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Updated: Sep 22, 2025

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
Channel Coupling Dynamics of Deep-Lying Orbitals in Molecular High-Harmonic Generation
Zheng Shu1, Hongjing Liang2, Yichen Wang2
1Institute of Applied Physics and Computational Mathematics, P.O. Box 8009, Beijing 100088, China.
Abstract:
Investigation on structures in the high-harmonic spectrum has provided profuse information of molecular structure and dynamics in intense laser fields, based on which techniques of molecular ultrafast dynamics imaging have been developed. Combining ab initio calculations and experimental measurements on the high-harmonic spectrum of the CO_{2} molecule, we find a novel dip structure in the low-energy region of the harmonic spectrum which is identified as fingerprints of participation of deeper-lying molecular orbitals in the process and decodes the underlying attosecond multichannel coupling dynamics. Our work sheds new light on the ultrafast dynamics of molecules in intense laser fields.
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