Potential energy surfaces for electron dynamics modeled by floating and breathing Gaussian wave packets with valence-bond spin-coupling: An analysis of high-harmonic generation spectrum

Abstract

A model of localized electron wave packets (EWPs), floating and breathing Gaussians with non-orthogonal valence-bond spin-coupling, is applied to compute the high-harmonic generation (HHG) spectrum from a LiH molecule induced by an intense laser pulse. The characteristic features of the spectrum, a plateau up to 50 harmonic-order and a cut-off, agreed well with those from the previous time-dependent complete active-space self-consistent-field calculation [T. Sato and K. L. Ishikawa, Phys. Rev. A \textbf{91}, 023417 (2015)]. In contrast with the conventional molecular orbital picture in which the Li 2s and H 1s atomic orbitals are strongly mixed, the present calculation indicates that an incoherent sum of responses of single electrons reproduces the HHG spectrum, in which the contribution from H 1s electron dominates the plateau and cut-off, whereas the Li 2s electron contributes to the lower frequency response. The results are comprehensive in terms of the shapes of single-electron potential energy curves constructed from the localized EWP model.

4 pages, 4 figures

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• Self-probing of Molecules with High Harmonic Generation
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• Strong-field absorption and emission of radiation in two-electron systems calculated with time-dependent natural orbitals
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Cited by in corpus (3)

• Theory of Moment Propagation for Quantum Dynamics in Single-Particle Description
• Single-electron quantum dynamics in high-harmonic generation spectrum from LiH molecule: analysis of potential energy surfaces for electrons constructed from a model of localized Gaussian wave packets with valence-bond spin-coupling
• Potential energy surfaces for electron dynamics from a model of localized Gaussian wave packets with valence-bond spin-coupling: high-harmonic generation spectra from H and He atoms