Electron Kinetic Energy Spectra Research Articles

HORTENSIA, a program package for the simulation of nonadiabatic autoionization dynamics in molecules.

We present a program package for the simulation of ultrafast vibration-induced autoionization dynamics in molecular anions in the manifold of the adiabatic anionic states and the discretized ionization continuum. This program, called HORTENSIA (Hopping Real-time Trajectories for Electron-ejection by Nonadiabatic Self-Ionization in Anions), is based on the nonadiabatic surface-hopping methodology, wherein nuclei are propagated as an ensemble along classical trajectories in the quantum-mechanical potential created by the electronic density of the molecular system. The electronic Schrödinger equation is numerically integrated along the trajectory, providing the time evolution of electronic state coefficients, from which switching probabilities into discrete electronic states are determined. In the case of a discretized continuum state, this hopping event is interpreted as the ejection on an electron. The derived diabatic and nonadiabatic couplings in the time-dependent electronic Schrödinger equation are calculated from anionic and neutral wavefunctions obtained from quantum-chemical calculations with commercially available program packages interfaced with our program. Based on this methodology, we demonstrate the simulation of autoionization electron kinetic energy spectra that are both time- and angle-resolved. In addition, the program yields data that can be interpreted easily with respect to geometric characteristics, such as bonding distances and angles, which facilitate the detection of molecular configurations important for the autoionization process. Furthermore, several useful extensions are included, namely, tools for the generation of initial conditions and input files as well as for the evaluation of output files, all of this both through console commands and a graphical user interface.

Threshold Photoionization and Density Functional Theory Investigations of Small Lanthanum Monoxide Clusters, LanO (n = 2-10).

Small lanthanum monoxide clusters, LanO (n = 2-10), have been studied by laser threshold photoionization (PI) spectroscopy and density functional theory (DFT). Ionization energies (IEs) gradually decrease with cluster size with oscillatory behavior at certain sizes at n = 4, 7, and 9, and the IEs are slightly lower than the corresponding bare Lan clusters. Mulliken charge analysis of the neutral and cation clusters indicates that the threshold PI occurs from a delocalized metal-based 5d orbital. The stable geometric structures and IEs for the LanO (n = 2-8) clusters have been determined from DFT. Zero electron kinetic energy and PI spectra have been calculated based on DFT calculations and compared with the experimental PI spectra. On the basis of favorable agreement between the simulated and experimental PI spectra, reliable ground-state geometric structures have been assigned. The O atom is negatively charged, equivalent to one electronic charge mainly transferred from La atoms bonded to it. Chemical bonding between the La and O atoms is ionic, whereas La atoms are mostly covalently bonded. No direct correlation is found between the electronic properties like the IE, electron affinity, and HOMO-LUMO gap and the stability of these clusters.

Multiphoton Ionization of Potassium Atoms in Femtosecond Laser FieldsSupported by the National Key R&D Program of China (Grant No. 2019YFA0307701), the National Natural Science Foundation of China (Grant Nos. 91850114, 11774131, 12074143, 11704148, 11704147, and 11904120), and the Science Challenge Project (Grant No. TZ2018005). D. Z. acknowledges the finical support of the starting grant from Jilin University.

We study the multiphoton ionization of potassium atoms in 800 nm and 400 nm femtosecond laser fields. In the 800 nm laser field, the potassium atom absorbs three photons and emits one electron via one photon resonance with the 4p intermediate state with the help of the ac-Stark shift. The resonance feature is clearly shown as an Autler–Townes (AT) splitting and is mapped out in the electron kinetic energy spectrum. In a 400 nm laser field, although one photon resonance is possible with the 5p state, no splitting is observed. The different transition amplitudes between 4s–4p and 4s–5p explain the observed results. Due to the AT effect, an unexpected peak in the photoelectron energy spectrum that violates the dipole transition rule is observed. A preliminary explanation involving the spin-orbit interaction in the p state is given to account for this component. The observed AT-splitting in the electron kinetic energy distribution can be used as an effective method to calibrate the intensity of a laser field.

On the Application of Pulsed Beams with a Wide Electron Kinetic Energy Spectrum

The application features of pulsed electron beams with a wide electron kinetic energy spectrum for solving practical problems are considered on the example of wheat seed treatment. The influence of the dose depth distribution determined by the beam spectrum on the efficiency of its application is shown. For the ASTRA-M electron accelerator based on a pulse transformer, an operating mode has been found (accelerating voltage of 260 kV at 0.15 kGy) in which the beam energy is released mainly in the surface layer of biological materials. This leads to a sharp decrease in the degree of infection with Penicillium spp. fungi while maintaining seed germination.

A comparative multi-state multi-dimensional quantum-classical dynamics on compact polycyclic aromatic hydrocarbons (CPAHs) by parallel TDDVR method

The newly implemented parallelized quantum–classical dynamical approach, namely, Time Dependent Discrete Variable Representation (TDDVR) method is applied to the spectroscopically important phenanthrene, acenaphthene and pyrene, where several conical intersections exist in their four lowest singlet excited electronic states (X, A, B and C), to illustrate their various dynamical aspects. This parallel version shows almost linear scalability with increasing number of computing processors. First principles dynamics is performed to the adopted Hamiltonians to obtain photoelectron (PE) spectra, zero electron kinetic energy (ZEKE) spectra, population dynamics and many other dynamical observables. The reduced densities of the wave packet (WP) in coupled electronic surfaces are used to elucidate the intrinsic dynamical features. The TDDVR calculated PE and assigned ZEKE spectra of all CPAHs are found to be good agreement with the previous experimental data and other available theoretical results.

Two-plasmon-decay induced fast electrons in intense femtosecond laser–solid interactions

The nonlinear coupling of intense laser pulse with plasma leads to excitation of several parametric instabilities, featuring plasmon, acoustic or electromagnetic modes. Specifically, the two-plasmon decay (TPD) instability, relevant to the generation of fast electrons, originates at the quarter critical surface, where the incident photon decays into a pair of electron plasmon waves. Although well explored by nanosecond lasers, the TPD instability is rarely seen in femtosecond laser–plasmas, mainly due to steep plasma profiles and the ultrashort duration of the driving pulse. Our experiments show TPD boosting of fast electrons in the femtosecond regime using low intensity contrast and temporally stretched laser pulses. The fast electron spectrum and 3ω0/2 harmonic emission from plasma show significant enhancement for stretched pulses (120 fs) in comparison to transform-limited short pulses (30 fs). The generation of fast electrons is found to be linked with the growth of 3ω0/2 harmonic. The effect of longer femtosecond pulses on TPD growth is observed using several fast electron diagnostics such as electron kinetic energy spectra, hard x-ray emission, rear side plasma emission, Cherenkov emission, and time-space resolved shadowgrams up to laser intensity of 1.5 × 1018 W cm−2. We, thus, provide robust and unambiguous demonstration of TPD instability driven generation of fast electrons in femtosecond laser–plasma interactions.

Hydration of Nucleobase as Probed by Electron Emission of Uridine-5′-Mono-Phosphate (UMP) in Aqueous Solution Induced by Nitrogen K-Shell Ionization

To identify the precise early radiation processes of DNA lesions, we measure electron kinetic energy spectra emitted from uridine-5′ monophosphate (UMP) in aqueous solution for the photoionization of the N 1s orbital electron and for the following Auger effect using a monochromatic soft X-ray synchrotron radiation at energies above the nitrogen K-shell ionization threshold. The change of photoelectron spectra for UMP in aqueous solutions at different proton concentrations (pH = 7.5 and 11.3) is ascribed to the chemical shift of the N3 nitrogen atom in uracil moiety of canonical and deprotonated forms. The lowest double ionization potentials for aqueous UMP at different pH obtained from the Auger electron spectra following the N 1s photoionization values show the electrostatic aqueous interaction of uracil moiety of canonical (neutral) and deprotonated (negatively charged) forms with hydrated water molecules.

Влияние спектра кинетических энергий электронов импульсного пучка на эффективное распределение поглощенной дозы по глубине мишени

Влияние спектра кинетических энергий электронов импульсного пучка на эффективное распределение поглощенной дозы по глубине мишени

Energy depth distribution of pulsed electron beam with wide electron kinetic energy spectrum for an aluminum target

Knowledges of pulsed electron beam characteristics is necessary for use it for scientific and practice applications. Current work analyses the pulsed electron beam extracted from the vacuum diode through a titanium foil (60 mkm) of the diode exit window. Electron beam energy depth distribution was measured for a target made of different number of aluminum foils. A pulsed electron beam with a wide range of kinetic energies was generated by the ASTRA-M accelerator (260 kV of accelerating voltage, up to 1 kA of beam current, 150 ns of beam pulse duration at FWHM). A calorimeter of total absorption and Faraday cup were used to measure beam characteristics. Calorimeter included two collectors: first one measures a beam energy after aluminum foils, and the second one measures a total beam energy. All measurements were performed at 10−5 Torr background pressure after the exit window foil. As a result, the electron kinetic energy spectrum of the beam out of diode has been reconstructed.

Changes in the Martian atmosphere induced by auroral electron precipitation

Typical auroral events in the Martian atmosphere, such as discrete and diffuse auroral emissions detected by UV spectrometers onboard ESA Mars Express and NASA MAVEN, are investigated. Auroral electron kinetic energy distribution functions and energy spectra of the upward and downward electron fluxes are obtained by electron transport calculations using the kinetic Monte Carlo model. These characteristics of auroral electron fluxes make it possible to calculate both the precipitation-induced changes in the atmosphere and the observed manifestations of auroral events on Mars. In particular, intensities of discrete and diffuse auroral emissions in the UV and visible wavelength ranges (Soret et al., 2016; Bisikalo et al., 2017; Gerard et al., 2017). For these conditions of auroral events, the analysis is carried out, and the contribution of the fluxes of precipitating electrons to the heating and ionization of the Martian atmosphere is estimated. Numerical calculations show that in the case of discrete auroral events the effect of the residual crustal magnetic field leads to a significant increase in the upward fluxes of electrons, which causes a decrease in the rates of heating and ionization of the atmospheric gas in comparison with the calculations without taking into account the residual magnetic field. It is shown that all the above-mentioned impact factors of auroral electron precipitation processes should be taken into account both in the photochemical models of the Martian atmosphere and in the interpretation of observations of the chemical composition and its variations using the ACS instrument onboard ExoMars.

Tracing transient charges in expanding clusters

We study transient charges formed in methane clusters following ionization by intense near-infrared laser pulses. Cluster ionization by 400 fs ($I=1 \times 10^{14}$ W/cm$^2$) pulses is highly efficient, resulting in the observation of a dominant C$^{3+}$ ion contribution. The C$^{4+}$ ion yield is very small, but is strongly enhanced by applying a time-delayed weak near-infrared pulse. We conclude that most of the valence electrons are removed from their atoms during the laser-cluster interaction, and that electrons from the nanoplasma recombine with ions and populate Rydberg states when the cluster expands, leading to a \textit{decrease} of the average charge state of individual ions. Furthermore, we find clear bound-state signatures in the electron kinetic energy spectrum, which we attribute to Auger decay taking place in expanding clusters. Such nonradiative processes lead to an \textit{increase} of the final average ion charge state that is measured in experiments. Our results suggest that it is crucial to include both recombination and nonradiative decay processes for the understanding of recorded ion charge spectra.

Correlated electronic decay in expanding clusters triggered by intense XUV pulses from a Free-Electron-Laser

Irradiation of nanoscale clusters and large molecules with intense laser pulses transforms them into highly-excited non- equilibrium states. The dynamics of intense laser-cluster interaction is encoded in electron kinetic energy spectra, which contain signatures of direct photoelectron emission as well as emission of thermalized nanoplasma electrons. In this work we report on a so far not observed spectrally narrow bound state signature in the electron kinetic energy spectra from mixed Xe core - Ar shell clusters ionized by intense extreme-ultraviolet (XUV) pulses from a free-electron-laser. This signature is attributed to the correlated electronic decay (CED) process, in which an excited atom relaxes and the excess energy is used to ionize the same or another excited atom or a nanoplasma electron. By applying the terahertz field streaking principle we demonstrate that CED-electrons are emitted at least a few picoseconds after the ionizing XUV pulse has ended. Following the recent finding of CED in clusters ionized by intense near-infrared laser pulses, our observation of CED in the XUV range suggests that this process is of general relevance for the relaxation dynamics in laser produced nanoplasmas.

Transition from SAMO to Rydberg State Ionization in C60 in Femtosecond Laser Fields.

The transition between two distinct ionization mechanisms in femtosecond laser fields at 785 nm is observed for C60 molecules. The transition occurs in the investigated intensity range from 3 to 20 TW/cm2 and is visualized in electron kinetic energy spectra below the one-photon energy (1.5 eV) obtained via velocity map imaging. Assignment of several observed broad spectral peaks to ionization from superatom molecular orbitals (SAMOs) and Rydberg states is based on time-dependent density functional theory simulations. We find that ionization from SAMOs dominates the spectra for intensities below 5 TW/cm2. As the intensity increases, Rydberg state ionization exceeds the prominence of SAMOs. Using short laser pulses (20 fs) allowed uncovering of distinct six-lobe photoelectron angular distributions with kinetic energies just above the threshold (below 0.2 eV), which we interpret as over-the-barrier ionization of shallow f-Rydberg states in C60.

Autoionization following nanoplasma formation in atomic and molecular clusters

Nanoplasmas resulting from the ionization of nano-scale particles by intense laser pulses are typically described by quasiclassical models, where electron emission is understood to take place via thermal processes. Recently, we discovered that, following the interaction of intense near-infrared (NIR) laser pulses with molecular oxygen clusters, electron emission from nanoplasmas can also occur from atomic bound states via autoionization [Schutte et al., Phys. Rev. Lett. 114, 123002 (2015)]. Here we extend these studies and demonstrate that the formation and decay of doubly-excited atoms and ions is a very common phenomenon in nanoplasmas. We report on the observation of autoionization involving spin-orbit excited states in molecular oxygen and carbon dioxide clusters as well as in atomic krypton and xenon clusters ionized by intense NIR pulses, for which we find clear bound-state signatures in the electron kinetic energy spectra. By applying terahertz (THz) streaking, we show that the observed autoionization processes take place on a picosecond to nanosecond timescale after the interaction of the NIR laser pulse with the clusters.

Inter- and intracycle interference effects in strong-field dissociative ionization

We theoretically study dissociative ionization of H$_2^+$ exposed to strong linearly polarized few-cycle visible, near-infrared and midinfrared laser pulses. We find rich energy-sharing structures in the combined electron and nuclear kinetic energy spectra with features that are a priori at odds with simple energy conservation arguments. We explain the structures as interferences between wave packets released during different optical cycles, and during the same optical cycle, respectively. Both inter- and intracycle interference structures are clearly visible in the joint energy spectra. The shapes of the interference structures depend on the dynamics leading to the double continuum, and carry sub-femtosecond information.

Correlated electronic decay following intense near-infrared ionization of clusters

We report on a novel correlated electronic decay process following extensive Rydberg atom formation in clusters ionized by intense near-infrared fields. A peak close to the atomic ionization potential is found in the electron kinetic energy spectrum. This new contribution is attributed to an energy transfer between two electrons, where one electron decays from a Rydberg state to the ground state and transfers its excess energy to a weakly bound cluster electron in the environment that can escape from the cluster. The process is a result of nanoplasma formation and is therefore expected to be important, whenever intense laser pulses interact with nanometer-sized particles.

Observation of correlated electronic decay in expanding clusters triggered by near-infrared fields.

When an excited atom is embedded into an environment, novel relaxation pathways can emerge that are absent for isolated atoms. A well-known example is interatomic Coulombic decay, where an excited atom relaxes by transferring its excess energy to another atom in the environment, leading to its ionization. Such processes have been observed in clusters ionized by extreme-ultraviolet and X-ray lasers. Here, we report on a correlated electronic decay process that occurs following nanoplasma formation and Rydberg atom generation in the ionization of clusters by intense, non-resonant infrared laser fields. Relaxation of the Rydberg states and transfer of the available electronic energy to adjacent electrons in Rydberg states or quasifree electrons in the expanding nanoplasma leaves a distinct signature in the electron kinetic energy spectrum. These so far unobserved electron-correlation-driven energy transfer processes may play a significant role in the response of any nano-scale system to intense laser light.

A low energy bound atomic electron Compton scattering model for Geant4

A two-body fully relativistic three-dimensional scattering framework has been utilised to develop an alternative Compton scattering computational model to those adapted from Ribberfors’ work for Monte Carlo modelling of Compton scattering. Using a theoretical foundation that ensures the conservation of energy and momentum in the relativistic impulse approximation, this new model, the Monash University Compton scattering model, develops energy and directional algorithms for both the scattered photon and ejected Compton electron from first principles. The Monash University Compton scattering model was developed to address the limitation of the Compton electron directionality algorithms of other computational models adapted from Ribberfors’ work. Here the development of the Monash University Compton scattering model, including its implementation in a Geant4 low energy electromagnetic physics class, G4LowEPComptonModel, is outlined. Assessment of the performance of G4LowEPComptonModel was undertaken in two steps: (1) comparison with respect to the two standard Compton scattering classes of Geant4 version 9.5, G4LivermoreComptonModel and G4PenelopeComptonModel, and (2) experimental comparison with respect to Compton electron kinetic energy spectra obtained from the Compton scattering of 662keV photons off the K-shell of gold. Both studies illustrate that the Monash University Compton scattering model, and in turn G4LowEPComptonModel, is a viable replacement for the majority of computational models that have been adapted from Ribberfors’ work. It was also shown that the Monash University Compton scattering model is able to reproduce the Compton scattering triply differential cross-section Compton electron kinetic energy spectra of 662keV photons K-shell scattering off of gold to within experimental uncertainty.

Terracelike structure in the above-threshold-ionization spectrum of an atom in an IR+XUV two-color laser field

Based on the frequency-domain theory, we investigate the above-threshold ionization (ATI) process of an atom in a two-color laser field with infrared (IR) and extreme ultraviolet (XUV) frequencies, where the photon energy of the XUV laser is close to or larger than the atomic ionization threshold. By using the channel analysis, we find that the two laser fields play different roles in an ionization process, where the XUV laser determines the ionization probability by the photon number that the atom absorbs from it, while the IR laser accelerates the ionized electron and hence widens the electron kinetic energy spectrum. As a result, the ATI spectrum presents a terrace-like structure. By using the saddle-point approximation, we obtain a classical formula which can predict the cutoff of each plateau in the terrace-like ATI spectrum. Furthermore, we find that the difference of the heights between two neighboring plateaus in the terrace-like structure of the ATI spectrum increases as the frequency of the XUV laser increases.

Resonant photoemission at the iron M-edge of Fe(CO)5

High resolution electron kinetic energy spectra of iron pentacarbonyl (Fe(CO)5) are studied in the photon energy range of 40-90 eV. The relative yield of photolines associated with the Fe 3d level shows a Fano line shape at photon energies of 61 eV. The increase in signal from the 3d level is indicative of resonant photoemission involving 3p-3d transitions at the M edge of iron. The signature of this resonance is also present in photolines typically attributed to be mostly CO in character. We use the modulation depth of the Fano resonances to reinterpret the photoelectron lines in the literature.