Excimer laser deposited CuO and Cu₂O films with third-order optical nonlinearities by femtosecond z-scan measurement

By controlling the oxygen pressure, single-phase CuO and Cu₂O thin films have been obtained on quartz substrates using a pulsed laser deposition technique. The structure properties and linear optical absorption of the films were characterized by X-ray diffraction and UV-VIS spectroscopy. By performing z-scan measurements using a femtosecond laser (800 nm, 50 fs), the real and imaginary parts of the third-order nonlinear susceptibility, Reχ⁽³⁾ and Imχ⁽³⁾, of the films were determined. Both CuO and Cu₂O films exhibited large optical nonlinearities, which is comparable to those in some representative semiconductor films such as ZnO and GaN films using femtosecond laser excitation. Compared with Cu₂O films, the CuO films showed larger third-order nonlinear optical effects under off-resonance excitation. Furthermore, the mechanisms of the optical nonlinearities in CuO and Cu₂O films are explained in the main text. It was suggested that the reasons of the difference in their nonlinear refractive effects may be related to the different electronic structure in CuO and Cu₂O materials.