We present results of high-resolution experiments on single ionization of He, Ne and Ar by ultra-short (25 fs, 6 fs) 795 nm laser pulses at intensities 0.15-2.0x10^15 W/cm^2. We show that the ATI-like pattern can survive deep in the tunneling regime and that the atomic structure plays an important role in the formation of the low-energy photoelectron spectra even at high intensities. The absence of ponderomotive shifts, the splitting of the peaks and their degeneration for few-cycle pulses indicate that the observed structures originate from a resonant process.
Using a three-dimensional quasiclassical technique we explore molecular double ionization by a linearly polarized, infrared (800~nm) 27~fs laser pulse. For intensities ranging from the tunneling to the over-the-barrier regime, we identify the double ionization pathways in a unified way as a function of total electron energy. For the tunneling regime, we discuss the differences in the interplay of double ionization (DI) pathways between strongly driven He and strongly driven $N_{2}$. For intermediate intensities in the over-the-barrier regime, we find that both the correlated momenta and the do…
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 …
The geometry-dependent ionization behavior of the ammonia molecule is investigated. Different theoretical approaches for obtaining the ionization yield are compared, all of them showing a strong dependence of the ionization yield on the inversion coordinate at long wavelengths ($\geq$ 800 nm). It is shown how this effect can be exploited to create and probe nuclear wave packets in neutral ammonia using Lochfraß. Furthermore, imaging of a wave packet tunneling through the barrier of a double-well potential in real time is discussed.
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 discuss the possibility of non-exponential tunneling ionization of atoms irradiated by intense laser field. This effect can occur at times, which are greater than the lifetime of a system under consideration. The mechanism for non-exponential depletion of an initial quasi-stationary state is the cutting of the energy spectrum of final continuous states at long times. We first consider the known examples of cold emission of electrons from metal, tunneling alpha-decay of atomic nuclei, spontaneous decay in two-level systems and the single-photon atomic ionization by a weak electromagnetic fie…
We propose a method to study the tunneling process by analyzing the time-dependent ionization yield in circularly polarized laser. A numerical calculation shows that for an atom exposed to a long laser pulse, if its initial electronic state wave function is non-spherical symmetric, the delayed phase shift of the ionization rate vs. the laser cycle period in real time in the region close to the peak intensity of the laser pulse can be used to probe the tunneling time. In this region, an obvious delay phase shift is observed, showing the tunneling time is in order of tens of attoseconds. Further…
The tunneling ionization of exotic atoms such as muonic hydrogen, muonium and positronium in a strong laser field of circular polarization is investigated taking into account the impact of the motion of the center of mass on the the tunneling ionization dynamics. The momentum partition between the ionization products is deduced. The effect of the center of mass motion for the momentum distribution of the ionization components is determined. The effect scales with the ratio of the electron (muon) to the atomic core masses and is nonnegligible for exotic atoms, while being insignificant for comm…
A new pathway of strong laser field induced ionization of an atom is identified which is based on recollisions under the tunneling barrier. With an amended strong field approximation, the interference of the direct and the under-the-barrier recolliding quantum orbits are shown to induce a measurable shift of the peak of the photoelectron momentum distribution. The scaling of the momentum shift is derived relating the momentum shift to the tunneling delay time according to the Wigner concept. This allows to extend the Wigner concept for the quasistatic tunneling time delay into the nonadiabatic…
Resonant two-photon ionization in a system consisting of two spatially well-separated atoms is studied. Due to two-center electron-electron correlations, the ionization may also proceed through photo-excitation of both atoms with subsequent interatomic Coulombic decay. We show that this channel may dominate the photoionization process and qualitatively change its dependence on the field intensity and the spectra of emitted electrons.
Recent attoclock experiments and theoretical studies regarding the strong-field ionization of atoms by few-cycle infrared pulses revealed new features that have attracted much attention. Here we investigate tunneling ionization and the dynamics of the electron probability using Bohmian Mechanics. We consider a one-dimensional problem to illustrate the underlying mechanisms of the ionization process. It is revealed that in the major part of the below-the-barrier ionization regime, in an intense and short infrared pulse, the electron does not tunnel \through" the entire barrier, but rather alrea…
The elaborate energy and momentum spectra of ionized electrons from atoms in laser fields suggest that the ionization dynamics described by tunneling theory should be modified. Although many efforts have been done within semiclassical models, there are few discussions describing multiphoton absorption process with quantum framework. In this letter, by comparing the results obtained with the time-dependent Schrodinger equation (TDSE) and Keldysh-Faisal-Reiss (KFR) theory, we have studied the nonperturbative effects of ionization dynamics beyond KFR theory. The difference in momentum spectra bet…
Pulsed field ionization of high-$n$ (90 $\leq n \leq$ 150) manifold states in Rb Rydberg atoms has been investigated in high slew-rate regime. Two peaks in the field ionization spectra were systematically observed for the investigated $n$ region, where the field values at the lower peak do not almost depend on the excitation energy in the manifold, while those at the higher peak increase with increasing excitation energy. The fraction of the higher peak component to the total ionization signals increases with increasing $n$, exceeding 80% at $n$ = 147. Characteristic behavior of the peak compo…
We study ionization of atoms in strong elliptically-polarized laser fields. We focus on the physical origin of the offset angle in the photoelectron momentum distribution and its possible relation to a specific time. By developing a model which is based on strong-field approximation and considers the classical Coulomb scattering, we are able to quantitatively explain recent attoclock experiments in a wide region of laser and atomic parameters. The offset angle can be understood as arising from the scattering of the electron by the ionic potential when the electron exits the laser-Coulomb-forme…
We study ionization of atoms in strong two-dimensional (2D) laser fields with various forms, numerically and analytically. We focus on the local most-probable tunneling routes (some specific electron trajectories) which are corresponding to the local maxima of photoelectron momentum distributions (PMDs). By making classic-quantum correspondence, we obtain a condition for these routes characterized by the electron position at the tunnel exit. With comparing the identified routes with the classical limit and the partial-decoupling approximation where it is assumed that tunneling is dominated by …
High-resolution photoelectron momentum distributions of Xe atoms ionized by 800-nm linearly polarized laser fields have been traced at intensities from 1.1*1013 to 3.5*1013W/cm2 using velocity-map imaging techniques. At certain laser intensities, the momentum spectrum exhibits a distinct double-ring structure for low-order above-threshold ionization, which appears to be absent at lower or higher laser intensities. By investigating the intensity-resolved photoelectron energy spectrum, we find that this double-ring structure originates from resonant multiphoton ionization involving multiple Rydb…
We present a theoretical study of the dissociative tunneling ionization process. Analytic expressions for the nuclear kinetic energy distribution of the ionization rates are derived. A particularly simple expression for the spectrum is found by using the Born-Oppenheimer (BO) approximation in conjunction with the reflection principle. These spectra are compared to exact non-BO ab initio spectra obtained through model calculations with a quantum mechanical treatment of both the electronic and nuclear degrees freedom. In the regime where the BO approximation is applicable imaging of the BO nucle…
Double ionization of an atom by single-photon absorption in the presence of a neighbouring atom is studied. The latter is, first, resonantly photoexcited and, afterwards, transfers the excitation energy radiationlessly to the other atom, leading to its double ionization. The process relies on the combined effect of interatomic and intraatomic electron correlations. It can dominate over the direct double photoionization by several orders of magnitude at interatomic distances up to few nanometers. The relative position of the neighbouring atom is shown to exert a characteristic influence on the …
We investigate the ionization dynamics of Argon atoms irradiated by an ultrashort intense laser of a wavelength up to 3100 nm, addressing the momentum distribution of the photoelectrons with near-zero-energy. We find a surprising accumulation in the momentum distribution corresponding to meV energy and a \textquotedblleft V"-like structure at the slightly larger transverse momenta. Semiclassical simulations indicate the crucial role of the Coulomb attraction between the escaping electron and the remaining ion at extremely large distance. Tracing back classical trajectories, we find the tunneli…
Recently, in a strong Coulomb field regime of tunneling ionization an unexpected large enhancement of photoelectron spectra due to the Coulomb field of the atomic core has been identified by numerical solution of time-dependent Schrödinger equation [Phys. Rev. Lett. \textbf{117}, 243003 (2016)] in the upper energy range of the tunnel-ionized direct electrons. We investigate the origin of the enhancement employing a classical theory with Monte Carlo simulations of trajectories, and a quantum theory of Coulomb-corrected strong field approximation based on the generalized eikonal approximation fo…
Photoelectron angular distributions following the non-resonant two-photon K-shell ionization of neutral atoms are studied theoretically. Using the independent particle approximation and relativistic second-order perturbation theory, the contributions of screening and relativistic effects to the photoelectron angular distribution are evaluated. A simple nonrelativistic expression is presented for the angle-differential cross section in dipole approximation for two-photon ionization by elliptically polarized photons, and its limitations are analyzed numerically. Moreover, we show that screening …
Interaction of a strong laser pulse with matter transfers not only energy but also linear momentum of the photons. Recent experimental advances have made it possible to detect the small amount of linear momentum delivered to the photoelectrons in strong-field ionization of atoms. We present numerical simulations as well as an analytical description of the subcycle phase (or time) resolved momentum transfer to an atom accessible by an attoclock protocol. We show that the light-field-induced momentum transfer is remarkably sensitive to properties of the ultrashort laser pulse such as its carrier…
Ionization of an atom or molecule presents surprising richness beyond our current understanding: strong-field ionization with low-frequency fields recently revealed unexpected kinetic energy structures (1, 2). A solid grasp on electron dynamics is however pre-requisite for attosecond-resolution recollision imaging (3), orbital tomography (4), for coherent sources of keV light (5), or to produce zeptosecond-duration x-rays (6). We present a methodology that enables scrutinizing strong-field dynamics at an unprecedented level. Our method provides high-precision measurements only 1 meV above the …
Interaction of a strong laser pulse with matter transfers not only energy but also linear momentum of the photons. Recent experimental advances have made it possible to detect the small amount of linear momentum delivered to the photoelectrons in strong-field ionization of atoms. Linear momentum transfer is a unique signature of the laser-atom interaction beyond its dipolar limit. Here, we present a decomposition of the subcycle time-resolved linear momentum transfer in term of its multipolar components. We show that the magnetic dipole contribution dominates the linear momentum transfer durin…
The non-resonant two-photon one-electron ionization of neutral atoms is studied theoretically in the framework of relativistic second-order perturbation theory and independent particle approximation. In particular, the importance of relativistic and screening effects in the total two-photon ionization cross section is investigated. Detailed computations have been carried out for the K-shell ionization of neutral Ne, Ge, Xe, and U atoms. The relativistic effects significantly decrease the total cross section, for the case of U, for example, they reduce the total cross section by a factor of two…
We study a feasibility of precision measurements of surface potentials at micrometer distances using resonant tunneling of cold atoms trapped in vertical optical lattices. A modulation of an amplitude of the lattice potential induces atomic tunneling among the lattice sites. The resonant modulation frequency corresponds to a difference of potential energy between latices sites which is defined by external force i.e. gravity. The vicinity of the surface alters the external potentials, and hence the resonant frequency. Application of this method allows accurate study of Casimir-type potentials a…
Molecules show a much increased multiple ionization rate in a strong laser field as compared to atoms of similar ionization energy. A widely accepted model attributes this to the action of the joint fields of the adjacent ionic core and the laser on its neighbor inside the same molecule. The underlying physical picture for the enhanced ionization is that the up-field atom that gets ionized. However, this is still debated and remains unproven. Here we report an experimental verification of this long-standing prediction. This is accomplished by probing the two-site double ionization of ArXe, whe…
The photoelectron momentum distribution in the strong-field ionization has a variety of structures that reveal the complicated dynamics of this process. Recently, we identified a low-energy interference structure in the case of a super-intense extreme ultraviolet (XUV) laser pulse and attributed it to the laser-induced electron Fresnel diffraction. This structure is determined by the laser-induced electron displacement [Geng L et al. 2021 Phys. Rev. A 104(2) L021102]. In the present work, we find that the Fresnel diffraction picture is also present in the tunneling and over-barrier regime of i…
In this paper, we theoretically study x-ray multiphoton ionization dynamics of heavy atoms taking into account relativistic and resonance effects. When an atom is exposed to an intense x-ray pulse generated by an x-ray free-electron laser (XFEL), it is ionized to a highly charged ion via a sequence of single-photon ionization and accompanying relaxation processes, and its final charge state is limited by the last ionic state that can be ionized by a single-photon ionization. If x-ray multiphoton ionization involves deep inner-shell electrons in heavy atoms, energy shifts by relativistic effect…
We theoretically study the pulse-width dependence of the photoelectron angular distribution (PAD) from the resonance-enhanced two-photon single ionization of He by femtosecond ($\lesssim 20$ fs) extreme-ultraviolet pulses, based on the time-dependent perturbation theory and simulations with the full time-dependent Schrödinger equation. In particular, we focus on the competition between resonant and nonresonant ionization paths, which leads to the relative phase $δ$ between the $S$ and $D$ wave packets distinct from the corresponding scattering phase shift difference. When the spectrally broade…
We investigate the physical processes in which an electron, upon return to its parent ion, promotes a second electron to an excited state, from which it subsequently tunnels. Employing the strong-field approximation and saddle-point methods, we perform a detailed analysis of the dynamics of the two electrons, in terms of quantum orbits, and delimit constraints for their momentum components parallel to the laser-field polarization. The kinetic energy of the first electron, upon return, exhibits a cutoff slightly lower than $10U_p$, where $U_p$ is the ponderomotive energy, as in rescattered abov…
Resonance ionization laser ion sources are efficient and element selective ion sources, which are particularly well suited for radioactive ion beam facilities. Using TRIUMF's off-line laser ion source test stand with a system of tunable titanium sapphire (Ti:Sa) lasers, laser resonance ionization schemes for lutetium and praseodymium have been investigated with a particular interest to autoionizing states. New ionization schemes via Rydberg states and autoionizing states were found. Their investigation and comparison of ion yields at the off-line test stand will be discussed, and the data of o…
Vortex photoelectron holography in strong-field tunneling ionization
School of Physics and Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology（华中科技大学物理科学与技术学院与武汉光电国家研究中心）；Moscow Institute of Physics and Technology（莫斯科物理技术学院）；Institute for Advanced Science, The University of Electro-Communications（电波大学高级科学研究所）；Hubei Fundamental Research Center for Physics（湖北物理基础研究中心）
The Salecker-Wigner-Peres quantum-clock approach is applied in order to determine the tunneling time of an electron in strong-field tunnel ionization via a time-dependent electric field. Our results show that the ionization of the electron takes a nonvanishing period of time. This tunneling time is of the order of the Keldysh time but strictly larger than the Keldysh time. Comparing the quantum-clock tunneling time to the mean tunneling time as obtained by the virtual-detector approach, one finds that these two complementary methods give very similar results. Due to the asymmetric distribution…
We present a detailed comparison of strong-field ionization of diatomic molecules and their companion atoms with nearly equal ionization potentials. We perform calculations in the length and velocity gauge formulations of the molecular strong-field approximation and with the molecular tunneling theory, and in both cases we consider effects of nuclear motion. A comparison of our results with experimental data shows that the length gauge strong-field approximation gives the most reliable predictions.
In the strong field molecular tunneling ionization theory of Tong et al. [Phys. Rev. A 66, 033402 (2002)], the ionization rate depends on the asymptotic wavefunction of the molecular orbital from which the electron is removed. The orbital wavefunctions obtained from standard quantum chemistry packages in general are not good enough in the asymptotic region. Here we construct a one-electron model potential for several linear molecules using density functional theory (DFT). We show that the asymptotic wavefunction can be improved with an iteration method and after one iteration accurate asymptot…
Tunneling times in atomic ionization are studied theoretically by a virtual detector approach. A virtual detector is a hypothetical device that allows one to monitor the wave function's density with spatial and temporal resolution during the ionization process. With this theoretical approach, it becomes possible to define unique moments when the electron enters and leaves with highest probability the classically forbidden region from first principles and a tunneling time can be specified unambiguously. It is shown that neither the moment when the electron enters the tunneling barrier nor when …
We revisit a recently proposed scheme [M.F. Ciappina et al 2019 Phys. Rev. A 99 043405] for accurate measurement of electromagnetic radiation intensities in a focus of high-power laser beams. The method is based on the observation of multiple sequential tunneling ionization of atoms and suggests the determination of the peak intensity value from the appearance in the focal area ions with a certain charge number. Here we study the sensitivity of the approach to two essential factors: the focal volume effect and the tunneling ionization model chosen to calculate ionization rates. We show, on the…
We coincidently measure the molecular frame photoelectron angular distribution and the ion sum-momentum distribution of single and double ionization of CO molecules by using circularly and elliptically polarized femtosecond laser pulses, respectively. The orientation dependent ionization rates for various kinetic energy releases allow us to individually identify the ionizations of multiple orbitals, ranging from the highest occupied to the next two lower-lying molecular orbitals for various channels observed in our experiments. Not only the emission of a single electron, but also the sequentia…
The intermediate domain of strong-field ionization between the tunneling and the multiphoton regimes is investigated using the strong field approximation and the imaginary-time method. An intuitive model for the dynamics is developed which describes the ionization process within a nonadiabatic tunneling picture with a coordinate dependent electron energy during the under-the-barrier motion. The nonadiabatic effects in the elliptically polarized laser field induce a transversal momentum shift of the tunneled electron wave packet at the tunnel exit, a delayed appearance in the continuum as well …
We use a quantum trajectory-based semi-classical method to account for Coulomb interaction between the photoelectron and the parent ion in the classically forbidden, sub-barrier region during strong-field tunneling ionization processes. We show that---besides the well-known modification of the tunneling ionization probability---there is also an influence on the interference pattern in the photoelectron spectra. In the long-wavelength limit, the shift of the intra-cycle interference fringes caused by sub-barrier Coulomb effects in the laser polarization direction can be derived analytically. We…
Classically allowed transport is shown to compete with quantum tunneling during the ionization of atoms by ultrashort and intense laser pulses, despite Keldysh parameters smaller than unity. This is done by comparing exact probability densities with the ones obtained from purely classical propagation using the Truncated Wigner Approximation. Not only is classical transport capable of moving trajectories away from the core, but it can also furnish ionization probabilities of the same order as the quantum ones for intensities currently employed in experiments. Our results have implications rangi…
We present a practical numerical technique for calculating tunneling ionization rates from arbitrary 1-D potential wells in the presence of a linear external potential by determining the widths of the resonances in the spectral density, rho(E), adiabatically connected to the field-free bound states. While this technique applies to more general external potentials, we focus on the ionization of electrons from atoms and molecules by DC electric fields, as this has an important and immediate impact on the understanding of the multiphoton ionization of molecules in strong laser fields.
The electron dynamics in the classically forbidden region during relativistic tunnel-ionization is investigated. The classical forbidden region in the relativistic regime is identified by defining a gauge invariant total energy operator. Introducing position dependent energy levels inside the tunneling barrier, we demonstrate that the relativistic tunnel-ionization can be well described by a one-dimensional intuitive picture. This picture predicts that, in contrast to the well-known nonrelativistic regime, the ionized electron wave packet arises with a momentum shift along the laser's propagat…
It is shown that it is feasible to use ultrashort time delay between two XUV femtosecond pulses in order to control two photon resonant ionization. The proposal is demonstrated on the spectrum of Helium, in terms of nonperturbative solutions of the time dependent Schroedinger equation. Comparison with results from second order time dependent perturbation theory provides additional insight.
The electron nondipole dynamics in tunneling ionization in an elliptically polarized laser field is investigated theoretically using a relativistic Coulomb-corrected strong-field approximation (SFA) based on the eikonal approximation of the Klein-Gordon equation. We calculate attoclock angle-resolved light-front momentum distributions at different ellipticities of the laser field in quasistatic and nonadiabatic regimes and analyze them with an improved Simpleman model. The nondipole correlations between longitudinal and transverse momentum components are examined. Deviations of the photoelectr…
Photoionization of an atom $A$, in the presence of a neighboring atom $B$, can proceed via resonant excitation of $B$ with subsequent energy transfer to $A$ through two-center electron-electron correlation. We demonstrate that this two-center mechanism can strongly outperform direct photoionization at nanometer internuclear distances and possesses characteristic features in its time development and the spectrum of emitted electrons.
We unravel the out-of-equilibrium quantum dynamics of a few interacting bosonic clouds in a two-dimensional asymmetric double-well potential at the resonant tunneling scenario. At the single-particle level of resonant tunneling, particles tunnel under the barrier from, typically, the ground-state in the left well to an excited state in the right well, i.e., states of different shapes and properties are coupled when their one-particle energies coincide. In two spatial dimensions, two types of resonant tunneling processes are possible, to which we refer to as longitudinal and transversal resonan…
We suggest that electron-laser interactions can give rise to resonance phenomena as the intensity varies. A new QED perturbation theory is developed, in which the coupling between an electron and the second quantized laser mode is treated nonperturbatively. We predict, for example, the above-threshold ionization rate shows peaks at intensities with integer ponderomotive parameter. Such quantum resonance effects may be exploited to calibrate laser intensities in appropriate range.
We study resonant two-color two-photon ionization of Helium via the 1s3p 1P1 state. The first color is the 15th harmonic of a tunable titanium sapphire laser, while the second color is the fundamental laser radiation. Our method uses phase-locked high-order harmonics to determine the {\it phase} of the two-photon process by interferometry. The measurement of the two-photon ionization phase variation as a function of detuning from the resonance and intensity of the dressing field allows us to determine the intensity dependence of the transition energy.
