The development of highly efficient flexible transparent electrodes (FTEs) supported on polymer substrates is of great importance to the realization of portable and bendable photovoltaic devices. Highly conductive, low-cost Cu has attracted attention as a promising alternative for replacing expensive indium tin oxide (ITO) and Ag. However, highly efficient, Cu-based FTEs are currently unavailable because of the absence of an efficient means of attaining an atomically thin, completely continuous Cu film that simultaneously exhibits enhanced optical transmittance and electrical conductivity. Here, strong two-dimensional (2D) epitaxy of Cu on ZnO is reported by applying an atomically thin (around 1 nm) oxygen-doped Cu wetting layer. Analyses of transmission electron microscopy images and X-ray diffraction patterns, combined with first-principles density functional theory calculations, reveal that the reduction in the surface and interface free energies of the wetting layers with a trace amount (1-2 atom %) of oxygen are largely responsible for the two-dimensional epitaxial growth of the Cu on ZnO. The ultrathin 2D Cu layer, embedded between ZnO films, exhibits a highly desirable optical transmittance of over 85% in a wavelength range of 400-800 nm and a sheet resistance of 11 Ω sq-1. The validity of this innovative approach is verified with a Cu-based FTE that contributes to the light-to-electron conversion efficiency of a flexible organic solar cell that incorporates the transparent electrode (7.7%), which far surpasses that of a solar cell with conventional ITO (6.4%).
Keywords: copper; flexible transparent electrode; organic solar cell; ultrathin film; wetting layer.