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Relativistic time-dependent configuration-interaction singles method

Zapata, Felipe LU ; Vinbladh, Jimmy LU ; Ljungdahl, Anton ; Lindroth, Eva and Dahlström, Jan Marcus LU (2022) In Physical Review A 105(1).
Abstract

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, where the negative energy states can be omitted... (More)

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, where 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 principles via the Dirac equation.

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author
; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Review A
volume
105
issue
1
article number
012802
publisher
American Physical Society
external identifiers
  • scopus:85122561115
ISSN
2469-9926
DOI
10.1103/PhysRevA.105.012802
language
English
LU publication?
yes
id
bab442ef-3e76-48f5-9b2b-357b686cde09
date added to LUP
2022-02-11 16:16:24
date last changed
2022-04-21 17:33:20
@article{bab442ef-3e76-48f5-9b2b-357b686cde09,
  abstract     = {{<p>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, where 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 principles via the Dirac equation. </p>}},
  author       = {{Zapata, Felipe and Vinbladh, Jimmy and Ljungdahl, Anton and Lindroth, Eva and Dahlström, Jan Marcus}},
  issn         = {{2469-9926}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{American Physical Society}},
  series       = {{Physical Review A}},
  title        = {{Relativistic time-dependent configuration-interaction singles method}},
  url          = {{http://dx.doi.org/10.1103/PhysRevA.105.012802}},
  doi          = {{10.1103/PhysRevA.105.012802}},
  volume       = {{105}},
  year         = {{2022}},
}