arXiv subjects

Sebastian Eckart

Publications and source records attributed to Sebastian Eckart.

18 recordsLinked to original sources

arXiv2026

Ultrafast electron vortex produced by a grating made of light

The generation of vortex matter waves carrying quantized orbital angular momentum is challenging and relies heavily on the material nanofabrication methods due to their extremely small de-Broglie wavelengths. Here, we introduce an all-optical method for generating an electron vortex by diffraction through a grating made of light. We realize the orbital angular momentum transfer between free electrons and photons by stimulated Compton scattering. The transferred angular momentum quantum number can be freely tuned. The method can be generalized to a broad range of charged particles, neutral atoms, and molecules of diverse masses. Our results open up novel opportunities for applications in free electron lasers and ultrafast electron microscopy by utilizing the orbital angular momentum degree of freedom of free electrons.

physics.atom-ph↗

arXiv2025

Dynamical phase evolution of Coulomb-focused electrons in strong-field ionization probed by a standing light wave

We investigate the dynamical phase evolution of Coulomb-focused electrons in strong-field ionization. We diffract the electrons with an ultrashort standing light wave to track their time-dependent phase. Our findings show that low-energy electrons exhibit a unique chromosome-shaped diffraction pattern, distinct from higher-energy electrons. Our numerical model quantitatively reproduces the experimental results, confirming this pattern maps the electron's time-dependent phase evolution as it escapes from a Coulomb potential. Our pulsed diffraction grating technique offers a new way to sense an electron's quantum phase without interfering its release mechanism.

physics.atom-ph↗

arXiv2024

Ultrafast Kapitza-Dirac effect

Similar to the optical diffraction of light passing through a material grating, the Kapitza-Dirac effect occurs when an electron is diffracted by a standing light wave. In its original description the effect is time-independent. In the present work, we extend the Kapitza-Dirac concept to the time domain. By tracking the spatiotemporal evolution of a pulsed electron wave packet diffracted by a femtosecond (10 15 second) standing wave pulse in a pump-probe scheme, we observe so far unseen time-dependent diffraction patterns. The fringe spacing in the observed pattern differs from that generated by the conventional Kapitza-Dirac effect, moreover it decreases as the pump-probe delay time increases. By exploiting this time-resolved diffraction scheme, we gather access to the time evolution of the previously inaccessible phase properties of a free electron.

physics.optics↗

arXiv2022

Non-adiabatic Strong Field Ionization of Atomic Hydrogen

We present experimental data on the non-adiabatic strong field ionization of atomic hydrogen using elliptically polarized femtosecond laser pulses at a central wavelength of 390 nm. Our measured results are in very good agreement with a numerical solution of the time-dependent Schrödinger equation (TDSE). Experiment and TDSE show four above-threshold ionization (ATI) peaks in the electron's energy spectrum. The most probable emission angle (also known as 'attoclock-offset angle' or 'streaking angle') is found to increase with energy, a trend that is opposite to standard predictions based on Coulomb interaction with the ion. We show that this increase of deflection-angle can be explained by a model that includes non-adiabatic corrections of the initial momentum distribution at the tunnel exit and non-adiabatic corrections of the tunnel exit position itself.

physics.atom-ph↗

arXiv2021

Magnetic-field effect in high-order above-threshold ionization

We experimentally and theoretically investigate the influence of the magnetic component of an electromagnetic field on high-order above-threshold ionization of xenon atoms driven by ultrashort femtosecond laser pulses. The nondipole shift of the electron momentum distribution along the light-propagation direction for high energy electrons beyond the classical cutoff is found to be vastly different from that below the cutoff. A V-shape structure in the momentum dependence of the nondipole shift above the cutoff is identified for the first time. With the help of classical and quantum-orbit analysis, we show that large-angle rescattering of the electrons strongly alters the partitioning of the photon momentum between electron and ion. The sensitivity of the observed nondipole shift to the electronic structure of the target atom is confirmed by three-dimensional time-dependent Schrödinger equation simulations for different model potentials.

physics.atom-ph↗

arXiv2021

Photoelectron energy peaks shift against the radiation pressure in strong field ionization

The photoelectric effect describes the ejection of an electron upon absorption of one or several photons. The kinetic energy of this electron is determined by the photon energy reduced by the binding energy of the electron and, if strong laser fields are involved, by the ponderomotive potential in addition. It has therefore been widely taken for granted that for atoms and molecules the photoelectron energy does not depend on the electron's emission direction but theoretical studies have questioned this since 1990. Here we provide experimental evidence, that the energies of photoelectrons emitted against the light-propagation direction are shifted towards higher values while those electrons that are emitted along the light-propagation direction are shifted to lower values. We attribute the energy shift to a nondipole contribution from the interaction of the moving electrons with the incident photons.

physics.atom-ph↗

arXiv2021

Quantum interference and imaging using intense laser fields

The interference of matter waves is one of the intriguing features of quantum mechanics that has impressed researchers and laymen since it was first suggested almost a century ago. Nowadays, attosecond science tools allow us to utilize it in order to extract valuable information from electron wavepackets. Intense laser fields are routinely employed to create electron wave packets and control their motion with sub-femtosecond and sub-nanometer precision. In this perspective article, we discuss some of the peculiarities of intense light-matter interaction. We review some of the most important techniques used in attosecond imaging, namely photoelectron holography and laser-induced electron diffraction. We attempt to ask and answer a few questions that do not get asked very often. For example, if we are interested in position space information, why are measurements carried out in momentum space? How to accurately retrieve photoelecron spactra from the numerical solution of the time-dependent Schrödinger equation? And, what causes the different coherence properties of high-harmonic generation and above-threshold ionization?

physics.chem-ph↗

arXiv2021

Measuring the photoelectron emission delay in the molecular frame

If matter absorbs a photon of sufficient energy it emits an electron. The question of the duration of the emission process has intrigued scientists for decades. With the advent of attosecond metrology, experiments addressing such ultrashort intervals became possible. While these types of studies require attosecond experimental precision, we present here a novel measurement approach that avoids those experimental difficulties. We instead extract the emission delay from the interference pattern generated as the emitted photoelectron is diffracted by the parent ion's potential. Targeting core electrons in CO, we measured a 2d map of photoelectron emission delays in the molecular frame over a wide range of electron energies. The measured emission times depend drastically on the emission direction and exhibit characteristic changes along the shape resonance of the molecule. Our approach can be routinely extended to other electron orbitals and more complex molecules.

physics.atom-ph↗

arXiv2021

Angular dependence of the Wigner time delay upon tunnel ionization of $H_{2}$

More than 100 years after its discovery and its explanation in the energy domain, the duration of the photoelectric effect is still heavily studied. The emission time of a photoelectron can be quantified by the Wigner time delay. Experiments addressing this time delay for single-photon ionization became feasible during the last 10 years. A missing piece, which has not been studied, so far, is the Wigner time delay for strong-field ionization of molecules. Here we show experimental data on the Wigner time delay for tunnel ionization of $H_{2}$ molecules and demonstrate its dependence on the emission direction of the electron with respect to the molecular axis. We find, that the observed changes in the Wigner time delay can be quantitatively explained by elongated/shortened travel paths of the electrons that are due to spatial shifts of the electron's birth position after tunneling. This introduces an intuitive perspective towards the Wigner time delay in strong-field ionization.

physics.atom-ph↗

arXiv2020

Swirling the weakly bound helium dimer from inside

Controlling the interactions between atoms with external fields opened up new branches in physics ranging from strongly correlated atomic systems to ideal Bose and Fermi gases and Efimov physics. Such control usually prepares samples that are stationary or evolve adiabatically in time. On the other hand, in molecular physics external ultrashort laser fields are employed to create anisotropic potentials that launch ultrafast rotational wave packets and align molecules in free space. Here we combine these two regimes of ultrafast times and low energies. We apply a short laser pulse to the helium dimer, a weakly bound and highly delocalized single bound state quantum system. The laser field locally tunes the interaction between two helium atoms, imparting an angular momentum of $2\hbar$ and evoking an initially confined dissociative wave packet. We record a movie of the density and phase of this wave packet as it evolves from the inside out. At large internuclear distances, where the interaction between the two helium atoms is negligible, the wave packet is essentially free. This work paves the way for future tomography of wave packet dynamics and provides the technique for studying exotic and otherwise hardly accessible quantum systems such as halo and Efimov states.

physics.atm-clus↗

arXiv2020

Kinematically complete experimental study of Compton scattering at helium atoms near the ionization threshold

Compton scattering is one of the fundamental interaction processes of light with matter. Already upon its discovery [1] it was described as a billiard-type collision of a photon kicking a quasi-free electron. With decreasing photon energy, the maximum possible momentum transfer becomes so small that the corresponding energy falls below the binding energy of the electron. Then ionization by Compton scattering becomes an intriguing quantum phenomenon. Here we report a kinematically complete experiment on Compton scattering at helium atoms below that threshold. We determine the momentum correlations of the electron, the recoiling ion, and the scattered photon in a coincidence experiment finding that electrons are not only emitted in the direction of the momentum transfer, but that there is a second peak of ejection to the backward direction. This finding links Compton scattering to processes as ionization by ultrashort optical pulses [2], electron impact ionization [3,4], ion impact ionization [5,6], and neutron scattering [7] where similar momentum patterns occur.

physics.atom-ph↗

arXiv2020

Zeptosecond Birth Time Delay in Molecular Photoionization

Photoionization is one of the fundamental light-matter interaction processes in which the absorption of a photon launches the escape of an electron. The time scale of the process poses many open questions. Experiments found time delays in the attosecond ($10^{-18}$ s) domain between electron ejection from different orbitals, electronic bands, or in different directions. Here, we demonstrate that across a molecular orbital the electron is not launched at the same time. The birth time rather depends on the travel time of the photon across the molecule, which is 247 zeptoseconds ($10^{-21}$ s) for the average bond length of H$_2$. Using an electron interferometric technique, we resolve this birth time delay between electron emission from the two centers of the hydrogen molecule.

physics.atom-ph↗

arXiv2020

Holographic Angular Streaking of Electrons and the Wigner-Time Delay

For a circularly polarized single-color field at a central frequency of $2ω$ the final electron momentum distribution upon strong field ionization does not carry any information about the phase of the initial momentum distribution. Adding a weak, co-rotating, circularly polarized field at a central frequency of $ω$ gives rise to a sub-cycle interference pattern (holographic angular streaking of electrons (HASE)). This interference pattern allows for the retrieval of the derivative of the phase of the initial momentum distribution after tunneling $ϕ^{\prime}_{\mathrm{off}}(p_i)$. A trajectory-based semi-classical model (HASE model) is introduced which links the experimentally accessible quantities to $ϕ^{\prime}_{\mathrm{off}}(p_i)$. It is shown that a change in $ϕ^{\prime}_{\mathrm{off}}$ is equivalent to a displacement in position space $Δx$ of the initial wave packet after tunneling. This offset in position space allows for an intuitive interpretation of the Wigner time delay $Δτ_W$ in strong field ionization for circularly polarized single-color fields. The influence of Coulomb interaction after tunneling is investigated quantitatively.

quant-ph↗

arXiv2020

Holographic detection of parity in atomic and molecular orbitals

We introduce a novel and concise methodology to detect the parity of atomic and molecular orbitals based on photoelectron holography, which is more general than the existing schemes. It fully accounts for the Coulomb distortions of electron trajectories, does not require sculpted fields to retrieve phase information and, in principle, is applicable to a broad range of electron momenta. By comparatively measuring the differential photoelectron spectra from strong-field ionization of N$_{2}$ molecules and their companion atoms of Ar, some photoelectron holography patterns are found to be dephased for both targets. This is well reproduced by the full-dimensional time-dependent Schrödinger equation and the Coulomb quantum-orbit strong-field approximation (CQSFA) simulation. Using the CQSFA, we trace back our observations to different parities of the 3$p$ orbital of Ar and the highest-occupied molecular orbital of N$_{2}$ via interfering Coulomb-distorted quantum orbits carrying different initial phases. This method could in principle be used to extract bound-state phases from any holographic structure, with a wide range of potential applications in recollision physics and spectroscopy.

physics.atom-ph↗

arXiv2020

Orientation Dependent Dissociative Ionization of H$_2$ in Strong Elliptic Laser Fields: Modification of the release time through molecular orientation

We investigate the photoelectron angular emission distributions obtained by strong field dissociative ionization of H$_2$ using cold target recoil ion momentum spectroscopy. In case of employing laser light with an ellipticity close to 0.9 and an intensity of 1.0 $\times$ 10$^{14}$ W/cm$^2$, we find that the most probable release-time of the electron does not generally coincide with the time when the laser field maximizes. The release-time is affected by the molecular orientation. In addition, we observe that the width of the release-time distribution depends on molecular orientation. We attribute this observation to the two-center-interference.

physics.atom-ph↗

arXiv2019

Correlation enhancement of high-order harmonics generation in Xe

We consider the process of high-order harmonics generation (HHG) in the xenon atom enhanced by the inter-shell correlation between the valence 5p and inner 4d shells. We derive the HHG spectrum from a numerical solution of the one-electron time-dependent Schrödinger equation multiplied by the enhancement factor taken as the photoionization cross-sections ratio calculated with and without the inter-shell correlation. Such a simplified approach is adequate to describe the experimental HHG spectrum reported by Shiner et al [Nat. Phys. 7, 464 (2011)] generated by a single color IR laser. Similarly, we find good agreement when applied to the two-color driven HHG spectra reported by Facciala et al [Phys. Rev. Lett. 117, 093902 (2016)].

physics.atom-ph↗

arXiv2018

Keldysh-Rutherford model for attoclock

We demonstrate a clear similarity between attoclock offset angles and Rutherford scattering angles taking the Keldysh tunnelling width as the impact parameter and the vector potential of the driving pulse as the asymptotic velocity. This simple model is tested against the solution of the time-dependent Schrödinger equation using hydrogenic and screened (Yukawa) potentials of equal binding energy. We observe a smooth transition from a hydrogenic to 'hard-zero' intensity dependence of the offset angle with variation of the Yukawa screening parameter. Additionally we make comparison with the attoclock offset angles for various noble gases obtained with the classical-trajectory Monte Carlo method. In all cases we find a close correspondence between the model predictions and numerical calculations. This suggests a largely Coulombic origin of the attoclock offset angle and casts further doubt on its interpretation in terms of a finite tunnelling time.

physics.atom-ph↗

arXiv2018

Ultrafast Preparation and Detection of Ring Currents in Single Atoms

Quantum particles can penetrate potential barriers by tunneling (1). If that barrier is rotating, the tunneling process is modified (2,3). This is typical for electrons in atoms, molecules or solids exposed to strong circularly polarized laser pulses (4,5). Here we measure how the transmission probability through a rotating tunnel depends on the sign of the magnetic quantum number m of the electron and thus on the initial sense of rotation of its quantum phase. We further show that the electron keeps part of that rotary motion on its way through the tunnel by measuring m-dependent modification of the electron emission pattern. These findings are relevant for attosecond metrology as well as for interpretation of strong field electron emission from atoms and molecules (6-13) and directly demonstrates the creation of ring currents in bound states of ions with attosecond precision. In solids, this could open a way to inducing and controlling ring-current related topological phenomena (14).

physics.atom-ph↗