Mn$_2$C MXene Functionalized by Oxygen is a Semiconducting Antiferromagnet and Efficient Visible Light Absorber (2406.01385v1)

Abstract: Manganese-based MXenes are promising two-dimensional materials due to the broad palette of their magnetic phases and the possibility of experimental preparation because the corresponding MAX phase was already prepared. Here, we systematically investigated geometrical conformers and spin solutions of oxygen-terminated Mn$_2$C MXene and performed subsequent many-body calculations to obtain reliable electronic and optical properties. Allowing energy-lowering using the correct spin ordering via supercell magnetic motifs is essential for the Mn$_2$CO$_2$ system. The stable ground-state Mn$_2$CO$_2$ conformation is antiferromagnetic (AFM) one with zigzag lines of up and down spins on Mn atoms. The AFM nature is consistent with the parent MAX phase and even the clean depleted Mn$_2$C sheet. Other magnetic states and geometrical conformations are energetically very close, providing state-switching possibilities in the material. Subsequent many-body GW and Bethe-Salpeter equation (BSE) calculations provide indirect semiconductor characteristics of AFM Mn$_2$CO$_2$ with a fundamental gap of 2.1 eV (and a direct gap of 2.4 eV), the first bright optical transition at 1.3 eV and extremely strongly bounded (1.1 eV) first bright exciton. Mn$_2$CO$_2$ absorbs efficiently the whole visible light range and near ultraviolet range (between 10 - 20%).