Electron Dynamics upon Ionization of Polyatomic Molecules: Coupling to Quantum Nuclear Motion and Decoherence. - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Physical Review Letters Année : 2017

Electron Dynamics upon Ionization of Polyatomic Molecules: Coupling to Quantum Nuclear Motion and Decoherence.

Michael Bearpark
  • Fonction : Auteur
Michael Robb
  • Fonction : Auteur
João Pedro Malhado
  • Fonction : Auteur

Résumé

Knowledge about the electronic motion in molecules is essential for our understanding of chemical reactions and biological processes. The advent of attosecond techniques opens up the possibility to induce electronic motion, observe it in real time, and potentially steer it. A fundamental question remains the factors influencing electronic decoherence and the role played by nuclear motion in this process. Here, we simulate the dynamics upon ionization of the polyatomic molecules paraxylene and modified bismethylene-adamantane, with a quantum mechanical treatment of both electron and nuclear dynamics using the direct dynamics variational multiconfigurational Gaussian method. Our simulations give new important physical insights about the expected decoherence process. We have shown that the decoherence of electron dynamics happens on the time scale of a few femtoseconds, with the interplay of different mechanisms: the dephasing is responsible for the fast decoherence while the nuclear overlap decay may actually help maintain it and is responsible for small revivals.

Dates et versions

hal-03018884 , version 1 (23-11-2020)

Identifiants

Citer

Morgane Vacher, Michael Bearpark, Michael Robb, João Pedro Malhado. Electron Dynamics upon Ionization of Polyatomic Molecules: Coupling to Quantum Nuclear Motion and Decoherence.. Physical Review Letters, 2017, 118 (8), pp.083001. ⟨10.1103/PhysRevLett.118.083001⟩. ⟨hal-03018884⟩
8 Consultations
0 Téléchargements

Altmetric

Partager

Gmail Facebook X LinkedIn More