Engineering and controlling heat and spin transport on the femtosecond timescale in spintronic devices opens up new ways to manipulate magnetization with unprecedented speed. Yet the underlying reversal mechanisms remain poorly understood due to the challenges of probing ultrafast, nonequilibrium spin dynamics. In this Letter, we demonstrate that typical magneto-optical experiments can be leveraged to access the time evolution of the spin accumulation generated within a magnetic multilayer following an ultrafast laser excitation. Furthermore, our analysis shows that the final magnetic state of the free layer in a spin valve is mainly dictated by the ultrafast dynamics of the reference-layer magnetization. Our results disentangle magnetization and spin transport dynamics within a multilayer stack and identify demagnetization and remagnetization-driven spin accumulation as the key mechanism for all-optical switching. These findings establish new design principles for ultrafast spintronic devices based on tailored spin current engineering.

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• Magnetization switching
• Magneto-optical effect
• Spin current
• Ultrafast demagnetization
• Spin valves