Single-Step Charge Transport through DNA over Long Distances
Quantum yields for charge transport across adenine tracts of increasing length have been measured by monitoring hole transport in synthetic oligonucleotides between photoexcited 2-aminopurine, a fluorescent analogue of adenine, and N_2-cyclopropyl guanine. Using fluorescence quenching, a measure of hole injection, and hole trapping by the cyclopropyl guanine derivative, we separate the individual contributions of single- and multistep channels to DNA charge transport and find that with 7 or 8 intervening adenines the charge transport is a coherent, single-step process. Moreover, a transition occurs from multistep to single-step charge transport with increasing donor/acceptor separation, opposite to that generally observed in molecular wires. These results establish that coherent transport through DNA occurs preferentially across 10 base pairs, favored by delocalization over a full turn of the helix.
© 2011 American Chemical Society. Received: August 5, 2010. Published: February 24, 2011. We are grateful to the National Institutes of Health (GM49216) for their support. We also thank the Caltech SURF program for a summer undergraduate fellowship (S.M.W.).
Accepted Version - nihms277098.pdf
Supplemental Material - ja107033v_si_001.pdf