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The objective of this work is to employ spin-polarized density functional theory (sDFT) calculations for the exploration of ultrathin magnetic films with large magnetic moments and a strong perpendicular anisotropy. Monolayer films of Fe1−xCox (with x = 0, 0.25, 0.5, 0.75, and 1) on Rh(001) were addressed to study their magnetic properties using the all-electron full-potential linearized augmented plane wave (FLAPW) method in film geometry. We studied the magnetic order of these films including structural relaxations of the topmost layers. Fe1−xCox monolayer films were found to be ferromagnetic (FM) in a broad range of Co content x with a maximum magnetic moment of 2.8 μB and of an out-of-plane magneto-crystalline anisotropy of 0.25 meV per magnetic atom at x = 0.5. The sDFT results were mapped onto a classical Heisenberg model, demonstrating FM Fe-Co and Co-Co couplings, while the Fe-Fe interaction is antiferromagnetic on Rh(001). The ordering temperature of the FeCo film was estimated to be well above room temperature (482 K).

Ab initioinvestigations of magnetic properties of FeCo monolayer alloy films on Rh(001)