Magnetism of Otherwise Nonmagnetic Elements: From Clusters to Monolayers.

ABSTRACT

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 UX6 (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 3µB in clusters and about 2µB in the 2D structure. In 2D UX4 (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.