Detection of the thietane precursor in the UVA formation of the DNA 6-4 photoadduct.

Nature Communications
Luis A Ortiz-RodríguezCarlos E Crespo-Hernández

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.

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Citations

Feb 16, 2021·Journal of the American Chemical Society·Luis A Ortiz-RodríguezCarlos E Crespo-Hernández
Jun 8, 2021·Chemical Science·Luis A Ortiz-Rodríguez, Carlos E Crespo-Hernández
Sep 5, 2021·Photochemistry and Photobiology·Luis A Ortiz-RodríguezCarlos E Crespo-Hernández
Nov 4, 2021·Physical Chemistry Chemical Physics : PCCP·Luis A Ortiz-RodríguezCarlos E Crespo-Hernández

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Methods Mentioned

BETA
phosphorescence spectroscopy

Software Mentioned

Gaussian
Glotaran
LabView
CASPT2

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