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

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  • Luis A. Ortiz-Rodríguez

    (Case Western Reserve University)

  • Christian Reichardt

    (Case Western Reserve University)

  • Sean J. Hoehn

    (Case Western Reserve University)

  • Steffen Jockusch

    (Columbia University)

  • Carlos E. Crespo-Hernández

    (Case Western Reserve University)

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.

Suggested Citation

  • Luis A. Ortiz-Rodríguez & Christian Reichardt & Sean J. Hoehn & Steffen Jockusch & Carlos E. Crespo-Hernández, 2020. "Detection of the thietane precursor in the UVA formation of the DNA 6-4 photoadduct," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-17333-y
    DOI: 10.1038/s41467-020-17333-y
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