Abstract
The search for new two-dimensional monolayers with diverse electronic properties has attracted growing interest in recent years. Here, we present an approach to construct MA(2)Z(4) monolayers with a septuple-atomic-layer structure, that is, intercalating a MoS2-type monolayer MZ(2) into an InSe-type monolayer A(2)Z(2). We illustrate this unique strategy by means of first-principles calculations, which not only reproduce the structures of MoSi2N4 and MnBi2Te4 that were already experimentally synthesized, but also predict 72 compounds that are thermodynamically and dynamically stable. Such an intercalated architecture significantly reconstructs the band structures of the constituents MZ(2) and A(2)Z(2), leading to diverse electronic properties for MA(2)Z(4), which can be classified according to the total number of valence electrons. The systems with 32 and 34 valence electrons are mostly semiconductors. Whereas, those with 33 valence electrons can be nonmagnetic metals or ferromagnetic semiconductors. In particular, we find that, among the predicted compounds, (Ca,Sr)Ga2Te4 are topologically nontrivial by both the standard density functional theory and hybrid functional calculations. While VSi2P4 is a ferromagnetic semiconductor and TaSi2N4 is a type-I Ising superconductor. Moreover, WSi2P4 is a direct gap semiconductor with peculiar spin-valley properties, which are robust against interlayer interactions. Our study thus provides an effective way of designing septuple-atomic-layer MA(2)Z(4) with unusual electronic properties to draw immediate experimental interest. The discovery of a new two-dimensional van der Waals layered MoSi2N4 material inspires many attentions. Here, the authors report intercalation strategies to explore a much wider range of MA(2)Z(4) family and predict amount of materials accessible to experimental verifications with emergent topological, magnetic or Ising superconductivity properties.