Subcycle electron-electron correlation effects on high-harmonic generation

ORAL

Abstract

High-harmonic generation (HHG) is one of the fundamental processes at the heart of attosecond physics. Traditionally viewed as an effective single-particle effect, recent advances have focused on contributions to the harmonic spectrum beyond this single-particle picture [1, 2], as well as on probing electron correlations through HHG in atoms, molecules, and solids [3, 4]. In this work, we quantify the influence of time-dependent electron-electron correlations on HHG using correlation measures from quantum information theory. By explicitly solving the time-dependent Schrödinger equation with the multi-configurational time-dependent Hartee-Fock method [5], we obtain fully correlated results for several multi-electron atoms. When comparing different atomic species, i.e. noble gas atoms (He, Ne) with alkaline-earth atoms (Be, Mg) we find the subcycle variation of correlation parameters to differ markedly for noble gases and alkaline-earth atoms. We provide an intuitive explanation of these surprising effects based on the dynamics of natural orbitals and discuss the effect of this ultrafast correlation dynamics on the HHG spectrum [6].

[1] A. D. Shiner et al., Nature Phys 7, 464–467 (2011).

[2] A. De Las Heras et al., Phys. Rev. Res. 2, 033047 (2020).

[3] D. R. Baykusheva et al., Phys. Rev. X 12, 011013 (2022).

[4] R. E. F. Silva et al., Nat. Photon. 12, 266 (2018).

[5] T. Sato et al., Phys. Rev. A 94, 023405 (2016).

[6] K. Buczolich et al., Phys. Rev. Res. 7, 043322 (2025).

*This research was funded by the FWF Grant No. P 35539-N, as well as by the FWF 10.55776/COE1. Support of K.B. via the IMPRS-APS is acknowledged. This research was supported in part by Grants No. JP19H00869, No. JP20H05670, No. JP22H05025, No. JP24H00427, and No. JP25K01688 from the MEXT of Japan, and the RIKEN TRIP initiative. This research was also partially supported by the MEXT Grant No. JPMXS0118067246 and JST COI-NEXT (Grant No. JPMJPF2221). Calculations were performed on the VSC4.

Publication: K. Buczolich et al., Phys. Rev. Res. 7, 043322 (2025).
https://doi.org/10.1103/zbfh-qfd2

Presenters

  • Katharin Buczolich

    • TU Wien

Authors

  • Katharin Buczolich

    • TU Wien
  • Takeshi Sato

    • Univ of Tokyo
  • Kenichi L. Ishikawa

    • Univ of Tokyo
  • Fabian Lackner

    • TU Wien
  • Joachim E Burgdoerfer

    • TU Wien
    • Vienna University of Technology
  • Iva Březinová

    • TU Wien