Effect of capping ligands on the optical properties and electronic energies of iron pyrite FeS2 nanocrystals and solid thin films

In this work, the optical and electronic properties of iron pyrite FeS2 nanocrystals and solid thin films with various capping ligands were systematically investigated by UV-Vis-NIR absorption spectroscopy, cyclic voltammetry and current density-voltage characteristic measurements. The iron pyrite nanocrystals with various ligands have an indirect band gap of around 1.05 eV and broad absorption spanning into the near-infrared region, exhibiting favorable optical properties for their photovoltaic applications. The electron affinities and ionization potentials of FeS2 nanocrystals determined through cyclic voltammetry measurements show strong ligand dependence. An energy level shift of up to 190 meV was obtained among the pyrite nanocrystals capped with the ligands employed in this work. The iron pyrite nanocrystal films capped with iodide and 1,2-ethanedithiol exhibit the largest band edge energy shift and conductivity, respectively. Our results not only provide several useful optical and electronic parameters of pyrite nanocrystals for their further use in optoelectronic devices as active layers and/or infrared optical absorption materials, but also highlight the relationship between their surface chemistry and electronic energies.