Analysis of Hazy Ga- and Zr-Co-Doped Zinc Oxide Films Prepared with Atmospheric Pressure Plasma Jet Systems

Co-doped ZnO thin films have attracted much attention in the field of transparent conductive oxides (TCOs) in solar cells, displays, and other transparent electronics. Unlike conventional single-doped ZnO, co-doped ZnO utilizes two different dopant elements, offering enhanced electrical properties and more controllable optical properties, including transmittance and haze; however, most previous studies focused on the electrical properties, with less attention paid to obtaining high haze using co-doping. Here, we prepare high-haze Ga- and Zr-co-doped ZnO (GZO:Zr or ZGZO) using atmospheric pressure plasma jet (APPJ) systems. We conduct a detailed analysis to examine the interplay between Zr concentrations and film properties. UV-Vis spectroscopy shows a remarkable haze factor increase of 7.19% to 34.8% (+384%) for the films prepared with 2 at% Zr and 8 at% Ga precursor concentrations. EDS analysis reveals Zr accumulation on larger and smaller particles, while SIMS links particle abundance to impurity uptake and altered electrical properties. XPS identifies Zr mainly as ZrO2 because of lattice stress from Zr doping, forming clusters at lattice boundaries and corroborating the SEM findings. Our work presents a new way to fabricate Ga- and Zr-co-doped ZnO for applications that require low electrical resistivity, high visible transparency, and high haze.