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Quantum mechanical calculations unveil the structure and properties of the absorbing and emitting excited electronic states of guanine quadruplex (66 views)

Improta R

Chemistry (ISSN: 0947-6539, 1521-3765, 1521-3765electronic), 2014 Jun 23; 20(26): 8106-8115.

Abstract
Herein, a full quantum mechanical study, in solution, of several models of guanine-quadruplex helices, both parallel and antiparallel, containing up to eight guanine residues, in their electronic excited state is reported. By exploiting TD-DFT calculations and including solvent effects by the polarizable continuum model, we provide the first atomistic description of the processes triggered by the absorption of UV light, reproducing and assigning the experimental optical and electronic circular dichroism spectra. The absorbing excited states are delocalized over multiple bases, whereas emission involves a stacked guanine dimer or a monomer. Several states, with a varying degree of localization and charge-transfer character, rule the photoexcited dynamics, which are deeply affected by the quadruplex topology. The lowest excited-state minimum for parallel quadruplex is an asymmetric excimer involving two stacked guanines, with a small charge transfer character, whereas for the anti-parallel structure, with the same topology of the thrombin binding aptamer, it is a fully symmetric excimer, characterized by a strong decrease of the stacking distance. A monomer-like decay path is the most relevant nonradiative decay pathway. Insights on the effect of the ions (K+ or Na+) on the excited state decay are also provided. Shedding light on quadruple helices: Quantum mechanical calculations show what happens when a guanine quadruplex absorbs UV radiation, allowing the assignment of the absorption and fluorescence spectra and giving insights into the factors ruling their photoexcited behavior (see figure). © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Affiliations ▼
*** IBB - CNR Affiliation

Istituto Biostrutture e Bioimmagini, Consiglio Nazionale Delle Ricerche, Via Mezzocannone 16, I-80134, Napoli, Italy

Details ▼
Impact factor: 5.731, 5-year impact factor: 5.635

Paper type: Journal Article, Research Support, Non-U. S. Gov'T,

Keywords: Density Functional Calculations, Excited States, Optical Spectra, Quadruplex, Charge Transfer, Continuum Mechanics, Density Functional Theory, Dimers, Electronic Properties, Monomers, Quantum Theory, Solvents, Topology, Absorption And Fluorescence Spectra, Electronic Circular Dichroism, Electronic Excited State, Polarizable Continuum Model, Quantum-Mechanical Calculation, Quantum-Mechanical Study, Positive Ions,

Url: http://www.scopus.com/inward/record.url?eid=2-s2.0-84902964600&partnerID=40&md5=e5609a4946c1249ebc6b6f499a5559ad

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Lech, C. J., Phan, A. T., Michel-Beyerle, M. -E., Voityuk, A. A., (2013) J. Phys. Chem. B, 117, p. 9851

Aquino, A. J. A., Nachtigallova, D., Hobza, P., Truhlar, D. G., Hattig, C., Lischka, H., (2011) J. Comput. Chem., 32, pp. 1217-1227

Szalay, P. G., Watson, T., Perera, A., Lotrich, V. F., Bartlett, R. J., (2012) J. Phys. Chem. A, 116, pp. 6702-6710

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Sobolewski, A. L., Domcke, W., (2004) Phys. Chem. Chem. Phys., 6, pp. 2763-2771

Frisch, M. J., Trucks, G. W., Schlegel, H. B., Scuseria, G. E., Robb, M. A., Cheeseman, J. R., Scalmani, G., Fox, D. J., (2009) Gaussian 09, , Revision A01 Gaussian, Inc., Wallingford CT


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16 Records (14 excluding Abstracts and Conferences).
Total impact factor: 73.28 (67.021 excluding Abstracts and Conferences).
Total 5-year impact factor: 79.549 (73.23 excluding Abstracts and Conferences).



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