Binder-Free Cu–In Alloy Nanoparticles Precursor and Their Phase Transformation to Chalcogenides for Solar Cell Applications

A low-cost, nonvacuum fabrication route for CuInSe2 and CuInS2 thin films is presented. To produce these films, binder-free colloidal precursors were prepared using Cu–In intermetallic nanoparticles that were synthesized via a chemical reduction method. The Cu–In alloy precursor films were transformed to CuInSe2 and CuInS2 by reactive annealing in chalcogen-containing atmospheres at atmospheric pressure. The as-synthesized nanoparticles and the annealed films were characterized by X-ray diffraction, transmission electron microscopy, scanning electron microscopy, energy dispersive X-ray spectrometry, electron probe X-ray microanalysis, Raman spectroscopy, and Auger electron spectroscopy depth profile measurements to elucidate the phase evolution pathway and the densification mechanism of the Cu–In–Se–S system. Solar cell devices made with CuInSe2 and CuInS2 absorbing layers exhibited power conversion efficiencies of 3.92% and 2.28%, respectively. A comparison of the devices suggested that the microstructure of the absorbing layer had a greater influence on the overall photovoltaic performance than the band gap energy. A diode analysis on the solar cell devices revealed that the high saturation current density and diode ideality factor caused lower open-circuit voltages than would be expected from the band gap energies. However, the diode analysis combined with the microstructural and compositional analysis offered guidance about how to improve the photovoltaic performance of these devices.