Electronic and Excitonic Properties of MSi₂Z₄ Monolayers

Abstract

MA₂ Z₄ monolayers form a new class of hexagonal non-centrosymmetric materials hosting extraordinary spin-valley physics. While only two compounds (MoSi₂ N₄ and WSi₂ N₄ ) are recently synthesized, theory predicts interesting (opto)electronic properties of a whole new family of such two-dimensional (2D) materials. Here, the chemical trends of band gaps and spin-orbit splittings of bands in selected MSi₂ Z₄ (M = Mo, W; Z = N, P, As, Sb) compounds are studied from first-principles. Effective Bethe-Salpeter-equation-based calculations reveal high exciton binding energies. Evolution of excitonic energies under external magnetic field is predicted by providing their effective g-factors and diamagnetic coefficients, which can be directly compared to experimental values. In particular, large positive g-factors are predicted for excitons involving higher conduction bands. In view of these predictions, MSi₂ Z₄ monolayers yield a new platform to study excitons and are attractive for optoelectronic devices, also in the form of heterostructures. In addition, a spin-orbit induced bands inversion is observed in the heaviest studied compound, WSi₂ Sb₄ , a hallmark of its topological nature.