Double Ionization Research Articles

Symmetry breaking in core-valence double ionisation of allene

Conventional electron spectroscopy is an established one-electron-at-the-time method for revealing the electronic structure and dynamics of either valence or inner shell ionized systems. By combining an electron-electron coincidence technique with the use of soft X-radiation we have measured a double ionisation spectrum of the allene molecule in which one electron is removed from a C1s core orbital and one from a valence orbital, well beyond Siegbahns Electron-Spectroscopy-for-Chemical-Analysis method. This core-valence double ionisation spectrum shows the effect of symmetry breaking in an extraordinary way, when the core electron is ejected from one of the two outer carbon atoms. To explain the spectrum we present a new theoretical approach combining the benefits of a full self-consistent field approach with those of perturbation methods and multi-configurational techniques, thus establishing a powerful tool to reveal molecular orbital symmetry breaking on such an organic molecule, going beyond Löwdins standard definition of electron correlation.

MP-CITDSE: A set of ab-initio programs for the simulation of hydrogenic and helium-like atom-laser interactions

MP-CITDSE is a package of programs which solves the time-dependent Schrödinger equation for hydrogenic and helium-like atomic systems interacting with an ultra-short laser pulse (of attosecond or femtosecond duration). The output of the computations – with some minimal processing – may be used to calculate excited populations, single and double ionisation yields, kinetic, angular and radial electron distributions, and harmonic yields. For the Helium atom, a full account of the inter-electronic correlation effects is included via a configuration interaction approach; for the time propagation of the wavefunction a spectral basis expansion on the eigenstates of the field-free Hamiltonian is used; for this reason post-processing of the expansion coefficients just after the pulse lead to simple formulas for quantities of experimental interest. Program summaryProgram Title: MP-CITDSECPC Library link to program files:https://doi.org/10.17632/gv4zxmfdx3.1Developer's repository link:https://github.com/aforembs/MP-CITDSELicensing provisions: GPLv3Programming language: C++Nature of problem: The ultra-fast high-intensity laser pulses of modern experimental sources require an ab-initio theoretical treatment, as the characteristics of such pulses are generally incompatible with the established Lowest-order Perturbation Theory (LOPT) approximation. Such a treatment can be quite cumbersome to not only implement, but also describe in a clear, intuitive manner. Its inherent complexity ensures that even in its simplest form, an ab-initio TDSE solver can easily consist of several thousand lines of code. As with any project of such scope a significant amount of effort is required to keep the code up to date, running on several platforms, compilers and operating systems. As such, while the numerical problem tackled by MP-CITDSE is that of the simulation of hydrogenic and helium-like atom-laser interactions on a single node computer/workstation; its main challenges are longevity and expandability. By doing away with unnecessary abstractions within the code, using a modern standard of a widely used and performant language (C++ 17) and hosting the source code on a publicly available GitHub repository we hope that the programs provided herein prove themselves useful to many current and future AMO Physicists.Solution method: The atomic systems are considered confined in a spherical box of finite size. In the one-electron case (hydrogen) the eigenstates are calculated in a spherical coordinate system by the direct diagonalisation of the field-free Hamiltonian matrix representation on a B-splines piecewise polynomial basis expansion of the radial part of the eigenfunctions; for the two-electron case (helium) the numerically calculated one-electron eigenstates are angularly coupled to form a zero-order (uncorrelated) two-electron numerical basis; then the latter basis is further coupled via a configuration-interaction approach to eventually calculate the helium's two-electron eigenstates.Following these steps, for both systems (hydrogen and helium) the computation proceeds by expanding the time-dependent wavefunction on the corresponding field-free eigenstate basis; thus, we end up to a system of first-order ordinary differential equations (ODEs) in time for the expansion (time-dependent) coefficients; the dynamical parameters for the ODEs time propagation, namely the eigenenergies and dipole matrix elements are calculated only once prior to the ODEs propagation [2]. The structure of the propagating matrix is block tridiagonal.Additional comments including restrictions and unusual features: This paper serves as the definitive reference for the MP-CITDSE code. In this version we solve the ODEs using a Runge-Kutta-Felnberg (RKF) algorithm. Also we have restricted the code to treat hydrogen and helium but with very little effort (non-relativistic) hydrogenic and helium-like atomic systems can also be simulated. The programs are supplied with two methods of compilation, via make and cmake to ensure greater portability.

Intermolecular Charge Transfer Induced Fragmentation of Formic Acid Dimers.

We investigate the intermolecular nonradiative charge transfer process in a double hydrogen-bonded formic acid (FA) dimer, initiated by electron-collision induced double ionization of one FA molecule. Through fragment ions and electron coincident momentum measurements and abinitio calculations, we obtain direct evidence that electron transfer from the neighboring FA molecule to fill one of the two vacancies occurs by a potential energy curve crossing of FA^{++}+FA with FA^{+}+FA^{+*} curves, forming an electronic excited state of dicationic dimers. This process causes the breaking of two hydrogen bonds and subsequently the cleavage of C─H and C─O covalent bonds in the dimers, which is expected to be a general phenomenon occurring in molecular complexes and can have important implications for radiation damage to biological matter.

Controlling multiple returnings in non-sequential double ionization with orthogonal two-color laser pulses

With the three-dimensional semi-classical ensemble model, we studied the non-sequential double ionization by orthogonal two-color laser pulses. Our calculations show that the proportion of events experiencing multiple returnings, the sum of the final energies of two electrons, and the ion momentum distribution depend on the relative phase of the two-color fields, exhibiting oscillatory behavior with a period of π. Back analysis of these trajectories reveals that we can control the recollision energy of the electron by changing the relative phase of the two-color laser pulse. As a consequence, the trajectories of multiple-returning ions change with the relative phase, resulting in relative-phase-dependent ion momentum distributions. The result shows that the momentum distribution of the ions in the trajectories of multiple returnings is clearly wider than that for the case of single returning. For the multiple-returning events, the binary recollision leads to a smaller scattering angle of the first electron.

Search for the interatomic Auger effect in Nitrous Oxide

The interatomic Auger effect following O 1s ionization in N2O has been experimentally investigated using multi-electron coincidence spectroscopy. The expected transition energies have been established by comparison to the measured N 1s−1v−1 core-valence double ionization energies. We describe a procedure to eliminate the background of two competing processes contributing spectroscopic signatures to the same energy range, namely double Auger decay of the O 1s vacancy and direct single-photon double ionization into the N 1s−1v−1 states. While the interatomic Auger transitions could not be successfully isolated, we provide an upper boundary of the transition probability of 0.07% with respect to the dominant single Auger decay after O 1s ionization.

L-Shell Photoionization of Magnesium-like Ions with New Results for Cl5+

This study reports on the absolute photoionization cross sections for the magnesium-like Cl5+ ion over the 190–370 eV photon energy range, corresponding to the L-shell (2s and 2p subshells) excitation regime. The experiments were performed using the Multi-Analysis Ion Apparatus (MAIA) on the PLéIADES beamline at the SOLEIL synchrotron radiation storage ring facility. Single and double ionization ion yields, produced by photoionization of the 2p subshell of the Cl5+ ion from the 2p63s2 1S0 ground state and the 2p63s3p 3P0,1,2 metastable levels, were observed, as well as 2s excitations. Theoretical calculations of the photoionization cross sections using the Multi-Configuration Dirac-Fock and R-matrix approaches were carried out, and the results were compared with the experimental data. The Cl5+ results were examined within the overall evolution of L-shell excitation for the early members of the Mg-like isoelectronic sequence (Mg, Al+, Si2+, S4+, Cl5+). Characteristic photon energies for P3+ were estimated by interpolation.

Theoretical investigation of electron-impact double ionization of B-like C+ to Ne5+ ions

Electron-impact double ionization (DI) including direct and indirect processes of B-like ${\mathrm{C}}^{+}$ to ${\mathrm{Ne}}^{5+}$ ions is investigated using a two-step approach. The direct process is treated as a primary single ionization (SI) and subsequent knockout mechanism. The indirect process is considered as a primary SI of an inner-shell $1s$ electron followed by a single autoionization. Based on the two-step approach, the DI cross sections are calculated using flexible atomic code with distorted-wave approximation. The potential of the intermediate ion is approximately equivalent to the mean potential constructed by three ions involved for calculating the cross section of the direct process, while using the potential of the ionizing ion in each step of the present two-step approach overestimates results. The present cross sections agree with available theoretical and experimental data.

Pulse length effects in long wavelength driven non-sequential double ionization

Pulse length effects in long wavelength driven non-sequential double ionization

Near- K -edge single and double photoionization of C2+ ions

Single and double ionization of berylliumlike ${\mathrm{C}}^{2+}$ by a single photon is investigated in the energy range from 292 to 350 eV in the vicinity of the $K$-shell single-ionization threshold. Energy resolutions range between 160 meV for overview scans and 11 meV for high-resolution spectroscopy. The experimental cross sections include contributions from the $1{s}^{2}2{s}^{2}\phantom{\rule{0.28em}{0ex}}^{1}S$ ground level and the $1{s}^{2}2s2p\phantom{\rule{0.28em}{0ex}}^{3}P$ metastable levels. A comparison of the experimentally derived cross-section function for photoabsorption by ${\mathrm{C}}^{2+}$ to a model based on previous $R$-matrix calculations shows very satisfying agreement.

Electron dynamics of molecular frustrated double ionization driven by strong laser fields* *Supported by the National Natural Science Foundation of China (Grant Nos. 12004323, 12074329, 12104389, 1174131 and 91850114), National Key R&D Program of China (2022YFE0134200) and Nanhu Scholars Program for Young Scholars of Xinyang Normal University, Natural Science Foundation of Jilin Province, China (Grant No. 20220101016JC), and the Open

We theoretically investigate the frustrated double ionization (FDI) of molecules with different alignment-dependence using a three-dimensional classical ensemble method. The numerical results show that the FDI probability decreases with increasing wavelength, which is similar to the wavelength dependence of the FDI probability of atoms. Tracing the classical trajectories reveals that the contributions to molecular FDI from single-recollision and multiple-recollision mechanisms are equal in the short wavelength regime. In the long wavelength regime, the single-recollision FDI channel dominates in FDI. The nature in which molecular FDI occurs is identified and explained.

Pulse length effects in long wavelength driven non-sequential double ionization

We present a joint experimental and theoretical study of non-sequential double ionization (NSDI) in argon driven by a 3100 nm laser source. The correlated photoelectron momentum distribution (PMD) shows a strong dependence on the pulse duration, and the evolution of the PMD can be explained by an envelope-induced intensity effect. Determined by the time difference between tunneling and rescattering, the laser vector potential at the ionization time of the bound electron will be influenced by the pulse duration, leading to different drift momenta. Such a mechanism is extracted through a classical trajectory Monte Carlo-based model and it can be further confirmed by quantum mechanical simulations. This work sheds light on the importance of the pulse duration in NSDI and improves our understanding of the strong field tunnel-recollision dynamics under mid-IR laser fields.

Fragmentation dynamics of electron-impact double ionization of helium

We study the double ionization dynamics of a helium atom impacted by electrons with full-dimensional classical trajectory Monte Carlo simulation. The excess energy is chosen to cover a wide range of values from 5 eV to 1 keV for comparative study. At the lowest excess energy, i.e., close to the double-ionization threshold, it is found that the projectile momentum is totally transferred to the recoil-ion while the residual energy is randomly partitioned among the three outgoing electrons, which are then most probably emitted with an equilateral triangle configuration. Our results agree well with experiments as compared with early quantum-mechanical calculation as well as classical simulation based on a two-dimensional Bohr’s model. Furthermore, by mapping the final momentum vectors event by event into a Dalitz plot, we unambiguously demonstrate that the ergodicity has been reached and thus confirm a long-term scenario conceived by Wannier. The time scale for such few-body thermalization, from the initial nonequilibrium state to the final microcanonical distribution, is only about 100 attoseconds. Finally, we predict that, with the increase of the excess energy, the dominant emission configuration undergoes a transition from equilateral triangle to T-shape and finally to a co-linear mode. The associated signatures of such configuration transition in the electron-ion joint momentum spectrum and triple-electron angular distribution are also demonstrated.

Generation of micro-Joule level coherent quasi-continuum extreme ultraviolet radiation using multi-cycle intense laser-atom interactions

In the present work we report on the current progress of the recently constructed GW attosecond extreme ultraviolet (XUV) source developed at the Institute of Electronic Structure and Laser of the Foundation for Research and Technology-Hellas (I.E.S.L-FO.R.T.H.). By the implementation of a compact-collinear polarization gating arrangement, the generation of a broadband, coherent XUV quasi-continuum produced by the interaction of a many-cycle infrared field with a gas phase medium is achieved. The spectral width of the XUV emission generated in Xenon, is spanning in the range of 17–32 eV and can support isolated pulses of duration in the range from 0.4 fs to 1.3 fs and pulse energy in the 1 μJ level. Theoretical calculations, taking into account the experimental conditions of this work, are supporting the observations, offering also an insight regarding the temporal profile of the emitted radiation. Finally, the high intensity of the produced XUV pulses has been confirmed by investigating the two-XUV-photon double ionization process of Argon atoms. The demonstrated results inaugurate the capability of the beamline of producing intense coherent quasi-continuum XUV radiation, supporting isolated as pulses, that can be exploited in studies of non-linear XUV processes, attosecond pulse metrology and XUV-pump–XUV-probe experiments.

Differential Description of Multiple Ionization of Uracil by 3.5 MeV/u C6+ Impact

In this work, a theoretical analysis of the impact of the multiple ionization of uracil by 3.5 MeV/u C6+ is developed in the framework of a classical trajectory Monte Carlo method, as recently introduced for multi-electronic targets. The electron emission contribution arising from the multiple electron ionization is explicitly determined and the emission geometries and the reaction regions for double and triple ionization are explicitly identified. The present results suggest that double ionization is mainly characterized by the emission of slow electrons with a relative angle of 80∘–120∘. For triple ionization, on the other hand, the emission seems to occur with the three electrons holding similar interelectronic angles.

Mechanisms of one-photon two-site double ionization after resonant inner-valence excitation in Ne clusters

Mechanisms of one-photon two-site double ionization after resonant inner-valence excitation in Ne clusters

Modeling the sequential dissociative double ionization of O2 by ultrashort intense infrared laser pulses

A density matrix approach for sequential double ionization (DM-SDI) of molecules has been developed recently and was applied to the ${\mathrm{N}}_{2}$ molecule [Yuen and Lin, Phys. Rev. A 106, 023120 (2022)]. In this article, we extended the DM-SDI model to ${\mathrm{O}}_{2}$, which is a more complicated system to model than ${\mathrm{N}}_{2}$, due to its electronic structures and spin-orbit and laser couplings in the manifold of doubly charged states. We obtained a good agreement on the kinetic energy release spectrum of ${\mathrm{O}}^{+}+{\mathrm{O}}^{+}$ from previous experiments. Thanks to the low computational cost of the model, we explored the mechanism behind the ionization and dissociation dynamics as well as the effects of lasers on the spectrum. This work will pave the way to model sequential dissociative double ionization of larger molecules and to probe molecular dynamics by measuring kinetic energy release spectra from this process.

Carrier-Envelope Phase Controlling of Ion Momentum Distributions in Strong Field Double Ionization of Methyl Iodide

In strong field ionization of methyl iodide initiated by elliptically polarized few-cycle pulses, a significant correlation was observed between the carrier-envelope phases (CEPs) of the laser and the preferred ejection direction of methyl cation arising from dissociative double ionization. This was attributed to the carrier-envelope phase dependent double ionization yields of methyl iodide. This observation provides a new way for monitoring the absolute CEPs of few-cycle pulses by observing the ion momentum distributions.

Searching for optimal THz generation through calculations of the asymmetry of photoelectron momentum distributions by an improved strong-field-approximation method

From the solution of the time-dependent Schr\"odinger equation (TDSE), it has been shown that in a two-color laser pulse the relative phase that optimizes terahertz (THz) radiation also optimizes the asymmetry of the angular distribution of photoelectrons. Here, we show that a second-order strong-field approximation can accurately calculate the asymmetry of photoelectrons and thus can locate the phase delay that optimizes THz generation, doing so four orders of magnitude faster than TDSE calculations. We further trace that this is possible because THz emission originates from a free-free radiative transition between the rescattered electron and the target ion, similar to other electron-ion collisions in the laser field, e.g., high-harmonic generation and nonsequential double ionization. Our results pave the way to locate the optimal phase delay for any typical laser pulses for maximal THz generation in the laboratory.

Strong field non-Franck–Condon ionization of H$$_2$$: a semi-classical analysis

Single ionization of H $$_2$$ molecules exposed to strong and short laser pulses is investigated by a semi-classical method. Three laser characteristics are considered: (i) The carrier-wave frequency corresponds to wavelengths covering and bridging the two ionization regimes: From tunnel ionization (TI) at 800 nm to multiphoton ionization (MPI) at 266 nm. (ii) Values of the peak intensity are chosen within a window to eliminate competing double ionization processes. (iii) Particular attention is paid to the polarization of the laser field, which can be linearly or circularly polarized. The results and their interpretation concern two observables, namely the end-of-pulse total ionization probability and vibrational distribution generated in the cation H $$_2^+$$ . The most prominent findings are an increased ionization efficiency in circular polarization and a vibrational distribution of the cation that favors lower-lying levels than those that would be populated in a vertical (Franck–Condon) ionization, leading to non-Franck–Condon distributions, both in linear and circular polarizations.

L-Shaped Double Gate Bipolar Impact Ionization MOSFET Based Energy Efficient Leaky Integrate and Fire Neuron for Spiking Neural Network

L-Shaped Double Gate Bipolar Impact Ionization MOSFET Based Energy Efficient Leaky Integrate and Fire Neuron for Spiking Neural Network