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Orbit-based methods are widespread in strong-field laser-matter interaction. They provide a framework in which photoelectron momentum distributions can be interpreted as the quantum interference between different semi-classical pathways the electron can take on its way to the detector, which brings with it great predictive power. The transition amplitude of an electron going from a bound state to a final continuum state is often written as multiple integrals, which can be computed either numerically, or by employing the saddle-point method. If one computes the momentum distribution via a saddle-point method, the obtained distribution is highly dependent on the time window from which the saddle points are selected for inclusion in the "sum over paths". In many cases, this leads to the distributions not even satisfying the basic symmetry requirements and often containing many more oscillations and interference fringes than their numerically integrated counterparts. Using the strong-field approximation, we find that the manual enforcement of the energy-conservation condition on the momentum distribution calculated via the saddle-point method provides a unique momentum distribution which satisfies the symmetry requirements of the system and which is in a good agreement with the numerical results. We illustrate our findings using the example of the Ar atom ionized by a selection of monochromatic and bichromatic linearly polarized fields., Comment: 11 pages, 10 figures

We perform a systematic analysis of single-channel quantum interference in laser-induced nonsequential double ionization with few-cycle pulses, using the strong-field approximation. We focus on a below-threshold intensity for which the recollision-excitation with subsequent ionization (RESI) mechanism is prevalent. We derive and classify several analytic interference conditions for single-channel RESI in arbitrary driving fields, and address specific issues for few-cycle pulses. Since the cycles in a short pulse are no longer equivalent, there are several events whose dominance varies. We quantify this dominance for single excitation channels by proposing a dominance parameter. Moreover, there will be many more types of superimposed interference fringes that must be taken into consideration. We find an intricate tapestry of patterns arising from phase differences related to symmetrization, temporal shifts and a combination of exchange and event interference., Comment: 34 pages, 24 figures; in the revised version, some references have been added, the introduction has been slightly altered and the conclusions have been considerably extended

We discuss the effect of using potentials with a Coulomb tail and different degrees of softening in the photoelectron momentum distributions (PMDs) using the recently implemented hybrid forward-boundary CQSFA (H-CQSFA). We show that introducing a softening in the Coulomb interaction influences the ridges observed in the PMDs associated with backscattered electron trajectories. In the limit of a hard-core Coulomb interaction, the re-scattering ridges close along the polarization axis, while for a soft-core potential, they are interrupted at ridge-specific angles. We analyze the momentum mapping of the different orbits leading to the ridges. For the hard-core potential, there exist two types of saddle-point solutions that coalesce at the ridge. By increasing the softening, we show that two additional solutions emerge as the result of breaking a hidden dynamical symmetry associated exclusively with the Coulomb potential. Further signatures of this symmetry breaking are encountered in subsets of momentum-space trajectories. Finally, we use scattering theory to show how the softening affects the maximal scattering angle and provide estimates that agree with our observations from the CQSFA. This implies that, in the presence of residual binding potentials in the electron's continuum propagation, the distinction between purely kinematic and dynamic caustics becomes blurred., Comment: 20 pages, 12 figures; some figures and an appendix were added in the revised version

We perform a systematic comparison between photoelectron momentum distributions computed with the rescattered-quantum orbit strong-field approximation (RQSFA) and the Coulomb-quantum orbit strong-field approximation (CQSFA). We exclude direct, hybrid, and multiple scattered CQSFA trajectories, and focus on the contributions of trajectories that undergo a single act of rescattering. For this orbit subset, one may establish a one-to-one correspondence between the RQSFA and CQSFA contributions for backscattered and forward-scattered trajectory pairs. We assess the influence of the Coulomb potential on the ionization and rescattering times of specific trajectory pairs, kinematic constraints determined by rescattering, and quantum interference between specific pairs of trajectories. We analyze how the Coulomb potential alters their ionization and return times, and their interference in photoelectron momentum distributions. We show that Coulomb effects are not significant for high or medium photoelectron energies and shorter orbits, while, for lower momentum ranges or longer electron excursion times in the continuum, the residual Coulomb potential is more important. We also assess the agreement of both theories for different field parameters, and show that it improves with the increase of the wavelength., Comment: 18 pages, 10 figures; accepted for publication in Physical Review A

We construct two strong-field path integral methods with full Coulomb distortion, in which the quantum pathways are mimicked by interfering electron orbits: the rate-based CQSFA (R-CQSFA) and the hybrid forward-boundary CQSFA (H-CQSFA). The methods have the same starting point as the standard Coulomb quantum-orbit strong-field approximation (CQSFA), but their implementation does not require pre-knowledge of the orbits' dynamics. These methods are applied to ultrafast photoelectron holography. In the rate-based method, electron orbits are forward propagated and we derive a non-adiabatic ionization rate from the CQSFA, which includes sub-barrier Coulomb corrections and is used to weight the initial orbit ensemble. In the H-CQSFA, the initial ensemble provides initial guesses for a subsequent boundary problem and serves to include or exclude specific momentum regions, but the ionization probabilities associated with individual trajectories are computed from sub-barrier complex integrals. We perform comparisons with the standard CQSFA and \textit{ab-initio} methods, which show that the standard, purely boundary-type implementation of the CQSFA leaves out whole sets of trajectories. We show that the sub-barrier Coulomb corrections broaden the resulting photoelectron momentum distributions (PMDs) and improve the agreement of the R-CQSFA with the H-CQSFA and other approaches. We probe different initial sampling distributions, uniform and otherwise, and their influence on the PMDs. We find that initial biased sampling emphasizes rescattering ridges and interference patterns in high-energy ranges, while an initial uniform sampling guarantees accurate modeling of the holographic patterns near the ionization threshold or polarization axis. Our results are explained using the initial to final momentum mapping for different types of interfering trajectories., Comment: 25 pages revtex, 14 figures; in the revised version, some explanations have been extended and some figures have been modified

We perform a systematic analysis of how ultrafast photoelectron holography is influenced by an elliptically polarized field, with emphasis on quantum interference effects. We find that the interplay of the external field and the binding potential leads to twisted holographic patterns for low ellipticities and recover well-known angular offsets for high ellipticities. Using the Coulomb quantum-orbit strong-field approximation (CQSFA), we assess how the field ellipticity affects specific holographic patterns, such as the fan and the spider. The interplay of the external field and the binding potential leads to twisted holographic patterns in the fan, and to loss of contrast in the spider. This behavior can be traced back to interfering electron trajectories, and unequal changes in tunneling probability due to non-vanishing ellipticity. We also derive tunneling times analytically using the strong-field approximation (SFA), provide estimates for ellipticy ranges for which interference is expected to be prominent, and discuss how to construct continuous electron momentum distributions exploring the rotation symmetry around the origin.

We investigate photoelectron holography in bichromatic linearly polarized fields of commensurate frequencies $r\omega$ and $s\omega$, with emphasis on the existing symmetries and for which values of the relative phase between the two driving waves they are kept or broken. Using group-theoretical methods, we show that, additionally to the well-known half-cycle symmetry, which is broken for $r+s$ odd, there are reflection symmetries around the field zero crossings and maxima, which may or may not be kept, depending on how both waves are dephased. The three symmetries are always present for monochromatic fields, while for bichromatic fields this is not guaranteed, even if $r+s$ is even and the half-cycle symmetry is retained. Breaking the half-cycle symmetry automatically breaks one of the other two, while, if the half-cycle symmetry is retained, the other two symmetries are either \textit{both} kept or broken. We analyze how these features affect the ionization times and saddle-point equations for different bichromatic fields. We also provide general expressions for the relative phases $\phi$ which retain specific symmetries. As an application, we compute photoelectron momentum distributions for $\omega-2\omega$ fields with the Coulomb Quantum Orbit Strong-Field approximation and assess how holographic structures such as the fan, the spider and interference carpets behave, focusing on the reflection symmetries. The features encountered can be traced back to the field gradient and amplitude affecting ionization probabilities and quantum interference in different momentum regions., Comment: 48 pages, 14 figures (including one in the appendix); figures have been included, there has been some restructuring and some discussions have been extended in the revised version

We analyze how bound-state excitation, electron exchange and the residual binding potential influence above-threshold ionization (ATI) in Helium prepared in an excited $p$ state, oriented parallel and perpendicular to a linearly polarized mid-IR field. Using ab initio B-spline Algebraic Diagrammatic Construction (ADC), and several one-electron methods with effective potentials, including the Schr\"odinger solver Qprop, modified versions of the Strong-Field Approximation and the Coulomb-Quantum Orbit Strong-Field Approximation (CQSFA), we find that these specific physical mechanisms leave significant imprints in ATI spectra and photoelectron momentum distributions. Examples are changes of up to two orders of magnitude in the high-energy photoelectron region, and ramp-like structures that can be traced back to Coulomb-distorted trajectories. The present work also shows that electron exchange renders rescattering less effective, causing suppressions in the ATI plateau. Due to the long-range potential, the electron continuum dynamics are no longer confined to the polarization axis, in contrast to the predictions of traditional approaches. Thus, one may in principle probe excited-state configurations perpendicular to the driving-field polarization without the need for orthogonally polarized fields., Comment: 26 pages, 8 figures. Fig. 5 has been compressed in order to meet the arXiV requirements. In the revised version, we have streamlined parts of the theory, modified some discussions and the conclusions, and added references

We provide a brief review of how phase space techniques are explored within strong-field and attosecond science. This includes a broad overview of the existing landscape, with focus on strong-field ionisation and rescattering, high-order harmonic generation, stabilisation and free-electron lasers. Furthermore, using our work on the subject, which deals with ionisation dynamics in atoms and diatomic molecules as well as high-order harmonic generation in inhomogeneous fields, we exemplify how such tools can be employed. One may for instance determine qualitatively different phase space dynamics, explore how bifurcations influence ionisation and high-harmonic generation, establish for which regimes classical and quantum correspondence works or fails, and what role different time scales play. Finally, we conclude the review highlighting the importance of the tools available in quantum optics, quantum information and physical chemistry to strong-field laser-matter interaction., Comment: 38 pages, 12 figures, submitted to EPJ D

We investigate the discrete orbital angular momentum (OAM) of photoelectrons freed in strongfield ionization. We use these `twisted' electrons to provide an alternative interpretation on existing experimental work of vortex interferences caused by strong field ionization mediated by two counterrotating circularly polarized pulses separated by a delay. Using the strong field approximation, we derive an interference condition for the vortices. In computations for a neon target we find very good agreement of the vortex condition with photoelectron momentum distributions computed with the strong field approximation, as well as with the time-dependent methods Qprop and R-Matrix. For each of these approaches we examine the OAM of the photoelectrons, finding a small number of vortex states localized in separate energy regions. We demonstrate that the vortices arise from the interference of pairs of twisted electron states. The OAM of each twisted electron state can be directly related to the number of arms of the spiral in that region. We gain further understanding by recreating the vortices with pairs of twisted electrons and use this to determine a semiclassical relation for the OAM. A discussion is included on measuring the OAM in strong field ionization directly or by employing specific laser pulse schemes as well as utilizing the OAM in time-resolved imaging of photo-induced dynamics., Comment: 14 pages, 4 figures, publication prepared for the the strong field theme of the Faraday Discussions conference: Time-resolved imaging of photo-induced dynamics

We propose an analytical approach for computing the eigenspectrum and corresponding eigenstates of a hyperbolic double well potential of arbitrary height or width, which goes beyond the usual techniques applied to quasi-exactly solvable models. We map the time-independent Schr\"odinger equation onto the Heun confluent differential equation, which is solved by using an infinite power series. The coefficients of this series are polynomials in the quantisation parameter, whose roots correspond to the system's eigenenergies. This leads to a quantisation condition that allows us to determine a whole spectrum, instead of individual eigenenergies. This method is then employed to perform an in depth analysis of electronic wave-packet dynamics, with emphasis on intra-well tunneling and the interference-induced quantum bridges reported in a previous publication [H. Chomet et al, New J. Phys. 21, 123004 (2019)]. Considering initial wave packets of different widths and peak locations, we compute autocorrelation functions and Wigner quasiprobability distributions. Our results exhibit an excellent agreement with numerical computations, and allow us to disentangle the different eigenfrequencies that govern the phase-space dynamics., Comment: 23 pages, 9 figures

We develop a new framework to optimize and understand uncertainty from in situ strong field measurements of laser field parameters. We present the first derivation of quantum and classical Fisher information for an electron undergoing strong-field ionization. This is used for parameter estimation and to characterize the uncertainty of the ponderomotive energy, directly proportional to laser intensity. In particular, the quantum and classical Fisher information for the momentum basis displays quadratic scaling over time. This can be linked to above-threshold ionization interference rings for measurements in the momentum basis and to the `ponderomotive phase' for the `ideal' quantum measurements. Preferential scaling is found for increasing laser pulse length and intensity. We use this to demonstrate for in situ measurements of laser intensity, that high resolution momentum spectroscopy has the capacity to reduce the uncertainty by over $25$ times compared to measurements employing the ionization rate, while using the `ideal' quantum measurement would reduce it by a further factor of $2.6$. A minimum uncertainty of the order $2.8 \times 10^{-3}~\%$ is theorized for this framework. Finally, we examine previous in situ measurements formulating a measurement that matches the experimental procedure and suggest how to improve this., Comment: 16 pages, 8 figures, 4 tables, 51 equations

We perform a phase-space analysis of strong-field enhanced ionisation in molecules, with emphasis on quantum-interference effects. Using Wigner quasi-probability distributions and the quantum Liouville equation, we show that the momentum gates reported in a previous publication [N. Takemoto and A. Becker, Phys. Rev. A \textbf{84}, 023401 (2011)] may occur for static driving fields, and even for no external field at all. Their primary cause is an interference-induced bridging mechanism that occurs if both wells in the molecule are populated. In the phase-space regions for which quantum bridges occur, the Wigner functions perform a clockwise rotation whose period is intrinsic to the molecule. This evolution is essentially non-classical and non-adiabatic, as it does not follow equienergy curves or field gradients. Quasi-probability transfer via quantum bridges is favoured if the electron's initial state is either spatially delocalised, or situated at the upfield molecular well. Enhanced ionisation results from the interplay of this cyclic motion, adiabatic tunnel ionisation and population trapping. Optimal conditions require minimising population trapping and using the bridging mechanism to feed into ionisation pathways along the field gradient., Comment: 27 pages, 13 figures; some figures have been simplified to comply with the arXiv requirements

Photoelectron holography constitutes a powerful tool for the ultrafast imaging of matter, as it combines high electron currents with subfemtosecond resolution, and gives information about transition amplitudes and phase shifts. Similarly to light holography, it uses the phase difference between the probe and the reference waves associated with qualitatively different ionization events for the reconstruction of the target and for ascertaining any changes that may occur. These are major advantages over other attosecond imaging techniques, which require elaborate interferometric schemes in order to extract phase differences. For that reason, ultrafast photoelectron holography has experienced a huge growth in activity, which has led to a vast, but fragmented landscape. The present review is an organizational effort towards unifying this landscape. This includes a historic account in which a connection with laser-induced electron diffraction (LIED) is established, a summary of the main holographic structures encountered and their underlying physical mechanisms, a broad discussion of the theoretical methods employed, and of the key challenges and future possibilities. We delve deeper in our own work, and place a strong emphasis on quantum interference, and on the residual Coulomb potential., Comment: Review article; 88 pages, 40 figures; the quality of some figures has been compromised in order to comply with the arxiv requirements

Most implementations of Coulomb-distorted strong-field approaches that contain features such as tunneling and quantum interference use real trajectories in continuum propagation, while a fully consistent approach must use complex trajectories throughout. A key difficulty in the latter case are branch cuts that appear due to the specific form of the Coulomb potential. We present a method for treating branch cuts in quantum-trajectory models, which is subsequently applied to photoelectron holography. Our method is not numerically intensive, as it does not require finding the location of all branching points and branch cuts prior to its implementation, and is applicable to Coulomb-free and Coulomb-distorted trajectories. We show that the presence of branch cuts leads to discontinuities and caustics in the holographic fringes in above-threshold ionization (ATI) photoelectron angular distributions (PAD). These artefacts are removed applying our method, provided they appear far enough from the polarization axis. A comparison with the full solution of the time-dependent Schr\"odinger equation is also performed, and a discussion of the applicability range of the present approach is provided., Comment: 13 pages, 8 figures. Some figure files have been reduced in order to comply with the arXiV requirements

We perform a detailed analysis of the different types of orbits in the Coulomb Quantum Orbit Strong-field Approximation (CQSFA), ranging from direct to those undergoing hard collisions. We show that some of them exhibit clear counterparts in the standard formulations of the strong-field approximation for direct and rescattered above-threshold ionization, and show that the standard orbit classification commonly used in Coulomb-corrected models is over-simplified. We identify several types of rescattered orbits, such as those responsible for the low-energy structures reported in the literature, and determine the momentum regions in which they occur. We also find formerly overlooked interference patterns caused by backscattered, Coulomb-corrected orbits and assess their effect on photoelectron angular distributions. These orbits improves the agreement of photoelectron angular distributions computed with the CQSFA with the outcome of ab-initio methods for high-energy phtotoelectrons perpendicular to the field-polarization axis., Comment: 19 pages, 9 figures

We provide approximate analytic expressions for above-threshold ionization (ATI) transition probabilities and photoelectron angular distributions (PADs). These analytic expressions are more general than those existing in the literature and include the residual binding potential in the electron continuum propagation. They successfully reproduce the ATI side lobes and specific holographic structures such as the near-threshold fan-shaped pattern and the spider-like structure that extends up to relatively high photoelectron energies. We compare such expressions with the Coulomb quantum orbit strong-field approximation (CQSFA) and the full solution of the time-dependent Schr\"odinger equation for different driving-field frequencies and intensities, and provide an in-depth analysis of the physical mechanisms behind specific holographic structures. Our results shed additional light on what aspects of the CQSFA must be prioritized in order to obtain the key holographic features, and highlight the importance of forward scattered trajectories. Furthermore, we find that the holographic patterns change considerably for different field parameters, even if the Keldysh parameter is kept roughly the same., Comment: 28 pages, 10 figures. The figures have been simplified in order to comply with the arXiV size requirements

Using the recently developed Coulomb Quantum Orbit Strong-Field Approximation (CQSFA), we perform a systematic analysis of several features encountered in above-threshold ionization (ATI) photoelectron angle-resolved distributions (PADs), such as side lobes, and intra- and intercycle interference patterns. The latter include not only the well-known intra-cycle rings and the near-threshold fan-shaped structure, but also previously overlooked patterns. We provide a direct account of how the Coulomb potential distorts different types of interfering trajectories and changes the corresponding phase differences, and show that these patterns may be viewed as generalized holographic structures formed by up to three types of trajectories. We also derive analytical interference conditions and estimates valid in the presence or absence of the residual potential, and assess the range of validity of Coulomb-corrected interference conditions provided in the literature., Comment: 17 pages, 11 figures. Some figures have been compressed in order to comply with the arXiv requirements

We investigate high-order harmonic generation in inhomogeneous media for reduced dimensionality models. We perform a phase-space analysis, in which we identify specific features caused by the field inhomogeneity. We compute high-order harmonic spectra using the numerical solution of the time-dependent Schr\"odinger equation, and provide an interpretation in terms of classical electron trajectories. We show that the dynamics of the system can be described by the interplay of high-frequency and slow-frequency oscillations, which are given by Mathieu's equations. The latter oscillations lead to an increase in the cutoff energy, and, for small values of the inhomogeneity parameter, take place over many driving-field cycles. In this case, the two processes can be decoupled and the oscillations can be described analytically., Comment: 11 pages, 8 figures. Some figures have been compressed in order to satisfy the arXiv requirements

We analyze the imprint of nodal planes in high-order harmonic spectra from aligned diatomic molecules in intense laser fields whose components exhibit orthogonal polarizations. We show that the typical suppression in the spectra associated to nodal planes is distorted, and that this distortion can be employed to map the electron's angle of return to its parent ion. This investigation is performed semi-analytically at the single-molecule response and single-active orbital level, using the strong-field approximation and the steepest descent method. We show that the velocity form of the dipole operator is superior to the length form in providing information about this distortion. However, both forms introduce artifacts that are absent in the actual momentum-space wavefunction. Furthermore, elliptically polarized fields lead to larger distortions in comparison to two-color orthogonally polarized fields. These features are investigated in detail for $\mathrm{O}_2$, whose highest occupied molecular orbital provides two orthogonal nodal planes., Comment: 11 pages, 6 figures

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 indistinguishability and intra-cycle events, and that stemming from different excitation channels. We find that interference is most prominent around the diagonal and anti-diagonal in the parallel-momentum plane and provide fully analytical expressions for most interference patterns encountered. We also show that this interference can be controlled by an appropriate choice of phase and excited-state geometry. This leads a to myriad of shapes for the RESI distributions including correlated, anti-correlated and ring-shaped., Comment: 14 pages, 13 figures

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 indistinguishability and intra-cycle events, and from different excitation channels., Comment: 5 pages, 4 figures

We investigate high-order harmonic spectra from aligned diatomic molecules in intense driving fields whose components have orthogonal polarizations. We focus on how the driving-field ellipticity influences structural interference patterns in a macroscopic medium. In a previous publication [Phys. Rev. A 88, 023404 (2013)] we have shown that the non-vanishing ellipticity introduces an effective dynamic shift in the angle for which the two-center interference maxima and minima occur, with regard to the existing condition for linearly polarized fields. In this work we show through simulation that it is still possible to observe this shift in harmonic spectra that have undergone macroscopic propagation, and discuss the parameter range for doing so. These features are investigated for $H_2$ in a bichromatic field composed of two orthogonally polarized waves. The shift is visible both in the near- and in the far-field regime, so that, in principle, it can be observed in experiments., Comment: 9 pages, 6 figures

We perform a detailed analysis of how the interplay between the residual binding potential and a strong laser field influences above-threshold ionization (ATI), employing a semi-analytical, Coulomb-corrected strong-field approximation (SFA) in which the Coulomb potential is incorporated in the electron propagation in the continuum. We find that the Coulomb interaction lifts the degeneracy of some SFA trajectories, and we identify a set of orbits which, for high enough photoelectron energies, may be associated with rescattering. Furthermore, by performing a direct comparison with the standard SFA, we show that several features in the ATI spectra can be traced back to the influence of the Coulomb potential on different electron trajectories. These features include a decrease in the contrast, a shift towards lower energies in the interference substructure, and an overall increase in the photoelectron yield. All features encountered exhibit a very good agreement with the \emph{ab initio} solution of the time-dependent Schr\"odinger equation., Comment: 12 pages, 10 figures

We assess the suitability of quantum and semiclassical initial value representations, exemplified by the coupled coherent states (CCS) method and the Herman Kluk (HK) propagator, respectively, for modeling the dynamics of an electronic wave packet in a strong laser field, if this wave packet is initially bound. Using Wigner quasiprobability distributions and ensembles of classical trajectories, we identify signatures of over-the-barrier and tunnel ionization in phase space for static and time-dependent fields and the relevant sets of phase-space trajectories in order to model such features. Overall, we find good agreement with the full solution of the time-dependent Schr\"odinger equation (TDSE) for Wigner distributions constructed with both initial-value representations. Our results indicate that the HK propagator does not fully account for tunneling and over-the-barrier reflections. However, it is able to partly reproduce features associated with the wave packet crossing classically forbidden regions, although the trajectories employed in its construction always obey classical phase-space constraints. We also show that the Coupled Coherent States (CCS) method represents a fully quantum initial value representation and accurately reproduces the results of a standard TDSE solver. Furthermore, we sow that both the HK propagator and the CCS approach may be successfully employed to compute the time-dependent dipole acceleration and high-harmonic spectra. Nevertheless, the semiclassical propagator exhibits a worse agreement with the TDSE than the outcome of the CCS method, as it neither fully accounts for tunneling nor for over-the-barrier reflections. This leads to a dephasing in the time-dependent wave function which becomes more pronounced for longer times., Comment: 23 pages (single column), 9 figures

We investigate the influence of intense, elliptically polarized driving fields on high-order harmonic spectra from aligned diatomic molecules. We derive a generalized two-center interference condition for elliptically polarized fields, which accounts for s-p mixing and the orbital symmetry, within the strong-field and the single-active electron approximation. We show that the non-vanishing ellipticity introduces an effective dynamic shift in the angle for which the two-center interference maxima and minima occur, with regard to the existing condition for linearly polarized fields. This shift depends on the ratio between the field-dressed momentum components of the returning electron parallel and perpendicular to the major ellipticity axis along each possible orbit. Because of this dependence, we find that there will be a blurring in the two-center interference minima, and that increasing ellipticity leads to splitting in such patterns. These features are investigated in detail for H2 and Ar2., Comment: 13 pages, 11 figures; some figures have been simplified in order to comply with the arXiV requirements

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 is caused by the electron velocity component perpendicular to the major polarization axis, while spatial interference is washed out as a consequence either of s-p mixing, or of the temporal dependence of the ionization prefactor. Both types of interference are analyzed in detail in terms of electron trajectories, and specific conditions for which sharp fringes occur are provided., Comment: 9, pages, 7 figures. Please note that some figures have been simplified in order to comply with the arXiv requirements

We perform a Bohmian-trajectory analysis of high-order harmonic generation (HHG), focusing on the fact that typical HHG spectra are best reproduced by the Bohmian trajectory starting at the innermost part of the core [Phys. Rev. A \textbf{88}, 023415 (2013)]. Using ensemble averages around this central trajectory, we show that, for the high-plateau and cutoff harmonics, small ensembles of Bohmian trajectories are sufficient for a quantitative agreement with the numerical solution of the time-dependent Schr\"odinger equation (TDSE), while larger ensembles are necessary in the low-plateau region. Furthermore, we relate the Bohmian trajectories to the "short" and "long" trajectories encountered in the Strong-Field Approximation (SFA), and show that the time-frequency maps from the central Bohmian trajectory overestimate the contributions of the long SFA trajectory, in comparison to the outcome of the TDSE computations. We also discuss how the time-frequency profile of the central trajectory may be influenced nonlocally by degrading the wave-packet propagation far from the core., Comment: 9 pages, 5 figures

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 dramatically with regard to the carrier-envelope phase. By performing a detailed analysis of the dynamics of the two active electrons in terms of quantum orbits, we relate the shapes and the momentum regions populated by such distributions to the dominant set of orbits along which rescattering of the first electron and ionization of the second electron occurs. These orbits can be manipulated by varying the carrier-envelope phase. This opens a wide range of possibilities for controlling correlated attosecond electron emission by an adequate pulse choice., Comment: 12 pages, 7 figures, 1 table

We investigate high-order harmonic generation from a Bohmian-mechanical perspective, and find that the innermost part of the core, represented by a single Bohmian trajectory, leads to the main contributions to the high-harmonic spectra. Using time-frequency analysis, we associate this central Bohmian trajectory to an ensemble of unbound classical trajectories leaving and returning to the core, in agreement with the three step model. In the Bohmian scenario, this physical picture builds up non-locally near the core via the quantum mechanical phase of the wavefunction. This implies that the flow of the wavefunction far from the core alters the central Bohmian trajectory. We also show how this phase degrades in time for the peripheral Bohmian trajectories as they leave the core region., Comment: 7 pages, 3 figures; the manuscript has been considerably extended and modified with regard to the previous versions

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 complex, the condition that recollision of the first electron occurs before tunnel ionization of the second electron translates into boundary conditions for the steepest-descent contours, and thus puts constraints on the saddles to be taken when computing the RESI transition amplitudes. We also show that this generalized causality condition has a dramatic effect in the shapes of the RESI electron momentum distributions for few-cycle laser pulses. Physically, causality determines how the dominant sets of orbits an electron returning to its parent ion can be combined with the dominant orbits of a second electron tunneling from an excited state. All features encountered are analyzed in terms of such orbits, and their quantum interference., Comment: 15 pages, 12 figures

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 the electron emission at spatially separated centers. We provide generalized analytical expressions for such maxima or minima, which take into account $s$ $p$ mixing and the orbital geometry. The patterns caused by the two-center interference are sharpest for vanishing alignment angle and get washed out as this parameter increases. Apart from that, there exist features due to the geometry of the lowest occupied molecular orbital (LUMO), which may be observed for a wide range of alignment angles. Such features manifest themselves as the suppression of probability density in specific momentum regions due to the shape of the LUMO wavefunction, or as an overall decrease in the RESI yield due to the presence of nodal planes., Comment: 11 pages revtex, 2 figures

The relation between high-harmonic spectra and the geometry of the molecular orbitals in position and momentum space is investigated. In particular we choose two isoelectronic pairs of homonuclear and heteronuclear molecules, such that the highest occupied molecular orbital of the former exhibit at least one nodal plane. The imprint of such planes is a strong suppression in the harmonic spectra, for particular alignment angles. We are able to identify two distinct types of nodal planes. If the nodal planes are determined by the atomic wavefunctions only, the angle for which the yield is suppressed will remain the same for both types of molecules. In contrast, if they are determined by the linear combination of atomic orbitals at different centers in the molecule, there will be a shift in the angle at which the suppression occurs for the heteronuclear molecules, with regard to their homonuclear counterpart. This shows that, in principle, molecular imaging, which uses the homonuclear molecule as a reference and enables one to observe the wavefunction distortions in its heteronuclear counterpart, is possible., Comment: 14 pages, 7 figures. Figs. 3, 5 and 6 have been simplified in order to comply with the arXiv size requirements

We make a detailed assessment of which form of the dipole operator to use in calculating high order harmonic generation within the framework of the strong field approximation, and look specifically at the role the form plays in the inclusion of multielectron effects perturbatively with regard to the contributions of the highest occupied molecular orbital. We focus on how these corrections affect the high-order harmonic spectra from aligned homonuclear and heteronuclear molecules, exemplified by $\mathrm{N}_2$ and CO, respectively, which are isoelectronic. We find that the velocity form incorrectly finds zero static dipole moment in heteronuclear molecules. In contrast, the length form of the dipole operator leads to the physically expected non-vanishing expectation value for the dipole operator in this case. Furthermore, the so called "overlap" integrals, in which the dipole matrix element is computed using wavefunctions at different centers in the molecule, are prominent in the first-order multielectron corrections for the velocity form, and should not be ignored. Finally, inclusion of the multielectron corrections has very little effect on the spectrum. This suggests that relaxation, excitation and the dynamic motion of the core are important in order to describe multielectron effects in molecular high-order high harmonic generation., Comment: Figures 2 and 4 have been simplified in order to fulfil the size requirements of arXiv; in the new version references have been added

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-field intensity threshold for the RESI physical mechanism. At the threshold, the kinetic energy of the first electron, upon return, is just sufficient to excite the second electron. We compute the distributions for helium and argon in the threshold and above-threshold intensity regime. In the latter case, we relate our findings to existing experiments. The electron-momentum distributions encountered are symmetric with respect to all quadrants of the plane spanned by the momentum components parallel to the laser-field polarization, instead of concentrating on only the second and fourth quadrants., Comment: 14 pages, 7 figures

We investigate the contributions from the $3\sigma_{g}$ and $1\pi_{u}$ and molecular orbitals in high-order harmonic generation in $N_{2}$, with particular emphasis on quantum-interference effects. We consider both the physical processes in which the electron is freed and returns to the same orbital, and those in which it is ionized off one orbital and recombines with the other. We show that the quantum-interference patterns observed in the high-order harmonic spectra are predominantly determined by the $3\sigma_{g}$ orbital. This holds both for the situation in which only the $1\pi_{ux}$ orbital is considered, and the dynamics of the electron is restricted to the plane $p_{x}p_{z},$ or in the full three-dimensional case, if the azimuthal angle is integrated over and the degeneracy of $1\pi_{u}$ is taken into account., Comment: 10 pages, 4 figures

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 above-threshold ionization (ATI). The second electron leaves the excited state in a direct ATI-like process, with the maximal energy of $2U_p$. We also compute electron-momentum distributions, whose maxima agree with our estimates and with other methods., Comment: 13 pages, 4 figures

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 the temporal region for which it is nearly linearly polarized. We show that, if the time delay $T_{d}$ is of the order of the pulse length, the electron-momentum distributions, as functions of the parallel momentum components, are highly asymmetric and dependent on the carrier-envelope (CE) phase. As this delay is decreased, this asymmetry gradually vanishes. We explain this behavior in terms of the available phase space, the quasi-static tunneling rate and the recollision rate for the first electron, for different sets of trajectories. Our results show that polarization-gating technique may provide an efficient way to study the NSDI dynamics in the single-cycle limit, without employing few-cycle pulses., Comment: 17 pages, 6 figures

We analyze the influence of different recombination scenarios, involving one or two centers, on high-order harmonic generation (HHG) in diatomic molecules, for different values of the internuclear separation. We work within the strong-field approximation, and employ modified saddle-point equations, in which the structure of the molecule is incorporated. We find that the two-center interference patterns, attributed to high-order harmonic emission at spatially separated centers, are formed by the quantum interference of the orbits starting at a center $C_{j}$ and finishing at a different center $C_{\nu }$ in the molecule with those starting and ending at a same center $C_{j}.$ Within our framework, we also show that contributions starting at different centers exhibit different orders of magnitude, due to the influence of additional potential-energy shifts. This holds even for small internuclear distances. Similar results can also be obtained by considering single-atom saddle-point equations and an adequate choice of molecular prefactors., Comment: 8 pages, 5 figures

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 starting at $C_{j}$ and ending at a different center $C_{\nu}$ leads to the same maxima as minima as if all possible scenarios are taken. There exist, however, quantitative differences as far as the gauge choice is concerned. Indeed, while the velocity-gauge distributions obtained employing only the above-mentioned processes are practically identical to the overall distributions, their length-gauge counterparts exhibit an asymmetry in the positive and negative momentum regions. This asymmetry is due to additional potential-energy shifts which are only present in the length-gauge formulation, and which, depending on the center, sink or increase the potential barrier through which the first electron tunnels. In contrast, the interference between topologically similar scenarios leads at most to patterns whose positions, in momentum space, do not agree with the overall interference condition, neither in the length nor in the velocity gauge., Comment: 17 pages, three figures; in the second revised version, some discussions have been extended and/or modified, Fig. 2 has been modified, a new figure has been inserted and some typos have been corrected. There are also changes in the abstract

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., Comment: 12 pages, 7 figures; some discussions have been extended and some figures slightly modified

We perform a detailed analysis of high-order harmonic generation in diatomic molecules within the strong-field approximation, with emphasis on quantum-interference effects. Specifically, we investigate how the different types of electron orbits, involving one or two centers, affect the interference patterns in the spectra. We also briefly address the influence of the choice of gauge, and of the initial and final electronic bound states on such patterns. For the length-gauge SFA and undressed bound states, there exist additional terms, which can be interpreted as potential energy shifts. If, on the one hand, such shifts alter the potential barriers through which the electron initially tunnels, and may lead to a questionable physical interpretation of the features encountered, on the other hand they seem to be necessary in order to reproduce the overall maxima and minima in the spectra. Indeed, for dressed electronic bound states in the length gauge, or undressed bound states in the velocity gauge, for which such shifts are absent, there is a breakdown of the interference patterns. In order to avoid such a problem, we provide an alternative pathway for the electron to reach the continuum, by means of an additional attosecond-pulse train. A comparison of the purely monochromatic case with the situation for which the attosecond pulses are present suggests that the patterns are due to the interference between the electron orbits which finish at different centers, regardless of whether one or two centers are involved., Comment: 14 pages, 9 figures; two figures have been modified, one figure and new results included, discussions extended

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 processes. However, around the boundary of the energy regions for which rescattering has a classical counterpart, such processes play a negligible role and very clear interference patterns are observed. In such energy regions, one is able to infer the internuclear distance from the energy difference between adjacent interference minima., Comment: 10 pages, 8 figures; discussions slightly modified and an additional figure inserted for clarity

In recent publications, it has been shown that high-order harmonic generation can be manipulated by employing a time-delayed attosecond pulse train superposed to a strong, near-infrared laser field. It is an open question, however, which is the most adequate way to approximate the attosecond pulse train in a semi-analytic framework. Employing the Strong-Field Approximation and saddle-point methods, we make a detailed assessment of the spectra obtained by modeling the attosecond pulse train by either a monochromatic wave or a Dirac-Delta comb. These are the two extreme limits of a real train, which is composed by a finite set of harmonics. Specifically, in the monochromatic limit, we find the downhill and uphill sets of orbits reported in the literature, and analyze their influence on the high-harmonic spectra. We show that, in principle, the downhill trajectories lead to stronger harmonics, and pronounced enhancements in the low-plateau region. These features are analyzed in terms of quantum interference effects between pairs of quantum orbits, and compared to those obtained in the Dirac-Delta limit., Comment: 10 pages, 7 figures (eps files). To appear in Laser Physics

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 $\Delta t$. 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 momenta obtained by the $N$ electrons when they reach the continuum at $t+\Delta t$, by moving such times towards or away from a crossing of the electric field. The contributions from both types of collisions are influenced in distinct ways, and the interplay between such trends determines the widths and the peak momenta of the distributions. Specifically in the few-cycle pulse case, we also show that such time delays do not affect the shapes of the momentum distributions in a radical fashion. Hence, even with a thermalization time $\Delta t$, nonsequential multiple ionization could in principle be used for absolute-phase diagnosis., Comment: 19 pages, 8 figures (eps files)

We perform a detailed analysis of how high-order harmonic generation (HHG) and above-threshold ionization (ATI) can be controlled by a time-delayed attosecond-pulse train superposed to a strong, near-infrared laser field. In particular we show that the high-harmonic and photoelectron intensities, the high-harmonic plateau structure and cutoff energies, and the ATI angular distributions can be manipulated by changing this delay. This is a direct consequence of the fact that the attosecond pulse train can be employed as a tool for constraining the instant an electronic wave packet is ejected in the continuum. A change in such initial conditions strongly affects its subsequent motion in the laser field, and thus HHG and ATI. In our studies, we employ the Strong-Field Approximation and explain the features observed in terms of interference effects between various electron quantum orbits. Our results are in agreement with recent experimental findings and theoretical studies employing purely numerical methods., Comment: 10 pages revtex and 6 figures (eps files)

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., Comment: 5 pages revtex and 4 figures (eps files)

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 by either a contact or a Coulomb-type interaction. We also perform an adequate treatment of the bound-state singularity which is present in this framework. We show that the momentum distributions are very sensitive with respect to spatially extended or localized wave functions, but are not considerably influenced by their shape. Furthermore, the modifications performed in order to overcome the bound-state singularity do not significantly alter the momentum distributions, apart from a minor suppression in the region of small momenta. The only radical changes occur if one employs effective form factors, which take into account the presence of the residual ion upon rescattering. If the ionic potential is of contact type, it outweighs the spreading caused by a long-range electron-electron interaction, or by spatially extended bound states. This leads to momentum distributions which exhibit a very good agreement with the existing experiments., Comment: 13 pages revtex, 11 figures (eps files)

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 asymmetric electron momentum distributions, which strongly depend on the absolute phase, i.e., on the phase difference between the pulse envelope and its carrier frequency. Around a particular value of this parameter, the distributions shift from the region of positive to that of negative momenta, or vice-versa, in a radical fashion. This behavior is investigated in detail for several driving-field parameters, and provides a very efficient method for measuring the absolute phase. Both models yield very similar distributions, which share the same physical explanation. There exist, however, minor discrepancies due to the fact that, beyond the region for which electron-impact ionization is classically allowed, the yields from the quantum mechanical computation decay exponentially, whereas their classical counterparts vanish., Comment: 12 pages revtex, 12 figures (eps files)

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 a (three-body) contact interaction or a Coulomb interaction, and we do or do not incorporate the mutual Coulomb repulsion of the two electrons in their final state. In particular, we investigate the correlation of the momentum components parallel to the laser-field polarization, with the transverse momentum components either restricted to certain finite ranges or entirely summed over. In the latter case, agreement with experimental data is best for the contact interaction and without final-state repulsion. In the former, if the transverse momenta are restricted to small values, comparison of theory with the data shows evidence of Coulomb effects. We propose that experimental data selecting events with small transverse momenta of \textit{both} electrons are particularly promising in the elucidation of the dynamics of NSDI. Also, a classical approximation of the quantum-mechanical $S$ matrix is formulated and shown to work very well inside the classically allowed region., Comment: 18 pages revtex, 13 figures (eps files; the files have been compressed due to memory problems)