A study of 8 MeV e-beam on localized defect states in ZnO nanostructures and its role on photoluminescence and third harmonic generation

In this article we have explored an effect of electron beam irradiation (EBI) on physical and nonlinear optical properties ZnO thin nano films. Nanostructured ZnO thin films were grown by low cost spray pyrolysis technique. The irradiation dosage has been fixed at 5 kGy, 10kGY, 15 kGy and 20 kGy. The structural investigation by Glancing angle X-Ray Diffractometer (GAXRD) confirms a polycrystalline phase of ZnO with wurtzite structure. The variation in the surface morphology upon EBI has been demonstrated using 2D and 3D Atomic force microscopy (AFM) images. Nanoscope software analysis quantifies the variation in surface roughness and average particle height upon EBI. The defect states created in the films upon irradiation experiments were investigated using UV-visible spectrophotometer, Room temperature Photoluminescence (RTPL), Raman and X-ray photo-electron spectroscopy (XPS). The increase in urbach tail validates the creation of localized defect states in the films The Gaussian fitting on RTPL spectra shows the quenching in the luminescent centers upon irradiation arised as result of recombination of vacancy defects. Phonon confinement model fitting on Raman spectra endorses that shift in the phonon modes observed on irradiation is due to spatial confinement of phonons. The elemental composition and impurity states of the EBI ZnO thin films were studied using XPS spectra. The shift in the binding energy of Zn and O elements infers the electron beam induced changes in the films. The electron beam irradiation has resulted in the increment of third order optical susceptibility chi(3) 3.5 x 10(-4) esu to 8.13 x 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 (CW) laser illumination. The enhanced THG signal investigated using Nd:YAG laser at 1064 nm and 8 ns pulse width shows the promising features of EBI ZnO films for frequency tripling applications.