Unveiling Orbital-mediated Ultrafast Demagnetization in Rare Earth-Transition-Metal Ferrimagnets

Abstract

The ultimate speed limit of magnetic recording and spintronic devices is set by the efficiency of angular-momentum transfer during ultrafast demagnetization, yet its microscopic pathway in Rare-Earth-Transition-Metal (RE-TM) ferrimagnets remains debated. Here, we establish an orbital-mediated framework in which 3d spin-orbit coupling (SOC) governs angular momentum (AM) dissipation. Strong 3d-SOC in RE-Co enables sub-picosecond, single-step demagnetization via direct orbital-to-lattice transfer, whereas weak 3d-SOC in RE-Fe redirects AM into 4f orbitals, producing slower two-step dynamics. The second-stage rate scales with 4f-SOC strength, revealing a distinct orbital-mediated dissipation channel. Using time-resolved magneto-optical Kerr measurements, supported by an extended four-temperature model, corroborate this picture across diverse RE-TM systems (RE = Sm, Gd, Tb, Dy, Ho and TM = Fe, Co, CoNi). Our results identify the SOC-driven competition between 3d and 4f orbital channels as the universal mechanism governing ultrafast demagnetization in RE-TM ferrimagnets, enabling rational design of the switching speed for next-generation spintronic devices.