Relationship between Charge Transfer and Charge Recombination Determines Photocurrent Efficiency through DNA Films

Takada, Tadao; Lin, Chunyan; Majima, Tetsuro

doi:10.1002/ange.200701525

Cited by 11 publications

(11 citation statements)

References 29 publications

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“…A 13-mer primer DNA (P2) possessing a hexylthiol group at the 5′-end was immobilized on the gold electrode through the Au−S bond linkage by the usual method. 28 A 10-mer oligo-dA (A 10 ) sequence containing the hexylthiol group at the 5′-end was used as a diluter to modulate the surface density of the primer (P2) on the electrode. A template DNA (T4) designed for the single-nucleotide extension was hybridized to P2 on the electrode.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…The photocurrent generation on an electrode modified with NI-conjugated dsDNA has been reported. 28,29 The excitation of NI upon irradiation generates a hole into DNA through charge separation process between excited NI and a nucleobase, and the generated hole migrates to the electrode through DNA and a reduced NI is recycled by a molecular oxygen dissolved in aqueous solution, resulting in the cathodic photocurrent response. 28,29 After the PEX reactions using dUTP NI , the prompt photocurrents were observed for the electrodes with P2/T4.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…A significant signal change in the photocurrent response by the mismatch base pair might be applied to discriminate the single-nucleotide sequence. 28,45 ■ CONCLUSION…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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Photoresponsive DNA Monolayer Prepared by Primer Extension Reaction on the Electrode

et al. 2015

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We describe a simple and convenient method for the preparation of photoresponsive DNA-modified electrodes using primer extension (PEX) reactions. A naphthalimide derivative was used as the photosensitizer that was attached to the C5-position of 2'-deoxyuridine-5'-triphosphate (dUTP(NI)). It has been found that dUTP(NI) is a good substrate for the PEX reactions using KOD Dash and Vent (exo-) enzymes in solutions to incorporate naphthalimide (NI) moieties into the DNA sequences. On the electrode surface immobilized with the primer/template DNA, the PEX reactions to incorporate dUTP(NI) molecules into the DNA sequence were found to efficiently proceed. With this solid-phase method, the DNA monolayers capable of generating photocurrent due to the photoresponsive NI molecule can be constructed. It was shown that the photocurrent generation was significantly suppressed by a single-nucleotide mismatch included in the primer/template DNA, which is applicable for the design of photoelectrochemical sensors to discriminate single-nucleotide sequences.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

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Photoresponsive DNA Monolayer Prepared by Primer Extension Reaction on the Electrode

et al. 2015

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“…7 Charge transfer is frequently associated with large dipole moment changes causing changes in local electric field magnitudes, which can then alter the molecular structure of the charge transfer system, rearrange neighboring species, and perturb the electronic states of both the charge transferred and neighboring species. 8 These responses to charge transfer events play a crucial role in determining photocurrent efficiency in photovoltaics, 9 bond activation in photocatalytic systems, 10 and reaction rates in biological systems. 1−5 Understanding the mechanism of charge transfer reactions on the molecular level can be challenging because systems in solution can be perturbed by solvent effects or by coupling to their heterogeneous environments.…”

Section: ■ Introductionmentioning

confidence: 99%

Orientation and Polarization Dependence of Ground- and Excited-State FSRS in Crystalline Betaine-30

et al. 2019

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Charge transfer reactions are frequently accompanied by large changes in dipole and are of instrumental importance in many biological and chemical processes. Understanding the mechanism and dynamics associated with charge transfer reactions has been the focus of decades of investigations; however, most studies have been done with solvated analytes in which the measurements can be significantly impacted by environmental broadening or solvent-mediated effects. Here, we study photoinduced intramolecular charge transfer in crystalline betaine-30, thus dramatically reducing environmental heterogeneities and solvent contributions to the charge transfer process. We use femtosecond stimulated Raman spectroscopy in a reflective microscope configuration to probe the ground and excited state structures in a well-characterized betaine-30 crystal, with a unit cell consisting of four nearly orthogonal betaine-30 molecules and six water molecules. This study highlights how changing the crystal orientation and laser polarization can impact the excited- and ground-state Raman signals due to differences in the unit cell net dipole moment along different crystal axes. We find that the forward charge transfer process (τ ∼ 500 fs) is unaffected by the crystalline environment, while the back electron transfer process (τ ∼ 20 ps) is delayed in the crystalline environment as compared to lifetimes obtained in a range of solvents. This work highlights the role of the net transition dipole orientation on signals resulting from charge transfer in an anisotropic system and should aid in guiding the rational design of solid-state photoactivated devices.

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“…Due to hybridisation specificity and the ability of oligonucleotides to self-assemble, they have been used as tools to arrange precise structures in the nanoscale range. [1][2][3] Many different methods have been developed that use DNA as a scaffold to orientate and assemble inorganic [4][5][6][7][8][9][10] as well as organic [11][12][13] compounds on nanometer scales. DNA block copolymers with both a DNA segment and an organic polymer unit were reported recently.…”

Section: Introductionmentioning

confidence: 99%

Enzymatic Synthesis of Organic‐Polymer‐Grafted DNA

Baccaro

Marx

2009

Chemistry A European J

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To create bioorganic hybrid materials, interdisciplinary work in the fields of chemistry, biology and materials science is conducted. DNA block copolymers are promising hybrid materials due to the combination of properties intrinsic to both the polymer and the nucleic acid blocks. Until now, the coupling of DNA and organic polymers has been exercised post-synthetically in solution or on solid support. Herein, we report the first enzyme-catalysed synthesis of DNA-organic polymer chimeras. For this purpose, four novel 2'-deoxyuridine triphosphates carrying polymer-like moieties linked to the nucleobase were synthesised. Linear polyethylene glycol monomethyl ethers of different sizes (1) and branched polyamido dendrons with varying terminal groups (2) were chosen as building blocks. We investigated the ability of DNA polymerases to accept the copolymers in comparison to the natural substrate and showed, through primer extensions, polymerase chain reactions and rolling circle amplification, that these building blocks could serve as a surrogate for the natural thymidine. By this method, DNA hybrid materials with high molecular weight, modification density, and defined structure are accessible.

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Relationship between Charge Transfer and Charge Recombination Determines Photocurrent Efficiency through DNA Films

Cited by 11 publications

References 29 publications

Photoresponsive DNA Monolayer Prepared by Primer Extension Reaction on the Electrode

Photoresponsive DNA Monolayer Prepared by Primer Extension Reaction on the Electrode

Orientation and Polarization Dependence of Ground- and Excited-State FSRS in Crystalline Betaine-30

Enzymatic Synthesis of Organic‐Polymer‐Grafted DNA

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