  The direct manipulation of spins via light may provide a path toward
ultrafast energy-efficient devices. However, distinguishing the microscopic
processes that can occur during ultrafast laser excitation in magnetic alloys
is challenging. Here, we study the Heusler compound Co2MnGa, a material that
exhibits very strong light-induced spin transfers across the entire M-edge. By
combining the element-specificity of extreme ultraviolet high harmonic probes
with time-dependent density functional theory, we disentangle the competition
between three ultrafast light-induced processes that occur in Co2MnGa:
same-site Co-Co spin transfer, intersite Co-Mn spin transfer, and ultrafast
spin-flips mediated by spin-orbit coupling. By measuring the dynamic magnetic
asymmetry across the entire M-edges of the two magnetic sublattices involved,
we uncover the relative dominance of these processes at different probe energy
regions and times during the laser pulse. Our combined approach enables a
comprehensive microscopic interpretation of laser-induced magnetization
dynamics on timescales shorter than 100 fs.
