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Spintronic structures are extensively investigated for their spin–orbit torque properties, required for magnetic commutation functionalities. Current progress in these materials is dependent on the interface engineering for the optimization of spin transmission. Here, we advance the analysis of ultrafast spin-charge conversion phenomena at ferromagnetic-transition metal interfaces due to their inverse spin-Hall effect properties. In particular, the intrinsic inverse spin-Hall effect of Pt-based systems and extrinsic inverse spin-Hall effect of Au: W and Au: Ta in NiFe/Au:(W, Ta) bilayers are investigated. The spin-charge conversion is probed by complementary techniques—ultrafast THz time-domain spectroscopy in the dynamic regime for THz pulse emission and ferromagnetic resonance spin-pumping measurements in the GHz regime in the steady state—to determine the role played by the material properties, resistivities …