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Lattice theory of ultrafast excitonic and charge-transfer dynamics in DNA

J. Chem. Phys. 125, 094909 (2006); doi:10.1063/1.2335452

Published 6 September 2006

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Eric R. Bittner
Department of Chemistry, University of Houston, Houston, Texas 77204 and Texas Center for Superconductivity, University of Houston, Houston, Texas 77204
We propose a lattice fermion model suitable for studying the ultrafast photoexcitation dynamics of ordered chains of deoxyribonucleic acid (DNA) polymers. The model includes both parallel (intrachain) and perpendicular (cross-chain) terms as well as diagonal cross-chain terms coupling neighboring bases. The general form of our Hamiltonian is borrowed from lattice fermion models of quantum chromodynamics. The band structure for this model can be determined analytically, and we use this as a basis for computing the singly excited states of the poly(dA)poly(dT) DNA duplex using configuration interaction singles. Parameters for the model are taken from various literature sources and our own ab initio calculations. Results indicate that the excited states consist of a low energy band of dark charge-separated states followed by separate bands of delocalized excitonic states which have weak mixing between the thymidine and adenosine sides of the DNA chain. We then propose a lattice exciton model based upon the transition dipole-dipole couplings between bases and compare the analytical results for the survival probability of an initially localized exciton to exact numerical results. The results herein underscore the competing role of excitonic and charge-transfer dynamics in these systems. ©2006 American Institute of Physics
History: Received 6 June 2006; accepted 14 July 2006; published 6 September 2006
Permalink: http://link.aip.org/link/?JCPSA6/125/094909/1
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KEYWORDS and PACS

Keywords
PACS
  • 87.14.Gg
    DNA, RNA
  • 87.15.Mi
    Spectra, photodissociation, and photoionization of biomolecules; bioluminescence
  • 87.15.He
    Biomolecular dynamics and conformational changes
  • 31.15.Ar
    Ab initio calculations (atoms and molecules)
  • YEAR: 2006

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PUBLICATION DATA

ISSN:
0021-9606 (print)   1089-7690 (online)
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