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Science 25 November 2005:
Vol. 310. no. 5752, pp. 1311 - 1313
DOI: 10.1126/science.1118316
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Reports

The Nature of Aqueous Tunneling Pathways Between Electron-Transfer Proteins

Jianping Lin, Ilya A. Balabin, David N. Beratan*

Structured water molecules near redox cofactors were found recently to accelerate electron-transfer (ET) kinetics in several systems. Theoretical study of interprotein electron transfer across an aqueous interface reveals three distinctive electronic coupling mechanisms that we describe here: (i) a protein-mediated regime when the two proteins are in van der Waals contact; (ii) a structured water-mediated regime featuring anomalously weak distance decay at relatively close protein-protein contact distances; and (iii) a bulk water–mediated regime at large distances. Our analysis explains a range of otherwise puzzling biological ET kinetic data and provides a framework for including explicit water-mediated tunneling effects on ET kinetics.

Departments of Chemistry and Biochemistry, Duke University, Durham, NC 27708, USA.

* To whom correspondence should be addressed. E-mail: david.beratan{at}duke.edu

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