Time-Dependent Multiconfiguration Self-Consistent-Field Study on Resonantly Enhanced High-Harmonic Generation from Transition Metal Elements

Abstract

We theoretically study high-harmonic generation (HHG) from transition metal elements Mn and Mn${}^{+}$, using full-dimensional, all-electron, first-principles simulations. The HHG spectra calculated with the time-dependent complete-active-space self-consistent-field (TD-CASSCF) and occupation-restricted multiple-active-space (TD-ORMAS) methods exhibit a prominent peak at $\sim 50$ eV, successfully reproducing resonant enhancement observed in previous experiments [R.A. Ganeev \textit{et al.}, Opt. Express \textbf{20}, 25239 (2012)]. Artificially freezing $3p$ orbitals in simulations results in its disappearance, which shows the essential role played by $3p$ electrons in the resonant harmonics (RH). Further transition-resolved analysis unambiguously identifies constructively interfering $3p$-$3d$ ($m=0,\pm 1$) giant resonance transitions as the origin of the RH, as also implied by its position in the spectra. Time-frequency analysis indicates that the recolliding electron combines with the parent ion to form the upper state of the transitions. In addition, this study shows that the TD-CASSCF and TD-ORMAS methods can be applied to open-shell atoms with many unpaired inner electrons.

7 pages, 8 figures

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• Dark and bright autoionizing states in resonant high harmonic generation: simulation via 1D helium model
• Strong-field ionization of atoms with $p^3$ valence shell: Two versus three active electrons
• Unexpected dipole instabilities in small molecules after ultrafast XUV irradiation
• Simulating real-time molecular electron dynamics efficiently using the time-dependent density matrix renormalization group
• Fano resonance in XUV generated by helium with few-cycle intense laser pulses and its classical analogy