Janus-functionalization induced magnetism and improved optoelectronic properties in two-dimension silicene and germanene: insights from first-principles calculations

Abstract In this paper, the structural stability, optoelectronic and magnetic properties of silicene and germanene monolayers Janus-functionalized simultaneously with hydrogen and alkali metal atoms (Li and Na) are investigated systematically by using first-principles calculations. The calculated results of the ab initio molecular dynamics simulations and cohesive energies indicate that all functionalized cases have good stability. Meanwhile, the calculated band structures show that all functionalized cases retain the Dirac cone. Particularly, the cases of HSiLi and HGeLi show metallic nature but retain semiconducting characteristics. Besides, the above two cases can present obvious magnetic behavior and their magnetic moments are mainly originated by the p states of Li atom. The metallic property and weak magnetic character can also be found in the case of HGeNa. While the case of HSiNa exhibits the nonmagnetic semiconducting property with a indirect band gap of 0.42 eV calculated by the HSE06 hybrid functional. It is also found that the optical absorption in the visible region of silicene and germanene can be effectively improved by Janus-functionalization. Specifically, a high optical absorption of visible light in an order of 4.5 × 10 5 cm −1 can be observed in the case of HSiNa. Furthermore, in the visible region, the reflection coefficients of all functionalized cases can also be enhanced. These results demonstrate the feasibility of the Janus-functionalization method to modulate the optoelectronic and magnetic properties of silicene and germanene, expanding their potential applications in the fields of spintronics and optoelectronics.