Covalent photofunctionalization and electronic repair of 2H-MoS2via nitrogen incorporation

Abstract

A route towards covalent functionalization of chemically inert 2H-MoS₂ exploiting sulfur vacancies is explored by means of (TD)DFT and GW/BSE calculations. Functionalization via nitrogen incorporation at sulfur vacancies is shown to result in more stable covalent binding than via thiol incorporation. In this way, defective monolayer MoS₂ is repaired and the quasiparticle band structure as well as the remarkable optical properties of pristine MoS₂ are restored. Hence, defect-free functionalization with various molecules is possible. Our results for covalently attached azobenzene, as a prominent photo-switch, pave the way to create photoresponsive two-dimensional (2D) materials.