期刊
CHEMICAL PHYSICS
卷 515, 期 -, 页码 572-579出版社
ELSEVIER
DOI: 10.1016/j.chemphys.2018.08.011
关键词
Modified DNA bases; 4-Thiouracil; Excited state dynamics; Internal conversion; Intersystem crossing; Photodynamics; Time-resolved spectroscopy; Pump-probe; Ultrafast spectroscopy
资金
- National Science Foundation [NSF-CHE-1362237, 1800050]
- Excellence Initiative of Aix-Marseille University (A*MIDEX) - French Government Investissements d'Avenir program
- project Equip@Meso - French Government Investissements d'Avenir program [ANR-10-EQPX-29-01]
- WSPLIT project [ANR-17-CE05-0005-01]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1800050] Funding Source: National Science Foundation
The ultraviolet (UV) photophysics of the natural and modified nucleobases can be surprisingly different In response to UV radiation, the natural pyrimidine nucleobases undergo ultrafast internal conversion back to the ground state, whereas their thiobase analogues, in which an oxygen has been replaced by sulfur, instead display efficient intersystem crossing to the triplet manifold. Here, the effect of the substituent position is investigated with time resolved photoelectron spectroscopy on 4-thiouracil, which is contrasted to previous work on 2-thiouracil. Although the photophysical pathway of both structural isomers is similar, i.e., leading from the S-2 ((1)pi pi*) state, via S-1 ((1)n pi*) to the triplet manifold and subsequently back to the ground state, the intersystem crossing dynamics are strongly influenced by the surrounding intramolecular environment of the sulfur atom.
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