期刊
NATURE CHEMISTRY
卷 10, 期 3, 页码 355-362出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.2916
关键词
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资金
- Deutsche Forschungsgemeinschaft [FOR1405, SFB749]
- Bundesministerium fur Bildung und Forschung [BMBF VUV-FAST/05K2014, 05K12GU1]
- DFG [FOR1405, SFB925]
- Cluster of Excellence 'Munich-Center for Advanced Photonics'
- Center for Integrated Protein Science (CIPSM)
- project ELI (Extreme Light Infrastructure) from the European Regional Development Fund [CZ.02.1.01/0.0/0.0/15_008/0000162]
- Rontgen Angstrom Cluster
- Chalmers Area of Advance Materials Science
- European XFEL
- Centre for Ultrafast Imaging
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.
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