Excitonic and Environmental Screening Effects in Two-Dimensional Janus MSO (M = Ga, In).

In this work, we investigate Janus monolayer MSO (M = Ga, In) systems using the state-of-the-art GW method within the framework of the many-body perturbation theory. Ground-state density functional theory calculations reveal that both the substitution of S atoms with O atoms and the chemisorption of the O atoms on a single side of the MS layer narrow the band gaps and reduce the carrier mobilities. Notably, one-shot GW calculations demonstrate that the GaSO-2 and InSO-1 systems exhibit optimal band gaps for visible light absorption. Based on the Bethe-Salpeter equation, the exciton binding energies of isolated Janus monolayer GaSO-2 and InSO-1 systems are lower than those of their prototype GaS and InS by 0.37 and 0.17 eV, respectively. Further calculations show that the exciton binding energies of the Janus GaSO-2 and InSO-1 systems can be precisely tuned by adjusting their thicknesses and the thicknesses of their substrates. A deep understanding of the mechanisms for tuning the exciton binding energies in Janus GaSO-2 and InSO-1 systems is crucial for the future design of advanced photovoltaic devices.