We present an experimental study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral argon atoms. Using 9.3 eV photons produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and ions produced from non-resonant two-photon ionization in coincidence. Photoionization from the $3p$ orbital produces a photoelectron scattering wave function with $p$ and $f$ partial wave components, which interfere and result in a photoelectron angular distribution with peak amplitude perpendicular to the VUV polarization. The comparison between the present results and two previous sets of theoretical calculations [Pan, C. & Starace, A. F. (1991). $\textit{Physical Review A}$, 44(1), 324., and Moccia, R., Rahman, N. K., & Rizzo, A. (1983). $\textit{Journal of Physics B: Atomic and Molecular Physics}$, 16(15), 2737.] indicates that electron-electron correlation contributes appreciably to the two-photon ionization dynamics.
The role of nucleus in strong-field nonsequential double ionization of Ar atoms is investigated using three-dimensional classical ensembles. By adjusting the nuclear Coulomb potential, we can excellently reproduce the experimental correlated electron and ion momentum spectra with laser intensities above the recollision threshold [Phys. Rev. Lett. 93, 263001 (2004)] and below the recollision threshold [Phys. Rev. Lett. 101, 053001 (2008)] quantitatively. Analysis reveals the detailed electronic dynamics when the nuclear Coulomb attraction plays a key role in the recollision process of nonsequen…
We explore the possibility of retrieving Auger spectra with FEL radiation. Using a laser pulse of 260 eV photon energy, we study the interplay of photo-ionization and Auger processes following the initial formation of a 2p inner-shell hole in Ar. Accounting for the fine structure of the ion states we demonstrate how to retrieve the Auger spectrum of $\mathrm{Ar^{+}\rightarrow Ar^{2+}}$. Moreover, considering two electrons in coincidence we also demonstrate how to retrieve the Auger spectrum of $\mathrm{Ar^{2+}\rightarrow Ar^{3+}}$.
We demonstrate kinematically complete measurements on frustrated double ionization of argon atoms in strong laser fields with a reaction microscope. We found that the electron trapping probability after strong field double ionization is much higher than that after strong field single ionization, especially in case of high laser intensity. The retrieved electron momentum distributions of frustrated double ionization show a clear transition from the nonsequential to the sequential regime, similar to those of strong field double ionization. The dependence of electron momentum width on the laser i…
Detailed understanding of the ionization process in noble liquid detectors is important for their use in applications such as the search for dark matter and coherent elastic neutrino-nucleus scattering. The response of noble liquid detectors to low-energy ionization events is poorly understood at this time. We describe a new simulation tool which predicts the ionization yield from electronic energy deposits (E < 10keV) in liquid Ar, including the dependence of the yield on the applied electric drift field. The ionization signal produced in a liquid argon detector from $^{37}$Ar beta decay and …
We report the observation of multiple ionization of Argon through multi-XUV-photon absorption induced by an unprecedentedly powerful laser driven high-harmonic-generation source. Comparing the measured intensity dependence of the yield of the different Argon charge states with numerical calculations we can infer the different channels -direct and sequential- underlying the interaction. While such studies were feasible so far only with FEL sources, this work connects highly-non-linear-XUV-processes with the ultra-short time scales, inherent to the harmonic pulses, and highlights the advanced pe…
Using a three-dimensional semiclassical method, we theoretically investigate frustrated double ionization (FDI) of Ar atoms subjected to strong laser fields. The double-hump photoelectron momentum distribution generated from FDI observed in a recent experiment [S. Larimian et al., Phys. Rev. Research 2, 013021 (2020)] is reproduced by our simulation. We confirm that the observed spectrum is due to recollision. The laser intensity dependence of FDI is investigated. We reveal that the doubly excited states of Ar atoms and excited states of Ar+ are the dominant pathways for producing FDI at relat…
Zhang and coworkers have recently reported results of experiments involving irradiation of argon clusters doped with bromofluorene chromophores by nanosecond-long pulses of 532 nm laser light. Multiply-charged ions of atomic argon (charge states, n, up to 7) and carbon (charge states up to 4) are observed which are sought to be rationalised using an evaporation model. The distinguishing facet of exploding clusters being progenitors of energetic ions and electrons constitutes the key driver for contemporary research in laser-cluster interactions; it is, therefore, important to point out inconsi…
We report an optical dipole trap for calcium. The trap is created by focusing a 488 nm argon-ion laser beam into a calcium magneto-optical trap. The argon-ion laser photo-ionizes atoms in the trap because of a near-resonance with the 4s4f 1F3 level. By measuring the dipole trap decay rate as a function of argon-ion laser intensity, we determine the 1F3 photo-ionization cross section at our wavelength to be approximately 230 Mb.
We demonstrate the controlled creation of a $\mathrm{^{174}Yb^{2+}}$ ion by photo-ionizing $\mathrm{^{174}Yb^+}$ with weak continuous-wave lasers at ultraviolet wavelengths. The photo-ionization is performed by resonantly exciting transitions of the $\mathrm{^{174}Yb^+}$ ion in three steps. Starting from an ion crystal of two laser-cooled $\mathrm{^{174}Yb^+}$ ions localized in a radio-frequency trap, the verification of the ionization process is performed by characterizing the properties of the resulting mixed-species ion-crystal. The obtained results facilitate fundamental studies of physics…
Atomic ionization by intense mid-infrared (mid-IR) pulses produces low electron energy features that the strong-field approximation, which is expected to be valid in the tunneling ionization regime characterized by small Keldysh parameters ($γ\ll 1$), cannot describe. These features include the low-energy structure (LES), the very-low-energy structure (VLES), and the more recently found zero-energy structure (ZES). They result from the interplay between the laser electric field and the atomic Coulomb field which controls the low-energy spectrum also for small $γ$. In the present joint experime…
When atoms or molecules are exposed to strong short-pulse infrared radiation, ionization as well as "frustrated tunneling ionization" (FTI) can occur, in which a portion of the almost ionized electrons recombine into the initial ground or an excited bound state. We analyze the ellipticity dependence of the relative signals that are predicted in a single-active electron approximation (SAE), the validity of which is checked against a parameter-free multi-electron \hbox{$R$-matrix} (close-coupling) with time dependence approach. We find good agreement between the results from both models, thereby…
We present a theoretical study of atomic ionization due to an XUV pulse in the presence of an infrared laser. Within the strong field approximation and considering the periodicity and symmetry of the transition matrix we show that the photoelectron spectrum can be described from the contribution during only one (or half) infrared cycle. These symmetry and periodicity properties impress selection rules which destructively cancel certain sideband orders favoring others. In particular, we analyze the photoionization of Argon in four geometrical arrangements of the polarization vector and the phot…
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 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.
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…
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.
We present an experimental and theoretical energy- and angle-resolved study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral N$_2$ molecules. Using 9.3 eV photons produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and ions produced from one-color two-photon ionization in coincidence. Photoionization of N$_2$ populates the X $^2Σ^+_g$, A $^2Π_u$, and B $^2Σ^+_u$ ionic states of N$_2^+$, where the photoelectron angular distributions associated with the X $^2Σ^+_g$ and A $^2Π_u$ state…
We investigate the relevance of multiple-orbital and multipole effects during high-harmonic generation (HHG). The time-dependent configuration-interaction singles (TDCIS) approach is used to study the impact of the detailed description of the residual electron-ion interaction on the HHG spectrum. We find that the shape and position of the Cooper minimum in the HHG spectrum of argon changes significantly whether or not interchannel interactions are taken into account. The HHG yield can be underestimated by up to 2 orders of magnitude in the energy regio of 30-50 eV. We show that the argument of…
Observation of molecular dynamics with quantum state resolution is one of the major challenges in chemical physics. Complete characterization of collision dynamics leads to the microscopic understanding and unraveling of different quantum phenomena such as scattering resonances. We present a new experimental approach for observing molecular dynamics involving neutral particles and ions that is capable in providing state-to-state mapping of the dynamics. We use Penning ionization reaction between argon and metastable helium to generate argon ion and ground state helium atom pairs at separation …
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…
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 …
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.
We investigate resonant strong field ionization of atomic hydrogen with respect to the 1s-2p-transition. By "strong" we understand that Rabi-periods are executed on a femtosecond time scale. Ionization and AC Stark shifts modify the bound state dynamics severely, leading to nonperturbative signatures in the photoelectron spectra. We introduce an analytical model, capable of predicting qualitative features in the photoelectron spectra such as the positions of the Autler-Townes peaks for modest field strengths. Ab initio solutions of the time-dependent Schroedinger equation show a pronounced shi…
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 …
K-line profiles emitted from a warm dense plasma environment are used for diagnostics of Ar droplet plasmas created by high energy laser pulses. We observe temperature gradients within the Ar droplet from cold temperatures of the order of some 10 eV up to higher temperatures of about 170 eV. Non-perturbative wave functions are calculated as well as ionization energies, binding energies and relevant emission energies using a chemical {\it ab initio} code. The plasma screening is considered within a perturbative approach to the Hamiltonian. The plasma effect influences the many-particle system r…
Two efficient and isotope-selective resonant two-photon ionization techniques for loading barium ions into radio-frequency (RF)-traps are demonstrated. The scheme of using a strong dipole-allowed transition at λ=553 nm as a first step towards ionization is compared to the established technique of using a weak intercombination line (λ=413 nm). An increase of two orders of magnitude in the ionization efficiency is found favoring the transition at 553 nm. This technique can be implemented using commercial all-solid-state laser systems and is expected to be advantageous compared to other narrowban…
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…
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 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.
The present tutorial provides an overview of the time-dependent configuration interaction singles (\acs{TDCIS}) scheme applied to nonlinear ionization over a broad photon-energy range. The efficient propagation of the wave function and the calculation of photoelectron spectra within this approach are described and demonstrated in various applications. Above-threshold ionization of argon and xenon in the extreme ultraviolet energy range is investigated as an example. A particular focus is put on the xenon $4d$ giant dipole resonance and the information that nonlinear ionization can provide abou…
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 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 study photoionization of argon atoms excited by attosecond pulses using an interferometric measurement technique. We measure the difference in time delays between electrons emitted from the $3s^2$ and from the $3p^6$ shell, at different excitation energies ranging from 32 to 42 eV. The determination of single photoemission time delays requires to take into account the measurement process, involving the interaction with a probing infrared field. This contribution can be estimated using an universal formula and is found to account for a substantial fraction of the measured delay.
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…
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.
In this paper we present Classical Trajectory Monte Carlo (CTMC) calculations for single and multiple electron ionization of Argon atoms and ions in the threshold region. We are able to recover the Wannier exponents a for the power-law behavior of the cross section s versus excess energy: the exact value of the exponent as well as the existence of its saturation for multiple ionization appear to be related to how the total binding energy is shared between target electrons.
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 study the resonant sequential two-photon ionization of neutral atoms by a combination of twisted- and plane-wave light within a fully relativistic framework. In particular, the ionization of an isotropic ensemble of neutral sodium atoms ($Z = 11$) from their ground $3^{2}S_{1/2}$ state via the $3^{2}P_{3/2}$ level is considered. We investigate in details the influence of the kinematic parameters of incoming twisted radiation on the photoelectron angular distribution and the circular dichroism. Moreover we study the influence of the geometry of the process on these quantities. This is perfor…
We study resonant two-photon ionization of helium atoms via the $1s3p$, $1s4p$ and $1s5p^1$P$_1$ states using the 15$^\mathrm{th}$ harmonic of a titanium-sapphire laser for the excitation and a weak fraction of the laser field for the ionization. The phase of the photoelectron wavepackets is measured by an attosecond interferometric technique, using the 17$^\mathrm{th}$ harmonic. We perform experiments with angular resolution using a velocity map imaging spectrometer and with high energy resolution using a magnetic bottle electron spectrometer. Our results are compared to calculations using th…
Relativistic effects in the non-resonant two-photon K-shell ionization of neutral atoms are studied theoretically within the framework of second-order perturbation theory. The non-relativistic results are compared with the relativistic calculations in the dipole and no-pair approximations as well as with the complete relativistic approach. The calculations are performed in both velocity and length gauges. Our results show a significant decrease of the total cross section for heavy atoms as compared to the non-relativistic treatment, which is mainly due to the relativistic wavefunction contract…
We demonstrate control over the localization of high-lying Rydberg wave packets in argon atoms with phase-locked orthogonally polarized two-color (OTC) laser fields. With a reaction microscope, we measured ionization signals of high-lying Rydberg states induced by a weak dc field and black-body radiation as a function of the relative phase between the two-color fields. We find that the dc-field ionization yields of high-lying Rydberg argon atoms oscillate with the relative two-color phase with a period of $2π$ while the photoionization signal by black-body radiation shows a period of $π$. Thes…
We perform numerical simulations for photoionization of the argon atom when exposed to a combined field of an infrared laser (abbreviated IR) and its 13th harmonic (H13) by solving the Time-Dependent Schrödinger Equation (TDSE)], noting that the associated energy spectrum displays a harmonic peak dressed by the IR and other peaks called side-bands SB+-n corresponds to the absorption (+n) and the emission (-n) of the n-infrared photons above the ionization threshold. In two-color H13+IR photoionization of argon, the analysis of the angular distribution of the ejected electron in the continuum, …
The ionization of atoms with sequences of attosecond pulses gives rise to excited ionic states that are entangled with the emitted photoelectron. Still, the ionic ensemble preserves some coherence that can be controlled through the laser parameters. In helium, control of the $2s/2p$ He$^+$ coherence is mediated by the autoionizing states below the $N=2$ threshold [Phys. Rev. Res. {\bf 3}, 023233 (2021)]. In the present work we study the role of the resonances both below and above the $N=3$ threshold on the coherence of the $N=3$ He$^+$ ion, in the attosecond pump-probe ionization of the helium…
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. …
We present a theoretical study of the photoelectron attosecond beating at the basis of RABBIT (Reconstruction of Attosecond Beating By Interference of Two-photon transitions) in the presence of autoionizing states. We show that, as a harmonic traverses a resonance, its sidebands exhibit a peaked phase shift as well as a modulation of the beating frequency itself. Furthermore, the beating between two resonant paths persists even when the pump and the probe pulses do not overlap, thus providing a sensitive non-holographic interferometric means to reconstruct coherent metastable wave packets. We …
The laser intensity dependence of the recoil energies from the Coulomb explosion of small argon clusters has been investigated by resolving the contributions of the individual charge states to the ion recoil energy spectra. Between $10^{14}$ and $10^{15}$ W/cm$^2$ the high-energy tail of the ion energy spectra changes its shape and develops into the well-known knee feature, which results from the cluster size distribution, laser focal averaging, and ionization saturation. Resolving the contributions of the different charge states to the recoil energies, the experimental data reveal that the ba…
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 a possible mechanism for the autoionization of ultracold Rydberg gases, based on the resonant coupling of Rydberg pair states to the ionization continuum. Unlike an atomic collision where the wave functions begin to overlap, the mechanism considered here involves only the long-range dipole interaction and is in principle possible in a static system. It is related to the process of intermolecular Coulombic decay (ICD). In addition, we include the interaction-induced motion of the atoms and the effect of multi-particle systems in this work. We find that the probability for this io…
We present ionization probability and line shape calculations for the two-step 3-photon ionization process, $1S \stackrel{2\hbar ω}{\longrightarrow}2S \stackrel{\hbar ω}{\longrightarrow}εP $, of the ground state of hydrogenic atoms in a non-monochromatic laser field with a time--dependent amplitude. Within the framework of a three--level model, the {\it AC Stark} shifts and non-zero ionization rates of all states involved were taken into account together with spatial and temporal inhomogeneities of the laser signal. In contrast with the usual perturbative technique, the time evolution of the a…
A new High Harmonic Generation (HHG) scheme, which doesn't rely on Tunnel-Ionization as the ionization mechanism but rather on Single-Photon Ionization, is theoretically proposed and numerically demonstrated. The scheme uses two driver fields: an extreme-ultraviolet driver which induces the ionization, and a circularly-polarized, co-rotating, two-color infrared driver carried at a fundamental frequency and its second harmonic which induces the recollision. Using Classical and time-dependent Schrödinger equation simulations of a model Argon atom, we show that in this scheme ionization is essent…
