Covalent nitrophenyl diazonium functionalized silicene for spintronics: a first-principles study

Abstract

We predict some novel electronic and magnetic properties of a functionalized silicene sheet by nitrophenyl diazonium (NPD) using first-principles calculations in the framework of density functional theory with dispersion corrections. Our calculations at the HSE06 level show that for the three coverage ratios of NPD considered in this work (i.e., NPD : Si = 1 : 8, 1 : 18 and 1 : 32), spin-polarized electronic structures can be always realized with NPD adsorption although the bandgap decreases upon reducing the NPD coverage ratio. The quasi-localized p_z electrons of Si are identified to be responsible for the ferrimagnetism in these two-dimensional systems. Remarkably, the system with the NPD : Si = 1 : 8 ratio is predicted to be a bipolar magnetic semiconductor. As such, half-metallicity can be realized by applying a gate voltage with reversible spin polarization, making NPD-1/8 a potential candidate for future spintronic applications. This work offers a new tailor-made functionalization approach to realize magnetic semiconducting silicene.