Probing magnetic properties of Pt/CrPS4 heterostructures via x-ray spectroscopy

Heterostructures composed of heavy metal and van der Waals (vdW) magnets serve as platforms to investigate magnetotransport properties, enabling the electric readout of the spin-flop transition in the vdW antiferromagnet. We investigate the spin and orbital contributions to magnetism in Pt/exfoliated multilayer CrPS4 heterostructure using the synchrotron-radiation based x-ray magnetic circular dichroism technique measured in the total electron yield (TEY) mode. The TEY detection, with probing depth of 5–10 nm, mainly reflects the interfacial magnetic behavior near the Pt/CrPS4 boundary. A spin-flop transition appears near 0.7 T in both the CrPS4 single crystal and the Pt/CrPS4 heterostructures. The total Cr moment remains ∼2 μB/f.u. in both systems at 14 T and 6 K. In Pt/CrPS4, the orbital moment is strongly modulated by Pt, as manifested in the enhancement from ∼0.1 μB/f.u. in CrPS4 to ∼0.5 μB/f.u. in Pt/CrPS4, an effect attributable to the strong spin–orbit coupling with Pt. At 25 K, the total Cr moment reduces to ∼1.1 μB/f.u. in both systems. The Cr orbital moment in CrPS4 remains low ∼0.1 μB/f.u., whereas in Pt/CrPS4 it remains high ∼0.5 μB/f.u. These findings provide qualitative evidence of robust spin–orbit coupling and orbital hybridization at Pt/CrPS4 interface, and highlight the potential of heavy metal/vdW antiferromagnet heterostructures for spin-orbitronic device applications.