Dr. Taran Driver, PULSE institute and SLAC National Accelerator Laboratory and Linac Coherent Light Source

Probing Correlated Multi-Electron Dynamics on the Attosecond Timescale

The interaction of light with matter is a fundamental process for probing and engineering the quantum properties of a molecule or material. This interaction is mediated by electrons, and understanding the many-body dynamics of electronic systems in the first moments following light-driven excitation is a frontier challenge. The characteristic timescale for this electron motion is set by the splitting of the relevant energy levels, which results in motion on the attosecond (10-18 s) timescale. It is now possible to generate pulses of light lasting on the order of one hundred attoseconds, both on the tabletop in the laboratory and at large free-electron laser facilities. I will present recent work using attosecond x-ray pulses to probe the ultrafast dynamics of multi-electron systems. We measured the photoemission delay in the core-level ionization of a molecule. This is the delay between the arrival of a photon and the emission of an electron in photoionization, which was long considered an instantaneous process. In fact, this delay reveals strong modulations due to electron correlation. We also time-resolved the response of an aromatic molecule, para-aminophenol, to impulsive photoionization. By accessing the dynamics within the first femtosecond following the removal of an electron, we observed the interplay between the sub-femtosecond decay of shake-up states and coherent charge density oscillation on the few-femtosecond timescale. I will also touch on future directions which will harness these new methods to develop ultrafast probes of electron motion and exotic light-engineered states in quantum materials.