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Synthesis, Electronic Structure, and Spectroscopy of Multinuclear Mn Complexes Relevant to the Oxygen Evolving Complex of Photosystem II

Lee, Heui Beom and Oyala, Paul H. and Agapie, Theodor (2019) Synthesis, Electronic Structure, and Spectroscopy of Multinuclear Mn Complexes Relevant to the Oxygen Evolving Complex of Photosystem II. In: Oxygen Production and Reduction in Artificial and Natural Systems. World Scientific Publishing , Singapore, pp. 259-283. ISBN 978-981-3276-91-8. https://resolver.caltech.edu/CaltechAUTHORS:20200122-092753618

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Abstract

Biochemical, spectroscopic, structural, and computational studies have provided insight into the biological water oxidation by the Oxygen Evolving Complex [OEC] of Photosystem II. Nevertheless, the atomic level mechanism of O₂ formation remains a matter of debate. Mechanistic proposals have been guided by the spectroscopic characterization of reaction intermediates. A key intermediate in the catalytic cycle, the S₂ state, features two characteristic EPR signals at g = 2 and g = 4.1, with the relative intensity of the two signals being condition-dependent. Two nearly isoenergetic structural isomers have been proposed as the source of these distinct signals, but relevant structure — electronic structure studies remain rare. In general, studies that probe the effect of small structural changes on the spectroscopic and magnetic properties of synthetic model clusters of S-states are rare, likely due to the synthetic challenges of accessing a series of isolable clusters that are suitable for comparisons. In this chapter, structurally characterized tetranuclear complexes with Mn oxidation states relevant to S₀–S₃ states are surveyed. In particular, magnetic and spectroscopic studies of a series of [Mn^(III)Mn₃ ^(IV)O₄] cuboidal complexes show that the electronic structure of tetranuclear Mn complexes is highly sensitive to small geometric changes and the nature of the bridging ligands. Thus, the deduction of the geometry of OEC S-state intermediates based on spectroscopic features needs to be complemented with appropriate structural determination.


Item Type:Book Section
Related URLs:
URLURL TypeDescription
https://doi.org/10.1142/9789813276925_0013DOIArticle
ORCID:
AuthorORCID
Lee, Heui Beom0000-0002-9550-2649
Oyala, Paul H.0000-0002-8761-4667
Agapie, Theodor0000-0002-9692-7614
Additional Information:© 2020 World Scientific Publishing Co Pte Ltd.
Record Number:CaltechAUTHORS:20200122-092753618
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200122-092753618
Official Citation:Synthesis, Electronic Structure, and Spectroscopy of Multinuclear Mn Complexes Relevant to the Oxygen Evolving Complex of Photosystem II. Heui Beom Lee, Paul H. Oyala, and Theodor Agapie. Oxygen Production and Reduction in Artificial and Natural Systems. April 2019, 259-283; doi: 10.1142/9789813276925_0013
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:100833
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:23 Jan 2020 00:17
Last Modified:28 Feb 2020 19:38

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