Magnetically driven anisotropic structural changes in the atomic laminateMn2GaC

Abstract

Inherently layered magnetic materials, such as magnetic ${M}_{n+1}A{X}_{n}$ (MAX) phases, offer an intriguing perspective for use in spintronics applications and as ideal model systems for fundamental studies of complex magnetic phenomena. The MAX phase composition ${{M}_{n}}_{+1}A{X}_{n}$ consists of ${M}_{n+1}{X}_{n}$ blocks separated by atomically thin $A$-layers where $M$ is a transition metal, $A$ an A-group element, $X$ refers to carbon and/or nitrogen, and $n$ is typically 1, 2, or 3. Here, we show that the recently discovered magnetic $\mathrm{M}{\mathrm{n}}_{2}\mathrm{GaC}$ MAX phase displays structural changes linked to the magnetic anisotropy, and a rich magnetic phase diagram which can be manipulated through temperature and magnetic field. Using first-principles calculations and Monte Carlo simulations, an essentially one-dimensional (1D) interlayer plethora of two-dimensioanl (2D) Mn-C-Mn trilayers with robust intralayer ferromagnetic spin coupling was revealed. The complex transitions between them were observed to induce magnetically driven anisotropic structural changes. The magnetic behavior as well as structural changes dependent on the temperature and applied magnetic field are explained by the large number of low energy, i.e., close to degenerate, collinear and noncollinear spin configurations that become accessible to the system with a change in volume. These results indicate that the magnetic state can be directly controlled by an applied pressure or through the introduction of stress and show promise for the use of $\mathrm{M}{\mathrm{n}}_{2}\mathrm{GaC}$ MAX phases in future magnetoelectric and magnetocaloric applications.