Abstract

Abstract : This research program explored time-resolved dynamics of molecular systems by femtosecond photoelectron spectroscopy using high order harmonics. Ultrafast soft x-ray laser pump/probe studies revealed changes in binding relations and atomic core level shifts in the molecules during chemical rearrangements by detecting the changes in photoelectron energies as a function of internuclear separation in dissociative states in real time. Harmonic pulses with photon energies up to 100 eV and femtosecond time resolution were produced with excellent efficiency and pulse-to-pulse stability. Valence and core photoelectron spectra were obtained on neutral atoms and molecules. Phase manipulation of high order harmonics was achieved. Photoelectron spectra and photoionization mass spectra of gas phase ionic liquids were obtained. Two color excitation spectra of bromine molecules were investigated, as well as Rydberg wave packet photoelectron angular distributions. Pump/probe experiments on the photodissociation of metal carbonyls, halogens, and aluminum halides were also under investigation.

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