Understanding ultrafast molecular dynamics that govern the evolution of excited systems allows modeling, predicting and in some cases controlling the outcome of chemical reactions. Using femtosecond (fs) laser pulses to initiate and probe dynamics, we provide insight into the important quantum mechanical mechanisms that control molecular dynamics. However, range of excited dynamics that can be addressed is limited by the wavelengths of readily available laser systems. Specifically, superexcited states, which are states that lie above the threshold for electron emission, can not be initiated directly from neutral molecular ground states with conventional laser systems. Such superexcited states exhibit extremely non Born-Oppenheimer dynamics, as electron and nuclear motion dynamics compete on ultrafast timescales, often leading to fragmentation rather than electron emission. Therefore, I propose to extend the range of investigated ultrafast phenomena to include superexcited state dynamics. Such states will be accessible with conventional fs lasers, not from neutral ground state molecules but from fast beams of negative ions or metastable neutral species that are energetically close to superexcited states. Furthermore, fast beam fragment imaging techniques will be used to record time resolved kinetic energies and correlations of fragmentation products. Specific objectives of this proposal are (i) to investigate time resolved dynamics of superexcited negatively charged water clusters; (ii) to investigate fragmentation dynamics of superexcited H3* states. The contribution of the MC-IRG will provide necessary funding to cover project expenses. In this way, MC-IRG will contribute to the training of students and to the transfer of knowledge I have acquired in the USA to researchers in Israel and the EU region. This grant will also enhance my own prospects of securing a tenure position at the Hebrew University in the end of the reintegration period.
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