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 integration over the transverse momenta for a small range of alignment angles, and are sharpest for parallel-aligned molecules. Due to the contributions of transverse-momentum components, these patterns become less defined as the alignment angle increases, until they disappear for perpendicular alignment. This behavior influences the shapes and the peaks of the electron momentum distributions.
Using a classical ensemble method, nonsequential double ionization is predicted to exist with elliptical and circular polarization. Recollision is found to be the underlying mechanism and it is only possible via elliptical trajectories.
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…
The influence of electron-electron Coulomb repulsion on nonsequential double ionization of rare-gas atoms is investigated. Several variants of the quantum-mechanical transition amplitude are evaluated that differ by the form of the inelastic electron-ion rescattering and whether or not Coulomb repulsion between the two electrons in the final state is included. For high laser intensity, an entirely classical model is formulated that simulates the rescattering scenario.
Nonsequential two-photon ionization of inner-shell $np$ subshell of neutral atoms by circularly polarized light is investigated. Detection of subsequent fluorescence as a signature of the process is proposed and the dependence of fluorescence degree of polarization on incident photon beam energy is studied. It is generally expected that the degree of polarization remains approximately constant, except when the beam energy is tuned to an intermediate $n's$ resonance. However, strong unexpected change in the polarization degree is discovered for nonsequential two-photon ionization at specific in…
We show through simulation that quantum interference in non-sequential double ionization can be used to control the recollision with subsequent ionization (RESI) mechanism. This includes the shape, localization and symmetry of RESI electron-momentum distributions, which may be shifted from a correlated to an anti-correlated distribution or vice versa, far below the direct ionization threshold intensity. As a testing ground, we reproduce recent experimental results by employing specific coherent superpositions of excitation channels. We examine two types of interference, from electron indisting…
We investigate differential electron distributions in nonsequential double ionization (NSDI) with linearly polarized, few-cycle pulses, using a classical model based on a laser-assisted inelastic $(e^-,2e^-)$ rescattering mechanism. We show that these yields, as functions of the momentum components parallel to the laser polarization, are highly asymmetric, and strongly influenced by the absolute phase, i.e., the phase difference between the carrier oscillation of a few-cycle laser pulse and its envelope. Indeed, around a critical phase, such distributions change their sign in a radical fashion…
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…
We examine correlated electron and doubly charged ion momentum spectra from strong field double ionization of Neon employing intense elliptically polarized laser pulses. An ellipticity-dependent asymmetry of correlated electron and ion momentum distributions has been observed. Using a 3D semiclassical model, we demonstrate that our observations reflect the sub-cycle dynamics of the recollision process. Our work reveals a general physical picture for recollision-impact double ionization with elliptical polarization, and demonstrates the possibility of ultrafast control of the recollision dynami…
We perform a systematic analysis of quantum interference in nonsequential double ionization focusing on the recollision-excitation with subsequent ionization (RESI) mechanism, employing the strong-field approximation (SFA). We find that interference has a major influence on the shape, localization and symmetry of the correlated electron momentum distributions. In particular, the fourfold symmetry with regard to the parallel momentum components observed in previous SFA studies is broken. Two types of interference are observed and thoroughly analyzed, namely that caused by electron indistinguish…
We examine the nature and statistical properties of electron-electron collisions in the recollision process in a strong laser field. The separation of the double ionization yield into sequential and nonsequential components leads to a bell-shaped curve for the nonsequential probability and a monotonically rising one for the sequential process. We identify key features of the nonsequential process and connect our findings in a simplified model which reproduces the knee shape for the probability of double ionization with laser intensity and associated trends.
We investigate laser induced nonsequential multiple ionization using a simple statistical model in which an electron recollides inelastically with its parent ion. In this collision, it thermalizes with the remaining $N-1$ bound electrons within a time interval $Δt$. Subsequently, all the $N$ electrons leave. We address the question of how the above time delays influence the individual contributions from the orbits in which the first electron, upon return, is accelerated or decelerated by the field, respectively, to the ion momentum distributions. In both cases, the time delays modify the drift…
The role of nucleus in strong-field nonsequential double ionization of Ar atoms is investigated using three-dimensional classical ensembles. By adjusting the nuclear Coulomb potential, we can excellently reproduce the experimental correlated electron and ion momentum spectra with laser intensities above the recollision threshold [Phys. Rev. Lett. 93, 263001 (2004)] and below the recollision threshold [Phys. Rev. Lett. 101, 053001 (2008)] quantitatively. Analysis reveals the detailed electronic dynamics when the nuclear Coulomb attraction plays a key role in the recollision process of nonsequen…
We develop an approximate model for the process of direct (nonsequential) two-photon double ionization of atoms. Employing the model, we calculate (generalized) total cross sections as well as energy-resolved differential cross sections of helium for photon energies ranging from 39 to 54 eV. A comparison with results of \textit{ab initio} calculations reveals that the agreement is at a quantitative level. We thus demonstrate that this complex ionization process is fully described by the simple model, providing insight into the underlying physical mechanism. Finally, we use the model to calcula…
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…
We investigate the physical processes in which an electron, upon return to its parent ion, promotes a second electron to an excited state, from which it subsequently tunnels. Employing the strong-field approximation and saddle-point methods, we perform a detailed analysis of the dynamics of the two electrons, in terms of quantum orbits, and delimit constraints for their momentum components parallel to the laser-field polarization. The kinetic energy of the first electron, upon return, exhibits a cutoff slightly lower than $10U_p$, where $U_p$ is the ponderomotive energy, as in rescattered abov…
We perform a detailed analysis of the importance of causality within the strong-field approximation and the steepest descent framework for the recollision-excitation with subsequent tunneling ionization (RESI) pathway in laser-induced nonsequential double ionization (NSDI). In this time-delayed pathway, an electron returns to its parent ion, and, by recolliding with the core, gives part of its kinetic energy to excite a second electron at a time $t^{\prime}$. The second electron then reaches the continuum at a later time $t$ by tunneling ionization. We show that, if $t^{\prime}$ and $t$ are co…
We perform a detailed analysis of the recollision-excitation-tunneling (RESI) mechanism in laser-induced nonsequential double ionization (NSDI), in which the first electron, upon return, promotes a second electron to an excited state, from which it subsequently tunnels, based on the strong-field approximation. We show that the shapes of the electron momentum distributions carry information about the bound-state with which the first electron collides, the bound state to which the second electron is excited, and the type of electron-electron interaction. Furthermore, one may define a driving-fie…
We investigate laser-induced nonsequential double ionization by a polarization-gated laser pulse, constructed employing two counter-rotating circularly polarized few cycle pulses with a time delay $T_{d}$. We address the problem within a classical framework, and mimic the behavior of the quantum-mechanical electronic wave packet by means of an ensemble of classical electron trajectories. These trajectories are initially weighted with the quasi-static tunneling rate, and with suitably chosen distributions for the momentum components parallel and perpendicular to the laser-field polarization, in…
We have investigated the energy correlation of the two electrons from nonsequential double ionization of helium atom in 800 nm laser fields at intensities below the recollision threshold by quantum calculations. The circular arcs structure of the correlated electron momentum spectra reveals a resonant double ionization process in which the two electrons transit from doubly excited states into continuum states by simultaneously absorbing and sharing excess energy in integer units of the photon energy. Coulomb repulsion between the two electrons in continuum states is responsible for the dominan…
With quantum calculations, we have investigated the multiphoton nonsequential double ionization of helium atoms in intense laser fields at ultraviolet wavelengths. Very surprisingly, we find a so-far unobserved double-circle structure in the correlated electron momentum spectra. The double-circle structure essentially reveals multiphoton Rabi oscillations of two electrons, which are strongly supported by the oscillating population of a certain doubly excited state and by the oscillating double ionization signals. This two-electron multiphoton Rabi effect provides profound understandings of ele…
We address nonsequential double ionization induced by strong, linearly polarized laser fields of only a few cycles, considering a physical mechanism in which the second electron is dislodged by the inelastic collision of the first electron with its parent ion. The problem is treated classically, using an ensemble model, and quantum-mechanically, within the strong-field and uniform saddle-point approximations. In the latter case, the results are interpreted in terms of "quantum orbits", which can be related to the trajectories of a classical electron in an electric field. We obtain highly asymm…
We perform a systematic analysis of how nonsequential double ionization in intense, linearly polarized laser fields is influenced by the initial states in which both electrons are bound, and by the residual ionic potential. We assume that the second electron is released by electron-impact ionization of the first electron with its parent ion, using an S-Matrix approach. We work within the Strong-Field Approximation, and compute differential electron momentum distributions using saddle-point methods. Specifically, we consider electrons in $1s$, $2p$, $3p$ and localized states, which are released…
Nonsequential double ionization (NSDI) of helium in an intense few-cycle laser pulse is investigated by applying the three-dimensional semi-classical re-scattering method. It is found that the momentum distribution of He$^{2+}$ shows a single-double-single peak structure as the pulse intensity increases. According to the different mechanisms dominating the NSDI process, the laser intensity can be classified into three regimes where the momentum distribution of He$^{2+}$ exhibits different characteristics. In the relatively high intensity regime, an NSDI mechanism named the "laser-assisted coll…
It is generally believed that the recollision mechanism of atomic nonsequential double ionization is suppressed in circularly polarized laser fields because the returning electron is unlikely to encounter the core. On the contrary, we find that recollision can and does significantly enhance double ionization, even to the extent of forming a "knee", the signature of the nonsequential process. Using a classical model, we explain two apparently contradictory experiments, the absence of a knee for helium and its presence for magnesium.
For the description of nonsequential double ionization (NSDI) of rare-gas atoms by a strong linearly polarized laser field, the quantum-mechanical $S$-matrix diagram that incorporates rescattering impact ionization is evaluated in the strong-field approximation. We employ a uniform approximation, which is a generalization of the standard saddle-point approximation. We systematically analyze the manifestations of the electron-electron interaction in the momentum distributions of the ejected electrons: for the interaction, by which the returning electron frees the bound electron, we adopt either…
We analyze two-photon double ionization of helium in both the nonsequential and sequential regime. We show that the energy spacing between the two emitted electrons provides the key parameter that controls both the energy and the angular distribution and reveals the universal features present in both the nonsequential and sequential regime. This universality, i.e., independence of photon energy, is a manifestation of the continuity across the threshold for sequential double ionization. For all photon energies, the energy distribution can be described by a universal shape function that contains…
In a fully classical simulation, we investigate the recollision mechanism of non-sequential double ionization (NSDI) and its manifestation in the end-of-pulse electron momentum distributions. We compare two different electron-electron potentials: a soft-core Coulombic potential and a Yukawa potential. We also implement the strong-field approximation (SFA), which is commonly made in quantum-mechanical $S$-matrix calculations, in our classical simulations and study its consequences. We find that, regardless of the form of the e-e potential, the SFA modifies the momentum distributions and recolli…
Consensus has been reached that recollision, as the most important post-tunneling process, is responsible for nonsequential double ionization process in intense infrared laser field, however, its effect has been restricted to interaction between the first ionized electron and the residual univalent ion so far. Here we identify the key role of recollision between the second ionized electron and the divalent ion in the below-threshold nonsequential double ionization process by introducing a Coulomb-corrected quantum-trajectories method, which enables us to well reproduce the experimentally obser…
We present accurate time-dependent ab initio calculations on fully differential and total integrated (generalized) cross sections for the nonsequential two-photon double ionization of helium at photon energies from 40 to 54 eV. Our computational method is based on the solution of the time-dependent Schroedinger equation and subsequent projection of the wave function onto Coulomb waves. We compare our results with other recent calculations and discuss the emerging similarities and differences. We investigate the role of electronic correlation in the representation of the two-electron continuum …
We perform theoretical investigations of laser-induced nonsequential double ionization with few cycle pulses, with particular emphasis on the dependence of the electron-momentum distributions on the carrier-envelope phase. We focus on the recollision-excitation with subsequent tunneling ionization (RESI) pathway, in which a released electron, upon return to its parent ion, gives part of its kinetic energy to promote a second electron to an excited state. At a subsequent time, the second electron is freed through tunneling ionization. We show that the RESI electron-momentum distributions vary d…
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 mo…
Recently introduced time-dependent renormalized natural orbital theory (TDRNOT) is tested on non-sequential double ionization (NSDI) of a numerically exactly solvable one-dimensional model He atom subject to few-cycle, 800-nm laser pulses. NSDI of atoms in strong laser fields is a prime example of non-perturbative, highly correlated electron dynamics. As such, NSDI is an important "worst-case" benchmark for any time-dependent few and many-body technique beyond linear response. It is found that TDRNOT reproduces the celebrated NSDI "knee," i.e., a many-order-of-magnitude enhancement of the doub…
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…
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…
The ionization of a one-dimensional model Helium atom in short laser pulses using time-dependent density functional theory is investigated. We calculate ionization probabilities as a function of laser intensity by approximating the correlation function of the system adiabatically with an explicit dependence on the fractional number of bound electrons. For the correlation potential we take the derivative discontinuity at integer numbers of bound electrons explicitly into account. This approach reproduces ionization probabilities from the solution of the time-dependent Schroedinger equation, in …
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 theoretically study frustrated double ionization (FDI) of atoms subjected to intense circularly polarized laser pulses using a three-dimensional classical model. We find a novel "knee" structure of FDI probability as a function of intensity, which is similar to the intensity dependence of nonsequential double ionization probability. The observation of FDI is more favourable when using targets with low ionization potentials and short driving laser wavelengths. This is attributed to the crucial role of recollision therein, which can be experimentally inferred from the photoelectron momentum d…
We demonstrate kinematically complete measurements on frustrated double ionization of argon atoms in strong laser fields with a reaction microscope. We found that the electron trapping probability after strong field double ionization is much higher than that after strong field single ionization, especially in case of high laser intensity. The retrieved electron momentum distributions of frustrated double ionization show a clear transition from the nonsequential to the sequential regime, similar to those of strong field double ionization. The dependence of electron momentum width on the laser i…
Quantum calculations of a 1+1-dimensional model for double ionization in strong laser fields are used to trace the time evolution from the ground state through ionization and rescattering to the two electron escape. The subspace of symmetric escape, a prime characteristic of nonsequential double ionization, remains accessible by a judicious choice of 1-d coordinates for the electrons. The time resolved ionization fluxes show the onset of single and double ionization, the sequence of events during the pulse, and the influences of pulse duration, and reveal the relative importance of sequential …
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.
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…
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…
A second plateau in the harmonic spectra of laser-driven two-electron atoms is observed both in the numerical solution of a low-dimensional model helium atom and using an extended strong field approximation. It is shown that the harmonics well beyond the usual cut-off are due to the simultaneous recombination of the two electrons, which were emitted during different, previous half-cycles. The new cut-off is explained in terms of classical trajectories. Classical predictions and the time-frequency analysis of the ab initio quantum results are in excellent agreement. The mechanism corresponds to…
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 …
Using a three-dimensional semiclassical method, we theoretically investigate frustrated double ionization (FDI) of Ar atoms subjected to strong laser fields. The double-hump photoelectron momentum distribution generated from FDI observed in a recent experiment [S. Larimian et al., Phys. Rev. Research 2, 013021 (2020)] is reproduced by our simulation. We confirm that the observed spectrum is due to recollision. The laser intensity dependence of FDI is investigated. We reveal that the doubly excited states of Ar atoms and excited states of Ar+ are the dominant pathways for producing FDI at relat…
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 describe first-principles in-plane calculations of non-sequential triple ionization (NSTI) of atoms in a linearly polarized intense laser pulse. In a fully classically correlated description, all three electrons respond dynamically to the nuclear attraction, the pairwise e-e repulsions and the laser force throughout the duration of a 780nm laser pulse. Nonsequential ejection is shown to occur in a multi-electron, possibly multi-cycle and multi-dimensional, rescattering sequence that is coordinated by a number of sharp transverse recollimation impacts.
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…
