Abstract:
:Notwithstanding the central biological role of the (6-4) photoadduct in the induction of skin cancer by sunlight, crucial mechanistic details about its formation have evaded characterization despite efforts spanning more than half a century. 4-Thiothymidine (4tT) has been widely used as an important model system to study its mechanism of formation, but the excited-state precursor, the intermediate species, and the time scale leading to the formation of the (6-4) photoadduct have remained elusive. Herein, steady-state and time-resolved spectroscopic techniques are combined with new and reported quantum-chemical calculations to demonstrate the excited state leading to the formation of the thietane intermediate, its rate, and the formation of the (6-4) photoadduct using the 5'-TT(4tT)T(4tT)TT-3' DNA oligonucleotide. Efficient, sub-1 ps intersystem crossing leads to the population of a triplet minimum of the thietane intermediate in as short as 3 ps, which intersystem crosses to its ground state and rearranges to form the (6-4) photoadduct.
journal_name
Nat Communjournal_title
Nature communicationsauthors
Ortiz-Rodríguez LA,Reichardt C,Hoehn SJ,Jockusch S,Crespo-Hernández CEdoi
10.1038/s41467-020-17333-ysubject
Has Abstractpub_date
2020-07-17 00:00:00pages
3599issue
1issn
2041-1723pii
10.1038/s41467-020-17333-yjournal_volume
11pub_type
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