Attosecond interferometry of shape resonances in the recoil frame of CF <sub>4</sub>
Saijoscha Heck, Denitsa Baykusheva, Meng Han, Jia-Bao Ji, Conaill Perry, Xiaochun Gong, Hans Jakob Wörner
Abstract
. This technique provides insights into the spatiotemporal photoionization dynamics of molecular shape resonances. We find delays of up to ∼600 as in the ionization out of the highest occupied molecular orbital (HOMO) with a strong dependence on the emission direction and a pronounced asymmetry along the dissociation axis. Comparison with quantum-scattering calculations traces the asymmetries to the interference of a small subset of partial waves at low kinetic energies and, additionally, to the interference of two overlapping shape resonances in the HOMO-1 channel. Our experimental and theoretical results establish a broadly applicable approach to space- and time-resolved photoionization dynamics in the molecular frame.