Mn2C MXene functionalized by oxygen is a semiconducting antiferromagnet and an efficient visible light absorber

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 Mn₂C 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 Mn₂CO₂ system. The stable ground-state Mn₂CO₂ conformation is antiferromagnetic (AFM) 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 Mn₂C 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 Mn₂CO₂ 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 bound (1.1 eV) first bright exciton. Mn₂CO₂ absorbs efficiently the whole visible light range and near ultraviolet range (between 10 and 20%).