Rational design of a two-dimensional high-temperature ferromagnet from HCP cobalt

• Published in: Physical chemistry chemical physics : PCCP 2024-08, Vol.26 (34), p.22715-22725
• Main Authors: Wang, Bo-Jing, Hou, Yi-Na, Jin, Chen-Dong, Zhang, Hu, Wang, Jiang-Long, Gong, Peng-Lai, Lian, Ru-Qian, Shi, Xing-Qiang, Wang, Rui-Ning
• Format: Article
• Language: English
• Subjects: Cobalt; Curie temperature; Ferromagnetism; High temperature; Insulation; Magnetization; Molecular dynamics; Monte Carlo simulation; Room temperature; Thickness
• ISSN: 1463-9076; 1463-9084; 1463-9084
• DOI: 10.1039/d4cp01390e

Cobalt has the highest Curie temperature ( T c ) among the elemental ferromagnetic metals and has a hexagonal close-packed (HCP) structure at room temperature. In this study, HCP Co was thinned to the thickness of several ( n ) unit cells along the c -axis and then passivated by halogen atoms, thus being named Co 2 n X 2 (X = F, Cl, Br and I). For Co 2 X 2 and Co 3 X 2 , all of them are not only kinetically but also thermodynamically stable from the viewpoint of the phonon spectra and molecular dynamics. Similar to HCP Co, two-dimensional (2D) Co 2 F 2 , Co 2 Cl 2 and Co 3 X 2 (X = Cl, Br and I) are still ferromagnetic metals within the Stoner model but Co 2 X 2 (X = Br and I) is a ferromagnetic half-metal with the coexistence of the metallic behavior for one spin and the insulating behavior for the other spin. Taking into account the spin-orbital coupling (SOC), the easy-magnetization axis is within the plane where the magnetization is isotropic, making it look like a 2D XY magnet. Applying a critical biaxial strain could lead to an easy-magnetization axis changing from the in-plane to the out-of-plane direction. Finally, we use classical Monte Carlo simulations to estimate the Curie temperature ( T c ) which is as high as 957 and 510 K for Co 2 F 2 and Co 2 Cl 2 , respectively, because of the strong direct exchange interaction. Different from being obtained by mechanical or liquid exfoliation from van der Waals layered structures, our study opens up new possibilities to search for novel 2D ferromagnets from the elemental ferromagnets and provides opportunities for realizing realistic ultra-thin spintronic devices. A novel family of 2D high-temperature ferromagnets (cobalt halides consisting of two or three close-packed Co layers with the surface coated with halogen atoms) with an in-plane easy-magnetization axis is designed using the first-principles method.