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