arXiv subjects

Eva Lindroth

Publications and source records attributed to Eva Lindroth.

At least 19 recordsLinked to original sources

arXiv2025

Photoionization time delays probe electron correlations

The photoelectric effect, explained by Einstein in 1905, is often regarded as a one-electron phenomenon. However, in multi-electron systems, the interaction of the escaping electron with other electrons, referred to as electron correlation, plays an important role. For example, electron correlations in photoionization of the outer $s$-subshells of rare gas atoms lead to a substantial minimum in the ionization probability, which was theoretically predicted in 1972 and experimentally confirmed using synchrotron radiation. However, recent attosecond photoionization time delay measurements in argon strongly disagree with theory, thus raising questions on the nature of electron correlations leading to this minimum. In this work, combining high-spectral resolution attosecond interferometry experiments and novel theoretical calculations allows us to identify the most essential electron correlations affecting the photoemission. The measurement of time delays gives unprecedented insight into the photoionization process, unraveling details of the atomic potential experienced by the escaping electron and capturing its dynamics.

physics.atom-ph↗

arXiv2024

The influence of final state interactions in attosecond photoelectron interferometry

Fano resonances are ubiquitous phenomena appearing in many fields of physics, e.g. atomic or molecular photoionization, or electron transport in quantum dots. Recently, attosecond interferometric techniques have been used to measure the amplitude and phase of photoelectron wavepackets close to Fano resonances in argon and helium, allowing for the retrieval of the temporal dynamics of the photoionization process. In this work, we study the photoionization of argon atoms close to the $3s^13p^64p$ autoionizing state using an interferometric technique with high spectral resolution. The phase shows a monotonic $2{\pi}$ increase across the resonance or a sigmo\"idal less than ${\pi}$ variation depending on experimental conditions, e.g. the probe laser bandwidth. Using three different, state-of-the-art calculations, we show that the measured phase is influenced by the interaction between final states reached by two-photon transitions.

physics.atom-ph↗

arXiv2024

Anisotropy parameters for two-color photoionization phases in randomly oriented molecules: theory and experiment in methane and deuteromethane

We present a combined theoretical and experimental work investigating the angle-resolved phases of the photoionization process driven by a two-color field consisting of an attosecond pulse train and an infrared pulse in an ensemble of randomly oriented molecules. We derive a general form for the two-color photoelectron (and time-delay) angular distribution valid also in the case of chiral molecules and when relative polarizations of the photons contributing to the attosecond photoelectron interferometer differ. We show a comparison between the experimental data and the theoretical predictions in an ensemble of methane and deuteromethane molecules, discussing the effect of nuclear dynamics on the photoionization phases. Finally, we demonstrate that the oscillating component and the phase of the two-color signal can be fitted using complex asymmetry parameters, in perfect analogy with the atomic case.

physics.chem-ph↗

arXiv2023

Measuring the quantum state of photoelectrons

A photoelectron, emitted due to the absorption of light quanta as described by the photoelectric effect, is often characterized experimentally by a classical quantity, its momentum. However, since the photoelectron is a quantum object, its rigorous characterization requires the reconstruction of the complete quantum state, the photoelectron's density matrix. Here, we use quantum state tomography to fully characterize photoelectrons emitted from helium and argon atoms upon absorption of ultrashort, extreme ultraviolet light pulses. While in helium we measure a pure photoelectronic state, in argon, spin-orbit interaction induces entanglement between the ion and the photoelectron, leading to a reduced purity of the photoelectron state. Our work shows how state tomography gives new insights into the fundamental quantum aspects of light-induced electronic processes in matter, bridging the fields of photoelectron spectroscopy and quantum information, and offering new spectroscopic possibilities for quantum technology.

quant-ph↗

arXiv2022

Autoionizing polaritons with the Jaynes-Cummings model

Intense laser pulses have the capability to couple resonances in the continuum, leading to the formation of a split pair of autoionizing polaritons. These polaritons can exhibit extended lifetimes due to interference between radiative and Auger decay channels. In this work, we show how an extension of the Jaynes-Cummings model to autoionizing states quantitatively reproduces the observed phenomenology. This extended model allows us to study how the dressing laser parameters can be tuned to control the ionization rate of the polariton multiplet.

physics.atom-ph↗

arXiv2022

Ionic Coherence in Resonant Above-Threshold Attosecond Ionization Spectroscopy

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 atom, which we simulate using the newstock \emph{ab initio} code. Due to the fine-structure splitting of the N=3 He$^+$ level, the ionic dipole beats on a picosecond timescale. We show how, from the dipole beating, it is possible to reconstruct the polarization of the ion at its inception.

physics.atom-ph↗

arXiv2022

Thomas--Reiche--Kuhn Correction for Truncated Configuration Interaction Spaces: Case of Laser-Assisted Dynamical Interference

The Thomas--Reiche--Kuhn sum rule is used to form an effective potential that is added to the time-dependent configuration interaction singles (TDCIS) equations of motion in velocity gauge. The purpose of the effective potential is to include virtual coupling from singles to doubles, which is required for size-consistent velocity gauge TDCIS results. The proposed method is compared to length gauge TDCIS results for laser-assisted photoionization. Finally, a novel dynamical interference effect controlled by two-color fields is predicted for atomic targets.

physics.atom-ph↗

arXiv2022

Resonant two-photon ionization of helium atoms studied by attosecond interferometry

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 the two-photon random phase approximation with exchange to account for electron correlation effects. We give an interpretation for the multiple $\pi$-rad phase jumps observed, both at and away from resonance, as well as their dependence on the emission angle.

physics.atom-ph↗

arXiv2021

Relativistic time-dependent configuration-interaction singles

In this work, a derivation and implementation of the relativistic time-dependent configuration interaction singles (RTDCIS) method is presented. Various observables for krypton and xenon atoms obtained by RTDCIS are compared with experimental data and alternative relativistic calculations. This includes energies of occupied orbitals in the Dirac-Fock ground state, Rydberg state energies, Fano resonances and photoionization cross sections. Diagrammatic many-body perturbation theory, based on the relativistic random phase approximation, is used as a benchmark with excellent agreement between RTDCIS reported at the Tamm-Dancoff level. Results from RTDCIS are computed in the length gauge, here the negative energy states can be omitted with acceptable loss of accuracy. A complex absorbing potential, that is used to remove photoelectrons far from the ion, is implemented as a scalar potential and validated for RTDCIS. The RTDCIS methodology presented here opens for future studies of strong-field processes, such as attosecond transient absorption and high-order harmonic generation, with electron and hole spin dynamics and other relativistic effects described by first principle via the Dirac equation.

physics.atom-ph↗

arXiv2021

Complete characterization of multi-channel single photon ionization

Ionization of atoms and molecules by absorption of a light pulse results in electron wavepackets carrying information on the atomic or molecular structure as well as on the dynamics of the ionization process. These wavepackets can be described as a coherent sum of waves of given angular momentum, called partial waves, each characterized by an amplitude and a phase. The complete characterization of the individual angular momentum components is experimentally challenging, requiring the analysis of the interference between partial waves both in energy and angle. Using a two-photon interferometry technique based on extreme ultraviolet attosecond and infrared femtosecond pulses, we characterize the individual partial wave components in the photoionization of the 2p shell in neon. The study of the phases of the angular momentum channels allows us to unravel the influence of short-range, correlation and centrifugal effects. This approach enables the complete reconstruction of photoionization electron wavepackets in time and space, providing insight into the photoionization dynamics.

physics.atom-ph↗

arXiv2021

Attosecond photoelectron spectroscopy of helium doubly excited states

We describe a numerical method that simulates the interaction of the helium atom with sequences of femtosecond and attosecond light pulses. The method, which is based on the close-coupling expansion of the electronic configuration space in a B-spline bipolar spherical harmonic basis, can accurately reproduce the excitation and single ionization of the atom, within the electrostatic approximation. The time dependent Schrödinger equation is integrated with a sequence of second-order split-exponential unitary propagators. The asymptotic channel-, energy- and angularly-resolved photoelectron distributions are computed by projecting the wavepacket at the end of the simulation on the multichannel scattering states of the atom, which are separately computed within the same close-coupling basis. This method is applied to simulate the pump-probe ionization of helium in the vicinity of the $2s/2p$ excitation threshold of the He$^+$ ion. This work confirms the qualitative conclusions of one of our earliest publications [L Argenti and E Lindroth, Phys. Rev. Lett. {\bf 105}, 53002 (2010)], in which we demonstrated the control of the $2s/2p$ ionization branching-ratio. Here, we take those calculations to convergence and show how correlation brings the periodic modulation of the branching ratios in almost phase opposition. The residual total ionization probability to the $2s+2p$ channels is dominated by the beating between the $sp_{2,3}^+$ and the $sp_{2,4}^+$ doubly excited states, which is consistent with the modulation of the complementary signal in the $1s$ channel, measured in 2010 by Chang and co-workers~[S Gilbertson~\emph{et al.}, Phys. Rev. Lett. {\bf 105}, 263003 (2010)].

physics.atom-ph↗

arXiv2021

Autoionizing Polaritons in Attosecond Atomic Ionization

Light-induced states are commonly observed in the photoionization spectra of laser-dressed atoms. The properties of autoionizing polaritons, entangled states of light and Auger resonances, however, are largely unexplored. We employ attosecond transient-absorption spectroscopy to study the evolution of autoionizing states in argon, dressed by a tunable femtosecond laser pulse. The avoided crossings between the $3s^{-1}4p$ and several light-induced states indicates the formation of polariton multiplets. We measure a controllable stabilization of the polaritons against ionization, in excellent agreement with \emph{ab initio} theory. Using an extension of the Jaynes-Cummings model to autoionizing states, we show that this stabilization is due to the destructive interference between the Auger decay and the radiative ionization of the polaritonic components. These results give new insights into the optical control of electronic structure in the continuum, and unlock the door to applications of autoionizing polaritons in poly-electronic systems.

physics.atom-ph↗

arXiv2021

Coherent control of an Helium-Ion ensemble

Attosecond pulses can ionize atoms in a coherent process. Since the emerging fragments are entangled, however, each preserves only a fraction of the initial coherence, thus limiting the chance of guiding the ion subsequent evolution. In this work, we use \emph{ab initio} simulations of pump-probe ionization of helium above the $2s/2p$ threshold to demonstrate how this loss of coherence can be controlled. Thanks to the participation of $2\ell n\ell'$ states, coherence between the ionic $2s$ and $2p$ states, which are degenerate in the non-relativistic limit, results in a stationary, delay-dependent electric dipole. From the picosecond real-time beating of the dipole, caused by the fine-structure splitting of the $n=2$ manifold, it is possible to reconstruct all original ion coherences, including between antiparallel-spin states, which are sensitive probe of relativistic effects in attosecond photoemission.

physics.atom-ph↗

arXiv2020

Implementation and validation of the relativistic transient absorption theory within the dipole approximation

A relativistic transient absorption theory is derived, implemented and validated within the dipole approximation based on the time-dependent Dirac equation. Time-dependent simulations have been performed using the Dirac equation and the Schrödinger equation for the Hydrogen atom in two different attosecond transient absorption scenarios. These simulations validate the present relativistic theory. The presented work can be seen as a first step in the development of a more general relativistic attosecond transient absorption spectroscopy method for studying heavy atoms, but it also suggests the possibility of studying relativistic effects, such as Zitterbewegung, in the time domain.

physics.atom-ph↗

arXiv2020

Attosecond electron-spin dynamics in Xe 4d photoionization

The photoionization of xenon atoms in the 70-100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe$^+$ states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide new insight into the complex electron-spin dynamics of photo-induced phenomena.

physics.atom-ph↗

arXiv2020

Non-exponential decay in Floquet-Bloch bands

Exponential decay laws describe systems ranging from unstable nuclei to fluorescent molecules, in which the probability of jumping to a lower-energy state in any given time interval is static and history-independent. These decays, involving only a metastable state and fluctuations of the quantum vacuum, are the most fundamental nonequilibrium process, and provide a microscopic model for the origins of irreversibility. Despite the fact that the apparently universal exponential decay law has been precisely tested in a variety of physical systems, it is a surprising truth that quantum mechanics requires that spontaneous decay processes have non-exponential time dependence at both very short and very long times. Cold-atom experiments both classic and recent have proven to be powerful probes of fundamental decay processes; in this paper, we propose the use of Bose condensates in Floquet-Bloch bands as a probe of long-time non-exponential decay in single isolated emitters. We identify a range of parameters that should enable observation of long-time deviations, and experimentally demonstrate a key element of the scheme: tunable decay between quasienergy bands in a driven optical lattice.

cond-mat.quant-gas↗

arXiv2019

Control of the Ion Polarization in the Pump-Probe Ionization of Helium

Attosecond pump-probe ionization process can be used to prepare atomic ions in the coherent superposition of states with opposite parity. The multiphoton shake-up ionization of Helium, in particular, generates ions with same principal quantum number and a net dipole moment that evolves on a time scale of few picoseconds, due to spin-orbit coupling. In this work we use an ab initio time-dependent close-coupling code to study how the coherence between levels of Helium ion can be controlled from the parameters of the ionizing-pulse sequence. The observed periodic revivals, on a picosecond time scale, of the ion dipole moment gives access to the study of the ionization of oriented targets.

physics.atom-ph↗

arXiv2019

Many-body calculations of two-photon, two color matrix elements for attosecond delays

We present calculations for attosecond atomic delays in photoionization of noble gas atoms based on full two-color two-photon Random-Phase Approximation with Exchange in both length and velocity gauge. Gauge invariant atomic delays are demonstrated for the complete set of diagrams. The results are used to investigate the validity of the common assumption that the measured atomic delays can be interpreted as a one-photon Wigner delay and a universal continuum--continuum contribution that depends only on the kinetic energy of the photoelectron, the laser frequency and the charge of the remaining ion, but not on the specific atom or the orbital from which the electron is ionized. Here we find that although effects beyond the universal IR--photoelectron continuum--continuum transitions are rare, they do occur in special cases such as around the $3s$ Cooper minimum in argon. We conclude also that in general the convergence in terms of many-body diagrams is considerably faster in length gauge than in velocity gauge.

physics.atom-ph↗