Few-femtosecond passage of conical intersections in the benzene cation - Université Claude Bernard Lyon 1 Accéder directement au contenu
Article Dans Une Revue Nature Communications Année : 2017

Few-femtosecond passage of conical intersections in the benzene cation

Résumé

Observing the crucial first few femtoseconds of photochemical reactions requires tools typically not available in the femtochemistry toolkit. Such dynamics are now within reach with the instruments provided by attosecond science. Here, we apply experimental and theoretical methods to assess the ultrafast nonadiabatic vibronic processes in a prototypical complex system—the excited benzene cation. We use few-femtosecond duration extreme ultraviolet and visible/near-infrared laser pulses to prepare and probe excited cationic states and observe two relaxation timescales of 11 ± 3 fs and 110 ± 20 fs. These are interpreted in terms of population transfer via two sequential conical intersections. The experimental results are quantitatively compared with state-of-the-art multi-configuration time-dependent Hartree calculations showing convincing agreement in the timescales. By characterising one of the fastest internal conversion processes studied to date, we enter an extreme regime of ultrafast molecular dynamics, paving the way to tracking and controlling purely electronic dynamics in complex molecules.
Fichier principal
Vignette du fichier
s41467-017-01133-y.pdf (572.36 Ko) Télécharger le fichier
Origine : Publication financée par une institution

Dates et versions

hal-02289271 , version 1 (04-02-2021)

Licence

Paternité

Identifiants

Citer

M. C. E. Galbraith, S. Scheit, N. V. Golubev, G. Reitsma, N. Zhavoronkov, et al.. Few-femtosecond passage of conical intersections in the benzene cation. Nature Communications, 2017, 8, pp.1018. ⟨10.1038/s41467-017-01133-y⟩. ⟨hal-02289271⟩
28 Consultations
45 Téléchargements

Altmetric

Partager

Gmail Facebook X LinkedIn More