title: Charge Transport across DNA-Based Three-Way Junctions.
abstract: DNA-based molecular electronics will require charges to be transported from one site within a 2D or 3D architecture to another. While this has been shown previously in linear, π-stacked DNA sequences, the dynamics and efficiency of charge transport across DNA three-way junction (3WJ) have yet to be determined. Here, we present an investigation of hole transport and trapping across a DNA-based three-way junction systems by a combination of femtosecond transient absorption spectroscopy and molecular dynamics simulations. Hole transport across the junction is proposed to be gated by conformational fluctuations in the ground state which bring the transiently populated hole carrier nucleobases into better aligned geometries on the nanosecond time scale, thus modulating the π-π electronic coupling along the base pair sequence.
authors.affiliation: †Department of Chemistry, Northwestern University, Evanston, Illinois 60208-3113, United States.|‡Argonne-Northwestern Solar Energy Research (ANSER) Center, Northwestern University, Evanston, Illinois 60208-3113, United States.
authors.forename: Ryan M
authors.initials: RM
authors.lastname: Young
authors.affiliation: †Department of Chemistry, Northwestern University, Evanston, Illinois 60208-3113, United States.
authors.forename: Arunoday P N
authors.initials: AP
authors.lastname: Singh
authors.affiliation: †Department of Chemistry, Northwestern University, Evanston, Illinois 60208-3113, United States.
authors.forename: Arun K
authors.initials: AK
authors.lastname: Thazhathveetil
authors.affiliation: †Department of Chemistry, Northwestern University, Evanston, Illinois 60208-3113, United States.
authors.forename: Vincent Y
authors.initials: VY
authors.lastname: Cho
authors.affiliation: §Departments of Chemistry, Biochemistry, and Physics, Duke University, Durham, North Carolina 27708, United States.
authors.forename: Yuqi
authors.initials: Y
authors.lastname: Zhang
authors.affiliation: ∥DelftChemTech, Delft University of Technology, Julianalaan 136, 2628 BL Delft, The Netherlands.
authors.forename: Nicolas
authors.initials: N
authors.lastname: Renaud
authors.affiliation: ∥DelftChemTech, Delft University of Technology, Julianalaan 136, 2628 BL Delft, The Netherlands.
authors.forename: Ferdinand C
authors.initials: FC
authors.lastname: Grozema
authors.affiliation: §Departments of Chemistry, Biochemistry, and Physics, Duke University, Durham, North Carolina 27708, United States.
authors.forename: David N
authors.initials: DN
authors.lastname: Beratan
authors.affiliation: †Department of Chemistry, Northwestern University, Evanston, Illinois 60208-3113, United States.
authors.forename: Mark A
authors.initials: MA
authors.lastname: Ratner
authors.affiliation: †Department of Chemistry, Northwestern University, Evanston, Illinois 60208-3113, United States.
authors.forename: George C
authors.initials: GC
authors.lastname: Schatz
authors.affiliation: †Department of Chemistry, Northwestern University, Evanston, Illinois 60208-3113, United States.
authors.forename: Yuri A
authors.initials: YA
authors.lastname: Berlin
authors.affiliation: †Department of Chemistry, Northwestern University, Evanston, Illinois 60208-3113, United States.
authors.forename: Frederick D
authors.initials: FD
authors.lastname: Lewis
authors.affiliation: †Department of Chemistry, Northwestern University, Evanston, Illinois 60208-3113, United States.|‡Argonne-Northwestern Solar Energy Research (ANSER) Center, Northwestern University, Evanston, Illinois 60208-3113, United States.
authors.forename: Michael R
authors.initials: MR
authors.lastname: Wasielewski
mesh_terms: D020029:Base Pairing; D004247:DNA / Q000737:chemistry*; D004579:Electron Transport; D007700:Kinetics; D008958:Models, Molecular; D056004:Molecular Dynamics Simulation; D013057:Spectrum Analysis
chemical_list: D004247:DNA