Tracking excited state decay mechanisms of pyrimidine nucleosides in real time.
Journal
Nature communications
ISSN: 2041-1723
Titre abrégé: Nat Commun
Pays: England
ID NLM: 101528555
Informations de publication
Date de publication:
14 12 2021
14 12 2021
Historique:
received:
17
06
2021
accepted:
24
11
2021
entrez:
15
12
2021
pubmed:
16
12
2021
medline:
11
1
2022
Statut:
epublish
Résumé
DNA owes its remarkable photostability to its building blocks-the nucleosides-that efficiently dissipate the energy acquired upon ultraviolet light absorption. The mechanism occurring on a sub-picosecond time scale has been a matter of intense debate. Here we combine sub-30-fs transient absorption spectroscopy experiments with broad spectral coverage and state-of-the-art mixed quantum-classical dynamics with spectral signal simulations to resolve the early steps of the deactivation mechanisms of uridine (Urd) and 5-methyluridine (5mUrd) in aqueous solution. We track the wave packet motion from the Franck-Condon region to the conical intersections (CIs) with the ground state and observe spectral signatures of excited-state vibrational modes. 5mUrd exhibits an order of magnitude longer lifetime with respect to Urd due to the solvent reorganization needed to facilitate bulky methyl group motions leading to the CI. This activates potentially lesion-inducing dynamics such as ring opening. Involvement of the
Identifiants
pubmed: 34907186
doi: 10.1038/s41467-021-27535-7
pii: 10.1038/s41467-021-27535-7
pmc: PMC8671501
doi:
Substances chimiques
Pyrimidine Nucleosides
0
Pyrimidines
0
Solvents
0
ribothymidine
1463-10-1
Uridine
WHI7HQ7H85
Types de publication
Journal Article
Research Support, Non-U.S. Gov't
Langues
eng
Sous-ensembles de citation
IM
Pagination
7285Informations de copyright
© 2021. The Author(s).
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