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  4. Spin cascade and doming in ferric hemes: Femtosecond X-ray absorption and X-ray emission studies
 
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research article

Spin cascade and doming in ferric hemes: Femtosecond X-ray absorption and X-ray emission studies

Bacellar, Camila  
•
Kinschel, Dominik  
•
Mancini, Giulia F.  
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September 8, 2020
Proceedings Of The National Academy Of Sciences Of The United States Of America (PNAS)

The structure-function relationship is at the heart of biology, and major protein deformations are correlated to specific functions. For ferrous heme proteins, doming is associated with the respiratory function in hemoglobin and myoglobins. Cytochrome c (Cyt c) has evolved to become an important electron-transfer protein in humans. In its ferrous form, it undergoes ligand release and doming upon photoexcitation, but its ferric form does not release the distal ligand, while the return to the ground state has been attributed to thermal relaxation. Here, by combining femtosecond Fe K-alpha and K-beta X-ray emission spectroscopy (XES) with Fe K-edge X-ray absorption near-edge structure (XANES), we demonstrate that the photocycle of ferric Cyt c is entirely due to a cascade among excited spin states of the iron ion, causing the ferric heme to undergo doming, which we identify. We also argue that this pattern is common to a wide diversity of ferric heme proteins, raising the question of the biological relevance of doming in such proteins.

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Type
research article
DOI
10.1073/pnas.2004490117
Web of Science ID

WOS:000572967300017

Author(s)
Bacellar, Camila  
•
Kinschel, Dominik  
•
Mancini, Giulia F.  
•
Ingle, Rebecca A.
•
Rouxel, Jeremy  
•
Cannelli, Oliviero  
•
Cirelli, Claudio
•
Knopp, Gregor
•
Szlachetko, Jakub
•
Lima, Frederico A.
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Date Issued

2020-09-08

Publisher

National Academy of Sciences

Published in
Proceedings Of The National Academy Of Sciences Of The United States Of America (PNAS)
Volume

117

Issue

36

Start page

21914

End page

21920

Subjects

Multidisciplinary Sciences

•

Science & Technology - Other Topics

•

ultrafast

•

x-ray spectroscopy

•

ferric hemoproteins

•

spin states

•

doming

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resolved resonance raman

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nitric-oxide-binding

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cytochrome-c

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electron-transfer

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carbon-monoxide

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low-temperature

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myoglobin recombination

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vibrational-relaxation

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spectroscopy

•

dynamics

Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LSU  
Available on Infoscience
October 10, 2020
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/172402
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