WG3 Photoinduced dynamics combines state-of-the-art time-resolved as well as stationary spectroscopic characterization techniques with theoretical chemistry to obtain a full description of photoinitiated reaction steps in supramolecular photocatalysts (SPCs). Photoinduced energy and electron transfer as well as proton-coupled electron transfer present central function-determining steps in SPC photocatalysis. In particular, multi-electron-transfer will be studied in detail as generally more than one redox-equivalents need to be accumulated for proton reduction and water oxidation to take place.

This challenge requires coordinated joint research activities towards a characterization of both electronic and structural changes on a wide range of time-scales, i.e. from the initial dynamics at the Franck-Condon-point to the second-to-minutes changes associated with formation and deactivation of photocatalytically active species. This will be achieved by combining resonance Raman spectroscopy, femtosecond transient absorption and fluorescence upconversion with nano-to-millisecond flash photolysis, coherent control and two-dimensional IR and UV/Vis spectroscopy, transient resonance Raman spectroscopy, transient EPR spectroscopy and time-resolved X-ray absorption, as well as time-resolved X-ray diffraction. To understand the function-determining ultrafast steps in detail and – in particular – to identify the nature of the relevant electronic states and their correlation with molecular (sub)structures, it is essential to support the experimental work with theoretical investigations. Theory, which will be an integral part of PERSPECT-H2O, will be focused on the characterization and prediction of electronic excited states of supramolecular photocatalysts also including explicit solvation, but also on the development of tools that allow identifying reaction coordinates for proton-coupled electron transfer, following radiationless dynamics after excitation in such complex systems, and finally modeling coherent control in SPCs.



Workgroup Leader: Prof. Antonin Vlcek

Queen Mary, University of London School of Biological and Chemical Sciences J. Priestley Bldg, Mile End Road  E1 4NS London United Kingdom

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Phone: +44 -(0) 20 - 7882 3260

Fax: +49 - (0) 20 - 7882 7427