Emergence of a Magnetic Semiconducting Phase in Hydrogenated Two-Dimensional SiGe Random Alloys

Two-dimensional (2D) group-IV materials are promising for spintronics due to their silicon compatibility and tunable properties. In this work, we investigate the structural, electronic, magnetic, and optical properties of semi-hydrogenated 2D SiGe random alloys—where hydrogen atoms saturate only one side of the atomic plane—using density functional theory and many-body perturbation theory (GW0). Substitutional disorder is modeled via representative high-symmetry configurations introduced by Baldereschi and co-workers to enable quasiparticle and optical simulations in large supercells. We demonstrate that these semi-hydrogenated alloys possess an intrinsic magnetic semiconducting ground state, arising from the electronic structure of the system, with an integer magnetic moment of 1μB per primitive cell. The spin-resolved electronic structure features nearly flat frontier bands and a finite energy gap, which is significantly renormalized by quasiparticle corrections while maintaining robust spin polarization. These properties remain remarkably stable across different realizations of chemical disorder and over a wide range of alloy compositions considered in this work. Optical spectra calculated within the random phase approximation reveal a composition-dependent red-shift of the low-energy onset in the imaginary part of the dielectric function, consistent with the evolution of the quasiparticle electronic structure and the persistence of flat spin-polarized frontier bands. Our findings establish semi-hydrogenated 2D SiGe random alloys as a resilient model platform to explore interaction-driven magnetism in disordered two-dimensional systems, while simultaneously offering realistic prospects for spintronic and magneto-optoelectronic applications in the presence of chemical disorder.