Unraveling the quantum nature of ultrafast spin injection at Co/Cu(001) interfaces

Microscopic spin-dependent charge transfer, backtransfer and scattering processes at interfaces are crucial for a broad range of dynamic spin phenomena in ferromagnetic heterostructures. We disentangle the fundamental quantum processes in optically induced spin transfer across a model epitaxial Co/Cu(001) interface by means of a direct comparison between femtosecond time-resolved interface-sensitive magnetization-induced second harmonic generation and parameter-free ab-initio time-dependent density functional theory. Due to agreement between theory and experiment, we identify transfer of majority electrons from the Co to the Cu, and simultaneous minority electron backtransfer from the Cu to the Co interface layers, as driving the spin dynamics in the first 30 fs after laser excitation. We separate this interfacial spin transfer from subsequently dominating spin flip processes induced by spin-orbit coupling, which reduce the total spin polarization in the heterostructure. Our combined experimental-theoretical approach shows the potential of a predictive theoretical description to elucidate spin injection and accumulation at ferromagnet/metal interfaces in conjunction with interface-sensitive magneto-optical experiments.