Solvent effect on the energetics of proton coupled electron transfer in guanine-cytosine pair in chloroform by mixed explicit and implicit solvation models

Lara Martinez-Fernandez 1, 2 Giacomo Prampolini 3 Javier Cerezo 4 Yanli Liu 5 Fabrizio Santoro 3 Roberto Improta 6
1 LIDyl - Laboratoire Interactions, Dynamique et Lasers (ex SPAM)
2 DICO - Biomolécules Excitées
IRAMIS - Institut Rayonnement Matière de Saclay, LIDyl - Laboratoire Interactions, Dynamique et Lasers (ex SPAM)
3 ICCOM-CNR - ICCOM
4 Universidad de Murcia
5 School of Physics and Optoelectronics Engineering
6 CNR – Istituto di Biostrutture e Bioimmagini
Abstract : The Watson-Crick hydrogen bonded pair formed by deoxyguanosine and deoxycytidine (GC) in chloroform has been analysed by classical Molecular Dynamics simulations, which shows the existence of several fairly stable solute/solvent hydrogen bonds. Time-Dependent Density Functional Theory (TD-DFT) calculations with M052X functional, including solvation effect by a mixed continuum/discrete model, show that solvent stabilizes G → C Charge Transfer excited states (CTGC). The Proton Transfer (PT) processes that can occur in CTGC have been mapped by TD-DFT combining State Specific and Linear Response implementations of the Polarizable Continuum Model. For the first time, the effect of explicit solute/solvent interactions on the PT is considered by studying models containing up to three CHCl3 molecules. Our study shows that PT from the N1 atom of G to the N3 of C is exoergonic also in solution but, at variance with what observed in gas-phase, a stable minimum is predicted for CTGC state in chloroform.
Type de document :
Article dans une revue
Chemical Physics, Elsevier, 2018, 515, pp.493-501
Liste complète des métadonnées
https://hal-cea.archives-ouvertes.fr/cea-01978120
Contributeur : Caroline Lebe <>
Soumis le : vendredi 11 janvier 2019 - 12:11:46
Dernière modification le : dimanche 13 janvier 2019 - 01:10:43

Identifiants

  • HAL Id : cea-01978120, version 1

Collections

CEA | DSM-IRAMIS | CEA-UPSAY | IRAMIS-LIDYL | CEA-DRF | UNIV-PARIS-SACLAY

Citation

Lara Martinez-Fernandez, Giacomo Prampolini, Javier Cerezo, Yanli Liu, Fabrizio Santoro, et al.. Solvent effect on the energetics of proton coupled electron transfer in guanine-cytosine pair in chloroform by mixed explicit and implicit solvation models. Chemical Physics, Elsevier, 2018, 515, pp.493-501. 〈cea-01978120〉

Exporter

BibTeX TEI DC DCterms EndNote

Partager

Métriques

Consultations de la notice

5

Contact

support.ccsd.cnrs.fr
hal.support@ccsd.cnrs.fr
Logo CCSD