Excess Electron Transfer Driven DNA Does Not Depend on the Transfer Direction

Haas, Clemens; Kräling, Katja; Cichon, Michaela; Rahe, Nicole; Carell, Thomas

doi:10.1002/anie.200353067

Cited by 40 publications

(13 citation statements)

References 30 publications

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“…[11] Even though the principle mechanism of excess-electron transfer, and in particular the distance dependence, [12][13][14][15][16][17][18] has been clarified, conflicting data still exist, for example, for the sequence dependence of the transfer reaction. [19][20][21][22][23][24][25][26][27] In addition, the question of whether excess-electron transfer depends on the transfer direction in the DNA duplex has not been satisfactorily investigated. Finally, we are just beginning to understand absolute hopping rates.…”

Section: Introductionmentioning

confidence: 99%

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Investigation of Excess‐Electron Transfer in DNA Double‐Duplex Systems Allows Estimation of Absolute Excess‐Electron Transfer and CPD Cleavage Rates

Fazio

Trindler

Heil

et al. 2010

Chemistry A European J

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To investigate the parameters and rates that determine excess-electron transfer processes in DNA duplexes, we developed a DNA double-duplex system containing a reduced and deprotonated flavin donor at the junction of two duplexes with either the same or different electron acceptors in the individual duplex substructures. This model system allows us to bring the two electron acceptors in the duplex substructures into direct competition for injected electrons and this enables us to decipher how the kind of acceptor influences the transfer data. Measurements with the electron acceptors 8-bromo-dA (BrdA), 8-bromo-dG (BrdG), 5-bromo-dU (BrdU), and a cyclobutane pyrimidine dimer, which is a UV-induced DNA lesion, allowed us to obtain directly the maximum overall reaction rates of these acceptors and especially of the T=T dimer with the injected electrons in the duplex. In line with previous observations, we detected that the overall dimer cleavage rate is about one order of magnitude slower than the debromination of BrdU. Furthermore, we present a more detailed explanation of why sequence dependence cannot be observed when a T=T dimer is used as the acceptor and we estimate the absolute excess-electron hopping rates.

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Section: Introductionmentioning

confidence: 99%

“…[27] This forces us to believe that dimer cleavage is slower than the multistep excess-electron transfer processes. This idea is supported by the result, from Giese, Carell and co-workers, that an electron can "overhop" a CPD lesion without opening it.…”

mentioning

confidence: 98%

Investigation of Excess‐Electron Transfer in DNA Double‐Duplex Systems Allows Estimation of Absolute Excess‐Electron Transfer and CPD Cleavage Rates

Fazio

Trindler

Heil

et al. 2010

Chemistry A European J

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“…Formation of inter‐ and intramolecular PDI dimers and oligomers upon duplex and hairpin formation or non‐covalent binding of PDI at abasic sites has also been reported. We previously reported that the PDI–DNA hairpin H8 , which possesses a PDI linker, exists as a monomer in water in the absence of salt but undergoes dimerization in the presence of 100 m m NaCl (Scheme a and b) . Similarly, the PDI–DNA dumbbell D8 exists predominantly as a monomer in water but undergoes self‐assembly into an end‐to‐end oligomer in the presence of added NaCl (Scheme c) .…”

Section: Introductionmentioning

confidence: 99%

Self‐Assembly of Perylenediimide–Single‐Strand‐DNA Conjugates: Employing Hydrophobic Interactions and DNA Base‐Pairing To Create a Diverse Structural Space

Mishra

Weissman

Krieg

et al. 2017

Chemistry A European J

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The self-assembly behavior of DNA conjugates possessing a perylenediimide (PDI) head group and an N-oligonucleotide tail has been investigated using a combination of optical spectroscopy and cryogenic transmission electron microscopy (cryo-TEM) imaging. To obtain insight into the interplay between PDI hydrophobic interactions and DNA base-pairing we employed systematic variation in the length and composition of the oligo tails. Conjugates with short (TA) or (CG) oligo tails (n≤3) form helical or nonhelical fibers constructed from π-stacked PDI head groups with pendent oligo tails in aqueous solution. Conjugates with longer (TA) oligo tails also form stacks of PDI head groups, which are further aggregated by base-pairing between their oligo tails, leading to fiber bundling and formation of bilayers. The longer (CG) conjugates form PDI end-capped duplexes, which further assemble into PDI-stacked arrays of duplexes leading to large scale ordered assemblies. Cryo-TEM imaging reveals that (CG) gives rise to both fibers and large assemblies, whereas (CG) assembles preferentially into large ordered structures.

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“…From electron spin resonance (ESR) studies on γ-ray radiated DNA, Sevilla et al estimated the β value of single-step EET at 77 K to be 0.8-1.2 Å -1 [27]. In addition, several research groups reported that the excess electron migrates in DNA by means of the multistep hopping mechanism [28][29][30][31][32][33][34][35][36][37][38][39][40][41][42][43][44][45]. Thus, the actual rate constant is necessary for further detailed understanding of EET in DNA.…”

Section: Excess Electron Transfer In Dnamentioning

confidence: 99%

Charge transfer in DNA

Fujitsuka

Majima

2013

Pure and Applied Chemistry

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In the past few decades, charge transfer in DNA has attracted considerable attention from researchers in a wide variety of fields ranging from bioscience and physical chemistry to nanotechnology. Charge transfer in DNA has been investigated using various techniques. Among them, time-resolved spectroscopic methods have provided information on chargetransfer dynamics in DNA, an important basis for therapy applications, nanomaterials, and so on. In charge transfer in DNA, holes and excess electrons act as positive and negative charge carriers, respectively. Hole-transfer (HT) dynamics have been investigated in detail, while the dynamics of excess electron transfer (EET) have only become clear rather recently. In the present paper, we summarize studies on the dynamics of HT and EET by several groups including ourselves.

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Excess Electron Transfer Driven DNA Does Not Depend on the Transfer Direction

Cited by 40 publications

References 30 publications

Investigation of Excess‐Electron Transfer in DNA Double‐Duplex Systems Allows Estimation of Absolute Excess‐Electron Transfer and CPD Cleavage Rates

Investigation of Excess‐Electron Transfer in DNA Double‐Duplex Systems Allows Estimation of Absolute Excess‐Electron Transfer and CPD Cleavage Rates

Self‐Assembly of Perylenediimide–Single‐Strand‐DNA Conjugates: Employing Hydrophobic Interactions and DNA Base‐Pairing To Create a Diverse Structural Space

Charge transfer in DNA

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