Unraveling the dominant role of phonons in the ultrafast non-local dynamics of a photoexcited metal/insulator heterostructure

Exploiting the element specificity of soft x-ray spectroscopy, we analyze the microscopic origin of ultrafast non-local dynamics induced by localized optical excitation in metal-insulator heterostructures. The performed ultraviolet pump - soft x-ray probe experiment is sensitive to all constituents of the [Fe/MgO]$_n$ heterostructures, and probes electronic as well as lattice excitations. Additional ultrafast electron diffraction experiments independently analyze the lattice dynamics of the Fe constituent, and provide in combination with the soft x-ray analysis and ab initio theory calculations comprehensive insight into the microscopic processes leading to local and non-local relaxation within one or among two constituents, respectively. Besides electronic excitations in Fe which relax within 1 ps by electron-phonon coupling, we identify a change at the oxygen K edge absorption at MgO sites which occurs already within 0.5 ps and is mediated by lattice excitations in Fe. This selective phonon transfer across the interface excites non-thermal, hot phonons in MgO. In addition a second, slower timescale is identified at the oxygen K pre-edge and the Fe L$_3$ edge. It represents heat transfer and thermalization of the heterostructure as a whole. Noteworthy, our experiments lack signatures of charge transfer across the interface and it is concluded that phononic processes dominate the competition of electronic and lattice excitations in these non-local dynamics.