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Ultrafast Excited-State Deactivation of 8-Hydroxy-2′-deoxyguanosine Studied by Femtosecond Fluorescence Spectroscopy and Quantum-Chemical Calculations (54 views)

Changenet-Barret P, Gustavsson T, Improta R, Markovitsi D

J Phys Chem A (ISSN: 1089-5639, 1520-5215electronic), 2015; 119(23): 6131-6139.

The fluorescence properties of the 8-hydroxy-2′-deoxyguanosine (8-oxo-dG) in aqueous solution at pH 6.5 are studied by steady-state spectroscopy and femtosecond fluorescence up-conversion and compared with those of 2′-deoxyguanine (dG) and 2′-deoxyguanine monophosphate (dGMP). The steady-state fluorescence spectrum of 8-oxo-dG is composed of a broad band that peaks at 356 nm and extends over the entire visible spectral region, and its fluorescence quantum yield is twice that of dG/dGMP. After excitation at 267 nm, the initial fluorescence anisotropy at all wavelengths is lower than 0.1, giving evidence of an ultrafast internal conversion (<100 fs) between the two lowest excited ππ∗ states (Lb and La). The fluorescence decays of 8-oxo-dG are biexponential with an average lifetime of 0.7 ± 0.1 ps, which is about two times longer than that of dGMP. In contrast with dGMP, only a moderate dynamical shift (∼1400 vs 10 000 cm-1) of the fluorescence spectra of 8-oxo-dG is observed on the time scale of a few picoseconds without modification of the spectral shape. PCM/TD-DFT calculations, employing either the PBE0 or the M052X functionals, provide absorption spectra in good agreement with the experimental one and show that the deactivation path is similar to that proposed for dGMP, with a fast motion toward an energy plateau, where the purine ring keeps an almost planar geometry, followed by decay to S0, via out-of-the plane motion of amino substituent. © 2015 American Chemical Society.

Affiliations ▼
*** IBB - CNR Affiliation

CNRS, IRAMIS, Laboratoire Francis Perrin, Gif sur Yvette, France

Consiglio Nazionale Delle Ricerche, Istituto di Biostrutture e Bioimmagini, Naples, Italy

Laboratoire d'Optique et Biosciences, Ecole Polytechnique, INSERM, Palaiseau cedex, France

Details ▼
Impact factor: 2.693, 5-year impact factor: 2.713

Paper type: Journal Article,

Keywords: Biomolecules, Fluorescence, Fluorescence Spectroscopy, Geometry, Quantum Chemistry, Quantum Theory, Femtosecond Fluorescence, Fluorescence Anisotropy, Fluorescence Properties, Fluorescence Quantum Yield, Quantum Chemical Calculations, Steady State Fluorescences, Steady State Spectroscopy, Visible Spectral Regions, Excited States,

Url: http://www.scopus.com/inward/record.url?eid=2-s2.0-84935884627&partnerID=40&md5=c89096d8210080e59a1053ce491c1deb

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* Photoinduced dynamics of guanosine monophosphate in water from broad-band transient absorption spectroscopy and quantum-chemical calculations (43 views)
Karunakaran V, Kleinermanns K, Improta R, Kovalenko SA
J Am Chem Soc (ISSN: 0002-7863, 0002-2786, 1520-5126), 2009; 131(16): 5839-5850.

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1 Records (1 excluding Abstracts and Conferences).
Total impact factor: 11.444 (11.444 excluding Abstracts and Conferences).
Total 5-year impact factor: 11.015 (11.015 excluding Abstracts and Conferences).

Your bibliography query: (([btitle, keywords, abstract] BIOMOLECULES AND [btitle, keywords, abstract] FLUORESCENCE AND [btitle, keywords, abstract] SPECTROSCOPY)) AND NOT [id] = 52895

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