First-principles modeling of 3d-transition-metal-atom adsorption on silicene: a linear-response DFT + U approach

By employing DFT  +  U calculations with the linear response method, we investigate the interactions between various 3d transition-metal atoms (Cr, Mn, Fe, Co) and silicene. In the cases of two-dimensional (2D) FeSi2 and CoSi2, the metal atoms tend to penetrate into the silicene layer. While CoSi2 is non-magnetic, FeSi2 exhibits a total magnetic moment of 2.21 μ(B)/cell. Upon the examination of 2D MSi6, a trend in anti-ferromagnetic (AFM) favorability in the z-direction is observed according to our DFT  +  U calculations. In the ferromagnetic (FM) states (less stable), each primary unit cell of CrSi6, MnSi6, and FeSi6 possesses different levels of total magnetization (4.01, 5.18, and 2.00 μ B/cell, respectively). The absolute magnetization given by AFM MSi6 structures varies in the range of 5.33-5.84 μ(B)/cell. A direct band gap in AFM MnSi6 (0.2 eV) is predicted, while the metastable FM FeSi6 structure has a wider band gap (0.85 eV). Interestingly, there are superexchange interactions between metal atoms in the MSi6 systems, which result in the AFM alignments.