Effects of oxygen partial pressure and annealing on dispersive optical nonlinearity in NiO thin films.

We report annealing induced sign reversal of dispersive optical nonlinearity in ion beam sputtered NiO thin films deposited at 30% and 70% oxygen partial pressures. In the Ultraviolet-visible spectra of the samples, the transmission peak corresponding to d-d transitions is observed near 2 eV. A shift in this peak towards higher energy was observed when the same films were annealed at 523 K. The near resonant photoinduced transitions produced giant nonlinear optical susceptibilities of both third- and fifth- orders when the annealed film was irradiated by a continuous wave 632.8 nm He-Ne laser. The role of the thermo-optic effect has been examined critically. Experimental studies further reveal that the oxygen partial pressure influences the growth direction of the grains in the thin films. The well known Z-scan experimental procedure has been followed for measurements of optical nonlinearities in all the NiO films. The nonlinear refractive indices of both the as-deposited and annealed NiO thin films are defined in terms of the thermo-optic coefficients (dn/dT)T=T0 and (d²n/dT²)T=T0. [ABSTRACT FROM AUTHOR]