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Direct observation of the gating step in protein electron transfer: Electric-field-controlled protein dynamics
Citation key ISI:000257902500046
Author Kranich, Anja and Ly, Hoang Khoa and Hildebrandt, Peter and Murgida, Daniel H.
Pages 9844-9848
Year 2008
ISSN 0002-7863
DOI 10.1021/ja8016895
Address 1155 16TH ST, NW, WASHINGTON, DC 20036 USA
Journal J. Am. Chem. Soc
Volume 130
Number 30
Month JUL 30
Publisher AMER CHEMICAL SOC
Abstract 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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