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Exploring ultrafast electronic coherences in metal-organic complexes in solution

Dr. Oliviero Cannelli (DESY) | Funding / PIER Seed Projects | 10/2024

Controlling the electronic motion at its intrinsic time scale is creating the conditions for innovative, light-induced chemical reaction routes via charge-directed reactivity, allowing to manipulate molecular functions at the microscopic level. Directing charge dynamics relies on the capability of generating electronic wave packets, which are coherent superposition of electronic excitations that follow classical-like trajectories, i.e. are spatially localized. As a consequence, the molecular reactivity in the presence of an electronic wave packet can significantly change with respect to conventional electronic excitations, potentially influencing photocatalytic activities. Since photoredox catalysis in solution is largely based on metal-organic complexes, controlling electronic wave packets in these systems could have a significant impact on their applications. In this project, we propose the study of specific metallic complexes whose peculiar electronic structure fully satisfies the conditions for long-living electronic coherences in solution. We will generate and detect electronic wave packets relying on transient absorption spectroscopy with extreme time resolution, using ultrathin liquid jets and a recirculation system for sample recovery. This project will open new perspectives for charge-directed photochemistry in metal-organic complexes.