unexpected l…
Recently it was pointed out that transition frequencies in certain diatomic molecules have an enhanced sensitivity to variations in the fine-structure constant $α$ and the proton-to-electron mass ratio $m_p/m_e$ due to a near cancellation between the fine-structure and vibrational interval in a ground electronic multiplet [V.~V.~Flambaum and M.~G.~Kozlov, Phys. Rev. Lett.~{\bf 99}, 150801 (2007)]. One such molecule possessing this favorable quality is silicon monobromide. Here we take a closer examination of SiBr as a candidate for detecting variations in $α$ and $m_p/m_e$. We analyze the rovi…
We study ionization dynamics of aligned diatomic molecules N$_2$ in strong elliptical laser fields experimentally and theoretically. The alignment dependence of photoelectron momentum distributions (PMDs) of N$_2$ measured in experiments is highlighted with comparing to Ar measured synchronously. Our results show that the PMDs of N$_2$ depend strongly on the alignment of the molecule, relative to the main axis of the laser ellipse. In particular, the most-probable electron-emission angle which is often used in attosecond measurement, differs remarkably when changing the molecular alignment. We…
Double ionization of diatomic molecules by short linearly polarized laser pulses is analyzed. We consider the final stage of the ionization process, that is the decay of a highly excited two electron molecule, which is formed after re-scattering. The saddles of the effective adiabatic potential energy close to which simultaneous escape of electrons takes place are identified. Numerical simulations of the ionization of molecules show that the process can be dominated by either sequential or non-sequential events. In order to increase the ratio of non-sequential to sequential ionizations very sh…
We have investigated the coherent phase control on the (3p^{2}) autoionizing state (AIS) resonantly coupled with the ground state for Mg through a two- and a four-photon transition simultaneously, using a bichromatic linearly polarized laser field. The frequency is chosen such that the lasers are tunable around resonance with the transition (3s^{2}(^{1}S^e)\rightarrow 3p^{2}(^{1}S^e)), which implies (ω_{f}=2.11) eV and (ω_{h}=4.22) eV. We are interested in the modification of autoionizing (AI) line shape through the relative phase and laser intensities. A strong phase dependence on the total i…
Diatomic polar molecules are one of the most promising platforms of quantum computing due to their rich internal states and large electric dipole moments. Here, we propose entangling rotational states of adjacent polar molecules via a strong electric dipole-dipole interaction. The splitting of 1.27 kHz between two entangled states is predicted for MgF molecules in an optical tweezer array. The resolution of the entangled states can be achieved in a magic potential for the molecules where the rotational states have the same trap frequencies. The magic potential can be formed by tuning the angle…
A theoretical study of the intense-field single ionization of molecular hydrogen or deuterium oriented either parallel or perpendicular to a linear polarized laser pulse (400 nm) is performed for different internuclear separations and pulse lengths in an intensity range of $(2-13)\times10^{13} $W cm$^{-2}$. The investigation is based on a non-perturbative treatment that solves the full time-dependent Schrödinger equation of both correlated electrons within the fixed-nuclei and the dipole approximation. The results for various internuclear separations are used to obtain the ionization yields of…
Diagonal Born--Oppenheimer correction in strong magnetic fields: finite-difference approach for light diatomic molecules
St. Petersburg State University（圣彼得堡国立大学）；Petersburg Nuclear Physics Institute named after B.P. Konstantinov of National Research Centre ’Kurchatov Institut’（俄罗斯国家研究中心库尔恰托夫研究所所属的以B.P.康斯坦丁诺夫命名的圣彼得堡核物理研究所）
Time-resolved x-ray scattering (TRXS) measures internuclear separations in a molecule following laser-induced photoexcitation. The molecular dynamics induced by the excitation laser may lie on one or several bound or dissociative electronic states. TRXS from these states can be difficult to isolate because they generally overlap in the angle-resolved x-ray scattering pattern $I(x,y,τ)$, where $τ$ is the pump-probe delay and $x,y$ are the physical pixel positions. Here we show how standard transform methods can isolate the dynamics from individual states. We form the temporal Fourier transform,…
For two-electron diatomic molecules, we investigate magnetic field effects in non-sequential double ionization where recollisions prevail. We do so by formulating a three-dimensional semi-classical model that fully accounts for the Coulomb singularities and for magnetic field effects during time propagation. Using this model, we identify a prominent signature of non-dipole effects. Namely, we demonstrate that the recolliding electron back-scatters along the direction of light propagation. Hence, this electron escapes opposite to the direction of change in momentum due to the magnetic field. Th…
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…
Time-delays in the photoionization of molecules are investigated. As compared to atomic ionization, the time-delays expected from molecular ionization present a much richer phenomenon, with a strong spatial dependence due to the anisotropic nature of the molecular scattering potential. We investigate this from a scattering theory perspective, and make use of molecular photoionization calculations to examine this effect in representative homonuclear and hetronuclear diatomic molecules, nitrogen and carbon monoxide. We present energy and angle-resolved maps of the Wigner delay time for single-ph…
The double-slit interference in single-photon ionization of the diatomic molecular ion $\mathrm{H}_2^+$ is theoretically studied beyond the dipole approximation. Via simulating and comparing the interactions of the prealigned $\mathrm{H}_2^+$ and the hydrogen atom with the xuv pulses propagating in different directions, we illustrate two kinds of effects that are encoded in the interference patterns of the photoelectrons from $\mathrm{H}_2^+$: (i) the photon-momentum transfer and (ii) the finite speed of light. While both effects could modify the maxima of the interference fringes, we show tha…
The tunneling model of ionization applies only to longitudinal fields: quasistatic electric fields that do not propagate. Laser fields are transverse: plane wave fields that possess the ability to propagate. Although there is an approximate connection between the effects of longitudinal and transverse fields in a useful range of frequencies, that equivalence fails completely at very low frequencies. Insight into this breakdown is given by an examination of radiation pressure, which is a unique transverse-field effect whose relative importance increases rapidly as the frequency declines. Radiat…
We investigate direct above-threshold ionization in diatomic molecules, with particular emphasis on how quantum interference is altered by a driving field of non-vanishing ellipticity. This interference may be either temporal, i.e., related to ionization events occurring at different times, or spatial, i.e., related to the electron emission at different centers in the molecule. Employing the strong-field approximation and saddle-point methods, we find that, in general, for non-vanishing ellipticity, there will be a blurring of the temporal and spatial interference patterns. The former blurring…
A new mechanism for the production of electron-positron pairs from the interaction of a laser field and a fully stripped diatomic molecule in the tunneling regime is presented. When the laser field is turned off, the Dirac operator has resonances in both the positive and the negative energy continua while bound states are in the mass gap. When this system is immersed in a strong laser field, the resonances move in the complex energy plane: the negative energy resonances are pushed to higher energies while the bound states are Stark shifted. It is argued here that there is a pair production enh…
Calculating the energy absorption of atomic clusters as a function of the laser pulse length $T$ we find a maximum for a critical $T^*$. We show that $T^*$ can be linked to an optimal cluster radius $R^*$. The existence of this radius can be attributed to the enhanced ionization mechanism originally discovered for diatomic molecules. Our findings indicate that enhanced ionization should be operative for a wide class of rare gas clusters. From a simple Coulomb explosion ansatz, we derive an analytical expression relating the maximum energy release to a suitably scaled expansion time which can b…
Accurate molecular imaging via high-order harmonic generation relies on comparing the harmonic emission from a molecule and an adequate reference system. However, an ideal reference atom with the same ionization properties as the molecule does not always exist. We show that for suitably designed, very short laser pulses, a one-to-one mapping between high-order harmonic frequencies and electron momenta in above-threshold ionization exists. Comparing molecular and atomic momentum distributions then provides the electron return amplitude in the molecule for every harmonic frequency. We show that …
In this work, we irradiate a superconducting artificial molecule composed of two coupled tunable transmons with microwave light while monitoring its state via joint dispersive readout. Performing high-power spectroscopy, we observe and identify a variety of single- and multiphoton transitions. We also find that at certain fluxes, the measured spectrum of the system deviates significantly from the solution of the stationary Schrödinger equation with no driving. We reproduce these unusual spectral features by solving numerically the full master equation for a steady-state and attribute them to a…
We present the development and performance of a newly built recoil ion momentum spectrometer to study the fragmentation dynamics of ionized molecules. The spectrometer is based on the two-stage Wiley-McLaren geometry and satisfies both time and velocity focusing conditions. An electrostatic lens has been introduced in the drift region to achieve velocity imaging and higher angular collection. The spectrometer is equipped with a 2D position-sensitive detector with multi-hit coincidence electronics. Ionic fragments with kinetic energy ~ 8 eV can be detected with 4π collection. The overall perfor…
When a diatomic molecule is ionized by an intense laser field, the ionization rate depends very strongly on the inter-nuclear separation. That dependence exhibits a pronounced maximum at the inter-nuclear separation known as the critical distance. This phenomenon was first demonstrated theoretically in H2+ and became known as charge-resonance enhanced ionization (CREI, in reference to a proposed physical mechanism) or simply enhanced ionisation (EI). All theoretical models of this phenomenon predict a double-peak structure in the R-dependent ionization rate of H2+. However, such double-peak st…
Based on the frequency-domain theory, we investigate the above-threshold ionization (ATI) process of an atom in a two-color laser field with infrared (IR) and extreme ultraviolet (XUV) frequencies, where the photon energy of the XUV laser is close to or larger than the atomic ionization threshold. By using the channel analysis, we find that the two laser fields play different roles in an ionization process, where the XUV laser determines the ionization probability by the photon number that the atom absorbs from it, while the IR laser accelerates the ionized electron and hence widens the electr…
Resonances are among the clearest quantum mechanical signatures of scattering processes. Previously, shape resonances and Feshbach resonances have been observed in inelastic and reactive collisions involving atoms or diatomic molecules. Structure in the integral cross section has been observed in a handful of elastic collisions involving polyatomic molecules. The present paper presents the observation of shape resonances in the reactive scattering of a polyatomic molecule, NH3. A merged-beam study of the gas phase He((3)S1) + NH3 Penning ionization reaction dynamics is described in the collisi…
We study the breakup of $\text{H}_2^+$ exposed to super-intense, femtosecond laser pulses with frequencies greater than that corresponding to the ionization potential. By solving the time-dependent Schrödinger equation in an extensive field parameter range, it is revealed that highly nonresonant dissociation channels can dominate over ionization. By considering field-dressed Born-Oppenheimer potential energy curves in the reference frame following a free electron in the field, we propose a simple physical model that characterizes this dissociation mechanism. The model is used to predict contro…
We present a simple exact analytical solution, using the Weyl-Titchmarsh-Kodaira spectral theorem, for the spectral function of the one-dimensional diatomic molecule model consisting of two attractive delta function wells in the presence of a static external electric field. For sufficiently deep and far apart wells, this molecule supports both an even and an odd state, and the introduction of a static electric field turns these bound states into quasi-bound states which are Stark shifted and broadened. The continuum spectrum also inherits an intricate pattern of resonances which reflect the co…
In the recent work of Vanne and Saenz [Phys. Rev. A 75, 063403 (2007)] the quasistatic limit of the velocity gauge strong-field approximation describing the ionization rate of atomic or molecular systems exposed to linearly polarized laser fields was derived. It was shown that in the low-frequency limit the ionization rate is proportional to the laser frequency (for a constant intensity of the laser field). In the present work I show that for circularly polarized laser fields the ionization rate is proportional to higher powers of the laser frequency for hydrogenic atoms. The new analytical ex…
We discuss the frequency and visibility of atom-molecule Ramsey fringes observed in recent experiments by Claussen et al.[Phys. Rev. A 67, 060701 (2003)]. In these experiments a 85Rb Bose-Einstein condensate was exposed to a sequence of magnetic field pulses on the high field side of the 155 G Feshbach resonance. The observed oscillation frequencies largely agree with the theoretically predicted magnetic field dependence of the binding energy of the highest excited diatomic vibrational state, except for a small region very close to the singularity of the scattering length. Our analytic treatme…
Angular distribution of photoelectrons released by the ionization of randomly-oriented molecules with two laser fields of carrier frequencies $ω$ and $2ω$, which are linearly polarized in two mutually-orthogonal directions, is analyzed in the perturbation limit for the case of one- vs two-photon ionization process. In particular, we focus on the recently predicted [Ph.V. Demekhin {\it et al.}, Phys. Rev. Lett. \textbf{121}, 253201 (2018)] forward-backward asymmetry in the photoelectron emission, which is induced by the interference of two fields and depends on the external relative phase betwe…
The quasistatic limit of the velocity-gauge strong-field approximation describing the ionization rate of atomic or molecular systems exposed to linear polarized laser fields is derived. It is shown that in the low-frequency limit the ionization rate is proportional to the laser frequency, if a Coulombic long-range interaction is present. An expression for the corresponding proportionality coefficient is given. Since neither the saddle-point approximation nor the one of a small kinetic momentum is used in the derivation, the obtained expression represents the exact asymptotic limit. This result…
The phenomenon of spatial (polar) asymmetry of produced photoelectron emission due to strong-field multiphoton process of above-threshold ionization (ATI) in atoms irradiated by a linearly polarized two-color (bichromatic) laser field consisting of coherent superposition of two commensurate harmonics (of frequencies and is considered and studied theoretically. The problem is addressed within the conventional strong-field approximation (SFA) in standard velocity gauge (VG) formulation under condition of arbitrary value of the so-called Keldysh parameter $γ$ , including both the multiphoton (for…
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…
