Facile control of giant green-emission in multifunctional ZnO quantum dots produced in a single-step process: femtosecond pulse ablation

Controlling both UV and visible emissions in ZnO quantum dots (QDs) poses a significant challenge due to the inherent introduction of defects during the growth process. We have refined the photoluminescence (PL) emission characteristics of ZnO QDs through a single-step, reagent-free femtosecond pulsed laser ablation in liquid (fs-PLAL) technique. The ratio of the near band edge (NBE) to deep-level emission (DLE), which determines the shape of the QDs' optical emission spectrum, is precisely controlled by the ablation laser pulse parameters-namely, pulse energy and temporal duration. Having established our ability to control the optical properties, we have investigated the mechanisms and physics involved in controlling optical emission. The key highlight of the work is that ablation with a fs-pulse induces substantial defect states without altering the particle size, with the extent of the effect being dependent on the pulse energy and pulse duration. The spectroscopic techniques inducing Raman spectroscopy, excitation power dependent PL and transient PL study provided deep insight into the PL emission properties of these similarly sized QDs. The improved DLE in these laser-ablated QDs is explained by a surface-recombination-layer approximation process employing steady-state and transient PL. Moreover, we have demonstrated the applicability of green emission for pH sensing within a linear range of 7-10 and highlight the inherent antibacterial properties of these QDs.