Long Range Electron Transfer in Blue Copper Proteins

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Abstract
Long range electron transfer (LRET) within proteins is investigated. Resolution of the detailed pathways and the effect of separating medium, distance and energetics on the rates are the focal questions. Two types of systems are studied: In azurins, it is the intramolecular LRET from an RS-SR− radical, produced pulse radiolytically, to the Cu(II) center. Differences in amino acid sequences amongst naturally occurring azurins make it possible to examine the parameters controling the reaction rates along this non physiological pathway. In the second system, the intramolecular LRET from the type 1 Cu(I) site to the type 3 binuclear center is studied in the multi sited blue copper oxidase, laccase. This enables a structure-reactivity correlation for the LRET along a pathway optimized by evolution.