arXiv subjects

Jimmy Vinbladh

Publications and source records attributed to Jimmy Vinbladh.

6 recordsLinked to original sources

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↗

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↗

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↗

arXiv2019

Fano's propensity rule in angle-resolved attosecond pump-probe photoionization

In a seminal article, Fano predicts that absorption of light occurs preferably with increase of angular momentum. Here we generalize Fano's propensity rule to laser-assisted photoionization, consisting of absorption of an extreme-ultraviolet photon followed by absorption or emission of an infrared photon. The predicted asymmetry between absorption and emission leads to incomplete quantum interference in attosecond photoelectron interferometry. It explains both the angular-dependence of the photoionization time delays and the delay-dependence of the photoelectron angular distributions. Our theory is verified by experimental results in Ar in the 20-40 eV range.

physics.atom-ph↗