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Direct observation of the gating step in protein electron transfer: Electric-field-controlled protein dynamics
Zitatschlüssel ISI:000257902500046
Autor Kranich, Anja and Ly, Hoang Khoa and Hildebrandt, Peter and Murgida, Daniel H.
Seiten 9844-9848
Jahr 2008
ISSN 0002-7863
DOI 10.1021/ja8016895
Adresse 1155 16TH ST, NW, WASHINGTON, DC 20036 USA
Journal J. Am. Chem. Soc
Jahrgang 130
Nummer 30
Monat JUL 30
Verlag AMER CHEMICAL SOC
Zusammenfassung Heterogeneous electron transfer of proteins at biomimetic interfaces is characterized by unusual distance dependences of the electron-transfer rates, whose origin has been elusive and controversial. Using a two-color, time-resolved, surface-enhanced resonance Raman spectroelectrochernical approach, we have been able to monitor simultaneously and in real time the structure, electron-transfer kinetics, and configurational fluctuations of cytochrome c electrostatically adsorbed to electrodes coated with selfassembled monolayers. Our results show that the overall electron-transfer kinetics is determined by protein dynamics rather than by tunnelling probabilities and that the protein dynamics in turn is controlled by the interfacial electric field. Implications for interprotein electron transfer at biological membranes are discussed.
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