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

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作者
Jan Kern
Rosalie Tran
Roberto Alonso-Mori
Sergey Koroidov
Nathaniel Echols
Johan Hattne
Mohamed Ibrahim
Sheraz Gul
Hartawan Laksmono
Raymond G. Sierra
Richard J. Gildea
Guangye Han
Julia Hellmich
Benedikt Lassalle-Kaiser
Ruchira Chatterjee
Aaron S. Brewster
Claudiu A. Stan
Carina Glöckner
Alyssa Lampe
Dörte DiFiore
Despina Milathianaki
Alan R. Fry
M. Marvin Seibert
Jason E. Koglin
Erik Gallo
Jens Uhlig
Dimosthenis Sokaras
Tsu-Chien Weng
Petrus H. Zwart
David E. Skinner
Michael J. Bogan
Marc Messerschmidt
Pieter Glatzel
Garth J. Williams
Sébastien Boutet
Paul D. Adams
Athina Zouni
Johannes Messinger
Nicholas K. Sauter
Uwe Bergmann
Junko Yano
Vittal K. Yachandra
机构
[1] Lawrence Berkeley National Laboratory,Physical Biosciences Division
[2] LCLS,undefined
[3] SLAC National Accelerator Laboratory,undefined
[4] Institutionen för Kemi,undefined
[5] Kemiskt Biologiskt Centrum,undefined
[6] Umeå Universitet,undefined
[7] Institut für Biologie,undefined
[8] Humboldt-Universität zu Berlin,undefined
[9] Max-Volmer-Laboratorium für Biophysikalische Chemie,undefined
[10] Technische Universität,undefined
[11] PULSE Institute,undefined
[12] SLAC National Accelerator Laboratory,undefined
[13] European Synchrotron Radiation Facility,undefined
[14] SSRL,undefined
[15] SLAC National Accelerator Laboratory,undefined
[16] National Energy Research Scientific Computing Center,undefined
[17] Lawrence Berkeley National Laboratory,undefined
[18] Present address: Diamond Light Source,undefined
[19] Harwell Science and Innovation Campus,undefined
[20] Didcot,undefined
[21] Oxfordshire OX11 0DE,undefined
[22] UK,undefined
[23] Present address: Synchrotron SOLEIL,undefined
[24] F-91192 Gif-Sur-Yvette,undefined
[25] France,undefined
[26] Present address: Department of Cell and Molecular Biology,undefined
[27] Uppsala Universitet,undefined
[28] 751 24 Uppsala,undefined
[29] Sweden,undefined
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摘要
The dioxygen we breathe is formed by light-induced oxidation of water in photosystem II. O2 formation takes place at a catalytic manganese cluster within milliseconds after the photosystem II reaction centre 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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