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Klaus Bartschat

Publications and source records attributed to Klaus Bartschat.

At least 19 recordsLinked to original sources

High-order harmonic generation in argon driven by short laser pulses: effects of post-pulse propagation and windowing

We present ab initio calculations using the $R$-matrix with time dependence (RMT) method for high-order harmonic generation (HHG) in argon in a short, intense pulse regime. The calculations employ a $6$-cycle $\sin^2$ pulse at $850$ nm with peak intensity $2.3\times 10^{14}$ W/cm$^2$ and, for comparison with the experiment by Guo et al. [J. Phys. B: At. Mol. Opt. Phys. 51, 034006 (2018)], a Gaussian pulse with the same frequency and peak intensity. Both pulse shapes yield the expected harmonic structure in the region above the ionization threshold (approximately $15.82$ eV in $LS$-coupling). The spectra exhibit strong carrier-envelope-phase (CEP) sensitivity. The energy region leading up to the ionization threshold contains spectral features arising from residual coherent dipole oscillations (free-induction decay) that strongly depend on spectral windowing and the post-pulse propagation time. We show that the HHG spectrum, particularly below the ionization threshold, is a defined quantity that depends on analysis choices rather than being a uniquely determined observable. Comparison between theoretical predictions and experimental observations in this energy regime, therefore, requires explicit specification of these parameters.

physics.atom-ph

Dichroic Electron Emission Patterns from Oriented Helium Ions

We report a joint experimental and theoretical study using a combination of polarization-controlled free-electron-laser (FEL) and near-infra\-red (NIR) pulses in a synchronized two-color photo\-ionization scheme. Excited He$^+$ ions, created by extreme ultraviolet (XUV) circularly polarized radiation from the XUV-FEL FERMI in the oriented $3p\, (m\!=\!+1)$ state, are exposed to circularly polarized 784-nm NIR radiation with peak intensities from $10^{12}\,\rm W/cm^2$ to $\rm 10^{13}\,W/cm^2$. The angular distribution of the ejected electrons exhibit a strong dichroism depending on the NIR intensity. While the co-rotating case is defined by a single path, for the counter-rotating case, there are two dominant pathways whose relative strength and phase difference are determined.

physics.atom-ph

Strong-Field Ionization Phenomena Revealed by Quantum Trajectories

We investigate the photoionization dynamics of atoms subjected to intense, ultrashort laser pulses through the use of quantum trajectories. This method provides a unique and consistent framework for examining electron dynamics within a time-dependent potential barrier. Our findings demonstrate that quantum trajectories offer additional insights into several key aspects of strong-field ionization, including the transition between ionization regimes, non-adiabatic effects under the barrier, the impact of the shape of the electronic potential, and the efficiency of over-the-barrier ionization.

physics.atom-ph

Circular Dichroism in Multiphoton Ionization of Resonantly Excited Helium Ions near Channel Closing

The circular dichroism (CD) of photoelectrons generated by near-infrared (NIR) laser pulses using multiphoton ionization of excited He$^+$ ions in the 3p(m=+1) state. The ions were prepared by circularly polarized extreme ultraviolet (XUV) pulses. For circularly polarized NIR pulses co- and counter-rotating relative to the polarization of the XUV pulse, a complex variation of the CD is observed as a result of intensity- and polarization-dependent Freeman resonances, with and without additional dichroic AC-Stark shifts. The experimental results are compared with numerical solutions of the time-dependent Schr\"odinger equation to identify and interpret the pronounced variation of the experimentally observed CD.

physics.atom-ph

Coherent control of multiphoton ionization of lithium atoms by a bichromatic laser field

We demonstrate a left-right asymmetry control of the photo\-electron angular distribution in multi\-photon ionization of Li atoms by a bichromatic laser field. By delaying the fundamental (780 nm) and its second harmonic relative to each other in steps of 130 atto\-seconds, we can vary the relative phase between the two laser fields with sub-wavelength accuracy and thereby steer the ejected electrons. Good agreement is found between the measurements and calculations at the appropriate intensities of the two harmonics.

physics.atom-ph

Opportunities for Gas-Phase Science at Short-Wavelength Free-Electron Lasers with Undulator-Based Polarization Control

Free-electron lasers (FELs) are the world's most brilliant light sources with rapidly evolving technological capabilities in terms of ultrabright and ultrashort pulses over a large range of accessible photon energies. Their revolutionary and innovative developments have opened new fields of science regarding nonlinear light-matter interaction, the investigation of ultrafast processes from specific observer sites, and approaches to imaging matter with atomic resolution. A core aspect of FEL science is the study of isolated and prototypical systems in the gas phase with the possibility of addressing well-defined electronic transitions or particular atomic sites in molecules. Notably for polarization-controlled short-wavelength FELs, the gas phase offers new avenues for investigations of nonlinear and ultrafast phenomena in spin orientated systems, for decoding the function of the chiral building blocks of life as well as steering reactions and particle emission dynamics in otherwise inaccessible ways. This roadmap comprises descriptions of technological capabilities of facilities worldwide, innovative diagnostics and instrumentation, as well as recent scientific highlights, novel methodology and mathematical modeling. The experimental and theoretical landscape of using polarization controllable FELs for dichroic light-matter interaction in the gas phase will be discussed and comprehensively outlined to stimulate and strengthen global collaborative efforts of all disciplines.

physics.atom-ph

High-Harmonic Generation in the Water Window from mid-IR Laser Sources

We investigate the harmonic response of neon atoms to mid-IR laser fields (2000-3000nm) using a single-active electron (SAE) model and the fully ab initio all-electron R-Matrix with Time-dependence (RMT) method. The laser peak intensity and wavelength are varied to find suitable parameters for high-harmonic imaging in the water window. Comparison of the SAE and RMT results shows qualitative agreement between them as well as parameters such as the cutoff frequency predicted by the classical three-step model. However, there are significant differences in the details, particularly in the predicted conversion efficiency. These details indicate the possible importance of multi-electron effects, as well as a strong sensitivity of quantitative predictions on specific aspects of the numerical model.

physics.atom-ph

Photoelectron momentum distributions in the strong-field ionization of atomic hydrogen by few-cycle elliptically polarized optical pulses

We investigate the strong-field ionization of atomic hydrogen in a few-cycle elliptically polarized infrared pulse by solving the time-dependent Schrödinger equation. The dependence of the photoelectron momentum distribution on the pulse intensity, ellipticity, length, envelope, and carrier envelope phase is analyzed. In particular, we explain the variation of the electron offset angle with asymptotic electron energy through the combined action of the field and the Coulomb potential, and demonstrate that low-ellipticity pulses make it possible to access the electron release time.

physics.atom-ph

Quantum control of entangled photon-pair generation in electron-atom collisions driven by laser-synthesized free-electron wave packets

We propose an extension of coherent control using laser-synthesized free-electron matter waves. In contrast to coherent control schemes exploiting optical coherences to steer the dynamics of matter waves, we analyze the opposite and investigate the control of quantum light emission driven by laser-sculpted coherent free-electron matter waves. We apply this concept to the control of entangled photon-pair emission in electron-atom collisions, in which the incident electron wave packet, colliding with a target atom $B$, is engineered by interferometric resonantly-enhanced multiphoton ionization of a parent atom $A$. Each ionization pathway leads to electron wave packets that coherently interfere during temporal evolution in the continuum. Their mutual coherence can be controlled by adjusting the relative phases or time delays of the frequency components of the ionizing field contributing to the interfering pathways. We report coherent control of entangled photon-pair generation in radiative photo-cascade emission upon decay of the target atom after inelastic excitation triggered by the collision with the synthesized electron wave packet.

quant-ph

Decomposition of the transition phase in multi-sideband RABBITT schemes

Reconstruction of Attosecond Beating By Interference of Two-photon Transitions (RABBITT) is a technique that can be used to determine the phases of atomic transition elements in photoionization processes. In the traditional RABBITT scheme, the so-called "asymptotic approximation" considers the measured phase as a sum of the Wigner phase linked to a single-photon ionization process and the continuum-continuum (cc) phase associated with further single-photon transitions in the continuum. In this paper, we explore the possibility of extending the asymptotic approximation to multi-sideband RABBITT schemes. The predictions from this approximation are then compared with results obtained by an {\it ab initio} calculation based on solving the time-dependent Schrödinger equation for atomic hydrogen.

quant-ph

Photoelectron spectroscopy of laser-dressed atomic helium

Photoelectron emission from excited states of laser-dressed atomic helium is analyzed with respect to laser intensity-dependent excitation energy shifts and angular distributions. In the two-color XUV (exteme ultra\-violet) -- IR (infrared) measurement, the XUV photon energy is scanned between \SI{20.4}{\electronvolt} and the ionization threshold at \SI{24.6}{\electronvolt}, revealing electric dipole-forbidden transitions for a temporally overlapping IR pulse ($\sim\!\SI{e12}{\watt\per \centi\meter\squared}$). The interpretation of the experimental results is supported by numerically solving the time-dependent Schrödinger equation in a single-active-electron approximation.

physics.atom-ph

Observation of Dynamic Stark Resonances in Strong-Field Excitation

We investigate AC Stark-shifted resonances in argon with ultrashort near-infrared pulses. Using 30 fs pulses we observe periodic enhancements of the excitation yield in the intensity regions corresponding to the absorption of 13 and 14 photons. By reducing the pulse duration to 6 fs with only a few optical cycles, we also demonstrate that the enhancements are significantly reduced beyond what is measurable in the experiment. Comparing these to numerical predictions, which are in quantitative agreement with experimental results, we find that even though the quantum-state distribution can be broad, the enhancements are largely due to efficient population of a select few AC Stark-shifted resonant states rather than the closing of an ionization channel. Because these resonances are dependent on the frequency and intensity of the laser field, the broad bandwidth of the 6 fs pulses means that the resonance condition is fulfilled across a large range of intensities. This is further exaggerated by volume-averaging effects, resulting in excitation of the $5g$ state at almost all intensities and reducing the apparent magnitude of the enhancements. For 30 fs pulses, volume averaging also broadens the quantum state distribution but the enhancements are still large enough to survive. In this case, selectivity of excitation to a single state is reduced below 25% of the relative population. However, an analysis of TDSE simulations indicates that excitation of up to 60% into a single state is possible if volume averaging can be eliminated and the intensity can be precisely controlled.

physics.atom-ph

Non-LTE analysis of K I in late-type stars

Older GCE models predict [K/Fe] ratios as much as 1 dex lower than those inferred from stellar observations. Abundances of potassium are mainly based on analyses of the 7698 $Å$ resonance line, and the discrepancy between models and observations is in part caused by the LTE assumption. We study the statistical equilibrium of KI, focusing on the non-LTE effects on the $7698 \ Å$ line. We aim to determine how non-LTE abundances of K can improve the analysis of its chemical evolution, and help to constrain the yields of models. We construct a model atom that employs the most up-to-date data. In particular, we calculate and present inelastic e+K collisional excitation cross-sections from the convergent close-coupling and the $B$-Spline $R$-matrix methods, and H+K collisions from the two-electron model. We constructed a fine grid of non-LTE abundance corrections that span $4000<\teff / \rm{K}<8000$, $0.50<\lgg<5.00$, $-5.00<\feh<+0.50$, and applied the corrections to abundances from the literature. In concordance with previous studies, we find severe non-LTE effects in the $7698 \ Å$ line, which is stronger in non-LTE with abundance corrections that can reach $\sim-0.7\,\dex$. We explore the effects of atmospheric inhomogeneity by computing a full 3D non-LTE stellar spectrum of KI for a test star. We find that 3D is necessary to predict a correct shape of the resonance 7698 $Å$ line, but the line strength is similar to that found in 1D non-LTE. Our non-LTE abundance corrections reduce the scatter and change the cosmic trends of literature K abundances. In the regime [Fe/H]$\lesssim-1.0$ the non-LTE abundances show a good agreement with the GCE model with yields from rotating massive stars. The reduced scatter of the non-LTE corrected abundances of a sample of solar twins shows that line-by-line differential analysis techniques cannot fully compensate for systematic modelling errors.

astro-ph.SR

Electron-impact excitation and ionization of atomic calcium at intermediate energies

We present a comprehensive study of electron collisions with calcium atoms by using the convergent \emph{B}-spline \emph{R}-matrix method. Elastic, excitation, and ionization cross sections were obtained for all transitions between the lowest 39 physical states of calcium (except for $3p^6 4s5g\ ^{3,1}G$) up to the $3p^6 4s8s\ ^1S$ state, for incident electron energies ranging from threshold to 100~eV. A multi\-configuration Hartree-Fock method with non\-orthogonal term-dependent orbitals was employed to generate accurate wave functions for the target states. Close-coupling expansions including the 39 physical states plus 444 pseudo-target states of calcium were used to check the sensitivity of the results to coupling to the target continuum. The cross-section dataset obtained from the large-scale calculations is expected to be sufficiently accurate and comprehensive for most current modeling applications involving neutral calcium.

physics.atom-ph

Attosecond angular streaking and tunnelling time in atomic hydrogen

Tunnelling, one of the key features of quantum mechanics, ignited an ongoing debate about the value, meaning and interpretation of 'tunnelling time'. Until recently the debate was purely theoretical, with the process considered to be instantaneous for all practical purposes. This changed with the development of ultrafast lasers and in particular, the 'attoclock' technique that is used to probe the attosecond dynamics of electrons. Although the initial attoclock measurements hinted at instantaneous tunnelling, later experiments contradicted those findings, claiming to have measured finite tunnelling times. In each case these measurements were performed with multi-electron atoms. Atomic hydrogen (H), the simplest atomic system with a single electron, can be 'exactly' (subject only to numerical limitations) modelled using numerical solutions of the 3D-TDSE with measured experimental parameters and acts as a convenient benchmark for both accurate experimental measurements and calculations. Here we report the first attoclock experiment performed on H and find that our experimentally determined offset angles are in excellent agreement with accurate 3D-TDSE simulations performed using our experimental pulse parameters. The same simulations with a short-range Yukawa potential result in zero offset angles for all intensities. We conclude that the offset angle measured in the attoclock experiments originates entirely from electron scattering by the long-range Coulomb potential with no contribution from tunnelling time delay. That conclusion is supported by empirical observation that the electron offset angles follow closely the simple formula for the deflection angle of electrons undergoing classical Rutherford scattering by the Coulomb potential. Thus we confirm that, in H, tunnelling is instantaneous (with an upperbound of 1.8 as) within our experimental and numerical uncertainty.

physics.atom-ph

Dynamics of Tunneling Ionization using Bohmian Mechanics

Recent attoclock experiments and theoretical studies regarding the strong-field ionization of atoms by few-cycle infrared pulses revealed new features that have attracted much attention. Here we investigate tunneling ionization and the dynamics of the electron probability using Bohmian Mechanics. We consider a one-dimensional problem to illustrate the underlying mechanisms of the ionization process. It is revealed that in the major part of the below-the-barrier ionization regime, in an intense and short infrared pulse, the electron does not tunnel \through" the entire barrier, but rather already starts from the classically forbidden region. Moreover, we highlight the correspondence between the probability of locating the electron at a particular initial position and its asymptotic momentum. Bohmian Mechanics also provides a natural definition of mean tunneling time and exit position, taking account of the time dependence of the barrier. Finally, we find that the electron can exit the barrier with significant kinetic energy, thereby corroborating the results of a recent study [Camus et al., Phys. Rev. Lett. 119 (2017) 023201].

physics.atom-ph

QDB: a new database of plasma chemistries and reactions

One of the most challenging and recurring problems when modelling plasmas is the lack of data on key atomic and molecular reactions that drive plasma processes. Even when there are data for some reactions, complete and validated datasets of chemistries are rarely available. This hinders research on plasma processes and curbs development of industrial applications. The QDB project aims to address this problem by providing a platform for provision, exchange, and validation of chemistry datasets. A new data model developed for QDB is presented. QDB collates published data on both electron scattering and heavy-particle reactions. These data are formed into reaction sets, which are then validated against experimental data where possible. This process produces both complete chemistry sets and identifies key reactions that are currently unreported in the literature. Gaps in the datasets can be filled using established theoretical methods. Initial validated chemistry sets for SF$_6$/CF$_4$/O$_2$ and SF$_6$/CF$_4$/N$_2$/H$_2$ are presented as examples.

physics.plasm-ph

Above-threshold ionization in neon produced by combining optical and bichromatic XUV femtosecond pulses

We consider the ionization of neon induced by a femtosecond laser pulse composed of overlapping, linearly polarized bichromatic extreme ultraviolet and infrared fields. In particular, we study the effects of the infrared light on a two-pathway ionization scheme for which Ne 2s22p53s1P is used as intermediate state. Using time-dependent calculations, supported by a theoretical approach based on the strong-field approximation, we analyze the ionization probability and the photoelectron angular distributions associated with the different sidebands of the ionization spectrum. Complex oscillations of the angular distribution anisotropy parameters as a function of the infrared light intensity are revealed. Finally, we demonstrate that coherent control of the asymmetry is achievable by tuning the infrared frequency to a nearby electronic transition.

physics.atom-ph