Zinc oxide is an important optoelectronic material, of particular interest due to its wide band gap (E_g ~ 3.3 eV at 300 K), large exciton binding energy (~66 meV) and especially for the variety of methods by which it can be processed. Moreover, ZnO is readily able to alloy with other metals in the oxide form and has a lattice that can facilitate interstitial doping. This gives ZnO a key role in the area of optoelectronics, metal oxide thin films and thin film transistor (TFT) technologies.

We demonstrate that crystalline, epitaxial-like and highly ordered ZnO thin films can be achieved from a precursor liquid at relatively low temperature via spin-coating. The synthesised films are smooth, stoichiometric ZnO with controllable thickness. An iterative layer-by-layer coating schematic is employed to demonstrate the effects of film thickness on structure, morphology as well as the surface and internal defects. Characterisation of the crystallinity, morphology, O-vacancy formation, stoichiometry, surface roughness and thickness variation was determined through X-ray diffraction, scanning and transmission electron and atomic force microscopy, X-ray photoelectron and photoluminescence spectroscopy, and the data of multi-layered ZnO correlated to defect formation and electrical conductivity.

It is imperative that high crystal quality epitaxial-like thin films can be formed from solution processing to compete with physical deposition methods. We demonstrate that iterative spin-coating of deposited ZnO films results in a transition in crystal texture with increasing thickness (number of layers) from the [] m-plane to the [] c-plane. The films attain a c-axis preferential orientation, with no other crystalline peaks present. Results show that the film’s surface morphology was very smooth, with average rms roughness <0.15 nm. Examination of these films also shows the consistency of the surface composition and defect level while highlighting the