Room-temperature deposition of nanocrystalline PbWO4 thin films by pulsed laser ablation

Pulsed laser ablation (PLA) was applied to synthesize nanocrystalline PbWO4 thin films onto glass substrates. The effects of Ar background gas pressure on phase evolution, microstructures and optical characteristics of PbWO4 thin films were investigated in detail. The PLA processes were carried out at room temperature without substrate heating or post-annealing treatment. XRD and HR-TEM results revealed that the PbWO4 thin films are composed of nanocrystalline and amorphous phases. Moreover, the films contained a high density of lattice defects such as twin boundaries and edge dislocations. The crystallite size and crystallinity increased, which were associated with a change in surface morphology as the Ar pressure increased. Reduced tungsten states W5+ or W4+ induced by oxygen vacancies were observed at 10 Pa and the atomic concentration of all constituent element was almost stoichiometric, especially the [Pb]/[W] ratio, which was nearly unity above 50 Pa. The optical energy band-gap was 3.03 eV at 50 Pa and increased to 3.35 eV at 100 Pa, which are narrower than the reported value (4.20 eV). This optical band-gap narrowing could be attributed to localized band-tail states and new energy levels induced by the amorphous structure and inherent lattice defects.