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Title: Quantum equilibration of the double-proton transfer in a model system Porphine
Author: Albareda, Guillermo
Riera, Arnau
González Pérez, Miguel
Bofill i Villà, Josep M.
Moreira, Ibério de Pinho Ribeiro
Valero Montero, Rosendo
Tavernelli, Ivano
Keywords: Química quàntica
Dinàmica molecular
Quantum chemistry
Molecular dynamics
Issue Date: 14-Sep-2020
Publisher: Royal Society of Chemistry
Abstract: There is a renewed interest in the derivation of statistical mechanics from the dynamics of closed quantum systems. A central part of this program is to understand how closed quantum systems, i.e., in the absence of a thermal bath, initialized far-from-equilibrium can share a dynamics that is typical to the relaxation towards thermal equilibrium. Equilibration dynamics has been traditionally studied with a focus on the so-called quenches of large-scale many-body systems. We consider here the equilibration of a two-dimensional molecular model system describing the double proton transfer reaction in porphine. Using numerical simulations, we show that equilibration indeed takes place very rapidly (about 200 fs) for initial states induced by pump-dump laser pulse control with energies well above the synchronous barrier. The resulting equilibration state is characterized by a strong delocalization of the probability density of the protons that can be explained, mechanistically, as the result of (i) an initial state consisting of a large superposition of vibrational states, and (ii) the presence of a very effective dephasing mechanism.
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It is part of: Physical Chemistry Chemical Physics, 2020, vol. 22, p. 22332-22341
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ISSN: 1463-9076
Appears in Collections:Articles publicats en revistes (Química Inorgànica i Orgànica)
Articles publicats en revistes (Ciència dels Materials i Química Física)

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