Direct evidence for grain boundary passivation in Cu(In,Ga)Se2 solar cells through alkali-fluoride post-deposition treatments

05 2019

Direct evidence for grain boundary passivation in Cu(In,Ga)Se2 solar cells through alkali-fluoride post-deposition treatments

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The properties and performance of polycrystalline materials depend critically on the properties of their grain boundaries. Polycrystalline photovoltaic materials - e.g. hybrid halide perovskites, copper indium gallium diselenide (CIGSe) and cadmium telluride - have already demonstrated high efficiencies and promise cost-effective electricity supply. For CIGSe-based solar cells, an efficiency above 23% has recently been achieved using an alkali-fluoride post-deposition treatment; however, its full impact and functional principle are not yet fully understood. Here, we show direct evidence for the passivation of grain boundaries in CIGSe treated with three different alkali-fluorides through a detailed study of the nanoscale optoelectronic properties. We determine a correlation of the surface potential change at grain boundaries with the open-circuit voltage, which is supported by numerical simulations. Our results suggest that heavier alkali elements might lead to better passivation by reducing the density of charged defects and increasing the formation of secondary phases at grain boundaries.


The use of polycrystalline materials for photovoltaic (PV) energy conversion promises fast fabrication and high cost-savings potential. However, the properties of polycrystalline semiconductors are frequently dominated by the properties of grain boundaries (GBs). In recent years, thin-film solar cells based on polycrystalline cadmium telluride (CdTe), Cu(In,Ga)Se2 (CIGSe), and lead-halide perovskite absorbers have surpassed the barrier of 22% power conversion efficiency. These outstanding efficiencies have been achieved through tedious materials and device optimization. It is obvious that in such high-efficiency devices the GBs are not leading to strong carrier recombination. In fact, some of the strategies for efficiency improvement have subsequently been identified to passivate GBs, e.g. a cadmium-chloride (CdCl2) treatment in CdTe solar cells and a polymer treatment in perovskite solar cells. For CIGSe solar cells an alkali-fluoride (AlkF) post-deposition treatment (PDT) has recently led to a significant increase in the efficiencies. Indeed, it has been reported that for a potassium-fluoride (KF)-PDT the electronic properties of the GBs are beneficially modified. However, a full understanding of the role of GBs in CIGSe is still lacking, especially in view of the heavier AlkF-PDT using rubidium-fluoride (RbF) and cesium-fluoride (CsF), which have led to higher record efficiencies in the last 2 years.

Most of the studies investigating the role of GBs in CIGSe were performed on material without any AlkF-PDT. The only alkali elements present in the absorber were those diffusing from the soda-lime glass substrate, mainly sodium (Na). Compositional studies at atomic level using atom probe tomography (APT) indicated Na accumulation at the GBs. More recent studies, where a KF-PDT was applied indicate also accumulation of K at GBs. As a consequence of the relative concentrations of the different alkali elements at GBs and in the grain interior, several effects have been observed, including Cu depletion, In and Se accumulation at GBs, a diminished downwardand increased upward band bending at GBs, increase or decreaseof carrier concentration, and an impact on the GB recombination velocity. A similar range of observations has been reported for RbF-PDT. The detailed composition, chemistry, and microstructure at GBs leads to different GB and possibly also bulk properties, explaining discrepancies in the literature. Different models have been suggested to explain the properties of GBs, however, there is no agreement about the relevance of the electronic properties of GBs for the device performance.

We present a comprehensive Kelvin probe force microscopy (KPFM) study of the electronic GB properties in CIGSe deposited by co-evaporation and compare the effect of KF-, RbF-, and CsF-PDT. A statistical analysis of more than 240 GBs shows distinct differences of the potential variation across the GBs between the samples. To isolate the effect of the different AlkF-PDTs, we use nominally identical CIGSe absorbers grown with the same processing conditions. To understand the impact of GBs on the device performance, we perform three-dimensional (3D) device simulations considering different GB electronic properties. Our results indicate that GBs exhibiting downward band bending (i.e. a hole transport barrier) have a negative impact on device performance. We also find that an optimized AlkF-PDT can lead to a passivation effect at GBs.

Full Article: https://www.nature.../s41467-019-11996-y

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