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Nanosecond near resonant excitation in As50S50 thin films leads to strongnonlinear optical response, i.e. nonlinear absorption coefficient up to 4 x 106cm/GW and nonlinear refractive index of 8.5 cm2/GW, both of which is thestrongest ever reported in amorphous semiconductors. We propose a five-levelenergy model to explain such effect which indicates that nonlinear process isreverse saturable absorption in nature, mediated by excited state absorptionfrom triplet-triplet transition. On the other hand, observation of negativenonlinear refractive index reveals the occurrence of self-defocusing effect.Finally, benefitting from the strong nonlinear response, we demonstrate apromising application of As50S50 thin films as an optical limiter foroptoelectronic sensors.

Near resonant nanosecond laser driven nonlinear optical response in As50S50 thin films