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Relativistic time-dependent configuration-interaction singles method
Stockholm University, Faculty of Science, Department of Physics. Lund University, Sweden.
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0002-7875-0544
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0003-3444-1317
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Number of Authors: 52022 (English)In: Physical Review A: covering atomic, molecular, and optical physics and quantum information, ISSN 2469-9926, E-ISSN 2469-9934, Vol. 105, no 1, article id 012802Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
2022. Vol. 105, no 1, article id 012802
National Category
Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:su:diva-204030DOI: 10.1103/PhysRevA.105.012802ISI: 000771583600007Scopus ID: 2-s2.0-85122561115OAI: oai:DiVA.org:su-204030DiVA, id: diva2:1652463
Available from: 2022-04-19 Created: 2022-04-19 Last updated: 2022-11-14Bibliographically approved

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Vinbladh, JimmyLjungdahl, AntonLindroth, Eva

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