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Excited state proton transfer is not involved in the ultrafast deactivation of Guanine-cytosine pair in solution (41 views)

Biemann L, Kovalenko SA, Kleinermanns K, Mahrwald R, Markert M, Improta R

J Am Chem Soc (ISSN: 0002-7863, 0002-2786, 1520-5126), 2011 Dec 14; 133(49): 19664-19667.

Abstract
Different derivatives of Guanine (G) and Cytosine (C), which sterically enforce the Watson-Crick (WC) conformer, have been studied in CHCl 3 by means of broad-band transient absorption spectroscopy. Our experiments rule out the involvement of an Excited State Proton Transfer (ESPT), which dominates the excited state decay of GC in the gas phase. Instead, the ultrafast dynamics via internal conversion occurs in a polar environment mainly by relaxation in the monomer moieties. Time-dependent density functional theory (TD-DFT) calculations in solution indeed indicate that population transfer from the bright excited states toward the charge transfer state is not effective in CHCl 3 and a noticeable energy barrier is associated with the ESPT reaction. ESPT is therefore not expected to be a main deactivation route for GC pairs within DNA. © 2011 American Chemical Society.

Affiliations ▼
*** IBB - CNR Affiliation

Department of Physical Chemistry, Heinrich-Heine University, University-str. 1, D-40225 Düsseldorf, Germany

Department of Chemistry, Humboldt-Universität zu Berlin, Brook-Taylor-Str. 2, D-12489 Berlin, Germany

Istituto Biostrutture e Bioimmagini-CNR, Via Mezzocannone 16, I-80134 Napoli, Italy

Details ▼
Impact factor: 9.907, 5-year impact factor: 9.766

Paper type: Journal Article,

Keywords: Broad Bands, Charge Transfer State, Excited-State Decay, Excited-State Proton Transfer, Gasphase, Guanine, Guanine Cytosines, Internal Conversions, Polar Environments, Population Transfer, Time Dependent Density Functional Theory, Transient Absorption Spectroscopies, Ultra-Fast, Ultra-Fast Dynamics, Population Statistics, Positive Ions, Excited States, Chloroform, Monomer, Article, Chemical Environment, Chemical Reaction, Energy, Excited State Proton Transfer, Molecular Dynamics, Proton Transport, Base Pairing, Quantum Theory, Solutions, Spectrum Analysis,

Url: http://www.scopus.com/inward/record.url?eid=2-s2.0-83055197004&partnerID=40&md5=badce0a8bbb0ea483904de0f64c1ad3b

References ▼
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Kovalenko, S.A., Schanz, R., Henning, H., Ernsting, N.P., (2001) J. Chem. Phys., 115, p. 3256

Karunakaran, V., Kleinermanns, K., Improta, R., Kovalenko, S.A., (2009) J. Am. Chem. Soc., 131, p. 5839

L wdin, P. O., (1963) Rev. Mod. Phys., 35, p. 72

L wdin, P. O., (1965) Mutat. Res., 2, p. 218

Kryachko, E. S., (2002) Int. J. Quantum Chem., 90, p. 910

Middleton, C. T., De La Harpe, K., Su, C., Law, Y. K., Crespo-Hern ndez, C. E., Kohler, B., (2009) Annu. Rev. Phys. Chem., 60, pp. 217-239

Nir, E., Pl tzer, Ch., Kleinermanns, K., De Vries, M., (2002) Eur. Phys. J. D., 20, pp. 317-329

Markwick, P. R. L., Doltsinis, N. L., (2007) J. Chem. Phys., 126, p. 175102

Groenhof, G., Sch fer, L. V., Boggio-Pasqua, M., Goette, M., Grubm ller, H., Robb, M. A., (2007) J. Am. Chem. Soc., 129, pp. 6812-6819

Schwalb, N. K., Michalak, T., Temps, F., (2009) J. Phys. Chem. B, 113, pp. 16365-16376

Schwalb, N. K., Temps, F., (2007) J. Am. Chem. Soc., 129, pp. 9272-9273

Miannay, F. -A., B ny sz, A., Gustavsson, T., Markovitsi, D., (2007) J. Am. Chem. Soc., 129, pp. 14574-14575

Vay, I., Changenet-Barret, P., Gustavsson, T., Zikich, D., Kotlyar, A. B., Markovitsi, D., (2010) Photochem. Photobiol. Sci., 9, pp. 1193-1195

Doorley, G. W., (2008) Ang. Chem., Int. Ed., 48, pp. 123-127

Kovalenko, S. A., Schanz, R., Henning, H., Ernsting, N. P., (2001) J. Chem. Phys., 115, p. 3256


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1 Records (1 excluding Abstracts and Conferences).
Total impact factor: 9.674 (9.674 excluding Abstracts and Conferences).
Total 5-year impact factor: 10.563 (10.563 excluding Abstracts and Conferences).



Your bibliography query: (([btitle, keywords, abstract] BROAD AND [btitle, keywords, abstract] BANDS AND [btitle, keywords, abstract] CHARGE AND [btitle, keywords, abstract] TRANSFER AND [btitle, keywords, abstract] STATE AND [btitle, keywords, abstract] EXCITED AND [btitle, keywords, abstract] DECAY)) AND NOT [id] = 9867



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