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Chemical interactions and dynamics with femtosecond X-ray spectroscopy and the role of X-ray free-electron lasers

X-ray free-electron lasers with intense, tuneable and short-pulse X-ray radiation are transformative tools for the investigation of transition-metal complexes and metalloproteins. This becomes apparent in particular when combining the experimental observables from X-ray spectroscopy with modern theo...

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Detalles Bibliográficos
Autor principal: Wernet, Philippe
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society Publishing 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6452048/
https://www.ncbi.nlm.nih.gov/pubmed/30929622
http://dx.doi.org/10.1098/rsta.2017.0464
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author Wernet, Philippe
author_facet Wernet, Philippe
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description X-ray free-electron lasers with intense, tuneable and short-pulse X-ray radiation are transformative tools for the investigation of transition-metal complexes and metalloproteins. This becomes apparent in particular when combining the experimental observables from X-ray spectroscopy with modern theoretical tools for calculations of electronic structures and X-ray spectra from first principles. The combination gives new insights into how charge and spin densities change in chemical reactions and how they determine reactivity. This is demonstrated for the investigations of structural dynamics with metal K-edge absorption spectroscopy, spin states in excited-state dynamics with metal 3p-3d exchange interactions, the frontier-orbital interactions in dissociation and substitution reactions with metal-specific X-ray spectroscopy, and studies of metal oxidation states with femtosecond pulses for ‘probe-before-destroy’ spectroscopy. The role of X-ray free-electron lasers is addressed with thoughts about how they enable ‘bringing back together’ different aspects of the same problem and this is thought to go beyond a conventional review paper where these aspects are formulated in italic font type in a prequel, an interlude and in a sequel. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays'.
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spelling pubmed-64520482019-04-18 Chemical interactions and dynamics with femtosecond X-ray spectroscopy and the role of X-ray free-electron lasers Wernet, Philippe Philos Trans A Math Phys Eng Sci Articles X-ray free-electron lasers with intense, tuneable and short-pulse X-ray radiation are transformative tools for the investigation of transition-metal complexes and metalloproteins. This becomes apparent in particular when combining the experimental observables from X-ray spectroscopy with modern theoretical tools for calculations of electronic structures and X-ray spectra from first principles. The combination gives new insights into how charge and spin densities change in chemical reactions and how they determine reactivity. This is demonstrated for the investigations of structural dynamics with metal K-edge absorption spectroscopy, spin states in excited-state dynamics with metal 3p-3d exchange interactions, the frontier-orbital interactions in dissociation and substitution reactions with metal-specific X-ray spectroscopy, and studies of metal oxidation states with femtosecond pulses for ‘probe-before-destroy’ spectroscopy. The role of X-ray free-electron lasers is addressed with thoughts about how they enable ‘bringing back together’ different aspects of the same problem and this is thought to go beyond a conventional review paper where these aspects are formulated in italic font type in a prequel, an interlude and in a sequel. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays'. The Royal Society Publishing 2019-05-20 2019-04-01 /pmc/articles/PMC6452048/ /pubmed/30929622 http://dx.doi.org/10.1098/rsta.2017.0464 Text en © 2019 The Authors. http://creativecommons.org/licenses/by/4.0/ Published by the Royal Society under the terms of the Creative Commons Attribution License http://creativecommons.org/licenses/by/4.0/, which permits unrestricted use, provided the original author and source are credited.
spellingShingle Articles
Wernet, Philippe
Chemical interactions and dynamics with femtosecond X-ray spectroscopy and the role of X-ray free-electron lasers
title Chemical interactions and dynamics with femtosecond X-ray spectroscopy and the role of X-ray free-electron lasers
title_full Chemical interactions and dynamics with femtosecond X-ray spectroscopy and the role of X-ray free-electron lasers
title_fullStr Chemical interactions and dynamics with femtosecond X-ray spectroscopy and the role of X-ray free-electron lasers
title_full_unstemmed Chemical interactions and dynamics with femtosecond X-ray spectroscopy and the role of X-ray free-electron lasers
title_short Chemical interactions and dynamics with femtosecond X-ray spectroscopy and the role of X-ray free-electron lasers
title_sort chemical interactions and dynamics with femtosecond x-ray spectroscopy and the role of x-ray free-electron lasers
topic Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6452048/
https://www.ncbi.nlm.nih.gov/pubmed/30929622
http://dx.doi.org/10.1098/rsta.2017.0464
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