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| Conference Presentation (Invited) | PUBDB-2024-05442 |
2024
Abstract: Observing molecules in action through the recording of 'molecular movies', i.e., their spatiotemporal evolution during chemical dynamics, with atomic spatial and temporal resolution promises to revolutionize our understanding of the molecular sciences and to provide a time-dependent basis of chemistry. Experimentally, we build upon our approaches to prepare highly controlled samples that enable advanced imaging methods of individual molecular species directly in the molecular frame. We prepare highly controlled molecular samples for advanced ultrafast imaging experiments. This includes the preparation of ensembles of individual molecular species, e.g., single microsolvation environments, single conformers, or even single quantum states. Furthermore, the generated very cold samples are ideally suited to fix the molecules in space in laser-alignment or mixed-field orientation approaches. Here, we used the electric deflector to spatially separate different molecular species in combination with pump-probe velocity-map-imaging experiments, including utilization of 4D 'cameras'. We demonstrated that this powerful experimental approach reveals intimate details, e.g., on the radiation damage and fragmentation of water-water and pyrrole-water dimers as well as on the UV-induced dynamics in the near-UV-absorbing prototypical biomolecular indole-water system. We determined the time-dependent appearance of the different reaction products and disentangled the occurring ultrafast processes. This novel approach ensures that the reactants are well-known and that detailed characteristics of the specific reaction products are accessible – moving further toward the complete chemical-reactivity experiment.
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