Magnetism of Otherwise Nonmagnetic Elements: From Clusters to Monolayers.

Atomic clusters are known to exhibit properties different from their bulk phase. However, when assembled or supported on substrates, clusters often lose their uniqueness. For example, uranium and coinage metals (Cu, Ag, Au) are nonmagnetic in their bulk. Herein, we show that UX 6 (X= Cu, Ag, Au) clusters, unlike their nonmagnetic bulk, are not only magnetic but also retain their magnetic character and structure when assembled into a two-dimensional (2D) material. The magnetic moment remains localized at the U site and is found to be 3μ B in clusters and about 2μ B in the 2D structure. In 2D UX 4 (X = Cu, Ag, Au) monolayers, U atoms are found to be coupled antiferromagnetically through an indirect exchange coupling mediated by the coinage metal atoms. Furthermore, hydrogenation of these monolayers can induce a transition from the antiferromagnetic to the ferromagnetic phase. These results, based on density functional theory, have predictive capability and can motivate experiments.