Design strategy and interface chemistry of ageing stable AZO films as high quality transparent conducting oxide

In this work, an attempt has been made to produce high quality Al-doped ZnO (AZO) transparent conductors by pulsed direct current (DC) magnetron sputtering under varied process conditions, namely sputtering power, sputtering pressure, doping level, and deposition time. The idea is to develop stable AZO films with excellent electro-optical properties, which can replace indium tin oxide (ITO) as transparent conducting oxide. The films are deposited on glass and polyethylene terephthalate (PET) substrates and characterized by X-ray diffraction (XRD), Raman spectroscopy, field emission scanning electron microscopy (FESEM), and energy dispersive X-ray spectroscopy (EDS) for material properties. The electronic and optical properties are investigated using UV-Vis-NIR absorption spectroscopy, photoluminescence spectroscopy, four probe resistivity and Hall measurements, which facilitate the design strategy to achieve promising electro-optical properties. AZO films under optimized process conditions possess sheet resistance below 5 Ω/sq. and maximum visible light transmittance close to 90%. The lowest value of electrical resistivity is found to be 2.1 × 10^-4 Ω·cm. The combination of low electrical resistivity and high optical transparency leading to the figure of merit of the order of 10^-2 Ω^-1 is critically dependent on the process conditions of sputtering as well as doping contents. High free carrier concentration in AZO films leads to the Burstein-Moss shift and this observed blue shift of the absorption spectrum as compared to that of ZnO with native defects depends on the doping contents and the process conditions. This work further explores the role of interface chemistry to achieve high stability of AZO films under ambient oxidizing conditions. The adsorption kinetics of cationic rhodamine 6G and anionic methyl orange at AZO surface with varying adsorption sites and ageing studies on the sheet resistance reveal that the excellent stability of AZO films is delicately linked to the process conditions as well as the content of the dopant material used in the preparation of the AZO sputtering targets. The findings of the study confirm that the sheet resistances of selective AZO films undergo no change and fixed at 4.5 Ω/sq. even for ageing period of over six months.