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The interplay between neutral exciton and charge transfer states in single-strand polyadenine: A quantum dynamical investigation (67 views)

Santoro F, Improta R, Avila Ferrer FJ, Segado M, Lami A

Photochem Photobiol Sci (ISSN: 1474-905x), 2013; 12(8): 1527-1543.

Abstract
We investigate the quantum dynamics of the internal conversion of excitons into charge transfer (CT) states in single-strand oligomers of adenine (A n) of different length (n up to 10 units) excited by a short-time laser pulse. Calculations are based on a model vibronic Hamiltonian whose parameters are fitted to accurate time-dependent density functional theory (TD-DFT) calculations, which was shown to reproduce the experimental absorption spectrum with the increase of n. As a first step, we analyze the impact of the vibrational motion on the population transfer in the dimer, highlighting that it causes loss of coherence and slows down the dynamics. For longer oligomers we resort to a simplified approach considering only electronic states and solving the equation of motion for the density matrix driven by inter-state couplings. In this way we are able also to include phenomenologically dephasing terms that mainly simulate intra-molecular effects, and lifetimes of local excitations mimicking monomer-like decay processes. Relaxation effects, whose role is to drive the system towards the thermal equilibrium allowing population exchange among states, are deliberately not considered here, since the focus is on very short-time dynamics. We consider both the cases of an instantaneous and of a finite-time (full width at half maximum 50 fs) laser pulse. According to our calculations, the photoexcited oligomers exhibit a complex dynamics and CT population rises on a 20-30 fs timescale and it persists even on the picosecond timescale. CT population increases with the length of the oligomer and it is only weakly dependent on the relative stability of CT and exciton states (within a range of 1500 cm-1). The chain length already modifies the photoexcited dynamics for A2 and A4 systems, but this effect saturates for small n so that the A10 oligomer is also representative of longer chains. © 2013 The Royal Society of Chemistry and Owner Societies.

Affiliations ▼
*** IBB - CNR Affiliation

CNR - Consiglio Nazionale Delle Ricerche, Istituto di Chimica Dei Composti Organo Metallici (ICCOM-CNR), UOS di Pisa Area della Ricerca, via G. Moruzzi 1, I-56124 Pisa, Italy

University of Málaga, Physical Chemistry, Faculty of Science, Málaga 29071, Spain

INSTM UdR Pisa, C/o Dipartimento di Chimica e Chimica Industriale, Università di Pisa, Via Risorgimento 35, I-56126 Pisa, Italy

University of M laga, Physical Chemistry, Faculty of Science, M laga 29071, Spain

Details ▼
Impact factor: 2.939, 5-year impact factor: 2.793

Paper type: Journal Article,

Keywords: Adenine, Chemistry, Dimerization, Electron, Laser, Light, Photochemistry, Quantum Theory, Article, Photochemical Processes,

Url: http://www.scopus.com/inward/record.url?eid=2-s2.0-84881093177&partnerID=40&md5=da255e7b5468519274f899d04c898d0f

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Kwok, W. M., Ma, C. S., Phillips, D. L., Femtosecond time- and wavelength-resolved fluorescence and absorption spectroscopic study of the excited states of adenosine and an adenine oligomer (2006) J. Am. Chem. Soc., 128, pp. 11894-11905

Schwalb, N. K., Temps, F., Base sequence and higher-order structure induce the complex excited-state dynamics in DNA (2008) Science, 322, pp. 243-245

Stuhldreier, M. C., Sch ler, C., Kleber, J., Temps, F., (2011) Ultrafast Phenomena XVII, pp. 553-555. , ed. M. Chergui, D. M. Jonas, E. Riedle, R. W. Schoenlein and A. J. Taylor, Oxford University Press, Oxford, UK

Lu, Y., Lan, Z. G., Thiel, W., Hydrogen bonding regulates the monomeric nonradiative decay of adenine in DNA strands (2011) Angew. Chem., Int. Ed., 50, pp. 6864-6867

Jones, K. E., Zewail, A. H., (1978) Advances in Laser Chemistry, 3, p. 196. , Springer Series in Chemical Physics, Springer, Berlin, Heidelberg New York

Bittner, E. R., Lattice theory of ultrafast excitonic and charge-transfer dynamics in DNA (2006) J. Chem. Phys., 125, pp. 094909-094920

Blankenship, R. E., Tiede, D. M., Barber, J., Brudvig, G. W., Fleming, G., Ghirardi, M., Gunner, M. R., Sayre, R. T., Comparing photosynthetic and photovoltaic efficiencies and recognizing the potential for improvement (2011) Science, 332, pp. 805-809

Clarke, T. M., Durrant, J. R., Charge photogeneration in organic solar cells (2010) Chem. Rev., 110, pp. 6736-6767

Merrifield, R. E., Ionized states in a one-dimensional molecular crystal (1961) J. Chem. Phys., 34, pp. 1835-1839

Bittner, E. R., Frenkel exciton model of ultrafast excited state dynamics in at DNA double helices (2007) J. Photochem. Photobiol., A, 190, pp. 328-334

Beck, H., J ckle, A., Worth, G. A., Meyer, H. -D., The multiconfiguration time-dependent Hartree (MCTDH) method: A highly efficient algorithm for propagating wavepackets (2000) Phys. Rep., 324, pp. 1-105

Meyer, H. -D., Gatti, F., Worth, G. A., (2009) Multidimensional Quantum Dynamics. MCTDH Theory and Applications, , ed., Wiley VCH, Weinheim

Balevi ius, Jr. V., Gelzinis, A., Abramavicius, D., Man al, T., Valkunas, L., Excitation dynamics and relaxation in a molecular heterodimer (2012) Chem. Phys., 404, pp. 94-102

Lange, A. W., Herbert, J. M., Both intra- and interstrand charge-transfer excited states in aqueous B-DNA are present at energies comparable to, or just above, the 1 * excitonic bright states (2009) J. Am. Chem. Soc., 131, pp. 3913-3922

Vay, I., Gustavsson, T., Douki, T., Berlin, Y., Markovitsi, D., Electronic excitation energy transfer between nucleobases of natural DNA (2012) J. Am. Chem. Soc., 134, pp. 11366-11368


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* The excited electronic states of adenine-guanine stacked dimers in aqueous solution: A PCM/TD-DFT study (49 views)
Santoro F, Barone V, Lami A, Improta R
Phys Chem Chem Phys (ISSN: 1463-9076, 1463-3907, 1463-9084electronic), 2010; 12(19): 4934-4948.

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* Vibronic model for the quantum dynamical study of the competition between bright and charge-transfer excited states in single-strand polynucleotides: the adenine dimer case (42 views)
Improta R, Santoro F, Barone V, Lami A
J Phys Chem A (ISSN: 1089-5639, 1520-5215electronic, 1089-5639linking), 2009 Dec 31; 113(52): 15346-15354.

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2 Records (2 excluding Abstracts and Conferences).
Total impact factor: 6.353 (6.353 excluding Abstracts and Conferences).
Total 5-year impact factor: 6.839 (6.839 excluding Abstracts and Conferences).



Your bibliography query: (([btitle, keywords, abstract] ADENINE AND [btitle, keywords, abstract] CHEMISTRY AND [btitle, keywords, abstract] DIMERIZATION AND [btitle, keywords, abstract] ELECTRON)) AND NOT [id] = 10631



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