Solvent effects on electron-driven proton-transfer processes: Adenine-thymine base pairs

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Solvent effects on electron-driven proton-transfer processes: Adenine-thymine base pairs (58 visite)

Dargiewicz M, Biczysko M, Improta R, Barone V

Phys Chem Chem Phys (ISSN: 1463-9076, 1463-3907, 1463-9084electronic), 2012; 14(25): 8981-8989.

Tipo di articolo: Journal Article,

Impact factor: 3.829

Impact factor a 5 anni: 3.976

Parole chiave: Adenine, Proton, Solvent, Thymine, Article, Base Pairing, Chemical Structure, Chemistry, Electron, Quantum Theory, Gases, Models, Molecular,

Url: http://www.scopus.com/inward/record.url?eid=2-s2.0-84862292644&partnerID=40&md5=73dfe0365d97fef2ebeadf50753c8231

Time-Dependent Density Functional Theory (TD-DFT) computations, with M05-2X and PBE0 functionals, have been employed for a detailed study of the Electron-Driven Proton-Transfer (PT) processes in an Adenine-Thymine Watson-Crick Base Pair in the gas phase and in solution, with the bulk solvent described by the polarizable continuum model. In the gas phase, TD-DFT computations predict that the Adenine → Thymine Charge Transfer (CT) excited state undergoes a barrierless PT reaction, in agreement with CC2 computations (S. Perun, A. Sobolewski, W. Domcke, J. Phys. Chem. A, 2006, 110, 9031.). The good agreement between the TD-DFT approach and CC2 results validates the former for the studies of excited state properties, excited state proton transfer reaction, and deactivation mechanisms in the DNA base pairs. Next, it is shown that inclusion of solvent effects significantly influences the possibility of both barrier-less excited state proton transfer and radiation-less deactivation through conical intersection with the ground state, affecting the energy of the CT excited state in the Franck-Condon region, the energy barrier associated to the PT process and the energy gap with the ground electronic state. These findings clearly indicate that environmental effects, with a special attention to proper treatment of dynamical solvation effects, have to be included for reliable computational analysis of photophysical and photochemical processes occurring in condensed phases. © 2012 the Owner Societies.

*** IBB - CNR ***

Dipartimento di Chimica Paolo Corradini, INSTM Village, Complesso Univ. Monte S. Angelo, via Cintia, 80126 Napoli, Italy

Center for Nanotechnology Innovation at NEST, Istituto Italiano di Tecnologia, Piazza San Silvestro 12, I-56127 Pisa, Italy

Istituto Biostrutture e Bioimmagini-CNRs, Via Mezzocannone 16, 80134 Napoli, Italy

Scuola Normale Superiore, piazza dei Cavalieri 7, 56126 Pisa, Italy

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