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Channel Coupling Dynamics of Deep-Lying Orbitals in Molecular High-Harmonic Generation.

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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… Click to show full 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 abĀ 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.

Keywords: deep lying; high harmonic; harmonic spectrum; coupling dynamics; dynamics deep; channel coupling

Journal Title: Physical review letters
Year Published: 2022

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