Approaching physical limits of ZnO:Al film performance for application in photovoltaics

ZnO:Al films which combine high optical transmittance in the visible, maximum carrier mobility (mu), moderate free electron densities (Ne) and high surface roughness are of special interest for application as transparent front electrode in thin film solar cells.
Present work focuses on systematic investigation of ZnO:Al films grown by reactive magnetron sputtering, a cost-efficient deposition method, using metal Zn-Al alloy targets with a wide range of Al target concentrations (c_Al). The observed dependence of the mobility on Ne is discussed in the framework of ionized impurity scattering and clustering as well as grain boundary limited transport which predicts a fundamental physical limit of mu. Precise control of growth parameters results in high quality polycrystalline and epitaxial ZnO:Al films exhibiting optimum mobility values (>45 and >55 cmK/Vs, respectively) approaching the upper limit set by ionized impurity scattering. A combination of ion beam analysis for Al quantification in the film with Hall effect measurements shows that above a critical Al concentration (~2.5 at.%) further Al enrichment in the films with increasing substrate temperature leads to deterioration of electrical properties. This approach also enables estimation of the fraction of electrically active Al in the ZnO matrix, which is rarely reported in a quantitative and systematic manner. It is shown that the Al donor activation in the ZnO:Al films does not exceed 40%.