Making Movies of Atomic Motion at the Angstrom and Femtosecond Scale

Realizing imaging of atomic motion de-novo within multiple molecular bonds in isolated molecules, with Angstrom and femtosecond resolutions is a grand challenge for the atomic molecular and optical physics community.  We will present several recent results in imaging quantum dynamics at the atomic length and time scales using ultrafast coherent x-ray diffraction at free electron lasers, photoelectron self-diffraction via strong field ionization, coincidence techniques, and advanced imaging and data analysis schemes that create such molecular movies without prior information of the system under study.  Time-resolved femtosecond x-ray diffraction patterns from laser-excited molecular iodine were used to create high fidelity molecular movies de-novo. We imaged electronic population transfer, vibrational motion, dissociation, rotational dephasing, Raman transitions, and non-adiabatic population transfer via coherent mixing of different electronic states.  We’ll also discuss results from photoelectron velocity map imaging and coincidence techniques as potential routes for table-top molecular movies. Finally, we will discuss using novel experimental and analysis methods, extending to the condensed phase and to systems of increased complexity.