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Hybrid lead halide perovskites are promising materials for future photovoltaics applications. Their spectral response can be readily tuned by controlling the halide composition, while their stability is strongly dependent on the film morphology and on the type of organic cation used. Mixed cation and mixed halide systems have led to the most efficient and stable perovskite solar cells reported, so far they are prepared exclusively by solutionprocessing. This might be due to the technical difficulties associated with the vacuum deposition from multiple thermal sources, requiring a high level of control over the deposition rate of each precursor during the film formation. In this report, thermal vacuum deposition with multiple sources (3 and 4) is used to prepare for the first time, multications/anions perovskite compounds. These thin-film absorbers are implemented into fully vacuum deposited solar cells using doped organic semiconductors. A maximum power conversion efficiency of 16% is obtained, with promising device stability. The importance of the control over the film morphology is highlighted, which differs substantially when these compounds are vacuum processed. Avenues to improve the morphology and hence the performance of fully vacuum processed multications/anions perovskite solar cells are proposed. [ABSTRACT FROM AUTHOR]

To improve the efficiency of existing perovskite solar cells (PSCs), a detailed understanding of the underlying device physics during their operation is essential. Here, a device model has been developed and validated that describes the operation of PSCs and quantitatively explains the role of contacts, the electron and hole transport layers, charge generation, drift and diffusion of charge carriers and recombination. The simulation to the experimental data of vacuum-deposited CH3NH3PbI3 solar cells over multiple thicknesses has been fit and the device behavior under different operating conditions has been studied to delineate the influence of the external bias, charge-carrier mobilities, energetic barriers for charge injection/extraction and, different recombination channels on the solar cell performance. By doing so, a unique set of material parameters and physical processes that describe these solar cells is identified. Trap-assisted recombination at material interfaces is the dominant recombination channel limiting device performance and passivation of traps increases the power conversion efficiency (PCE) of these devices by 40%. Finally, guidelines to increase their performance have been issued and it is shown that a PCE beyond 25% is within reach. [ABSTRACT FROM AUTHOR]

Efficient monolithic perovskite/perovskite tandem solar cells are fabricated using two perovskite absorbers with complementary bandgaps. By employing doped organic semiconductors, an efficient and selective extraction of the charge carriers is ensured. This study demonstrates perovskite/perovskite tandem cells delivering a maximum efficiency of 18%, highlighting the potential of vacuum‐deposited multilayer structures in overcoming the efficiency of single‐junction perovskite devices. [ABSTRACT FROM AUTHOR]