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Intramolecular vibrational redistribution in the non-radiative excited state decay of uracil in the gas phase: An ab initio molecular dynamics study (80 visite)

Carbonniere P, Pouchan C, Improta R

Phys Chem Chem Phys (ISSN: 1463-9076, 1463-3907, 1463-9084electronic), 2015; 17(17): 11615-11626.

Tipo di articolo: Journal Article,

Impact factor: 4.449

Impact factor a 5 anni: 4.273


Parole chiave: Non disponibili.

Url: http://www.scopus.com/inward/record.url?eid=2-s2.0-84928476420&partnerID=40&md5=c1318067c44f8f568811e51d335d27c4

We report a study of intramolecular vibrational distribution (IVR) occurring in the electronic ground state of uracil (S0) in the gas phase, following photoexcitation in the lowest energy bright excited state (Sπ) and decay through the ethylene-like Sπ/S0 Conical Intersection (CI-0π). To this aim we have performed 20 independent ab initio molecular dynamics simulations starting from CI-0π (ten of them with 1 eV kinetic energy randomly distributed over the different molecular degrees of freedom) and 10 starting from the ground state minimum (Franck-Condon, FC, point), with the excess kinetic energy equal to the energy gap between CI-0π and the FC point. The simulations, exploiting PBE0/6-31G(d) calculations, were performed over an overall period of 10 ps. A thorough statistical analysis of the variation of the geometrical parameters of uracil during the simulation time and of the distribution of the kinetic energy among the different vibrational degrees of freedom provides a consistent picture of the IVR process. In the first 0-200 fs the structural dynamics involve mainly the recovery of the average planarity. In the 200-600 fs time range, a substantial activation of CO and NH degrees of freedom is observed. After 500-600 fs most of the geometrical parameters reach average values similar to those found after 10 ps, though the system cannot be considered to be in equilibrium yet. © 2015 the Owner Societies.
*** IBB - CNR ***

Université de Pau et des Pays de l'Adour UMR5254, IPREM, Equipe Chimie-Physique Hélioparc, 2 av. Président Angot, Pau Cedex 09, France

CNR-Consiglio Nazionale Delle Ricerche, Istituto di Biostrutture Biommagini (IBB-CNR), Via Mezzocannone 16, Napoli, Italy
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