Probing Charge Transport Kinetics in a Plasmonic Environment with Cyclic Voltammetry
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Possible modifications in electrochemical reaction kinetics are explored in a nanostructured plasmonic environment with and without additional light illumination using a cyclic voltammetry (CV) method. In nanostructured gold, the effect of light on anodic and cathodic currents is much pronounced than that in a flat system. The electron-transfer rate shows a 3-fold increase under photoexcitation. The findings indicate a possibility of using plasmonic excitations for controlling electrochemical reactions.Keywords:
Photoexcitation
Electrochemical kinetics
Photocurrent
Single-turnover electron transfer within the mitochondrial complex III has been studied by combining, in solution, the isolated complex from bovine heart with detergent-solubilized reaction centers of Rhodopseudomonas sphaeroides. Initiation of electron transfer by short flash activation resulted in the prompt oxidation of cytochrome c and reduction of cytochrome b. The subsequent reduction of ferricytochrome c was observed to be concomitant with the oxidation of the ferrocytochrome b, both reactions being inhibited by the addition of actimycin A. The rate of electron transfer through complex III is dependent upon the ambient redox potential poise in a way that is consistent with the presence of a redox component, presumably analogous to the photosynthetic ubiquinone Qz, which is an obligatory intermediate in electron transfer between cytochromes b and c. These results demonstrate cyclic electron transfer in a constructed assembly of mitochondrial complex III, cytochrome c, and photochemical reaction centers.
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Abstract The construction of one‐dimensional chromophore aggregates of naphthalenediimide (NDI) and bis(2‐thienyl)diketopyrrolopyrrole (TDPP) using 40‐mer oligodeoxythymidines (dT 40 ) as a scaffold was previously reported. Furthermore, the chromophore‐aggregate (NDI‐dT 40 /TDPP‐dT 40 ) co‐immobilized heterojunction gold electrode exhibited a more efficient photocurrent than the TDPP–dT 40 ‐immobilized electrode with selective photoexcitation of TDPP‐dT 40 . In this work, a system comprising three components (in which the chromophore aggregates of diphenyl‐diketopyrrolopyrrole (PDPP‐dT 40 ) are employed as a third component) was examined in order to enhance photocurrent efficiency. Selective photoexcitation of TDPP‐dT 40 on the NDI‐dT 40 /TDPP‐dT 40 /PDPP‐dT 40 electrode shows photocurrent responses with greater quantum yield than those of the TDPP‐dT 40 , NDI‐dT 40 /TDPP‐dT 40 and TDPP‐dT 40 /PDPP‐dT 40 electrodes. The results suggest the addition of PDPP‐dT 40 can control charge separation and charge recombination between the electron and the hole (generated by an electron transfer from the photoexcited TDPP‐dT 40 to NDI‐dT 40 ).
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Low-frequency ( f < 50 Hz) photocurrent noise caused by the breakdown of the low-temperature freeze-out of neutral shallow donors at 4.2 K has been investigated under resonant photoexcitation in n -GaAs. At the onset of the breakdown (∼4 V/cm), the photocurrent noise was selectively generated by the resonant photoexcitation at the photon energies of the ( D 0 , X ) n =1,2 lines and the ( D + , X ) line. The observed results are explained by the current-filament formation.
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All biological energy (and, thus, all fossil energy) is ultimately derived from a series of basic electron transfer reactions, starting with the primary charge separation in photosynthesis. The subsequent energy flow proceeds through a series of subsequent redox reactions, largely involving metallo-proteins in which the energy of reduction is coupled to proton transport and manufacture of ATP for biosyntheses. (Fig 1). 1Mitochondral electron transport chain. Despite the obvious importance of such redox reactions, until recently such reactions remained rather poorly characterised, and poorly understood. Within the past few years, however, rapid advances have occurred in several key areas, including: 1) electron transfer theory1-3 2) experiments on model reactions (eg: electron transfer at long, fixed distance),4-6 3) experimental techniques for monitoring rapid biological electron transfer,7-10 and 4) structural charaterization of the redox proteins themselves,11-15 including detailed models for the protein-protein complexes within which electron transfer occurs. As a result of these advances, rapid experimental
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