Giant Stokes shift for charged vacancies in monolayer SnS

Abstract

We perform first-principles density-functional theory calculations to determine the equilibrium defect structures, formation energies, charge transition levels, and electronic structures of Sn and S vacancies in monolayer SnS. Both Sn and S vacancies exhibit multiple charge transition levels and in-gap defect states, indicating that they may be stable in different charge states depending on the Fermi level in the system. Depending on the charge state of the vacancy, the easily distorted SnS lattice undergoes different relaxations, and in some cases, symmetry-breaking reconstructions, creating defect states within the gap that electrons can occupy at a lower energetic cost. Due to significant atomic relaxations between the equilibrium defect structures in different charge states, optical charge transitions involving both types of vacancies exhibit significant Stokes shifts of over 1 eV, which may provide opportunities for increased efficiency in light emission diode, solar cell, and solar concentrator applications.