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The direct manipulation of spins via light may provide a path towardultrafast energy-efficient devices. However, distinguishing the microscopicprocesses that can occur during ultrafast laser excitation in magnetic alloysis challenging. Here, we study the Heusler compound Co2MnGa, a material thatexhibits very strong light-induced spin transfers across the entire M-edge. Bycombining the element-specificity of extreme ultraviolet high harmonic probeswith time-dependent density functional theory, we disentangle the competitionbetween three ultrafast light-induced processes that occur in Co2MnGa:same-site Co-Co spin transfer, intersite Co-Mn spin transfer, and ultrafastspin-flips mediated by spin-orbit coupling. By measuring the dynamic magneticasymmetry across the entire M-edges of the two magnetic sublattices involved,we uncover the relative dominance of these processes at different probe energyregions and times during the laser pulse. Our combined approach enables acomprehensive microscopic interpretation of laser-induced magnetizationdynamics on timescales shorter than 100 fs.

Optically controlling the competition between spin flips and intersite spin transfer in a Heusler half-metal on sub-100 fs timescales