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

Kern, Jan ; Tran, Rosalie ; Alonso-Mori, Roberto ; Koroidov, Sergey ; Echols, Nathaniel ; Hattne, Johan ; Ibrahim, Mohamed ; Gul, Sheraz ; Laksmono, Hartawan and Sierra, Raymond G , et al. (2014) In Nature Communications 5. p.4371-4371
Abstract
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 $s 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 $s after the third flash. Diffraction data of all states studied exhibit an anomalous scattering signal from Mn but show no... (More)
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 $s 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 $s 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. (Less)
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@article{6308ceda-e1a2-4a60-afd4-392f6291b59b,
  abstract     = {{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 $s 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 $s 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.}},
  author       = {{Kern, Jan and Tran, Rosalie and Alonso-Mori, Roberto and Koroidov, Sergey and Echols, Nathaniel and Hattne, Johan and Ibrahim, Mohamed and Gul, Sheraz and Laksmono, Hartawan and Sierra, Raymond G and Gildea, Richard J and Han, Guangye and Hellmich, Julia and Lassalle-Kaiser, Benedikt and Chatterjee, Ruchira and Brewster, Aaron S and Stan, Claudiu A and Glöckner, Carina and Lampe, Alyssa and DiFiore, Dörte and Milathianaki, Despina and Fry, Alan R and Seibert, M Marvin and Koglin, Jason E and Gallo, Erik and Uhlig, Jens and Sokaras, Dimosthenis and Weng, Tsu-Chien and Zwart, Petrus H and Skinner, David E and Bogan, Michael J and Messerschmidt, Marc and Glatzel, Pieter and Williams, Garth J and Boutet, Sébastien and Adams, Paul D and Zouni, Athina and Messinger, Johannes and Sauter, Nicholas K and Bergmann, Uwe and Yano, Junko and Yachandra, Vittal K}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  month        = {{01}},
  pages        = {{4371--4371}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Taking snapshots of photosynthetic water oxidation using femtosecond X-ray diffraction and spectroscopy.}},
  url          = {{http://dx.doi.org/10.1038/ncomms5371}},
  doi          = {{10.1038/ncomms5371}},
  volume       = {{5}},
  year         = {{2014}},
}