Revisiting the optoelectronic properties of sputtered aluminium-doped zinc oxide: a study combining advanced optical dispersion models

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Abstract Aluminium-doped zinc oxide (AZO) thin films with different aluminium (Al) concentrations were grown by RF-magnetron sputtering with substrate active cooling. Sputtering induced sample heating was aimed to be mitigated by the applied cooling, achieving films with electrical resistivities as low as 3.3 × 10 − 3 Ω ⋅ cm , in the as-deposited state. Subsequently, an annealing treatment was performed to enhance the electrical properties and assess the effect of the Al concentration. The absorption coefficient spectra of zinc oxide (ZnO) exhibits an excitonic absorption contribution to the fundamental absorption that is typically not considered in AZO when determining the optical bandgap. Nevertheless, here we show that this free exciton band remains visible in AZO even at Al concentrations greater than 4 at.%. Additionally, the doping-induced defect states increases the width of tail states. These two factors have a substantial effect on the absorption edge, and thus must be considered with adequate models when attempting to determine the optical bandgap. In this work, we use a recently developed Elliot-based optical dispersion model to accurately determine the optical bandgap, exciton binding energy and Urbach energy of AZO thin films. On the other hand, we assess the infrared free carrier absorption, typically modeled by the Drude dispersion formula, by considering a complex frequency-dependent dynamical resistivity and the polar nature of the ZnO lattice. Normally, the real part of the dynamical resistivity follows a power law dependence and the exponent is assumed to be −1.5 for highly-doped semiconductors. Notwithstanding, here we let this exponent as a free fitting parameter to assess the effect of distinct scattering mechanisms present in sputtered AZO thin films and its dependence with the Al doping concentration. We believe these results can be extended to other degenerated semiconductors and are relevant for the understanding and tailoring of their fundamental optoelectronic properties.