TY - JOUR
T1 - Direct observation of the hole carriers in DNA photoinduced charge transport
AU - Harris, Michelle A.
AU - Mishra, Ashutosh Kumar
AU - Young, Ryan M.
AU - Brown, Kristen E.
AU - Wasielewski, Michael R.
AU - Lewis, Frederick D.
PY - 2016/5/4
Y1 - 2016/5/4
N2 - The excited state behavior of DNA hairpins possessing a diphenylacetylenedicarboxamide (DPA) linker separated from a single guanine-cytosine (G-C) base pair by zero-to-six adenine-thymine (A-T) base pairs has been investigated. In the case of hairpins with zero or one A-T separating DPA and G, formation of both DPA anion radical (DPA-·) and G cation radical (G+·) are directly observed and characterized by their transient absorption and stimulated Raman spectra. For hairpins with two or more intervening A-T, the transient absorption spectra of DPA-·) and the adenine polaron (An+·) are observed. In addition to characterization of the hole carriers, the dynamics of each step in the charge separation and charge recombination process as well as the overall efficiency of charge separation have been determined, thus providing a complete account of the mechanism and dynamics of photoinduced charge transport in these DNA hairpins.
AB - The excited state behavior of DNA hairpins possessing a diphenylacetylenedicarboxamide (DPA) linker separated from a single guanine-cytosine (G-C) base pair by zero-to-six adenine-thymine (A-T) base pairs has been investigated. In the case of hairpins with zero or one A-T separating DPA and G, formation of both DPA anion radical (DPA-·) and G cation radical (G+·) are directly observed and characterized by their transient absorption and stimulated Raman spectra. For hairpins with two or more intervening A-T, the transient absorption spectra of DPA-·) and the adenine polaron (An+·) are observed. In addition to characterization of the hole carriers, the dynamics of each step in the charge separation and charge recombination process as well as the overall efficiency of charge separation have been determined, thus providing a complete account of the mechanism and dynamics of photoinduced charge transport in these DNA hairpins.
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U2 - 10.1021/jacs.6b00702
DO - 10.1021/jacs.6b00702
M3 - Article
C2 - 27082662
AN - SCOPUS:84968813265
SN - 0002-7863
VL - 138
SP - 5491
EP - 5494
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 17
ER -