Susanne Siebentritt

Record efficiency in chalcopyrite-based solar cells Cu(In,Ga)(S,Se)2 is achieved using a gallium gradient to increase the bandgap of the absorber toward the back side. Although this structure has successfully reduced recombination at the back contact, we demonstrate that in industrial absorbers grown in the pilot line of Avancis, the back part is a source of non-radiative recombination. Depth-resolved photoluminescence (PL) measurements reveal two main radiative recombination paths at 1.04 eV and 1.5–1.6 eV, attributed to two phases of low and high bandgap material, respectively. Instead of a continuous change in the bandgap throughout the thickness of the absorber, we propose a model where discrete bandgap phases interlace, creating an apparent gradient. Cathodoluminescence and Raman scattering spectroscopy confirm this result. Additionally, deep defects associated with the high gap phase reduce the absorber's performance. Etching away the back part of the absorber leads to an increase of one order of magnitude in the PL intensity, i.e., 60 meV in quasi-Fermi level splitting. Non-radiative voltage losses correlate linearly with the relative contribution of the high energy PL peak, suggesting that reducing the high gap phase could increase the open circuit voltage by up to 180 mV.

As Si-based solar cell technologies approach their theoretical efficiency limits, alternative photovoltaic systems, such as tandem solar cells, are gathering increased attention due to their potential to reach higher efficiencies by better use of the solar spectrum. Cu(In,Ga)S2 (CIGS) is a promising material for the top cell due to its large, tunable bandgap energy (Eg), stability, and already established high efficiencies. However, the deficit in open circuit voltage is still large; therefore, an improved understanding of the efficiency losses is required. Scanning electron microscopy cathodoluminescence was used to study the role of the polycrystalline nature for radiative recombination in CIGS samples of varying Cu-content. Considerable differences between neighboring grains were observed in the emission energy and the emission intensity, with significant drops in emission energy at the grain boundaries. Lateral homogeneity in the near band edge (NBE) energy was found to reduce for samples with Cu-poor compositions, with its standard deviation halving (σNBE ∼ 20 meV) compared to the more stoichiometric films (σNBE ∼ 50 meV), which corresponds to an open circuit voltage loss contribution that is nearly an order of magnitude lower. Such inhomogeneities can be attributed mainly to local variations of the Ga concentration. Hence, the differences between the samples could be explained by the different deposition times at elevated temperature allowing for different extents of homogeneity. Thus, Cu-poor films are not only favorable because of lower concentrations of deep defects but also because of reduced bandgap variations.