Computational search for efficient single-photon emitters among the substitutional doping defects in two-dimensional GaSe

Abstract

Single photon emitters (SPE) in the near-infrared (NIR) spectrum range are critical elements in quantum communication technology. We apply here computational methods to reveal local defects in the GaSe monolayer with properties favorable for such SPEs. Based on an educated guess, we selected twelve defects YX in GaSe, where the Y dopant substitutes the X host atom, X = Ga or Se, and Y = C, Si, Ge, N, P, or As. Our calculations show that two defects, NGa, and PGa, are dynamically unstable. For the remaining defects, we apply the linear response GW method and Bethe-Salpeter equation (BSE) to calculate the electronic structure and optical excitation spectra. Some defects are found to have two sharp peaks (occupied and unoccupied) of the density of the electronic states within the band gap. The NSe-, PSe-, and AsSe-defects have intense sharp an optical excitation peak at energies around 0.8 eV (λ = 1550 nm). Analysis of the formation of the BSE eigenstates associated with these peaks suggests that these excitations can cause a narrow zero-phonon line emission. We thus propose the NSe-, PSe-, and AsSe-defects in the GaSe monolayer as promising SPE in NIR region.