Resolving Ultra-Fast Spin-Orbit Dynamics in Heavy Many-Electron Atoms

Jack Wragg, Daniel D. A. Clarke, Gregory S. J. Armstrong, Andrew C. Brown, Connor P. Ballance, Hugo W. Van Der Hart

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Abstract

We use R-Matrix with Time-dependence (RMT) theory, with spin-orbit effects included, to study krypton irradiated by two time-delayed XUV ultrashort pulses. The first pulse excites the atom to 4s$^2$4p$^5$5s. The second pulse then excites 4s4p65s autoionising levels, whose population can be observed through their subsequent decay. By varying the time delay between the two pulses, we are able to control the excitation pathway to the autoionising states. The use of cross-polarised light pulses allows us to isolate the two-photon pathway, with one photon taken from each pulse.
Original languageEnglish
Number of pages6
JournalPhysical Review Letters
DOIs
Publication statusPublished - 15 Oct 2019

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Keywords

  • First-principles calculations
  • atoms
  • Spin-orbit coupling
  • Single- and few-photon ionization & excitation

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