Relaxation dynamics of photoexcited calcium deposited on argon clusters: theoretical simulation of time-resolved photoelectron spectra. - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Journal of Physical Chemistry A Année : 2010

Relaxation dynamics of photoexcited calcium deposited on argon clusters: theoretical simulation of time-resolved photoelectron spectra.

Résumé

Relaxation dynamics following photoexcitation of a calcium atom deposited on an icosahedral-like argon cluster Ar(n) (n approximately = 55) is investigated through theoretical simulations. Based on ab initio calculations of the CaAr molecule, a diatomics-in-molecules model is set up to efficiently describe the electronic excited states of the system. The excited state dynamics is studied using molecular dynamics with electronic transitions (Tully, J. C. J. Chem. Phys. 1990, 93, 1061). The signature of this dynamics in the time-resolved photoelectron spectra is investigated, to assess the possibility of detecting competing vibrational and electronic relaxations through pump-probe experiments. The vibrational relaxation, influenced by nonadiabatic transitions, can clearly be seen in the time-resolved photoelectron spectra. The details of the electronic relaxation, as well as the possible ejection of the chromophore, are found to be sensitive to the local environment of the calcium atom deposited on the argon cluster.

Domaines

Autre
Fichier non déposé

Dates et versions

hal-00842663 , version 1 (09-07-2013)

Identifiants

Citer

Marie-Catherine Heitz, Laurent Teixidor, Van-Oanh Nguyen-Thi, Fernand Spiegelman. Relaxation dynamics of photoexcited calcium deposited on argon clusters: theoretical simulation of time-resolved photoelectron spectra.. Journal of Physical Chemistry A, 2010, 114 (9), pp.3287-96. ⟨10.1021/jp909443p⟩. ⟨hal-00842663⟩
60 Consultations
0 Téléchargements

Altmetric

Partager

Gmail Facebook X LinkedIn More