Na-Mediated Stoichiometry Control of FeS2 Thin Films: Suppression of Nanoscale S-Deficiency and Improvement of Photoresponse.

Control of the constituent phase and stoichiometry of iron pyrite (FeS2) is a prerequisite for high-performance photovoltaic devices based on this material. If the pyrite contains sulfur-deficiency-related secondary phases which have a metallic character and a high possibility of coexistence in pyrite films, then significant carrier recombination is expected. In this work, the beneficial role of Na in suppressing the formation of nanoscale or amorphous sulfur-deficient secondary phases is reported with experimental evidence, leading to a higher phase purity for solution-processed pyrite films. The potential reduction of charge recombination via these metallic secondary phases results in significant improvements in both the photopotential and photocurrent intensity of Na-modified pyrite films compared with reference samples.