Author
Listed:
- Dominik Kinschel
(Ecole Polytechnique Fédérale de Lausanne (EPFL))
- Camila Bacellar
(Ecole Polytechnique Fédérale de Lausanne (EPFL))
- Oliviero Cannelli
(Ecole Polytechnique Fédérale de Lausanne (EPFL))
- Boris Sorokin
(Ecole Polytechnique Fédérale de Lausanne (EPFL))
- Tetsuo Katayama
(Japan Synchrotron Radiation Research Institute (JASRI))
- Giulia F. Mancini
(Ecole Polytechnique Fédérale de Lausanne (EPFL))
- Jérémy R. Rouxel
(Ecole Polytechnique Fédérale de Lausanne (EPFL))
- Yuki Obara
(Tokyo University of Agriculture and Technology (TUAT))
- Junichi Nishitani
(Kyoto University)
- Hironori Ito
(Tokyo University of Agriculture and Technology (TUAT))
- Terumasa Ito
(Tokyo University of Agriculture and Technology (TUAT))
- Naoya Kurahashi
(Sofia University)
- Chika Higashimura
(Kyoto University)
- Shotaro Kudo
(Kyoto University)
- Theo Keane
(Newcastle University)
- Frederico A. Lima
(European XFEL)
- Wojciech Gawelda
(European XFEL
Adam Mickiewicz University)
- Peter Zalden
(European XFEL)
- Sebastian Schulz
(European XFEL)
- James M. Budarz
(Ecole Polytechnique Fédérale de Lausanne (EPFL))
- Dmitry Khakhulin
(European XFEL)
- Andreas Galler
(European XFEL)
- Christian Bressler
(European XFEL)
- Christopher J. Milne
(Paul-Scherrer-Institut (PSI))
- Thomas Penfold
(Newcastle University)
- Makina Yabashi
(Japan Synchrotron Radiation Research Institute (JASRI))
- Toshinori Suzuki
(Kyoto University)
- Kazuhiko Misawa
(Tokyo University of Agriculture and Technology (TUAT))
- Majed Chergui
(Ecole Polytechnique Fédérale de Lausanne (EPFL))
Abstract
In haemoglobin the change from the low-spin (LS) hexacoordinated haem to the high spin (HS, S = 2) pentacoordinated domed deoxy-myoglobin (deoxyMb) form upon ligand detachment from the haem and the reverse process upon ligand binding are what ultimately drives the respiratory function. Here we probe them in the case of Myoglobin-NO (MbNO) using element- and spin-sensitive femtosecond Fe Kα and Kβ X-ray emission spectroscopy at an X-ray free-electron laser (FEL). We find that the change from the LS (S = 1/2) MbNO to the HS haem occurs in ~800 fs, and that it proceeds via an intermediate (S = 1) spin state. We also show that upon NO recombination, the return to the planar MbNO ground state is an electronic relaxation from HS to LS taking place in ~30 ps. Thus, the entire ligand dissociation-recombination cycle in MbNO is a spin cross-over followed by a reverse spin cross-over process.
Suggested Citation
Dominik Kinschel & Camila Bacellar & Oliviero Cannelli & Boris Sorokin & Tetsuo Katayama & Giulia F. Mancini & Jérémy R. Rouxel & Yuki Obara & Junichi Nishitani & Hironori Ito & Terumasa Ito & Naoya K, 2020.
"Femtosecond X-ray emission study of the spin cross-over dynamics in haem proteins,"
Nature Communications, Nature, vol. 11(1), pages 1-8, December.
Handle:
RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-17923-w
DOI: 10.1038/s41467-020-17923-w
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Citations
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Cited by:
- Jie Zhang & Linshan Liu & Chaofeng Zheng & Wang Li & Chunru Wang & Taishan Wang, 2023.
"Embedded nano spin sensor for in situ probing of gas adsorption inside porous organic frameworks,"
Nature Communications, Nature, vol. 14(1), pages 1-10, December.
- R. Mincigrucci & J. R. Rouxel & B. Rossi & E. Principi & C. Bottari & S. Catalini & J. S. Pelli-Cresi & D. Fainozzi & L. Foglia & A. Simoncig & A. Matruglio & G. Kurdi & F. Capotondi & E. Pedersoli & , 2023.
"Element- and enantiomer-selective visualization of molecular motion in real-time,"
Nature Communications, Nature, vol. 14(1), pages 1-8, December.
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