Importance of Green Density of Nanoparticle Precursor Film in Microstructural Development and Photovoltaic Properties of CuInSe2 Thin Films

We demonstrate here that an improvement in precursor film density (green density) leads to a great enhancement in the photovoltaic performance of CuInSe2 (CISe) thin film solar cells fabricated with Cu-In nanoparticle precursor films via chemical solution deposition. A cold-isostatic pressing (CIP) technique was applied to uniformly compress the precursor film over the entire surface (measuring 3~4 cm2) and was found to increase its relative density (particle packing density) by ca. 20%, which resulted in an appreciable improvement in the microstructural features of the sintered CISe film in terms of lower porosity, reduced grain boundaries, and a more uniform surface morphology. The low-bandgap (Eg=1.0 eV) CISe PV devices with the CIP-treated film exhibited greatly enhanced open-circuit voltage (VOC, from 0.265 V to 0.413 V) and fill factor (FF, from 0.34 to 0.55), as compared to the control devices. As a consequence, an almost 3-fold increase in the average power conversion efficiency, 3.0 to 8.2% (with the highest value of 9.02%), was realized without an anti-reflection coating. A diode analysis revealed that the enhanced VOC and FF were essentially attributed to the reduced reverse saturation current density (j0) and diode ideality factor (n). This is associated with the suppressed recombination, likely due to the reduction in recombination sites such as grain/air surfaces (pores), inter-granular interfaces, and defective CISe/CdS junctions in the CIP-treated device. From the temperature dependences of VOC, it was confirmed that the CIP-treated devices suffer less from interface recombination.