Journal
APPLIED MAGNETIC RESONANCE
Volume 44, Issue 6, Pages 691-720Publisher
SPRINGER WIEN
DOI: 10.1007/s00723-012-0437-3
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Funding
- Natural Sciences and Engineering Research Council (NSERC) of Canada
- Federal Ministry of Education and Research of Germany (BMBF) [03SF0355C]
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This article provides an overview of the application of electron paramagnetic resonance (EPR) and related hyperfine spectroscopies for the investigation of the electronic and geometric structure of the tetramanganese cluster that constitutes the oxygen-evolving complex (OEC) of photosystem II. Starting from the spin physics of Mn ions, a quantum-mechanical description of exchange-coupled oligonuclear Mn systems is given. Then, the focus shifts to the characterization of the OEC with emphasis on the two half-integer spin states of its catalytic cycle, namely the S-0 and S-2. The development of electronic models based on EPR and related spectroscopies, such as electron nuclear double resonance (ENDOR), is described in detail. The role of broken-symmetry density functional theory (BS-DFT) is also outlined. The characterization of Mn ligands and bound substrate waters via electron nuclear magnetic interactions is illustrated. Implications for the mechanism of water oxidation catalysis are discussed.
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