Multielectron double ionization with elliptically polarized light is examined theoretically using a classical ensemble method going beyond the single-active-electron approximation. A knee structure in the ion signal is found. Our analysis provides an explanation for newly observed SDI phenomena.
We present theoretical calculations of orientation-dependent total ionization yields from the highest occupied molecular orbitals of the oriented OCS molecule by solving the time-dependent Schrödinger equation in three dimensions. The calculations were performed within the single-active-electron approximation including multielectron polarization. The multielectron polarization term was represented by an induced dipole term which contains the polarizability of the OCS + cation parallel to the laser polarization. Upon accounting for multielectron polarization, the calculated total ionization yie…
We revisit strong-field ionization of aligned O$_2$, CO$_2$, and CS$_2$ molecules in light of recent advances in the field of strong-field physics, in particular the inclusion of multielectron polarization in the numerical solution of the time-dependent Schr{ö}dinger equation (TDSE) within the singe-active-electron approximation. Upon inclusion of multielectron polarization and the associated induced dipole potential in the TDSE model, we obtain angular distributions of total ionization yields which are in better agreement with the available experimental results for CO$_2$ and CS$_2$. For the …
We extend the semiclassical two-step model [Phys. Rev. A 94, 013415 (2016)] to include a multielectron polarization-induced dipole potential. Using this model we investigate the imprints of multielectron effects in the momentum distributions of photoelectrons ionized by a linearly polarized laser pulse. We predict narrowing of the longitudinal momentum distributions due to electron focusing by the induced dipole potential. We show that the polarization of the core also modifies interference structures in the photoelectron momentum distributions. Specifically, the number of fanlike interference…
We discuss the mechanism by which the inclusion of multielectron polarization improves the solution of the time-dependent Schrödinger equation (TDSE) for the oriented CO molecule in a strong external laser pulse within the single-active-electron (SAE) approximation. A challenging problem of using the SAE approximation is that the active electron, instead of undergoing ionization, may be driven by the external field to lower-lying orbitals. For the oriented CO molecule, dipole coupling to the lower-lying bound states of the potential depends on the orientation angle, thereby affecting the orien…
We present a novel approach to calculating strong field ionization dynamics of multielectron molecular targets. Adopting a multielectron wavefunction ansatz based on field-free ab initio neutral and ionic multielectron states, a set of coupled time-dependent single-particle Schroedinger equations describing the neutral amplitude and continuum electron are constructed. These equations, amenable to direct numerical solution or further analytical treatment, allow one to study multielectron effects during strong field ionization, recollision, and high harmonic generation. We apply the method to st…
We report fully differential photoelectron spectra from an {\it ab-inito} coupled channels treatment of CO$_2$. Photoionization by laser pulses centered at 400 nm and 800 nm wavelength are considered, with arbitrary molecular alignment and polarization (linear and elliptic). Calculations reveal significant excited state channel contributions that are, at certain molecular orientations, an order of magnitude larger than the ground state channel in the rescattering plateau. Partial wash out of the multiphoton structure in the ATI spectra and of the nodal features in angle resolved spectra is obs…
Multiple electron processes occur widely in atoms, molecules, clusters, and condensed matters when they are interacting with energetic particles or intense laser fields. In this work, a unified and accurate theoretical formalism is proposed on the direct multielectron processes of atoms including the multiple Auger decay and multiple ionization by an impact of an energetic electron or a photon based on the atomic collision theory described by a correlated many-body Green's function. Such a practical treatment is made possible due to different coherence features of the particles (matter waves) …
We solve the hydrodynamic-ballistic equations of motion for a one-dimensional time-dependent Thomas-Fermi model of Cl_2 exposed to an intense subpicosecond laser field, and observe simultaneous multielectron ionization and molecular dissociation. The fragment kinetic energy defect with respect to the simple Coulomb explosion picture is found to originate in ejected-electron screening of the escaping fragments; its magnitude agrees with that observed in recent experiments.
We consider the final stage of multiple ionization of atoms in a strong linearly polarized laser field within a classical model. We propose that non-sequential multiple ionization is dominated by symmetric escape from a highly excited intermediate complex. For a configuration of N electrons with C_Nv symmetry in a plane perpendicular to the electric field we analyze the classical motion in phase space and discuss the final momentum distribution parallel and perpendicular to the polarization axis. The results are in good agreement with recent experiment of multiple ionization in Ne.
High harmonic spectroscopy has the potential to combine attosecond temporal with sub-Angstrom spatial resolution of the early nuclear and multielectron dynamics in molecules. It involves strong field ionization of the molecule by the IR laser field followed by time-delayed recombination of the removed electron with the molecular ion. The time-delay is controlled on the attosecond time scale by the oscillation of the IR field and is mapped into the harmonic number, providing a movie of molecular dynamics between ionization and recombination. One of the challenges in the analysis of high harmoni…
Carrier envelope phase (CEP) stabilized 5 fs and 22 fs pulses of intense 800 nm light are used to probe the strong-field ionization dynamics of multielectron entities, xenon and carbon disulfide. We compare ion yields obtained with and without CEP-stabilization: with 8-cycle (22 fs) pulses, Xe$^{6+}$ yields are suppressed (relative to Xe$^+$ yields) by between 30% and 50%, depending on phase, reflecting the phase dependence of non-sequential ionization and its contribution to the formation of higher charge states. On the other hand, ion yields for Xe$^{q+}$ ($q$=2-4) with CEP-stablized pulses …
Visualizing intense laser field driven electron dynamics in a multielectron molecule: dynamic electron localization, bonding properties and multiple ionization bursts
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.
Direct evidence for projectile electronic structure effects in slow multielectron capture collisions
Indian Institute of Science Education and Research Pune(印度科学教育研究所浦那分校);Université Caen Normandie, ENSICAEN, CNRS, CEA, Normandie Univ., CIMAP UMR6252(卡昂诺曼底大学,ENSICAEN,法国国家科学研究中心,法国原子能和替代能源委员会,诺曼底大学,CIMAP联合研究实验室)
The degree of elliptical polarization of intense short laser pulses is shown to be related to the timing of strong-field non-sequential double ionization. Higher ellipticity is predicted to force the initiation of double ionization into a narrower time window, and this "pins" the ionizing field strength in an unexpected way, leading to the first experimentally testable formula for double ionization probability as a function of ellipticity.
We predict new end-of-pulse behavior in high-field atomic double ionization. Calculations of atomic electron trajectories in short intense laser pulses confirm our analysis of elliptical polarization. We exhibit a four-band structure in ion momentum distributions under various ellipticities, and predict that sequential and non-sequential double ionization can be cleanly distinguished under elliptical polarization.
Important information about strong-field atomic or molecular ionization can be missed when using linearly polarized laser fields. The field strength at which an electron was ionized, or the time during a pulse of the ionization event are examples of such missing information. In treating single, double, and triple ionization events we show that information of this kind is made readily available by use of elliptical polarization.
Elliptical dichroism is known in atomic photoionization as the difference in the photoelectron angular distributions produced in nonlinear ionization of atoms by left- and right-handed elliptically polarized light. We theoretically demonstrate that the maximum dichroism |Δ_{ED}|=1 always appears in two-photon ionization of any atom if the photon energy is tuned in so that the electron emission is dominantly determined by two intermediate resonances. We propose the two-photon ionization of atomic helium in order to demonstrate this remarkable phenomenon. The maximum elliptical dichroism could b…
We join the tribute to Professor N.B. Delone in this memorial issue by presenting the results of new calculations on the effects of ellipticity on double ionization by short and strong near-optical laser pulses.
Based on the strong-field approximation, we obtain analytical expressions for the initial momentum at the tunnel exit and instantaneous ionization rate of tunneling ionization in elliptically polarized laser fields with arbitrary ellipticity. The tunneling electron reveals a nonzero offset of the initial momentum at the tunnel exit in the elliptically polarized laser field. We find that the transverse and longitudinal components of this momentum offset with respect to the instantaneous field direction are directly related to the time derivatives of the instantaneous laser electric field along …
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 investigate the strong-field ionization of atomic hydrogen in a few-cycle elliptically polarized infrared pulse by solving the time-dependent Schrödinger equation. The dependence of the photoelectron momentum distribution on the pulse intensity, ellipticity, length, envelope, and carrier envelope phase is analyzed. In particular, we explain the variation of the electron offset angle with asymptotic electron energy through the combined action of the field and the Coulomb potential, and demonstrate that low-ellipticity pulses make it possible to access the electron release time.
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 …
We numerically study models of $\mathrm{H}_2$ and $\mathrm{LiH}$ molecules, aligned collinearly with the linear polarization of the external field, to elucidate the possible role of correlation in the enhanced-ionization phenomena. Correlation is considered at different levels of approximation with the time-dependent generalized-active-space configuration-interaction method. The results of our studies show that enhanced ionization occurs in multielectron molecules, that correlation is important and they also demonstrate significant deviations between the results of the single-active-electron a…
Employing recent developed magneto-optical trap recoil ion momentum spectroscopy (MOTRIMS) combining cold atom, strong laser pulse, and ultrafast technologies, we study momentum distributions of the multiply ionized cold rubidium (Rb) induced by the elliptically polarized laser pulses (35 fs, $1.3 \times 10^{15}$ W/cm$^2$). The complete vector momenta of Rbn+ ions up to charge state n = 4 are recorded with extremely high resolution (0.12 a.u. for Rb$^+$). Variations of characteristic multi-bands displayed in momentum distributions, as the ellipticity varies from the linear to circular polariza…
We report the formulation of a new, cost-effective approximation method in the time-dependent optimized coupled-cluster (TD-OCC) framework [T. Sato et al., J. Chem. Phys. 148, 051101 (2018)] for first-principles simulations of multielectron dynamics in an intense laser field. The method, designated as TD-OCCD(T), is a time-dependent, orbital-optimized extension of the "gold-standard" CCSD(T) method in the ground-state electronic structure theory. The equations of motion for the orbital functions and the coupled-cluster amplitudes are derived based on the real-valued time-dependent variational …
An improved quantum trajectory Monte Carlo method involving the Stark shift of the initial state, Coulomb potential, and multielectron polarization-induced dipole potential is used to revisit the origin of the low-energy interference structure in the photoelectron momentum distribution of the xenon atom subjected to an intense laser field, and resolve the different contributions of these three effects. In addition to the well-studied radial finger-like interference structure, a ring-like interference structure induced by interference among electron wave packets emitted from multi-cycle time wi…
It is well-known from numerical and experimental results that the fraction of Rydberg states (excited neutral atoms) created by tunnel ionization declines dramatically with increasing ellipticity of laser light. We present a method to analyze this dependence on ellipticity, deriving a probability distribution of Rydberg states that agrees closely with recent experimental [1] and numerical results. In particular, contradicting the existing proposed mechanism [1] and general expectations, our results indicate that the dependence of Rydberg yield on laser ellipticity is not caused by a rescatteri…
We study static-field ionization of He-like ions with nuclear charge number in the range of $2\le Z \le 36$. Both the tunneling and over-the-barrier regimes are considered. We calculate the ionization rates by three approximate methods: a fitting formula based on the Perelemov-Popov-Terent'ev (PPT) formula, a perturbative expansion in powers of $1/Z$, and a single-active electron approximation, and compare them with reference ionization rates computed by the multiconfiguration time-dependent Hartree-Fock (MCTDHF) approach. The relative deviation of the rates computed by the PPT-based fitting f…
A general model and toolkit for the ionization of three or more electrons in strongly driven molecules using an effective Coulomb potential for the interaction between bound electrons
The sub-cycle dynamics of electrons driven by strong laser fields is central to the emerging field of attosecond science. We demonstrate how the dynamics can be probed through high-order harmonic generation, where different trajectories leading to the same harmonic order are initiated at different times, thereby probing different field strengths. We find large differences between the trajectories with respect to both their sensitivity to driving field ellipticity and resonant enhancement. To accurately describe the ellipticity dependence of the long trajectory harmonics we must include a sub-c…
Strong-field ionization and rescattering beyond the long-wavelength limit of the dipole approximation is studied with elliptically polarized mid-IR pulses. We have measured the full three-dimensional photoelectron momentum distributions (3D PMDs) with velocity map imaging and tomographic reconstruction. The ellipticity-dependent 3D-PMD measurements revealed an unexpected sharp, thin line-shaped ridge structure in the polarization plane for low momentum photoelectrons. With classical trajectory Monte Carlo (CTMC) simulations and analytical methods we identified the associated ionization dynamic…
The role of Coulomb focusing in above-threshold ionization in an elliptically polarized mid-infrared strong laser field is investigated within a semiclassical model incorporating tunneling and Coulomb field effects. It is shown that Coulomb focusing up to moderate ellipticity values is dominated by multiple forward scattering of the ionized electron by the atomic core that creates a characteristic low-energy structure in the photoelectron spectrum and is responsible for the peculiar energy scaling of the ionization normalized yield along the major polarization axis. At higher ellipticities, th…
Relativistic tunnel ionization of atoms by intense, elliptically polarized light is considered. The relativistic version of the Landau-Dykhne formula is employed. The general analytical expression is obtained for the relativistic photoelectron spectra. The most probable angle of electron emission, the angular distribution near this angle, the position of the maximum and the width of the energy spectrum are calculated. In the weak field limit we obtain the familiar non-relativistic results. For the case of circular polarization our analytical results are in agreement with recent derivations of …
We study the formation of highly excited neutral atoms during the break-up of strongly-driven molecules. Past work on this significant phenomenon has shown that during the formation of highly excited neutral atoms ($\mathrm{H^{*}}$) during the break-up of H$_{2}$ in a linear laser field the electron that escapes does so either very quickly or after remaining bound for a few periods of the laser field. Here, we address the electron-nuclear dynamics in $\mathrm{H^{*}}$ formation in elliptical laser fields, through Coulomb explosion. We show that with increasing ellipticity two-electron effects a…
We have performed classical trajectory Monte Carlo (CTMC) studies of electron capture and ionization in multiply charged (Q=8) ion-Rydberg atom collisions at intermediate impact velocities. Impact parallel to the minor and to the major axis, respectively, of the initial Kepler electron ellipse has been investigated. The important role of the initial electron momentum distribution found for singly charged ion impact is strongly disminished for higher projectile charge, while the initial spatial distribution remains important for all values of Q studied.
We describe an ab initio and non-perturbative $R$-matrix with time-dependence theory for ultrafast atomic processes in light fields of arbitrary polarization. The theory is applicable to complex, multielectron atoms and atomic ions subject to ultrashort (particularly few-femtosecond and attosecond) laser pulses with any given ellipticity, and generalizes previous time-dependent $R$-matrix techniques restricted to linearly polarized fields. We discuss both the fundamental equations, required to propagate the multielectron wavefunction in time, as well as the computational developments necessary…
We employ a recently developed three-dimensional semiclassical model to identify nondipole effects in triple ionization of Ne driven by infrared laser pulses at intensities where electron-electron correlation prevails. This model fully accounts for the Coulomb interaction of each electron with the core and avoids artificial autoionization by employing effective Coulomb potentials to describe the interaction between bound electrons (ECBB). Using the ECBB model, we identify a prominent signature of nondipole effects. Namely, the component along the direction of light propagation of the average s…
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…
RMT is a program which solves the time-dependent Schrodinger equation for general, multielectron atoms, ions and molecules interacting with laser light. As such it can be used to model ionization (single-photon, multi-photon and strong-field), recollision (high-harmonic generation, strong-field rescattering), and more generally absorption or scattering processes with a full account of the multielectron correlation effects in a time-dependent manner. Calculations can be performed for targets interacting with ultrashort, intense laser pulses of long-wavelength and arbitrary polarization. Calcula…
We take advantage of the information provided by use of elliptical polarization in a recent two-electron release time experiment [A.N. Pfeiffer et al., Nature Physics 7, 428 (2011)]. This allows a comparative test of the currently dominant conjectures regarding independent-electron tunneling theory vs. fully electron-correlated classical release theory to describe electron release in strong-field double ionization.
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…
We provide theoretical investigations of the response of the Ar and H atoms to an intense elliptically polarized few-cycle laser pulse, as a function of light ellipticity. The time-dependent Schr{ö}dinger equation describing the least-bound electron is solved numerically, and differential quantities such as the momentum distribution, the electron density in the continuum, and the above-threshold ionization spectra are computed. These quantities provide insight into the ionization dynamics and the electron rescattering process as a function of light ellipticity, and reveal great similarities be…
With a classical ensemble model that including electron correlations during the whole ionization process, we investigated strong-field sequential double ionization of Ar by elliptically polarized pulses at the quantitative level. The experimentally observed intensity-dependent three-band or four-band structures in the ion momentum distributions are well reproduced with this classical model. More importantly, the experimentally measured ionization time of the second electrons [A. N. Pfeiffer et al., Nature Phys. 7, 428 (2011)], which can not be predicted by the standard independent-electron mod…
The total ionization rate of biharmonic ($ω+ 3ω$) ionization is studied within the independent particle approximation and the third order perturbation theory. Particular attention is paid to how the polarization of the biharmonic light field affects the total rate. The ratios of the biharmonic ionization rates for linearly and circularly polarized beams as well as for corotating and counterrotating elliptically polarized beams are analyzed, and how they depend on the beam parameters, such as photon frequency or phase between $ω$ and $3ω$ light beams. We show that the interference of the biharm…
We study ionization of aligned H$_2^+$ in strong elliptically-polarized laser fields numerically and analytically. The calculated offset angle in photoelectron momentum distribution is several degrees larger for the molecule than a model atom with similar ionization potential at diverse laser parameters. Using a strong-field model that considers the properties of multi-center and single-center Coulomb potentials, we are able to quantitatively reproduce this angle difference between the molecule and the atom. Further analyses based on this model show that the response time of electron to light …
Using a three-dimensional semiclassical model, we study double ionization for strongly-driven He fully accounting for magnetic field effects. For linearly and slightly elliptically polarized laser fields, we show that recollisions and the magnetic field combined act as a gate. This gate favors more transverse - with respect to the electric field - initial momenta of the tunneling electron that are opposite to the propagation direction of the laser field. In the absence of non-dipole effects, the transverse initial momentum is symmetric with respect to zero. We find that this asymmetry in the t…
We perform high-resolution measurements of momentum distribution on Rb$^{n+}$ recoil ions up to charge state $n=4$, where laser-cooled rubidium atoms are ionized by femtosecond elliptically polarized lasers with the pulse duration of 35 fs and the intensity of 3.3$\times$10$^{15}$ W/cm$^2$ in the over-barrier ionization (OBI) regime. The momentum distributions of the recoil ions are found to exhibit multi-band structures as the ellipticity varies from the linear to circular polarizations. The origin of these band structures can be explained quantitatively by the classical OBI model and dedicat…
Increasing ellipticity usually suppresses the recollision probability drastically. In contrast, we report on a recollision channel with large return energy and a substantial probability, regardless of the ellipticity. The laser envelope plays a dominant role in the energy gained by the electron, and in the conditions under which the electron comes back to the core. We show that this recollision channel eciently triggers multiple ionization with an elliptically polarized pulse.
A recent paper reported elliptically polarized high-order harmonics from aligned N$_2$ using a linearly polarized driving field [X. Zhou \emph{et al.}, Phys. Rev. Lett. \textbf{102}, 073902 (2009)]. This observation cannot be explained in the standard treatment of the Lewenstein model and has been ascribed to many-electron effects or the influence of the Coulomb force on the continuum electron. We show that non-vanishing ellipticity naturally appears within the Lewenstein model when using a multi-center stationary phase method for treating the dynamics of the continuum electron. The reason for…
Double ionization (DI) is a fundamental process that despite its apparent simplicity provides rich opportunities for probing and controlling the electronic motion. Even for the simplest multielectron atom, helium, new DI mechanisms are still being found. To first order in the field strength, a strong external field doubly ionizes the electrons in helium such that they are ejected into the same direction (front-to-back motion). The ejection into opposite directions (back-to-back motion) cannot be described to first order, making it a challenging target for control. Here, we address this challen…
The nondirect product discrete variable representation (npDVR) is developed for the time-dependent Schrödinger equation with nonseparable angular variables and is applied to a hydrogen atom in elliptically polarized strong laser fields. The 2D npDVR is constructed on spherical harmonics orthogonalized on the 2D angular grids of the Popov and Lebedev 2D cubatures for the unit sphere. With this approach we have investigated the dynamics of a hydrogen atom initially in its ground state in elliptically polarized laser fields with the intensity up to $I=10^{14}$ W/{cm}$^2$ and wavelength of $λ=800$…