Cooperative two-photon effects in chalcogenide photoresists

Photosensitive chalcogenide glasses are very promising materials for pulsed holography, pulsed photolithography and pulsed optical information recording due to their exceptional sensitivity to pulsed light excitation. We present a comprehensive study of the dynamics of the pulse photoresponse of 0.3-1.0 μm thick chalcogenide glassy As₅₀Se₅₀ thin films using a transient-grating method. Both the decrease of transparency and a change of the dissolution rate were recorded after single Nd:YAG and ArF laser pulse and about (1-5)×1000 times larger energy was necessary to obtain the same changes using CW radiation. We show that when excited by a short laser pulse, two different time scales behavior and different intensity dependence of short- and long-time scale signals are present: the short-time signal behaves linearly with the input power but the long-time signal behaves quadratically with the input power. Such behavior reflects a fast electronic process followed by a slow structural rearrangement (the after-pulse effect). The obtained data indicate that the strong increase of photosensitivity following a short intense pulsed light excitation is due to a two-photon effect that aids the process of structural rearrangement as when two photons weaken or break the neighboring bonds, the probability of structural transformation increases significantly.