High-order harmonic transient grating spectroscopy of SF6 molecular vibrations - Laboratoire Collisions Agrégats Réactivité - LCAR Accéder directement au contenu
Article Dans Une Revue Journal of Physics B: Atomic, Molecular and Optical Physics Année : 2014

High-order harmonic transient grating spectroscopy of SF6 molecular vibrations

Résumé

Strong field transient grating spectroscopy has shown to be a very versatile tool in time-resolved molecular spectroscopy. Here we use this technique to investigate the high-order harmonic generation from SF6 molecules vibrationally excited by impulsive stimulated Raman scattering. Transient grating spectroscopy enables us to reveal clear modulations of the harmonic emission. This heterodyne detection shows that the harmonic emission generated between 14 to 26 eV is mainly sensitive to two among the three active Raman modes in SF6, i.e. the strongest and fully symmetric nu 1-A1g mode (774 cm-1, 43 fs) and the slowest mode nu5-T2g (524 cm-1, 63 fs). A time-frequency analysis of the harmonic emission reveals additional dynamics: the strength and central frequency of the nu 1 mode oscillate with a frequency of 52 cm-1 (640 fs). This could be a signature of the vibration of dimers in the generating medium. Harmonic 11 shows a remarkable behavior, oscillating in opposite phase, both on the fast (774 cm-1) and slow (52 cm-1) timescales, which indicates a strong modulation of the recombination matrix element as a function of the nuclear geometry. These results demonstrate that the high sensitivity of high-order harmonic generation to molecularvibrations, associated to the high sensitivity of transient grating spectroscopy, make their combination a unique tool to probe vibrational dynamics.
Fichier principal
Vignette du fichier
Arxiv_SF6_TGS.pdf (1.43 Mo) Télécharger le fichier
Origine : Fichiers produits par l'(les) auteur(s)
Loading...

Dates et versions

hal-00957658 , version 1 (10-03-2014)

Identifiants

Citer

Amélie Ferré, David Staedter, Frédéric Burgy, Michal Dagan, Dominique Descamps, et al.. High-order harmonic transient grating spectroscopy of SF6 molecular vibrations. Journal of Physics B: Atomic, Molecular and Optical Physics, 2014, 47 (12), pp.124023. ⟨10.1088/0953-4075/47/12/124023⟩. ⟨hal-00957658⟩
376 Consultations
335 Téléchargements

Altmetric

Partager

Gmail Facebook X LinkedIn More