Emerging Two-Dimensional Magnetism in Nonmagnetic Electrides Hf2X (X = S, Se, Te)

TL;DR

This paper predicts that nonmagnetic layered electrides Hf2X can exhibit 2D magnetism and topological surface states due to surface-induced Stoner instability, revealing a new pathway for discovering 2D magnetic materials.

Contribution

It demonstrates, through first-principles calculations, that Hf2X electrides develop surface ferromagnetism and topological states, linking surface effects with 2D magnetism and band topology.

Findings

Surface ferromagnetism in Hf2X monolayers and surfaces.

Shift of hybridized states toward Fermi level causes Stoner instability.

Presence of strongly spin-polarized topological surface states.

Abstract

Recent experimental discoveries of two-dimensional (2D) magnets have triggered intense research activities to search for atomically thin magnetic systems. Using first-principles calculations, we predict the emergence of 2D magnetism in the monolayers (MLs), few layers, and surfaces of nonmagnetic layered electrides Hf2X (X = S, Se, Te) consisting of three-atom-thick Hf-X-Hf stacks. It is revealed that each bulk Hf2X hosts a novel quantum state of Dirac nodal lines with a high density of states arising from Hf-5d cationic and interlayer anionic electrons around -0.9 eV below the Fermi level EF. However, for the MLs, few layers, and surfaces of Hf2X, such hybridized states are shifted toward EF to generate van Hove singularities, leading to a Stoner instability. The resulting surface ferromagnetism gives rise to strongly spin-polarized topological surface states at Hf2X(001), demonstrating that anionic electrons, 2D magnetism, and band topology are entangled with each other. Our findings will open new perspectives for the discovery of 2D magnets via exploiting surface effects in nonmagnetic layered electrides.