Magnetic structure determination of rare-earth based, high moment, atomic laminates; potential parent materials for 2D magnets

We report muon spin rotation ($\mu$SR) and neutron diffraction on the rare-earth based magnets (Mo$_{2/3}$RE$_{1/3}$)$_2$AlC, also predicted as parent materials for 2D derivatives, where RE = Nd, Gd (only ($\mu$SR), Tb, Dy, Ho and Er. By crossing information between the two techniques, we determine the magnetic moment ($m$), structure, and dynamic properties of all compounds. We find that only for RE = Nd and Gd the moments are frozen on a microsecond time scale. Out of these two, the most promising compound for a potential 2D high ($m$) magnet is the Gd variant, since the parent crystals are pristine with $m = 6.5 \pm 0.5 \mu_B$, N\'eel temperature of $27.4 \pm 0.8$ K, and magnetic anisotropy smaller than $10^{-8}$ between in and out of plane coupling. This result suggests that magnetic ordering in the Gd variant is dominated by in-plane magnetic interactions and should therefore remain stable if exfoliated into 2D sheets.