Please use this identifier to cite or link to this item: http://hdl.handle.net/2067/46441
Title: Tracking excited state decay mechanisms of pyrimidine nucleosides in real time
Authors: Borrego-Varillas, Rocío
Nenov, Artur
Kabaciński, Piotr
Conti, Irene
Ganzer, Lucia
Oriana, Aurelio
Jaiswal, Vishal Kumar
Delfino, Ines 
Weingart, Oliver
Manzoni, Cristian
Rivalta, Ivan
Garavelli, Marco
Cerullo, Giulio
Journal: NATURE COMMUNICATIONS 
Issue Date: 2021
Abstract: 
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 1nπ* state is found to be negligible.
URI: http://hdl.handle.net/2067/46441
ISSN: 2041-1723
DOI: 10.1038/s41467-021-27535-7
Rights: Attribution-NonCommercial-NoDerivatives 4.0 International
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