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Mapping the ultrafast dynamics of adenine onto its nucleotide and oligonucleotides by time-resolved photoelectron imaging

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Chatterley, Adam S., West, Christopher A., Roberts, Gareth M., Stavros, Vasilios G. and Verlet, Jan R. R. (2014) Mapping the ultrafast dynamics of adenine onto its nucleotide and oligonucleotides by time-resolved photoelectron imaging. The Journal of Physical Chemistry Letters, 5 (5). pp. 843-848. doi:10.1021/jz500264c ISSN 1948-7185.

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Official URL: http://dx.doi.org/10.1021/jz500264c

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Abstract

The intrinsic photophysics of nucleobases and nucleotides following UV absorption presents a key reductionist step toward understanding the complex photodamage mechanisms occurring in DNA. The decay mechanism of adenine in particular has been the focus of intense investigation, as has how these correlate to those of its more biologically relevant nucleotide and oligonucleotides in aqueous solution. Here, we report on time-resolved photoelectron imaging of the deprotonated 3′-deoxy-adenosine-5′-monophosphate nucleotide and the adenosine di- and trinucleotides. Through a comparison of gas- and solution-phase experiments and available theoretical studies, the dynamics of the base are shown to be relatively insensitive to the surrounding environment. The decay mechanism primarily involves internal conversion from the initially populated 1ππ* states to the ground state. The relaxation dynamics of the adenosine oligonucleotides are similar to those of the nucleobase, in contrast to the aqueous oligonucleotides, where a fraction of the ensemble forms long-lived excimer states.

Item Type: Journal Article
Subjects: Q Science > QH Natural history
Divisions: Faculty of Science, Engineering and Medicine > Science > Mathematics
Library of Congress Subject Headings (LCSH): DNA damage, Photoelectrons spectroscopy
Journal or Publication Title: The Journal of Physical Chemistry Letters
Publisher: American Chemical Society
ISSN: 1948-7185
Official Date: 11 February 2014
Dates:
DateEvent
11 February 2014Published
11 February 2014Accepted
7 February 2014Submitted
Volume: 5
Number: 5
Number of Pages: 6
Page Range: pp. 843-848
DOI: 10.1021/jz500264c
Status: Peer Reviewed
Publication Status: Published
Access rights to Published version: Restricted or Subscription Access
Funder: Leverhulme Trust (LT), Engineering and Physical Sciences Research Council (EPSRC), Royal Society (Great Britain), European Research Council (ERC)
Grant number: F/00215/BH (LT), EP/ D073472/1 (EPSRC), 306536 (ERC)

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