Long-Range Charge Transfer through DNA by Replacing Adenine with Diaminopurine

Kawai, Kiyoshi; Kodera, Haruka; Majima, Tetsuro

doi:10.1021/ja907409z

Cited by 37 publications

(43 citation statements)

References 56 publications

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“…72,73 In a more extensive study, a good correlation was observed between the rate of formation of PTZ •+ in NI–PTZ systems and Δ HOMO between the low potential sites G, D, and 8-bromoguanine, and the high potential sites 2-aminopurine (Ap), A, 8-bromoadenine, and thymine when low and high potential sites were placed in alternating sequences. 74 In this study, it was the difference in HOMO energies, rather than the absolute HOMO energies, that affected the rate of CT.…”

Section: Dna Ct In Solutionmentioning

confidence: 97%

Solution, surface, and single molecule platforms for the study of DNA-mediated charge transport

Muren

Olmon

Barton

2012

Phys. Chem. Chem. Phys.

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The structural core of DNA, a continuous stack of aromatic heterocycles, the base pairs, which extends down the helical axis, gives rise to the fascinating electronic properties of this molecule that is so critical for life. Our laboratory and others have developed diverse experimental platforms to investigate the capacity of DNA to conduct charge, termed DNA-mediated charge transport (DNA CT). Here, we present an overview of DNA CT experiments in solution, on surfaces, and with single molecules that collectively provide a broad and consistent perspective on the essential characteristics of this chemistry. DNA CT can proceed over long molecular distances but is remarkably sensitive to perturbations in base pair stacking. We discuss how this foundation, built with data from diverse platforms, can be used both to inform a mechanistic description of DNA CT and to inspire the next platforms for its study: living organisms and molecular electronics.

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Section: Dna Ct In Solutionmentioning

confidence: 97%

Solution, surface, and single molecule platforms for the study of DNA-mediated charge transport

Muren

Olmon

Barton

2012

Phys. Chem. Chem. Phys.

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“…Recent experiments have demonstrated that the rates of CT processes in DNA hairpins depend not only on the distance between the donor and the acceptor sites but on the base pair sequence (32)(33)(34)(35)(36)(37). In particular, it has been found that sequences containing both guanine:cytosine (G:C) and adenine:thymine (A:T) base pairs exhibit a faster hole transfer between S a and S b than sequences involving only A:T base pairs (32,33).…”

mentioning

confidence: 99%

Impact of a single base pair substitution on the charge transfer rate along short DNA hairpins

Renaud

Berlin

Ratner

2013

Proc. Natl. Acad. Sci. U.S.A.

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Numerical studies of hole migration along short DNA hairpins were performed with a particular emphasis on the variations of the rate and quantum yield of the charge separation process with the location of a single guanine:cytosine (G:C) base pair. Our calculations show that the hole arrival rate increases as the position of the guanine:cytosine base pair shifts from the beginning to the end of the sequence. Although these results are in agreement with recent experimental findings, the mechanism governing the charge migration along these sequences is revisited here. Instead of the phenomenological two-step hopping mechanism via the guanine base, the charge propagation occurs through a delocalization of the hole density along the base pair stack. Furthermore, the variations of the charge transfer with the position of the guanine base are explained by the impact of the base pair substitutions on the delocalized conduction channels.quantum filling | photoinduced hole transfer | stochastic surrogate Hamiltonian D espite a rather long history, investigations of excess charge carriers in DNA remain an area of intensive experimental and theoretical research (reviewed in refs. 1-3). This interest is mainly due to the relevance of the charge transfer (CT) phenomenon to the oxidation damage (4, 5) and to the potential application of DNA in nanoelectronics (6, 7). Experimentally, charge migration through DNA can be probed either by steady-state methods based on measurements of the damage ratio (8-10) or by time-resolved spectroscopic techniques (11)(12)(13)(14). The latter experimental approach was shown to be particularly efficient for monitoring charge motion in DNA hairpins (13). To carry out time-resolved spectroscopic experiments on these small DNA model systems, the opposite ends of the hairpin are capped with stilbene linkers S a and S b , serving as the hole donor and acceptor, respectively. It has been demonstrated that photoexcitation of S a results in the formation of a bound electron-hole pair initially localized on the hole donor. The separation of this pair occurs via the migration of the hole along the hairpin and the subsequent reaction of the positive charge with the stilbene acceptor. Kinetics of the hole arrival at S b , monitored by a second pulse, enable one to deduce the hole arrival rate, k a , and the quantum yield, Φ a , of the charge separation process.Hole migration along hairpins with less than three base pairs is discussed in terms of a single-step superexchange (15-18). In contrast, multistep sequential hopping is assumed to be responsible for charge propagation along longer hairpins (19-23). The competition between these two mechanisms leads to a distance dependence of the hole arrival rate given by:where N is the number of base pairs in the sequence, κ 1 and κ 2 are scaling factors, R 0 = 3:4 A is the mean interbase pair distance, β = 0:5 − 1:0 A −1 is the exponential falloff parameter for the superexchange mechanism (24-29), and η = 1:5 − 2:0 is the exponent of the power law characteristic f...

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“…Recent ultrafast nonlinear optical spectroscopy has revealed the temporal behavior of relaxation process of the photoexcited molecular chain [7,8]. Also in biomolecules, such as α-helix protein and DNA strands, which consist of molecular chain structures, the transport process in a nonequilibrium state have been extensively studied in order to clarify the biofunctions of these molecules from a microscopic viewpoint [9][10][11][12][13].…”

Section: Introductionmentioning

confidence: 99%

Nonequilibrium transport on a quantum molecular chain in terms of the complex Liouvillian spectrum

Tanaka

Kanki²,

Petrosky³

2011

Phys. Rev. E

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The transport process in a molecular chain in a nonequilibrium stationary state is theoretically investigated. The molecule is interacting at both ends with thermal baths of different temperatures, while no dissipation mechanism is contained inside the molecular chain. We have first obtained the nonequilibrium stationary state outside the Hilbert space in terms of the complex spectral representation of Liouvillian. The nonequilibrium stationary state is obtained as an eigenstate of the Liouvillian, which is constructed through the collision invariant of the kinetic equation. The eigenstate of the Liouvillian contains information on the spatial correlation between the molecular chain and the thermal baths. While energy flow in the nonequilibrium state which is due to the first-order correlation can be described by the Landauer formula, the particle current due to the second-order correlation cannot be described by the Landauer formula. The present method provides a simple way to evaluate the energy transport in a molecular chain in a nonequilibrium situation.

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Long-Range Charge Transfer through DNA by Replacing Adenine with Diaminopurine

Cited by 37 publications

References 56 publications

Solution, surface, and single molecule platforms for the study of DNA-mediated charge transport

Solution, surface, and single molecule platforms for the study of DNA-mediated charge transport

Impact of a single base pair substitution on the charge transfer rate along short DNA hairpins

Nonequilibrium transport on a quantum molecular chain in terms of the complex Liouvillian spectrum

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