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Kohärente multidimensionale Spektroskopie von kontrollierten isolierten Systemen (COCONIS)

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Fundamental quantum mechanical processes determine the properties of matter and their functionality. In order to understand complex processes such as light harvesting in photosynthesis and photovoltaics, a detailed knowledge of coherent effects in excitation and charge transfer processes and related dynamics is required. To a large extent, the complexity of the systems induces too many interactions and perturbations of the processes to isolate and understand individual mechanisms. Advanced experimental methods, capable of detecting quantum coherences, so far are not applicable to quantum state controlled molecular complexes isolated from the perturbing environment, due to the low density of such targets. In this project we employ for the first time coherent femtosecond multidimensional spectroscopy to dilute isolated molecular complexes. For a specific heterogeneous synthesis, we use aggregation in superfluid helium at millikelvin temperatures. In order to reach the needed sensitivity we set up a novel phase modulation technique including lock-in demodulation in combination with mass-resolved ionization and photoelectron detection. Advanced mathematical methods are furthermore developed and applied, boosting efficient collection of multidimensional datasets.


This research is carried out in the projects: PHANCY, SAPPHIRE, CHOISE.