Unveiling a Chemisorbed Crystallographically Heterogeneous Graphene/L1(0)-FePd Interface with a Robust and Perpendicular Orbital Moment

[Image: see text] A crystallographically heterogeneous interface was fabricated by growing hexagonal graphene (Gr) using chemical vapor deposition (CVD) on a tetragonal FePd epitaxial film grown by magnetron sputtering. FePd was alternately arranged with Fe and Pd in the vertical direction, and the outermost surface atom was identified primarily as Fe rather than Pd. This means that FePd has a high degree of L1(0)-ordering, and the outermost Fe bonds to the carbon of Gr at the interface. When Gr is grown by CVD, the crystal orientation of hexagonal Gr toward tetragonal L1(0)-FePd selects an energetically stable structure based on the van der Waals (vdW) force. The atomic relationship of Gr/L1(0)-FePd, which is an energetically stable interface, was unveiled theoretically and experimentally. The Gr armchair axis was parallel to FePd [100](L10), where Gr was under a small strain by chemical bonding. Focusing on the interatomic distance between the Gr and FePd layers, the distance was theoretically and experimentally determined to be approximately 0.2 nm. This shorter distance (≈0.2 nm) can be explained by the chemisorption-type vdW force of strong orbital hybridization, rather than the longer distance (≈0.38 nm) of the physisorption-type vdW force. Notably, depth-resolved X-ray magnetic circular dichroism analyses revealed that the orbital magnetic moment (M(l)) of Fe in FePd emerged at the Gr/FePd interface (@inner FePd: M(l) = 0.16 μ(B) → @Gr/FePd interface: M(l) = 0.32 μ(B)). This interfacially enhanced M(l) showed obvious anisotropy in the perpendicular direction, which contributed to interfacial perpendicular magnetic anisotropy (IPMA). Moreover, the interfacially enhanced M(l) and interfacially enhanced electron density exhibited robustness. It is considered that the shortening of the interatomic distance produces a robust high electron density at the interface, resulting in a chemisorption-type vdW force and orbital hybridization. Eventually, the robust interfacial anisotropic M(l) emerged at the crystallographically heterogeneous Gr/L1(0)-FePd interface. From a practical viewpoint, IPMA is useful because it can be incorporated into the large bulk perpendicular magnetic anisotropy (PMA) of L1(0)-FePd. A micromagnetic simulation assuming both PMA and IPMA predicted that perpendicularly magnetized magnetic tunnel junctions (p-MTJs) using Gr/L1(0)-FePd could realize 10-year data retention in a small recording layer with a circular diameter and thickness of 10 and 2 nm, respectively. We unveiled the energetically stable atomic structure in the crystallographically heterogeneous interface, discovered the emergence of the robust IPMA, and predicted that the Gr/L1(0)-FePd p-MTJ is significant for high-density X nm generation magnetic random-access memory (MRAM) applications.