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Solvent effect on the singlet excited-state lifetimes of nucleic acid bases: A computational study of 5-fluorouracil and uracil in acetonitrile and water (69 visite) J Am Chem Soc (ISSN: 0002-7863, 0002-2786, 1520-5126), 2006 Dec 20; 128(50): 16312-16322. Tipo di articolo: Journal Article, Impact factor: 7.696 Impact factor a 5 anni: 11.015 Parole chiave: Absorption, Acetonitrile, Emission Spectroscopy, Mathematical Models, Microscopic Examination, Probability Density Function, Quantum Theory, Solvents, Water, Excited States, Lowest Energy Excited States, Polarizable Continuum Model (pcm), Uracil, Nucleic Acids, Fluorouracil, Nucleic Acid Base, Aqueous Solution, Article, Calculation, Density Functional Theory, Flame Photometry, Hydrogen Bond, Molecular Dynamics, Quantum Mechanics, Computer Simulation, Fluorine, Molecular Conformation, Time Factors, Url: http://www.scopus.com/inward/record.url?eid=2-s2.0-33845573545&partnerID=40&md5=2e2651b7040fe5b1f92e2f4892f8589f The first comprehensive quantum mechanical study of solvent effects on the behavior of the two lowest energy excited states of uracil derivatives is presented. The absorption and emission spectra of uracil and 5-fluorouracil in acetonitrile and aqueous solution have been computed at the time-dependent density-functional theory level, using the polarizable continuum model (PCM) to take into account bulk solvent effects. The computed spectra and the solvent shifts provided by our method are close to their experimental counterpart. The S0/S1 conical intersection, located in the presence of hydrogen-bonded solvent molecules by CASSCF (8/8) calculations, indicates that the mechanism of ground-state recovery, involving out-of-plane motion of the 5 substituent, does not depend on the nature of the solvent. Extensive explorations of the excited-state surfaces in the Franck-Condon (FC) region show that solvent can modulate the accessibility of an additional decay channel, involving a dark n/π* excited state. This finding provides the first unifying explanation for the experimental trend of 5-fluorouracil excited-state lifetime in different solvents. 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