Driving force dependence of electron transfer dynamics in synthetic DNA hairpins

F. D. Lewis, R. S. Kalgutkar, Y. Wu, X. Liu, J. Liu, R. T. Hayes, S. E. Miller, M. R. Wasielewski

Research output: Contribution to journalArticlepeer-review

169 Citations (Scopus)

Abstract

The driving force dependence of photoinduced electron-transfer dynamics in duplex DNA has been investigated for 16 synthetic DNA hairpins in which an acceptor chromophore serves as a linker connecting two complementary oligonucleotide arms containing a single donor nucleobase located either adjacent to the linker or separated from the linker by two unreactive base pairs. The rate constants for both charge separation and charge recombination processes have been determined by means of subpicosecond time-resolved transient absorption spectroscopy and the results analyzed using quantum mechanical Marcus theory. This analysis provides intimate details about electron-transfer processes in DNA including the distance dependence of the electronic coupling between the acceptor and nucleobase donor and the solvent and nuclear reorganization energies.

Original languageEnglish
Pages (from-to)12346-12351
Number of pages6
JournalJournal of the American Chemical Society
Volume122
Issue number49
DOIs
Publication statusPublished - Dec 13 2000

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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