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Optically driven intersite and interlayer spin transfer are individuallyknown as the fastest processes for manipulating the spin order of magneticmaterials on the sub 100 fs time scale. However, their competing influence onthe ultrafast magnetization dynamics remains unexplored. In our work, we showthat optically induced intersite spin transfer (also known as OISTR) dominatesthe ultrafast magnetization dynamics of ferromagnetic alloys such as Permalloy(Ni80Fe20) only in the absence of interlayer spin transfer into a substrate.Once interlayer spin transfer is possible, the influence of OISTR issignificantly reduced and interlayer spin transfer dominates the ultrafastmagnetization dynamics. This provides a new approach to control themagnetization dynamics of alloys on extremely short time scales by fine-tuningthe interlayer spin transfer.

Competing signatures of intersite and interlayer spin transfer in the ultrafast magnetization dynamics