Sub-Ablative Femtosecond Laser Modification of the Nonlinear Optical Response of Amorphous TiO2 Thin Films

Femtosecond laser processing has emerged as a promising post-deposition method for tailoring the properties of dielectric thin films, offering localized modification without thermal damage. This study investigates the effect of sub-ablative femtosecond laser irradiation on the nonlinear optical response of a TiO2 single-layer coating deposited on soda-lime glass by electron-beam evaporation. The coating was modified using 35 fs pulses at 800 nm delivered at a repetition rate of 1 kHz and a fluence of 0.083 J/cm2 while varying the number of pulses per spot. The effective nonlinear refractive index (n2,eff) and effective nonlinear absorption coefficient (βeff) were measured using the z-scan technique with femtosecond excitation. The as-deposited TiO2 coating exhibited a negative effective nonlinear refractive index, signifying a self-defocusing nonlinear response, while femtosecond laser irradiation leads to pronounced changes in the effective nonlinear parameters. An increase in the magnitude of both effective nonlinear coefficients and a reversal of the sign of the effective nonlinear refractive index are experimentally observed after irradiation with higher pulse numbers. These findings provide experimental evidence that sub-ablative femtosecond laser processing can be used as a post-deposition tool to control the nonlinear optical response of TiO2 thin films.