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Tandem solar cells can surpass the limitations of single‐junction devices, promising increased performance due to lower thermalization losses. Even though many research and industrial upscaling efforts are based on perovskite‐Si tandems, all‐thin‐film photovoltaic (PV) devices, for instance with chalcopyrite (CIGSe) and perovskite, can offer many advantages such as significant cost and material savings and access to niche markets like building integrated‐ and flexible PV. However, long‐term stability and outdoor performance of perovskite‐based tandem devices is to this day challenging. This work presents the first data analysis of year‐round outdoor measurements (mpp‐tracked) of a perovskite‐chalcopyrite tandem device with a starting efficiency of about 23.14% before encapsulation. The maximum outdoor performance of the tandem device changed during the period of observation, reaching the peak performance in April and then decreased due to the device degradation. At its maximum outdoor performance, the tandem could reach up to 68% higher instantaneous power output, relative to its single‐junction reference (CIGSe‐SJ). In addition, a quantitative time series performance analysis, exemplary qualitative imaging characterization of the tandem before and after outdoor exposure, is shown. Finally, the possibility of predicting the immediate performance of an all‐thin‐film tandem is verified by using a multiple linear regression model with accuracies generally exceeding 90%. This work presents the first data analysis of year‐round measurements under outdoor conditions of a perovskite‐CIGS tandem solar cell. In addition, the data acquired is used to verify the possibility of predicting the immediate performance of an all‐thin‐film tandem using a multiple linear regression model with accuracies generally exceeding 90%.

We report a route to deposit In2S3 thin films from air-stable, low-cost molecular precursor inks for Cd-free buffer layers in chalcopyrite-based thin film solar cells. Different precursor compositions and processing conditions were studied to define a reproducible and robust process. By adjusting the ink properties, this method can be applied in different printing and coating techniques. Here we report on two techniques, namely spin-coating and inkjet printing. Active area efficiencies of 12.8% and 12.2% have been achieved for In2S3-buffered solar cells respectively, matching the performance of CdS-buffered cells prepared with the same batch of absorbers.

The influence of absorber grain boundaries on the photocurrent transport in chalcopyrite based thin film solar cells has been calculated using a two dimensional numerical model. Considering extreme cases, the variation in red response is more expressed than in one dimensional models. These findings may offer an explanation for the strong influence of buffer layer preparation on the spectral response of cells with small grained absorbers.

The crystallisation of sputter-deposited, amorphous In2O3:H films was investigated. The influence of deposition and crystallisation parameters onto crystallinity and electron hall mobility was explored. Significant precipitation of metallic indium was discovered in the crystallised films by electron energy loss spectroscopy. Melting of metallic indium at ~160 °C was suggested to promote primary crystallisation of the amorphous In2O3:H films. The presence of hydroxyl was ascribed to be responsible for the recrystallization and grain growth accompanying the inter-grain In-O-In bounding. Metallic indium was suggested to provide an excess of free electrons in as-deposited In2O3 and In2O3:H films. According to the ultraviolet photoelectron spectroscopy, the work function of In2O3:H increased during crystallisation from 4 eV to 4.4 eV, which corresponds to the oxidation process. Furthermore, transparency simultaneously increased in the infraredspectral region. Water was queried to oxidise metallic indium in UHV at higher temperature as compared to oxygen in ambient air. Secondary ion mass-spectroscopy results revealed that the former process takes place mostly within the top ~50 nm. The optical band gap of In2O3:H increased by about 0.2 eV during annealing, indicating a doping effect. This was considered as a likely intra-grain phenomenon caused by both (In0)O•• and (OH−)O• point defects. The inconsistencies in understanding of In2O3:H crystallisation, which existed in the literature so far, were considered and explained by the multiplicity and disequilibrium of the processes running simultaneously.