Time-resolved studies on the dynamics of electronic charge transfer processes in bioinorganic complexes - development of technological foundations

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The dynamics of charge transfer processes and the connected catalytic activities in bioinorganic model compounds require studies of time-resolved spectroscopic techniques such as resonance Raman and X-ray absorption spectroscopy (XAS) in a wide range of time domains from sub picosecond time scales to minutes. SP1 lays the technological foundation to supply samples under cooled anaerobic conditions and to develop measurement procedures that will allow the effective study of bioinorganic complexes such as Tyrosinase, CuA, and TypeZero model complexes. The supply of samples to the experimental interaction region of pump and probe beams has been accomplished within the first funding period by the design, construction and first operation of three different chambers that can be supplied with three different jet and aerosol injection systems. First XAS and Raman measurements show the ground breaking potential of these delivery systems as they avoid sample radiation damage and enable pump-flow-probe experiments for intermediate time domains. In the second funding period we will build on our expertise to improve the experiments on two crucial aspects. Firstly, we will implement a cooler and shaker system to increase the sample stability for longer measurement times on temperature sensitive systems and secondly we will upgrade the experimental conditions for instance for pump-probe XAS in order to enhance the signal to noise by e.g. measuring the shot noise of the x-rays. Together with our initial results we expect to accomplish our goal to measure and understand the charge transfer dynamics of ground and excited states in bioinorganic model compounds. Furthermore, we supply crucial experimental measurement techniques to enable and support the structural and electronic characterization within the subprojects 3, 4, and 5.