Signatures of light-induced nonadiabaticity in the field-dressed vibronic spectrum of formaldehyde

• Verfasst von: Fábri, Csaba [VerfasserIn]
• Verfasst von: Halász, Gábor J. [VerfasserIn]
• Verfasst von: Cederbaum, Lorenz S. [VerfasserIn]
• Verfasst von: Vibók, Ágnes [VerfasserIn]
• Titel: Signatures of light-induced nonadiabaticity in the field-dressed vibronic spectrum of formaldehyde
• Verf.angabe: Csaba Fábri, Gábor J. Halász, Lorenz S. Cederbaum, and Ágnes Vibók
• E-Jahr: 2021
• Jahr: 24 March 2021
• Umfang: 13 S.
• Teil: volume:154
• Teil: year:2021
• Teil: number:12
• Teil: elocationid:124308
• Teil: pages:1-13
• Teil: extent:13
• Fussnoten: Gesehen am 27.04.2021
• Titel Quelle: Enthalten in: The journal of chemical physics
• Ort Quelle: Melville, NY : American Institute of Physics, 1933
• Jahr Quelle: 2021
• Band/Heft Quelle: 154(2021), 12, Artikel-ID 124308, Seite 1-13
• ISSN Quelle: 1089-7690
• DOI: doi:10.1063/5.0045069
• Datenträger: Online-Ressource
• Sprache: eng
• K10plus-PPN: 1755991991

Abstract

Nonadiabatic coupling is absent between the electronic ground X and first excited (singlet) A states of formaldehyde. As laser fields can induce conical intersections between these two electronic states, formaldehyde is particularly suitable for investigating light-induced nonadiabaticity in a polyatomic molecule. The present work reports on the spectrum induced by light—the so-called field-dressed spectrum—probed by a weak laser pulse. A full-dimensional ab initio approach in the framework of Floquet-state representation is applied. The low-energy spectrum, which without the dressing field would correspond to an infrared vibrational spectrum in the X-state, and the high-energy spectrum, which without the dressing field would correspond to the X → A spectrum, are computed and analyzed. The spectra are shown to be highly sensitive to the frequency of the dressing light allowing one to isolate different nonadiabatic phenomena.