TY - JOUR
T1 - Hole transport in DNA hairpins via base mismatches and strand crossings
T2 - Efficiency and dynamics
AU - Thazhathveetil, Arun K.
AU - Harris, Michelle A.
AU - Young, Ryan M.
AU - Wasielewski, Michael R.
AU - Lewis, Frederick D.
N1 - Funding Information:
This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division under Award DE-FG02-96ER14604 (F.D.L.) and the U.S. Office of Naval Research MURI grant no. N00014-11-1-0729 (M.R.W.).
PY - 2016/12/1
Y1 - 2016/12/1
N2 - The efficiency and dynamics of hole transport via base mismatches and strand crossings have been determined for 10 DNA hairpins by means of femtosecond transient absorption spectroscopy. The hairpins possess a stilbenedicarboxamide hole donor and stilbenediether hole acceptor separated by seven base pairs. Hole transport occurs via an intra- or interstrand A3G4 diblock purine sequence that contains either a single base pair mismatch or strand crossing. Pyrimidine-pyrimidine mismatches (TT or CC) effectively block intrastrand hole transport; whereas purine-purine mismatches (AA or GG) permit efficient interstrand hole transport. Purine-to-purine intrastrand hole transport between adjacent matched base pairs is also moderately efficient (AG > AA > GG). Based upon these results AA mismatches are being employed in the design of three-way junctions for incorporation in prototype charge splitting and charge combining devices.
AB - The efficiency and dynamics of hole transport via base mismatches and strand crossings have been determined for 10 DNA hairpins by means of femtosecond transient absorption spectroscopy. The hairpins possess a stilbenedicarboxamide hole donor and stilbenediether hole acceptor separated by seven base pairs. Hole transport occurs via an intra- or interstrand A3G4 diblock purine sequence that contains either a single base pair mismatch or strand crossing. Pyrimidine-pyrimidine mismatches (TT or CC) effectively block intrastrand hole transport; whereas purine-purine mismatches (AA or GG) permit efficient interstrand hole transport. Purine-to-purine intrastrand hole transport between adjacent matched base pairs is also moderately efficient (AG > AA > GG). Based upon these results AA mismatches are being employed in the design of three-way junctions for incorporation in prototype charge splitting and charge combining devices.
KW - Base-pair mismatch
KW - DNA
KW - Donor-acceptor systems
KW - Hole transport
KW - Transient absorption spectroscopy
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U2 - 10.1016/j.jphotochem.2016.03.002
DO - 10.1016/j.jphotochem.2016.03.002
M3 - Article
AN - SCOPUS:84977151300
VL - 331
SP - 160
EP - 164
JO - Journal of Photochemistry and Photobiology A: Chemistry
JF - Journal of Photochemistry and Photobiology A: Chemistry
SN - 1010-6030
ER -