Kinetics of charge separation in poly(A)-Poly(T) DNA hairpins

Gail S. Blaustein, Frederick D Lewis, Alexander L. Burin

Research output: Contribution to journalArticlepeer-review

22 Scopus citations

Abstract

A kinetics model is designed to investigate the charge separation (CT) process in stilbene-capped DNA hairpins composed of AT base pairs. This model combines standard tunneling and hopping electron transport with exciplex formation upon photoexcitation of the acceptor stilbene and its neighboring adenine and is capable of interpreting the CT rate and yield data within experimental accuracy. An analysis of hopping transport within the framework of a 1-D diffusion model results in a calculation of the nearest-neighbor CT rate to be approximately 1.2 ns-1. In agreement with previous experimental and theoretical work, it is ascertained through a novel application of an extension to classical Marcus theory that the nearest-neighbor CT is adiabatic with reorganization energy λ ∼ 0.83 eV. The kinetics model can be extended to accurately characterize CT in other poly(A)-poly(T) systems with different hole donors (naphthaldiimide and 2-aminopurine) and acceptors (phenothiazine and guanine).

Original languageEnglish (US)
Pages (from-to)6732-6739
Number of pages8
JournalJournal of Physical Chemistry B
Volume114
Issue number19
DOIs
StatePublished - May 20 2010

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

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