The structural, optical, morphological and nonlinear optical properties of Cu:ZnO spraycoated films are studied. The surface morphology of Cu:ZnO thin films turned out to be homogenous, crack free and well covered with pea-shaped grains. The peak shift observed in the xray photoelectron spectroscopy spectra of the Cu:ZnO thin films infers the defect states present in the films. The satellite peak observed at 939.9 eV for Cu2P core-level spectra confirms the +2 oxidation state of Cu in the films. The formation of additional defect levels in the nanostruc-tures upon Cu doping was investigated using photoluminescence (PL) and Raman spectroscopy studies. The luminescent centers in the violet, blue and green spectral region were observed. The most prominent emission was centered at the blue color center for 5% Cu:ZnO thin films. The enhancement in the PL emission intensity confirms the increase in the defect state density upon Cu doping. The shifting of the UV emission peak to the visible region validates the increase in the nonradiative recombination process in the films upon doping. The phonon modes observed in Raman analysis around 439, 333 and 558 cm −1 confirm the improvement in the crystallinity and formation of defect states in the films. X-ray diffraction reveals that the deposited films are of single-phase wurtzite ZnO structure with preferential growth orientation parallel (0 0 2) to the C-axis. The thirdorder optical susceptibility χ(3) has been increased from 3.5 × 10 −4 to 2.77 × 10 −3 esu due to the enhancement of electronic transition to different defect levels formed in the films and through local heating effects arising due to continuous wave laser illumination. The enhanced third harmonic generation signal investigated using a Nd:YAG laser at 1064 nm and 8 ns pulse width shows the credibility of Cu:ZnO films in frequency tripling applications.

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