Achieving highly-enhanced UV photoluminescence and its origin in ZnO nanocrystalline films

ZnO is an efficient luminescent material in the UV-range similar to 3.4 eV with a wide range of applications in optical technologies. Sputtering is a cost-effective and relatively straightforward growth technique for ZnO films; however, most as-grown films are observed to contain intrinsic defects which can significantly diminish the desirable UV-emission. In this research the defect dynamics and optical properties of ZnO sputtered films were studied via post-growth annealing in Ar or O-2 ambient, with X-ray diffraction (XRD), imaging, transmission and Urbach analysis, Raman scattering, and photoluminescence (PL). The imaging, XRD, Raman and Urbach analyses indicate significant improvement in crystal morphology and band-edge characteristics upon annealing, which is nearly independent of the annealing environment. The native defects specific to the as-grown films, which were analyzed via PI, are assigned to Zn-i related centers that luminesce at 2.8 eV. Their presence is attributed to the nature of the sputtering growth technique, which supports Zn-rich growth conditions. After annealing, in either environment the 2.8 eV center diminished accompanied by morphology improvement, and the desirable UV-PL significantly increased. The 02 ambient was found to introduce nominal O-i centers while the Ar ambient was found to be the ideal environment for the enhancement of the UV-light emission: an enhancement of similar to 40 times was achieved. The increase in the UV-PL is attributed to the reduction of Zn-i-related defects, the presence of which in ZnO provides a competing route to the UV emission. Also, the effect of the annealing was to decrease the compressive stress in the films. Finally, the dominant UV-PL at the cold temperature regime is attributed to luminescent centers not associated with the usual excitons of ZnO, but rather to structural defects. (C) 2016 The Authors. Published by Elsevier B.V.