Resolving Ultrafast Spin-Orbit Dynamics in Heavy Many-Electron Atoms

Phys Rev Lett. 2019 Oct 18;123(16):163001. doi: 10.1103/PhysRevLett.123.163001.

Abstract

We use R-matrix with time-dependence theory, with spin-orbit effects included, to study krypton irradiated by two time-delayed extreme ultraviolet ultrashort pulses. The first pulse excites the atom to 4s^{2}4p^{5}5s. The second pulse then excites 4s4p^{6}5s autoionizing levels, whose population can be observed through their subsequent decay. By varying the time delay between the two pulses, we are able to control the excitation pathway to the autoionizing states. The use of cross-polarized light pulses allows us to isolate the two-photon pathway, with one photon taken from each pulse.