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Transferring the entatic-state principle to copper photochemistry

Dicke, B
Autor Dicke, B Institute of Nanostructure and Solid State Physics, University of Hamburg, 22761 Hamburg, Germany Center for Free-Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg, Germany
Hoffmann, A
Autor Hoffmann, A Institute for Inorganic Chemistry, RWTH Aachen University, 52074 Aachen, Germany
Stanek, J
Autor Stanek, J Institute for Inorganic Chemistry, RWTH Aachen University, 52074 Aachen, Germany
Rampp, M S
Autor Rampp, M S Institute for BioMolecular Optics and Center for Integrated Protein Science (CIPSM), Ludwig-Maximilians-Universität Munich, Oettingenstraße 67, 80538 Munich, Germany
Grimm-Lebsanft, B
Autor Grimm-Lebsanft, B ORCID Institute of Nanostructure and Solid State Physics, University of Hamburg, 22761 Hamburg, Germany Center for Free-Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg, Germany
Biebl, F
Autor Biebl, F Institute of Nanostructure and Solid State Physics, University of Hamburg, 22761 Hamburg, Germany Center for Free-Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg, Germany
Rukser, D
Autor Rukser, D Institute of Nanostructure and Solid State Physics, University of Hamburg, 22761 Hamburg, Germany Center for Free-Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg, Germany
Maerz, B
Autor Maerz, B Institute for BioMolecular Optics and Center for Integrated Protein Science (CIPSM), Ludwig-Maximilians-Universität Munich, Oettingenstraße 67, 80538 Munich, Germany
Göries, D
Autor Göries, D Deutsches Elektronensynchrotron (DESY), Notkestraße 85, 22607 Hamburg, Germany
Naumova, M
Autor Naumova, M Institute of Nanostructure and Solid State Physics, University of Hamburg, 22761 Hamburg, Germany Department of Chemistry, University of Paderborn, 33098 Paderborn, Germany
Biednov, M
Autor Biednov, M Institute of Nanostructure and Solid State Physics, University of Hamburg, 22761 Hamburg, Germany Center for Free-Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg, Germany
Neuber, G
Autor Neuber, G Institute of Nanostructure and Solid State Physics, University of Hamburg, 22761 Hamburg, Germany Center for Free-Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg, Germany
Wetzel, A
Autor Wetzel, A Institute of Nanostructure and Solid State Physics, University of Hamburg, 22761 Hamburg, Germany Center for Free-Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg, Germany
Hofmann, S M
Autor Hofmann, S M Institute for BioMolecular Optics and Center for Integrated Protein Science (CIPSM), Ludwig-Maximilians-Universität Munich, Oettingenstraße 67, 80538 Munich, Germany
Roedig, P
Autor Roedig, P Deutsches Elektronensynchrotron (DESY), Notkestraße 85, 22607 Hamburg, Germany
Meents, A
Autor Meents, A Deutsches Elektronensynchrotron (DESY), Notkestraße 85, 22607 Hamburg, Germany
Bielecki, J
Autor Bielecki, J Laboratory of Molecular Biophysics, Department of Cell and Molecular Biology, Uppsala University, Husargatan 3 (Box 596), SE-751 24 Uppsala, Sweden European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany
Andreasson, J
Autor Andreasson, J Laboratory of Molecular Biophysics, Department of Cell and Molecular Biology, Uppsala University, Husargatan 3 (Box 596), SE-751 24 Uppsala, Sweden ELI Beamlines, Institute of Physics, Czech Academy of Science, Na Slovance 2, 182 21 Prague, Czech Republic Condensed Matter Physics, Department of Physics, Chalmers University of Technology, Göteborg, Sweden
Beyerlein, K R
Autor Beyerlein, K R ORCID Center for Free-Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg, Germany
Chapman, H N
Autor Chapman, H N ORCID Center for Free-Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg, Germany Deutsches Elektronensynchrotron (DESY), Notkestraße 85, 22607 Hamburg, Germany
Bressler, C
Autor Bressler, C European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany Department of Physics, Technical University of Denmark, Fysikvej 307, Kongens Lyngby 2800, Denmark The Hamburg Center for Ultrafast Imaging, Universität Hamburg, Luruper Chaussee 149, 22761 Hamburg, Germany
Zinth, W
Autor Zinth, W ORCID Institute for BioMolecular Optics and Center for Integrated Protein Science (CIPSM), Ludwig-Maximilians-Universität Munich, Oettingenstraße 67, 80538 Munich, Germany
Rübhausen, M
Autor Rübhausen, M ORCID Institute of Nanostructure and Solid State Physics, University of Hamburg, 22761 Hamburg, Germany Center for Free-Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg, Germany
Herres-Pawlis, S
Autor Herres-Pawlis, S ORCID Institute for Inorganic Chemistry, RWTH Aachen University, 52074 Aachen, Germany

Nature chemistry. 2018 Mar ; 10 (3) : 355-362. [epub] 20180115

Nat Chem
ISSN 1755-4349 | 1755-4330
Zdroj

Jazyk angličtina Země Velká Británie, Anglie Médium print-electronic

Typ dokumentu časopisecké články, práce podpořená grantem

Perzistentní odkaz https://www.medvik.cz/link/pmid29461525

PubMed 29461525
DOI 10.1038/nchem.2916
PII: nchem.2916
Knihovny.cz E-zdroje

The entatic state denotes a distorted coordination geometry of a complex from its typical arrangement that generates an improvement to its function. The entatic-state principle has been observed to apply to copper electron-transfer proteins and it results in a lowering of the reorganization energy of the electron-transfer process. It is thus crucial for a multitude of biochemical processes, but its importance to photoactive complexes is unexplored. Here we study a copper complex-with a specifically designed constraining ligand geometry-that exhibits metal-to-ligand charge-transfer state lifetimes that are very short. The guanidine-quinoline ligand used here acts on the bis(chelated) copper(I) centre, allowing only small structural changes after photoexcitation that result in very fast structural dynamics. The data were collected using a multimethod approach that featured time-resolved ultraviolet-visible, infrared and X-ray absorption and optical emission spectroscopy. Through supporting density functional calculations, we deliver a detailed picture of the structural dynamics in the picosecond-to-nanosecond time range.

Center for Free Electron Laser Science Luruper Chaussee 149 22761 Hamburg Germany

Condensed Matter Physics Department of Physics Chalmers University of Technology Göteborg Sweden

Department of Chemistry University of Paderborn 33098 Paderborn Germany

Department of Physics Technical University of Denmark Fysikvej 307 Kongens Lyngby 2800 Denmark

Deutsches Elektronensynchrotron Notkestraße 85 22607 Hamburg Germany

ELI Beamlines Institute of Physics Czech Academy of Science Na Slovance 2 182 21 Prague Czech Republic

European XFEL Holzkoppel 4 22869 Schenefeld Germany

Institute for BioMolecular Optics and Center for Integrated Protein Science Ludwig Maximilians Universität Munich Oettingenstraße 67 80538 Munich Germany

Institute for Inorganic Chemistry RWTH Aachen University 52074 Aachen Germany

Institute of Nanostructure and Solid State Physics University of Hamburg 22761 Hamburg Germany

Laboratory of Molecular Biophysics Department of Cell and Molecular Biology Uppsala University Husargatan 3 SE 751 24 Uppsala Sweden

The Hamburg Center for Ultrafast Imaging Universität Hamburg Luruper Chaussee 149 22761 Hamburg Germany