Rare earth monopnictides and monochalcogenides from first principles: Towards an electronic phase diagram of strongly correlated materials

Abstract

We present the results of an ab initio study of the electronic structure of 140 rare earth compounds. Specifically, we predict an electronic phase diagram of the entire range of rare earth monopnictides and monochalcogenides, composed of metallic, semiconducting and heavy fermion-like regions and exhibiting valency transitions brought about by a complex interplay between ligand chemistry and lanthanide contraction. The calculations exploit the combined effect of a first-principles methodology, which can adequately describe the dual character of electrons, itinerant versus localized, and high-throughput computing made possible by the increasing available computational power. Our findings, including the predicted 'intermediate valent' compounds SmO and TmSe, are in excellent overall agreement with the available experimental data. The accuracy of the approach, proven e.g. through the lattice parameters calculated to within ∼1.5% of the experimental values, and its ability to describe localization phenomena in solids, makes it a competitive atomistic simulation approach in the search for and design of new materials with specific physical properties and possible technological applications. © IOP Publishing Ltd and Deutsche Physikalische Gesellschaft.