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Resolving Ultrafast Photoinduced Deactivations in Water-Solvated Pyrimidine Nucleosides (10 views)

Pepino AJ, Segarra-marti J, Nenov A, Improta R, Garavelli M

J Phys Chem Lett (ISSN: 1948-7185electronic, 1948-7185linking), 2017 Apr 20; 8(8): 1777-1783.

Abstract
For the first time, ultrafast deactivations of photoexcited water-solvated pyrimidine nucleosides are mapped employing hybrid QM(CASPT2)/MM(AMBER) optimizations that account for explicit solvation, sugar effects, and dynamically correlated potential energy surfaces. Low-energy S1/S0 ring-puckering and ring-opening conical intersections (CIs) are suggested to drive the ballistic coherent subpicosecond (<200 fs) decays observed in each pyrimidine, the energetics controlling this processes correlating with the lifetimes observed. A second bright 1pi2pi* state, promoting excited-state population branching and leading toward a third CI with the ground state, is proposed to be involved in the slower ultrafast decay component observed in Thd/Cyd. The transient spectroscopic signals of the competitive deactivation channels are computed for the first time. A general unified scheme for ultrafast deactivations, spanning the sub- to few-picosecond time domain, is eventually delivered, with computed data that matches the experiments and elucidates the intrinsic photoprotection mechanism in solvated pyrimidine nucleosides.

Affiliations ▼
*** IBB - CNR Affiliation

Dipartimento di Chimica Industriale "Toso Montanari" Viale del Risorgimento, 4, 40136 Bologna, Italy., Laboratoire de Chimie UMR 5182, Universite Lyon, ENS de Lyon, CNRS, Universite Lyon 1 , F-69342 Lyon, France., Istituto di Biostrutture e Bioimmagini CNR , Via Mezzocannone 16, I-80134 Napoli, Italy.,

Details ▼
Impact factor: 9.353, 5-year impact factor: 8.334

Paper type: Journal Article,

Keywords: Not available.

Url: Not available.

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5 Records (5 excluding Abstracts and Conferences).
Total impact factor: 11.415 (11.415 excluding Abstracts and Conferences).
Total 5-year impact factor: 12.837 (12.837 excluding Abstracts and Conferences).



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