A simple model for sequential multiphoton ionization by ultra-intense x-rays is presented. The derived scaling of the ion yield with pulse energy quantitatively reproduces the experimental data, which shows that the ion yield increases according to the "power law" behavior typical of multiphoton ionization, followed by saturation at high pulse energies. The calculated average time interval between ionizations for producing ions at a certain charge state is found to be proportional to the pulse duration and independent of all other x-ray pulse parameters. This agrees with previous studies where the kinetic energy of fragment ions with a given charge state produced by intense x-ray ionization of molecules was found to be independent of the pulse energy, but to increase with smaller pulse duration due to the smaller time interval between ionizations.
We present a theory illuminating the cross-over from strong-field tunnelling ionization to weak-field multiphoton ionization in the interaction of a classical laser field with a hydrogen atom. A simple formula is derived in which the ionization amplitude appears as a product of two separate amplitudes. The first describes the initial polarization of the atom by virtual multiphoton absorption and the second the subsequent tunnelling out of the polarized atom. Tunnelling directly from the ground state and multiphoton absorption without tunnelling appear naturally as the limits of the theory.
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…
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…
The multiphoton ionization and photoelectron spectra of magnesium were studied at laser intensities of up to 6x10^{13} Wcm^{-2} using 150 fs laser pulses of a wavelength of 400 nm. The results indicated that a variety of different ionization mechanisms played a role in both types of spectra. A theoretical model describing the processes is presented and the routes to ionization are identified. The work demonstrates the significance of the two-electron nature of the atom in interpreting the experimental results.
We present a theoretical method for calculating multiphoton ionization amplitudes and cross sections of few-electron atoms. The present approach is based on an extraction of partial wave amplitudes from a scattering wave function, which is calculated by solving a system of driven Schroedinger equations. The extraction relies on a description of partial waves in terms of a small number of Coulomb waves with fixed wave numbers. The method can be used for photon energies below and above the ionization threshold and to treat resonance-enhanced multiphoton ionization. We use it to calculate two-, t…
We theoretically study multiphoton ionization through the triplet states of Mg by linearly polarized (LP) and circularly polarized (CP) fs laser pulses. After the construction of the atomic basis using the frozen-core Hartree-Fock potential (FCHFP) as well as the model potential (MP) approaches for both singlet and triplet series which show rather good agreements with the existing data in terms of state energies and dipole matrix elements, we solve time-dependent Schrödinger equations with $3s3p$ $^{3}P_{1}$ as an initial state, and calculate the total ionization yield and photoelectron energy…
Multiphoton ionization of sodium by femtosecond laser pulses of 800 nm wavelength in the range of laser peak intensities entering over-the-barrier ionization domain is studied. Photoelectron momentum distributions and the energy spectra are determined numerically by solving the time dependent Schroedinger equation for three values of the laser intensity from this domain. The calculated spectra agree well with the spectra obtained experimentally by Hart et al (Phys. Rev. A 2016 93 063426). A partial wave analysis of the spectral peaks related to Freeman resonances has shown that each peak is a …
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…
The dynamics of the electron impact multiphoton ionization of a hydrogen atom in the presence of an intense laser field has been studied theoretically, with a view to comparing (qualitatively) the results with the recent kinematically complete experiments of Horr et al [ Phys. Rev. Lett., vol. 94, 153201, (2005) ] for the He target. Significant laser modifications are noted in the present doubly (DDCS) and the fully differential cross sections (TDCS). For most of the explored kinematics (chosen in accordance with the experiment), the present binary peak intensity of the laser-assisted TDCS is …
Multiphoton ionization of sodium by laser pulses of 800 nm wavelength and 57 fs duration is studied in the range of laser peak intensities belonging to over-the-barrier ionization regime. Photoelectron momentum distributions (PMD) and the energy spectra are determined numerically by solving the time dependent Schrödinger equation. The calculated spectra agree well with the spectra obtained experimentally by Hart et al. [Phys. Rev. A 93, 063426 (2016)]. The contributions of photoelectrons with different values of the orbital quantum number in the PMD are determined by expanding the photoelectro…
We provide a detailed quantitative study of the possible role of a small admixture of harmonics on resonant two-photon ionization. The motivation comes from the occasional presence of 2nd and 3rd harmonics in FEL radiation. We obtain the dependence of ionic yields on the intensity of the fundamental, the percentage of 2nd harmonic and the detuning of the fundamental from resonance. Having examined the cases of one and two intermediate resonances, we arrive at results of general validity and global behavior, showing that even a small amount of harmonic may seem deceptively innocuous.
We report on the observation of phase space modulations in the correlated electron emission after strong field double ionization of helium using laser pulses with a wavelength of 394~nm and an intensity of $3\cdot10^{14}$W/cm$^2$. Those modulations are identified as direct results of quantum mechanical selection rules predicted by many theoretical calculations. They only occur for an odd number of absorbed photons. By that we attribute this effect to the parity of the continuum wave function.
We calculate two-dimensional photoelectron momentum distributions and energy spectra after multiphoton ionization of Li atoms subject to intense laser fields in one-photon Rabi-flopping regime. The time-dependent Schrödinger equation is solved within the single-active-electron approximation using a model potential which reproduces accurately the binding energies and dipole matrix elements of the Li atom. Interaction with the external electromagnetic field is treated within the dipole approximation. We show that the Rabi oscillations of the population between the ground $2s$ state and the excit…
The Autler-Townes effect due to near resonance transition between 4s-4p states in potassium atoms is mapped out in the photo-electron-momentum distribution and manifests itself as a splitting in the photo-electron kinetic energy spectra. The energy splitting fits well with the calculated Rabi frequency at low laser intensities and shows clear deviation at laser intensities above 1.5x10^11 W/cm^2. An effective Rabi frequency formulae including the ionization process explains the observed results. Our results reveal the possibility to tune the effective coupling strength with the cost of the num…
We theoretically study multiphoton ionization of the Ca atom irradiated by the second (photon energy 3.1 eV) and third (photon energy 4.65 eV) harmonics of Ti:sapphire laser pulses (photon energy 1.55 eV). Because of the dense energy level structure the second and third harmonics of a Ti:sapphire laser are nearly single-photon resonant with the ${4s4p}$ $^1P^o$ and ${4s5p}$ $^1P^o$ states, respectively. Although two-photon ionization takes place through the near-resonant intermediate states with the same symmetry in both cases, it turns out that there are significant differences between them. …
With quantum calculations, we have investigated the multiphoton nonsequential double ionization of helium atoms in intense laser fields at ultraviolet wavelengths. Very surprisingly, we find a so-far unobserved double-circle structure in the correlated electron momentum spectra. The double-circle structure essentially reveals multiphoton Rabi oscillations of two electrons, which are strongly supported by the oscillating population of a certain doubly excited state and by the oscillating double ionization signals. This two-electron multiphoton Rabi effect provides profound understandings of ele…
In this paper we report the theoretical results obtained for partial ionization yields and the above-threshold ionization (ATI) spectra of Magnesium in a Ti:sapphire laser field (804 nm) in the range of short pulse duration (20-120 fs). Ionization yield, with linearly polarized light for a 120 fs laser pulse, is obtained as a function of the peak intensity motivated by recent experimental data \cite{gillen:2001}. For this, we have solved the time-dependent Schrödinger equation nonperturbatively on a basis of discretized states obtained with two different methods; one with the two-electron wave…
We apply time-dependent R-matrix theory to study inner-shell ionization of C atoms in ultra-short high-frequency light fields with a photon energy between 170 and 245 eV. At an intensity of 10$^{17}$ W/cm$^2$, ionization is dominated by single-photon emission of a $2\ell$ electron, with two-photon emission of a 1s electron accounting for about 2-3\% of all emission processes, and two-photon emission of $2\ell$ contributing about 0.5-1\%. Three-photon emission of a 1s electron is estimated to contribute about 0.01-0.03\%. Around a photon energy of 225 eV, two-photon emission of a 1s electron, l…
We present a study of multiphoton dissociative ionization from molecules. By solving the time-dependent Schrödinger equation for H$_2^+$ and projecting the solution onto double continuum scattering states, we observe the correlated electron-nuclear ionization dynamics in detail. We show --- for the first time --- how multiphoton structure prevails as long as the energies of all fragments are accounted for. Our current work provides a new avenue to analyze strong-field fragmentation that leads to a deeper understanding of the correlated molecular dynamics.
We have investigated multiphoton multiple ionization dynamics of argon and xenon atoms using a new x-ray free electron laser (XFEL) facility, SPring-8 Angstrom Compact free electron LAser (SACLA) in Japan, and identified that highly charged Xe ions with the charge state up to +26 are produced predominantly via four-photon absorption as well as highly charged Ar ions with the charge state up to +10 are produced via two-photon absorption at a photon energy of 5.5 keV. The absolute fluence of the XFEL pulse, needed for comparison between theory and experiment, has been determined using two-photon…
We address the concept of direct multiphoton multiple ionization in atoms exposed to intense, short wavelength radiation and explore the conditions under which such processes dominate over the sequential. Their contribution is shown to be quite robust, even under intensity fluctuations and interaction volume integration, and reasonable agreement with experimental data is also found.
In this paper, we extend the results of an earlier paper in which we had demonstrated the limitations of the notion of non-resonant multiphoton ionization, in the exploration of photon statistics effects in non-linear processes. Through the quantitative analysis of specific realistic processes, we provide the connection to conditions of intensity and pulse duration necessary in relevant experiments, including a recent seminal experiment demonstrating the effect of superbunching found in squeezed radiation.
Despite inherently complex multiphoton dynamics, our observations show that Ba double ionization with an infrared laser (8800-8920 cm^{-1}) resembles a single-photon process; namely, its probability is proportional to the laser intensity. In this regime, single-electron ionization is due to a four-photon resonant transition through the highly perturbed state 6p^2 1D_2, whereas double ionization is realized by the two-electron mechanism. Furthermore, we argue that these conclusions are valid for other alkaline-earth-metal atoms and other parameters of laser radiation.
The coherent radiation spectrum of two-level polar molecules with UV transition is studied at the multiphoton resonant excitation by a moderately strong laser field. The spectrum corresponding to harmonic generation and low-frequency radiation is investigated both analytically and numerically. Specifically, a mechanism for generation of intense smoothly tunable terahertz radiation by two-level molecular configurations (with dynamic Stark shifts) possessing permanent dipole moments, is considered.
Approximate scaling laws with respect to the nuclear charge are introduced for the time-dependent Dirac equation describing hydrogen-like ions subject to laser fields within the dipole approximation. In particular, scaling relations with respect to the laser wavelengths and peak intensities are discussed. The validity of the scaling relations is investigated for two-, three-, four-, and five-photon ionization of hydrogen-like ions with the nuclear charges ranging from $Z=1$ to $92$ by solving the corresponding time-dependent Dirac equations adopting the properly scaled laser parameters. Good a…
We report on the production of cold, state-selected H$_2^+$ molecular ions in a linear RF trap. The ions are produced by (3+1) resonance-enhanced multi-photon ionisation (REMPI) of H$_2$, and sympathetically cooled by laser-cooled Be$^+$ ions. After demonstrating and characterizing the REMPI process, we use photodissociation by a deep UV laser at 213~nm to verify the high vibrational purity of the produced H$_2^+$ ion samples. Moreover, the large difference between the photodissociation efficiencies of ions created in the $v=0$ and $v=1$ levels provides a way to detect a $v=0 \to 1$ transition…
A theoretical study of the intense-field multiphoton ionization of hydrogenlike systems is performed by solving the time-dependent Dirac equation within the dipole approximation. It is shown that the velocity-gauge results agree to the ones in length gauge only if the negative-energy states are included in the time propagation. On the other hand, for the considered laser parameters, no significant difference is found in length gauge if the negative-energy states are included or not. Within the adopted dipole approximation the main relativistic effect is the shift of the ionization potential. A…
In a recent experiment at the VUV free-electron laser facility at DESY in Hamburg, the generation of multiply charged ions in a gas of atomic xenon was observed. This paper develops a theoretical description of multiphoton ionization of xenon and its ions. The numerical results lend support to the view that the experimental observation may be interpreted in terms of the nonlinear absorption of several VUV photons. The method rests on the Hartree-Fock-Slater independent-particle model. The multiphoton physics is treated within a Floquet scheme. The continuum problem of the photoelectron is solv…
Ab initio simulations of a range of interferometric experiments are used to identify a strong dependence on multiphoton phase shifts in above-threshold ionization. A simple rule of thumb for interaction phase shifts is derived to explain both the conservation of photoelectron yield and its absolute CEP-dependence. For instance, it is found that interferometric above-threshold ionization experiments are shifted by $π/4$ relative to RABBIT experiments, and that there is no RABBIT-term in a laser-assisted photoionization experiment with odd and even harmonics. Thus, our work helps to resolve the …
Anomalous Autler-Townes Splitting in Resonant Multiphoton Ionization Driven by Bright Squeezed Vacuum
Huazhong University of Science and Technology（华中科技大学）；Shanghai Jiao Tong University（上海交通大学）；Technion–Israel Institute of Technology（以色列理工学院）；Guangdong Technion–Israel Institute of Technology（广东以色列理工学院）
We investigate molecular dynamics of multiple ionization in N2 through multiple core-level photoabsorption and subsequent Auger decay processes induced by intense, short X-ray free electron laser pulses. The timing dynamics of the photoabsorption and dissociation processes is mapped onto the kinetic energy of the fragments. Measurements of the latter allow us to map out the average internuclear separation for every molecular photoionization sequence step and obtain the average time interval between the photoabsorption events. Using multiphoton ionization as a tool of multiple-pulse pump-probe …
Here, we report on the nonlinear ionization of argon atoms in the short wavelength regime using ultraintense x rays from the European XFEL. After sequential multiphoton ionization, high charge states are obtained. For photon energies that are insufficient to directly ionize a $1s$ electron, a different mechanism is required to obtain ionization to Ar$^{17+}$. We propose this occurs through a two-color process where the second harmonic of the FEL pulse resonantly excites the system via a $1s \rightarrow 2p$ transition followed by ionization by the fundamental FEL pulse, which is a type of x-ray…
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 report on a kinematically complete experiment on strong field double ionization of helium using laser pulses with a wavelength of 394\,nm and intensities of $3.5-5.7\times10^{14}\,W/cm^2$. Our experiment reaches the most complete level of detail which previously has only been reached for single photon double ionization. We give an overview over the observables on many levels of integration, starting from the ratio of double to single ionization, the individual electron and ion momentum distributions over joint momentum and energy distributions to fully differential cross sections showing th…
The coherent control of electron beams and ultrafast electron wave packets dynamics have attracted significant attention in electron microscopy as well as in atomic physics. In order to unify the conceptual pictures developed in both fields, we demonstrate the generation and manipulation of tailored electron orbital angular momentum (OAM) superposition states either by employing customized holographic diffraction masks in a transmission electron microscope or by atomic multiphoton ionization utilizing pulse-shaper generated carrier-envelope phase stable bichromatic ultrashort laser pulses. Bot…
Ionization by relativistically intense laser pulses of finite duration is considered in the framework of strong-field quantum electrodynamics. Our main focus is on the formation of ionization supercontinua. More specifically, when studying the energy distributions of photoelectrons ionized by circularly polarized pulses, we observe the appearance of broad structures lacking the interference patterns. These supercontinua extend over hundreds of driving photon energies, thus corresponding to high-order nonlinear processes. The corresponding polar-angle distributions show asymmetries which are at…
Application of a parallel-projection inversion technique to z-scan spectra of multiply charged xenon and krypton ions, obtained by non-resonant field ionization of neutral targets, has for the first time permitted the direct observation of intensity-dependent ionization probabilities. These ionization efficiency curves have highlighted the presence of structure in the tunnelling regime, previously unobserved under full-volume techniques.
Trapping cold, chemically important molecules with electromagnetic fields is a useful technique to study small molecules and their interactions. Traps provide long interaction times that are needed to precisely examine these low density molecular samples. However, the trapping fields lead to non-uniform molecular density distributions in these systems. Therefore, it is important to be able to experimentally characterize the spatial density distribution in the trap. Ionizing molecules in different locations in the trap using resonance enhanced multiphoton ionization (REMPI) and detecting the re…
We provide theoretical investigations of the response of the Ar and H atoms to an intense elliptically polarized few-cycle laser pulse, as a function of light ellipticity. The time-dependent Schr{ö}dinger equation describing the least-bound electron is solved numerically, and differential quantities such as the momentum distribution, the electron density in the continuum, and the above-threshold ionization spectra are computed. These quantities provide insight into the ionization dynamics and the electron rescattering process as a function of light ellipticity, and reveal great similarities be…
We present a multichannel photoelectron interferometry technique based on trichromatic pulse shaping for unambiguous determination of quantum phases in multiphoton ionization (MPI) of potassium atoms. The colors of the laser field are chosen to produce three energetically separated photoelectron interferograms in the continuum. While the red pulse is two-photon resonant with the $3d$-state resulting in a (2+1) resonance-enhanced MPI (REMPI), a (1+2) REMPI occurs via the non-resonant intermediate $4p$-state with an initial green or blue pulse. We show that ionization via a non-resonant intermed…
The alignment- and internuclear-distance dependent ionization of H$_2$ exposed to intense, ultrashort laser fields is studied by solving the time-dependent two-electron Schrödinger equation. In the regime of perturbative few-photon ionization, a strong dependence of the ionization yield on the internuclear distance is found. While this finding confirms a previously reported breakdown of the fixed-nuclei approximation for parallel alignment, a simpler explanation is provided and it is demonstrated that this breakdown is not due to vibrational dynamics during the laser pulse. The persistence of …
We examine the nature and statistical properties of electron-electron collisions in the recollision process in a strong laser field. The separation of the double ionization yield into sequential and nonsequential components leads to a bell-shaped curve for the nonsequential probability and a monotonically rising one for the sequential process. We identify key features of the nonsequential process and connect our findings in a simplified model which reproduces the knee shape for the probability of double ionization with laser intensity and associated trends.
This paper concerns the theory of non-recollisional ionization or detachment of atoms or ions by intense few-cycle pulses. It is shown that in certain conditions of pulse duration, peak intensity and carrier-envelope phase, the ionization probability integrated over ejection angle varies almost periodically with energy, with a period roughly equal to the photon energy for slow enough outgoing electrons. This modulation is found both in calculations based on the strong field approximation (SFA) and in ab initio time-dependent calculations. It is explained as resulting from the interference betw…
We examine correlated electron and doubly charged ion momentum spectra from strong field double ionization of Neon employing intense elliptically polarized laser pulses. An ellipticity-dependent asymmetry of correlated electron and ion momentum distributions has been observed. Using a 3D semiclassical model, we demonstrate that our observations reflect the sub-cycle dynamics of the recollision process. Our work reveals a general physical picture for recollision-impact double ionization with elliptical polarization, and demonstrates the possibility of ultrafast control of the recollision dynami…
We 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…
The ionization probability of N$_2$, O$_2$, and CO$_2$ in intense laser fields is studied theoretically as a function of the alignment angle by solving the time-dependent Schrödinger equation numerically assuming only the single-active-electron approximation. The results are compared to recent experimental data [D.~Pavi{č}i{ć} et al., Phys.\,Rev.\,Lett.\ {\bf 98}, 243001 (2007)] and good agreement is found for N$_2$ and O$_2$. For CO$_2$ a possible explanation is provided for the failure of simplified single-active-electron models to reproduce the experimentally observed narrow ionization dist…
We investigate the dynamics of electron-electron recollisions in the double ionization of atoms in strong laser fields. The statistics of recollisions can be reformulated in terms of an area-preserving map from the observation that the outer electron is driven by the laser field to kick the remaining core electrons periodically. The phase portraits of this map reveals the dynamics of these recollisions in terms of their probability and efficiency.
In this paper a 4-component Dirac theory of ionization of hydrogen molecular ion in a super-intense laser field is developed. Simple analytic expressions for the spin specific as well as the total ionization currents emitted from the ground state of the ion are derived. The results are given for all polarization and finite propagation vectors of the field. They apply for inner-shell ionization of analogous heavier molecular ions as well. The presence of molecular two-slit interference effect, first found in the non-relativistic case, and the spin-flip ionization current, and an asymmetry of th…
Diatomic molecules (e.g., O$_2$) in intense laser field exhibit a peculiar suppressed ionization behavior compared to their companion atoms. Several physical models have been proposed to account for this suppression while no consensus has been achieved. In this letter, we aim to clarify the underlying mechanisms behind this molecular ionization suppression. Experimental data recorded at midinfrared laser wavelength and its comparison with that at near-infrared wavelength revealed a peculiar wavelength and intensity dependence of the suppressed ionization of O$_2$ with respect to its companion …
Ionization and excitation of water molecules in intense laser pulses is studied theoretically by solving the three-dimensional time-dependent electronic Schrödinger equation within the single-active-electron approximation. The possibility to image orbital densities by measurement of the orientation-dependent ionization of H2O in few-cycle, 800nm linear-polarized laser pulses is investigated. While the highest-occupied molecular orbital 1b1 is found to dominate the overall ionization behavior, contributions from the energetically lower lying 3a1 orbital dominate the ionization yield in the noda…
