Enhancing Reverse Saturable Absorption in SnS₂ Nanosheets by Plasma Treatment

The knowledge concerning the influence of defects on the nonlinear optical response of materials remains scarce so far. In this work, we have successfully introduced defects into SnS₂ nanosheets by plasma treatment and shown that a defect generation is an effective approach to significantly improve the reverse saturable absorption of SnS₂. The SnS₂ nanosheets treated with Ar plasma for 40 s exhibit a nonlinear absorption coefficient (β₀) as large as (2.9 ± 0.12) × 10⁴ cm GW^-1, which is nearly 9 times that of the untreated sample. The influence of Ar-plasma-treatment time, defect type, and defect number on the nonlinear absorption of SnS₂ nanosheets are also studied. Structure and spectroscopy characterization confirms the introduction of S and Sn vacancies with Ar-plasma etching. Surface photovoltage spectroscopy and density functional theory calculation indicate that S vacancies can induce in-gap states in the band gap. These in-gap states act as intermediate states for the successive absorption of photons during femtosecond laser excitation (namely, excited-state absorption). In contrast, Sn defects cannot lead to in-gap states and have a limited contribution to nonlinear absorption. Our result would provide a promising way to improve optical nonlinearities.