Taking snapshots of photosynthetic water oxidation using femtosecond X-ray diffraction and spectroscopy.

Taking snapshots of photosynthetic water oxidation using femtosecond X-ray diffraction and spectroscopy.
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DOI:
10.1038/ncomms5371
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发表时间:
2014-07-09
影响因子:
16.6
通讯作者:
Yachandra, Vittal K.
Yachandra, Vittal K.
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Kern, Jan;Tran, Rosalie;Alonso-Mori, Roberto;Koroidov, Sergey;Echols, Nathaniel;Hattne, Johan;Ibrahim, Mohamed;Gul, Sheraz;Laksmono, Hartawan;Sierra, Raymond G.;Gildea, Richard J.;Han, Guangye;Hellmich, Julia;Lassalle-Kaiser, Benedikt;Chatterjee, Ruchira;Brewster, Aaron S.;Stan, Claudiu A.;Gloeckner, Carina;Lampe, Alyssa;DiFiore, Doertee;Milathianaki, Despina;Fry, Alan R.;Seibert, M. Marvin;Koglin, Jason E.;Gallo, Erik;Uhlig, Jens;Sokaras, Dimosthenis;Weng, Tsu-Chien;Zwart, Petrus H.;Skinner, David E.;Bogan, Michael J.;Messerschmidt, Marc;Glatzel, Pieter;Williams, Garth J.;Boutet, Sebastien;Adams, Paul D.;Zouni, Athina;Messinger, Johannes;Sauter, Nicholas K.;Bergmann, Uwe;Yano, Junko;Yachandra, Vittal K.

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我们呼吸的双氧是由水在光系统II中光诱导氧化形成的。O2的形成发生在催化锰簇的光系统II反应中心被三个单周转闪光激发后的毫秒内。在这里,我们提出了结合X射线发射光谱和衍射数据的2闪光(2F)和3闪光(3F)的光系统II样品,和瞬态3F′状态(第三闪光后250 μs),收集功能条件下使用X射线自由电子激光。光谱表明,在第三次闪光后的250 μs内,初始O-O键的形成与Mn还原相结合,尚未发生。所有研究状态的衍射数据表现出从Mn的异常散射信号,但在目前的分辨率为4.5 μ m没有显着的结构变化。这项研究代表了光系统II催化反应过程中结构变化的分子电影中的初始帧。
The dioxygen we breathe is formed from water by its light-induced oxidation in photosystem II. O2 formation takes place at a catalytic manganese cluster within milliseconds after the photosystem II reaction center is excited by three single-turnover flashes. Here we present combined X-ray emission spectra and diffraction data of 2 flash (2F) and 3 flash (3F) photosystem II samples, and of a transient 3F′ state (250 μs after the third flash), collected under functional conditions using an X-ray free electron laser. The spectra show that the initial O-O bond formation, coupled to Mn-reduction, does not yet occur within 250 μs after the third flash. Diffraction data of all states studied exhibit an anomalous scattering signal from Mn but show no significant structural changes at the present resolution of 4.5 Å. This study represents the initial frames in a molecular movie of the structural changes during the catalytic reaction in photosystem II.
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