Symmetry and Vibrational Control of Multi-Channel HHG in Methane
- 1Dipartimento di Scienze Chimiche e Farmaceutiche, Università di Trieste, via L. Giorgieri 1, 34127 Trieste, Italy
- 2Laboratoire de Chimie Théorique, Sorbonne Université, CNRS, Paris F-75005, France
Abstract
High-harmonic generation (HHG) driven by tailored bicircular laser fields has emerged as a powerful tool for probing structural and dynamical properties of complex molecules. We compute HHG spectra of methane (CH4) interacting with intense ω/2ω counter-rotating bicircular fields using an all-electron approach based on the time-dependent Schrödinger equation. The emitted harmonics are explained as the interplay between the dynamical symmetries of the driving field and the tetrahedral spatial symmetry of the molecule. We unravel the critical role of molecular normal modes in modulating population dynamics across distinct ionization and recombination channels. The appearance of forbidden harmonics under asymmetric stretching of methane is analyzed, showing a clear interplay between such harmonics and the spatial displacement. This work provides insights for experimental investigations of aligned molecular systems, with a view toward a pump–probe setup.
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BibTeX
@article{marchetta2026symmetry,
title = {{Symmetry and Vibrational Control of Multi-Channel HHG in Methane}},
author = {Marco Marchetta and Eleonora Luppi and Emanuele Coccia},
journal = {The Journal of Physical Chemistry Letters},
year = {2026},
month = oct,
doi = {10.1021/acs.jpclett.6c02522},
url = {https://doi.org/10.1021/acs.jpclett.6c02522},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Symmetry and Vibrational Control of Multi-Channel HHG in Methane
AU - Marco Marchetta
AU - Eleonora Luppi
AU - Emanuele Coccia
PY - 2026
DA - 2026/10/08
JO - The Journal of Physical Chemistry Letters
DO - 10.1021/acs.jpclett.6c02522
UR - https://doi.org/10.1021/acs.jpclett.6c02522
AB - High-harmonic generation (HHG) driven by tailored bicircular laser fields has emerged as a powerful tool for probing structural and dynamical properties of complex molecules. We compute HHG spectra of methane (CH4) interacting with intense ω/2ω counter-rotating bicircular fields using an all-electron approach based on the time-dependent Schrödinger equation. The emitted harmonics are explained as the interplay between the dynamical symmetries of the driving field and the tetrahedral spatial symmetry of the molecule. We unravel the critical role of molecular normal modes in modulating population dynamics across distinct ionization and recombination channels. The appearance of forbidden harmonics under asymmetric stretching of methane is analyzed, showing a clear interplay between such harmonics and the spatial displacement. This work provides insights for experimental investigations of aligned molecular systems, with a view toward a pump–probe setup.
SN - 1948-7185
ER -