First-Principles Study of Two-Dimensional CeN: Interplay between Structural Stability, Electronic Structure, and Magnetism

Abstract

In this work, the structural stability, and the electronic and magnetic properties of a novel CeN monolayer derived from the (111) surface of bulk rock salt CeN are investigated using first-principles calculations. Dimensional reduction produces substantial changes in the local atomic environment, decreasing the Ce-N coordination from sixfold in the bulk to threefold in the monolayer and shortening the Ce-N bond length, while preserving an essentially planar hexagonal structure. Moreover, the electronic and magnetic properties are significantly modified, which may be useful for practical applications. Both ferromagnetic (FM) and antiferromagnetic (AFM) configurations were investigated and found to be strongly bound, with the FM state slightly lower in energy. The magnetic moments are predominantly localized on the Ce atoms and mainly originated from the Ce 4f states. The electronic structure also exhibits a pronounced dependence on magnetic ordering, highlighting the connection between localized 4f states and the spin-dependent electronic properties of the system. In addition, the calculated elastic properties confirm the mechanical stability of the monolayer, while phonon calculations support its dynamical stability. Ab initio molecular dynamics simulations further indicate that the two-dimensional structure preserves its integrity under finite-temperature conditions. Overall, these results demonstrate that dimensional reduction significantly modifies the structural, electronic, and magnetic behavior of CeN without compromising the stability of the resulting two-dimensional lattice. The combination of structural robustness, localized Ce 4f magnetism, and spin-dependent electronic properties make the CeN monolayer an interesting system for further exploration in two-dimensional magnetism and spin-dependent applications.