The interaction between O2 and ZnO thin films prepared by atomic layer deposition has been investigated by time-dependent second-harmonic generation, by probing the electric field induced by adsorbed oxygen molecules on the surface. The second-harmonic generated signal decays upon laser exposure due to two-photon assisted desorption of O2. Blocking and unblocking the laser beam for different time intervals reveals the adsorption rate of O2 onto ZnO. The results demonstrate that electric field induced second-harmonic generation provides a versatile non-contact probe of the adsorption kinetics of molecules on ZnO thin films.
It is demonstrated that as-grown e-beam deposited SiOx thin films on fused silica substrates show a second-order nonlinear response that is dependent on film thickness. Using a Maker fringes method the effective nonlinear coefficient for a SiO thin film is estimated to be comparable to that of crystalline quartz. Variation of process parameters has been used to investigate the origin of the nonlinear response. The second-harmonic signal is very sensitive to annealing of the film and can be totally removed by annealing at a few hundred degrees. It is also demonstrated that a retarding grid that traps charged particles between the crucible and the sample reduces the nonlinear signal from a SiO thin film significantly. It is suggested that oriented dipoles arise during deposition due to a negatively charged film from oxygen ions, thus, resulting in a non-centrosymmetric film. Finally, using e-beam lithography, well-defined nonlinear 2D structures can be synthesized, thus opening the door to a new and practical way to create nonlinear structures for planar waveguide technology.
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