We quantify recombination losses in the bulk and interfaces for different perovskite compositions and popular charge transport layers.

Copper-zinc-tin-chalcogenide kesterites, Cu(2)ZnSnS(4) and Cu(2)ZnSnSe(4) (CZTS(e)) are ideal candidates for the production of thin film solar cells on large scales due to the high natural abundance of all constituents, a tunable direct band gap ranging from 1.0 to 1.5 eV, a large absorption coefficient, and demonstrated power conversion efficiencies close to 10%. However, Sn losses through desorption of SnS(e) from CZTS(e) at elevated temperatures (above 400 °C) impede the thorough control of film composition and film homogeneity. No robust and feasible fabrication process is currently available. Here we show that understanding the formation reaction of the kesterite absorber is the key to control the growth process and to drastically improve the solar cell efficiency. Furthermore, we demonstrate that this knowledge can be used to simplify the four-dimensional parameter space (spanned by the four different elements) to an easy and robust two-dimensional process. Sufficiently high partial pressures of SnS(e) and S(e) (a) prevent the decomposition reaction of the CZTS(e) at elevated temperatures and (b) introduce any missing Sn into a Sn-deficient film. This finding enables us to simplify the precursor to a film containing only Cu and Zn, whereas Sn and S(e) are introduced from the gas phase by a self-regulating process.

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Time‐resolved photoluminescence (TRPL) is a powerful characterization technique to study carrier dynamics and quantify absorber quality in semiconductors. The minority carrier lifetime, which is critically important for high‐performance solar cells, is often derived from TRPL analysis. However, here it is shown that various nonideal absorber properties can dominate the TRPL signal making reliable extraction of the minority carrier lifetime not possible. Through high‐resolution intensity‐, temperature‐, voltage‐dependent, and spectrally resolved TRPL measurements on absorbers and devices it is shown that photoluminescence (PL) decay times for kesterite materials are dominated by minority carrier detrapping. Therefore, PL decay times do not correspond to the minority carrier lifetime for these materials. The lifetimes measured here are on the order of hundreds of picoseconds in contrast to the nanosecond lifetimes suggested by the decay curves. These results are supported with additional measurements, device simulation, and comparison with recombination limited PL decays measured on Cu(In,Ga)Se2. The kesterite material system is used as a case study to demonstrate the general analysis of TRPL data in the limit of various measurement conditions and nonideal absorber properties. The data indicate that the current bottleneck for kesterite solar cells is the minority carrier lifetime.

Cu 2 ZnSnSe 4 (CZTSe) thin films are grown by coevaporation. Composition depth profiles reveal that a Zn rich phase is present at the CZTSe/Mo interface. Raman measurements on the as grown films are used to study the near surface region and the CZTSe/Mo interface, after mechanically removing the thin film from the Mo coated glass. These measurements provide direct experimental evidence of the formation of a ZnSe phase at the CZTSe/Mo interface. While the Raman spectra at the surface region are dominated by CZTSe modes, those measured at the CZTSe/Mo interface are dominated by ZnSe and MoSe2 modes.