The S2 State of the Oxygen-Evolving Complex of Photosystem II Explored by QM/MM Dynamics: Spin Surfaces and Metastable States Suggest a Reaction Path Towards the S3 State

被引：141
作者：
Bovi, Daniele [1 ]
Narzi, Daniele [1 ]
Guidoni, Leonardo [1 ,2 ]
机构：
[1] Univ Roma La Sapienza, Dipartimento Fis, I-00185 Rome, Italy
[2] Univ Aquila, Dipartimento Sci Fis & Chim, I-67100 Laquila, Italy
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2013年 / 52卷 / 45期
基金：
欧洲研究理事会;
关键词：
abinitio calculations; density functional calculations; Kok cycle; photosystemII; water splitting; PARAMAGNETIC-RESONANCE SIGNALS; O BOND FORMATION; NEAR-INFRARED LIGHT; MANGANESE COMPLEX; CRYSTAL-STRUCTURE; SUBSTRATE WATER; SYNECHOCOCCUS-ELONGATUS; O-2-EVOLVING COMPLEX; PROTONATION STATES; STRUCTURAL MODELS;
D O I：
10.1002/anie.201306667
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Split and polish: Quantum mechanics/molecular mechanics simulations reveal the role of spin surfaces, kinetics, and thermodynamics on the interconversion between two structural models of the {Mn4CaO5} cluster (see picture) in the S2 state of the water-splitting Kok's cycle in photosystem-II. The results account for the temperature, illumination, and procedure dependence of historical EPR experiments and suggest a detailed pathway for the S2 to S3 transition. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
引用
收藏
页码：11744 / 11749
页数：6
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