Journal Article

PUBDB-2018-00754

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Transferring the entatic-state principle to copper photochemistry

Dicke, B.CFEL*Extern* ; Hoffmann, A. ; Stanek, J. ; Rampp, M. S. ; Grimm-Lebsanft, B.Extern* ; Biebl, F.CFEL* ; Rukser, D.CFEL*Extern* ; Maerz, B. ; Göries, D.XFEL.EU* ; Naumova, M.DESY* ; Biednov, M.CFEL*Extern* ; Neuber, G.CFEL*Extern* ; Wetzel, A. ; Hofmann, S. M. ; Roedig, P.DESY* ; Meents, A.CFEL*DESY* ; Bielecki, J.XFEL.EU* ; Andreasson, J.Extern* ; Beyerlein, K. R.CFEL*MPG* ; Chapman, H. N.CFEL*DESY* ; Bressler, C. ; Zinth, W. (Corresponding author) ; Rübhausen, M. (Corresponding author) ; Herres-Pawlis, S. (Corresponding author)

2018
Nature Publishing Group London

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Please use a persistent id in citations: doi:10.1038/nchem.2916  doi:10.3204/PUBDB-2018-00754

Abstract: 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.

Note: © Macmillan Publishers Limited, part of Springer Nature

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)
2. UNI/INF (CFEL-AO)
3. Attosecond Science and Technology (FS-ATTO)
4. FS-Photon Science (FS-PS)
5. CFEL-Coherent X-Ray Imaging (FS-CFEL-1)
6. European XFEL Projekt Team (Eur.XFEL)

Research Program(s):

1. 6215 - Soft Matter, Health and Life Sciences (POF3-621) (POF3-621)
2. 6G3 - PETRA III (POF3-622) (POF3-622)
3. SWEDEN-DESY - SWEDEN-DESY Collaboration (2020_Join2-SWEDEN-DESY) (2020_Join2-SWEDEN-DESY)

Experiment(s):

1. PETRA Beamline P11 (PETRA III)

Appears in the scientific report 2018

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Database coverage:
; ; BIOSIS Previews ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; IF >= 25 ; JCR ; NCBI Molecular Biology Database ; Nationallizenz ; SCOPUS ; Science Citation Index ; Science Citation Index Expanded ; Thomson Reuters Master Journal List ; Web of Science Core Collection

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