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Updated: Jun 8, 2026

Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization
Published on: August 6, 2018
Multichannel molecular high-order harmonic generation from asymmetric diatomic molecules
Xue-Bin Bian1, André D Bandrauk
1Département de Chimie, Université de Sherbrooke, Sherbrooke, Quebéc J1K 2R1, Canada.
Multichannel molecular high-order harmonic generation (MHOHG) in HeH2+ ions shows resonant excitation via laser-induced electron transfer (LIET). This LIET process leads to fractional-order harmonics from excited states, confirmed by time series analysis.
Area of Science:
- Quantum Optics
- Molecular Physics
- Attosecond Science
Background:
- High-order harmonic generation (HHG) is a key process in strong-field physics.
- Molecular HHG offers insights into electron dynamics and molecular structure.
- Asymmetric molecular ions present unique HHG characteristics.
Purpose of the Study:
- To numerically investigate multichannel molecular high-order harmonic generation (MHOHG) in the HeH2+ system.
- To explore the role of laser-induced electron transfer (LIET) in generating novel harmonic spectra.
- To confirm the MHOHG channel through time-resolved analysis.
Main Methods:
- Numerical simulations of electron dynamics in the HeH2+ ion under intense laser fields.
- Analysis of harmonic spectra, focusing on fractional-order harmonics.
- Time series analysis to identify and confirm the MHOHG pathway.
Main Results:
- Significant resonant excitation via LIET to neighboring ions was observed.
- Multiple frequency (fractional-order) harmonics were generated from energy-shifted excited states.
- Interference between recombination pathways from ground and excited states was confirmed.
Conclusions:
- LIET is a crucial mechanism for multichannel HHG in asymmetric molecular ions.
- Fractional-order harmonics provide evidence of excited-state contributions.
- The study confirms a novel MHOHG channel involving LIET and state interference.
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