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Transferring the entatic-state principle to copper photochemistry
Univ Hamburg, Inst Nanostruct & Solid State Phys, D-22761 Hamburg, Germany.;Ctr Free Electron Laser Sci CFEL, Luruper Chaussee 149, D-22761 Hamburg, Germany..
Rhein Westfal TH Aachen, Inst Inorgan Chem, D-52074 Aachen, Germany..
Rhein Westfal TH Aachen, Inst Inorgan Chem, D-52074 Aachen, Germany..
Ludwig Maximilians Univ Munchen, Inst Biomol Opt, Oettingenstr 67, D-80538 Munich, Germany.;Ludwig Maximilians Univ Munchen, Ctr Integrated Prot Sci CIPSM, Oettingenstr 67, D-80538 Munich, Germany..
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2018 (English)In: Nature Chemistry, ISSN 1755-4330, E-ISSN 1755-4349, Vol. 10, no 3, p. 355-362Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
NATURE PUBLISHING GROUP , 2018. Vol. 10, no 3, p. 355-362
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Physical Chemistry
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URN: urn:nbn:se:uu:diva-348833DOI: 10.1038/NCHEM.2916ISI: 000425589000018PubMedID: 29461525OAI: oai:DiVA.org:uu-348833DiVA, id: diva2:1200025
Available from: 2018-04-23 Created: 2018-04-23 Last updated: 2018-04-23Bibliographically approved

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Bielecki, JohanAndreasson, Jakob

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