Unusual Optoelectronic Properties of Hydrogenated Bilayer Silicene: From Solar Absorber to Light-emitting Diode Applications

Silicon is arguably the greatest electronic material, but not so good an optoelectronic material. By employing first-principles calculations and cluster-expansion approach, we discover that hydrogenated bilayer silicene (BS) shows promising potential as new optoelectronic materials. Most significantly, hydrogenation will covert the intrinsic BS, a strongly indirect semiconductor, into a direct-gap semiconductor with a widely tunable band gap. At low hydrogen concentrations, four ground states of single- and double-side hydrogenated BS are characterized with dipole-allowed direct (or quasidirect) band gaps in the desirable range from 1 to 1.5 eV, suitable for solar applications. At high hydrogen concentrations, three well-ordered double-side hydrogenated BS structures exhibit direct (or quasidirect) band gaps in the range of red, green, and blue colors, respectively, affording white light emitting diodes. Our findings open a door to the search of new silicon-based light-absorption and light-emitting materials for earth-abundant high-efficiency optoelectronic applications.