KEYWORDS: Perovskite, Tandem solar cells, Temperature metrology, External quantum efficiency, Solar cells, Data modeling, Silicon, Absorption, Solar energy, Glasses
Perovskite/silicon tandem solar cells promise power conversion efficiencies (PCE) beyond the thermodynamic limit of single-junction devices. This potential has been unveiled via several champion devices, however, their actual outdoor performance is yet to be investigated. Here, we fabricate 25 %-efficient two-terminal (2T) monolithic perovskite/silicon tandem solar cells and test them outdoors to reveal the characteristics of these devices specifically in hot and sunny climates, which are the ideal locations to operate such efficient photovoltaic devices. In this article, we summarize our observation on the perovskite/silicon tandem solar cells under actual operational conditions and discuss the lessons we take from our interpretations.
Mixed halide, mixed cation lead perovskite films have been demonstrated to benefit tremendously from the addition of Cs and Rb into the perovskite formulation, resulting in high performance, enhanced reproducibility and stability. However, the root cause of these effects in these complicated systems is not well understood. We address the above challenge by tracking in situ the solidification of perovskite precursors during solution-casting using time-resolved grazing incidence wide-angle X-ray scattering (GIWAXS). In doing so, we can directly link the formation or suppression of different crystalline phases to the presence of Cs and/or Rb. In the absence of these elements, the multi-component perovskite film is inherently unstable, phase segregating into a solvated MAI-rich phase and a FABr-rich phase. Adding even one of the two (Cs or Rb) is shown to alter the solidification quite dramatically, promoting different solidification pathways. Importantly, the addition of both components in the optimal ratio can drastically suppress phase segregation and promotes the spontaneous formation of the desired perovskite phase. This result is also confirmed by elemental mapping of organic cations (FA+, MA+) and halide anions (I-, Br-) via time-of-flight secondary ion mass spectroscopy (ToF-SIMS). Perovskite precursors with an optimal combination of additives (7% Cs, 3% Rb) result in solar cells with 20.1% power conversion efficiency (PCE), outperforming formulation excluding Cs and Rb (PCE=14.6%). We propose that the synergistic effect is due to the collective benefits of Cs and Rb on the formation kinetics of the perovskite phase, and on the halides redistribution throughout the film. Importantly, our study points to new design rules for tuning the crystallization pathway of multi-component hybrid perovskites.
Cesium lead halide perovskite materials have recently attracted attention in view of their optical and electronic properties which make them excellent candidates for potential applications in lasers, light emitting diodes and photodetectors. In this work, we provide the experimental and theoretical evidence for sequential photon absorption/re-emission in CsPbBr3 perovskite microwires. Using two-photon excitation, we recorded PL lifetimes and emission spectra as a function of the lateral distance between PL excitation and collection positions along the microwire, with separations exceeding 100 µm. As the propagation length increases, the PL spectrum develops a new emission peak that is red-shifted by 20 nm from the main emission and is accompanied by the appearance of the well-resolved rise times in the PL kinetics. We undertake quantitative modeling that accounts for bimolecular recombination and photon recycling within the microwire waveguide, and find that it is sufficient to account for the observed decay modifications. The model relies on a high radiative efficiency in CsPbBr3 perovskite microwires to explain the photon recycling observed. Such findings provide crucial information about the potential impact of photon recycling and waveguide trapping on optoelectronic properties of cesium lead halide perovskite materials
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