Exciton decay mechanism in DNA single strands: back-electron transfer and ultrafast base motions.
Journal
Chemical science
ISSN: 2041-6520
Titre abrégé: Chem Sci
Pays: England
ID NLM: 101545951
Informations de publication
Date de publication:
11 May 2022
11 May 2022
Historique:
received:
18
11
2021
accepted:
09
04
2022
entrez:
3
6
2022
pubmed:
4
6
2022
medline:
4
6
2022
Statut:
epublish
Résumé
The photochemistry of DNA systems is characterized by the ultraviolet (UV) absorption of π-stacked nucleobases, resulting in exciton states delocalized over several bases. As their relaxation sensitively depends on local stacking conformations, disentangling the ensuing electronic and structural dynamics has remained an experimental challenge, despite their fundamental role in protecting the genome from potentially harmful UV radiation. Here we use transient absorption and transient absorption anisotropy spectroscopy with broadband femtosecond deep-UV pulses (250-360 nm) to resolve the exciton dynamics of UV-excited adenosine single strands under physiological conditions. Due to the exceptional deep-UV bandwidth and polarization sensitivity of our experimental approach, we simultaneously resolve the population dynamics, charge-transfer (CT) character and conformational changes encoded in the UV transition dipoles of the π-stacked nucleotides. Whilst UV excitation forms fully charge-separated CT excitons in less than 0.3 ps, we find that most decay back to the ground state
Identifiants
pubmed: 35655577
doi: 10.1039/d1sc06450a
pii: d1sc06450a
pmc: PMC9093102
doi:
Types de publication
Journal Article
Langues
eng
Pagination
5230-5242Informations de copyright
This journal is © The Royal Society of Chemistry.
Déclaration de conflit d'intérêts
There are no conflicts to declare.
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