Engineering 2D high-temperature ferromagnets with large in-plane anisotropy via alkali-metal decoration in a tetragonal CoSe monolayer

TL;DR

This study uses first-principles calculations to show that alkali-metal decoration of tetragonal CoSe monolayers creates stable 2D ferromagnets with high Curie temperatures and large in-plane magnetic anisotropy, suitable for spintronics.

Contribution

It introduces alkali-metal decoration as a novel method to engineer high-$T_c$ 2D ferromagnets with large MAE in tetragonal CoSe monolayers, enhancing magnetic properties significantly.

Findings

LiCoSe is a half-metal with high $T_c$ > 300 K.

Alkali-metal decoration enhances ferromagnetism and MAE.

NaCoSe exhibits the highest MAE and strain-tunable $T_c$.

Abstract

Two-dimensional (2D) ferromagnetic materials with high Curie temperature ($T_{\rm c}$) and large magnetic anisotropy energy (MAE) are critical for nanoscale spintronics but remain rare. We propose, via first-principles calculations, that adsorbing alkali atoms ($A$ = Li, Na, K, Rb, Cs) onto a tetragonal CoSe monolayer transforms it into a series of stable 2D ferromagnetic metals, $A$CoSe, with an in-plane easy axis. Notably, LiCoSe is a half-metal. These functionalized monolayers exhibit dramatically enhanced ferromagnetism compared to the pristine layer, with $T_{\rm c}$ > 300 K and MAE > 800 $\mu$eV/Co. The coupled alkali atoms amplify the local magnetic moment of Co ions, reinforce ferromagnetic Ruderman-Kittel-Kasuya-Yosida (RKKY) and superexchange couplings, and concurrently weaken the direct antiferromagnetic exchange between Co ions. Furthermore, tensile strain can further elevate the MAE (via band shifting) and increase $T_{c}$ (by strengthening the nearest-neighbor exchange $J_1$). Among them, NaCoSe exhibits the highest MAE and excellent strain-modulated $T_{c}$, rendering it the most promising candidate material. Our results establish alkali-metal decoration as an effective strategy for realizing 2D ferromagnets with high $T_{\rm c}$ and large MAE in tetragonal lattices.