Réaction par transfert de charge métal-ligand femtochimie aux temps ultra-courts et spectroscopie de l'état de transition en gouttelette d'hélium

Abstract : The dynamics of the interaction of an atom or a molecule with a large cluster has been studied in this manuscript in view of characterising the exchange of electronic vibrational and kinetic energy between a small system with another having a large number of degrees of freedom, the cluster.We have first studied experimentally and theoretically, the real time dynamicsof a barium atom deposited on argon clusters , (BaArn). The Ba atom was excited in high Rydberg states. A rich dynamics ensues between the chromophore an the cluster. For the theoretical interpretation a new method has been developed. It its designed to take into account the large number of electronically accessed states and their coupling with the numerous nuclear degrees of freedom of the atomic movements. The combination of the experimental and theoretical informations has allowed the characterisation of a reaction path for these dynamics. The second system studied is the photodissociation of the Ca2 molecule deposited on helium clusters pure or doped with argon (Ca2Hen or Ca2ArmHen), fluorescence emission. A comparison is also made with the Ca2Hen system. Important differences appear depending upon the nature of the solvating medium be it quantal (helium) or classical (argon). Several reaction channels have been characterised and measured for the formation of the resulting calcium atom in helium or argon solvating media.
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Antoine Masson. Réaction par transfert de charge métal-ligand femtochimie aux temps ultra-courts et spectroscopie de l'état de transition en gouttelette d'hélium. Autre [cond-mat.other]. Université Paris Sud - Paris XI, 2011. Français. ⟨NNT : 2011PA112209⟩. ⟨tel-00649169⟩

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