The most efficient organic-inorganic perovskite solar cells (PSCs) contain the conventional n-i-p mesoscopic device architecture using a semiconducting TiO scaffold combined with a compact TiO blocking layer for selective electron transport. These devices achieve high power conversion efficiencies (15-22%) but mainly require high-temperature sintering (>450 °C), which is not possible for temperature-sensitive substrates. Thus far, comparably little effort has been spent on alternative low-temperature (<150 °C) routes to realize high-efficiency TiO-based PSCs; instead, other device architectures have been promoted for low-temperature processing. In this paper the compatibility of the conventional mesoscopic TiO device architecture with low-temperature processing is presented for the first time with the combination of electron beam evaporation for the compact TiO and UV treatment for the mesoporous TiO layer. Vacuum evaporation is introduced as an excellent deposition technique of uniform compact TiO layers, adapting smoothly to the rough fluorine-doped tin oxide substrate surface. Effective removal of organic binders by UV light is shown for the mesoporous scaffold. Entirely low-temperature-processed PSCs with TiO scaffold reach encouraging stabilized efficiencies of up to 18.2%. This process fulfills all requirements for monolithic tandem devices with high-efficiency silicon heterojunction solar cells as the bottom cell.

Relating crystallization of the absorber layer in a perovskite solar cell (PSC) to the device performance is a key challenge for the process development and in-depth understanding of these types of high efficient solar cells. A novel approach that enables real-time photo-physical and electrical characterization using a graphite-based PSC is introduced in this work. In our graphite-based PSC, the device architecture of porous monolithic contact layers creates the possibility to perform photovoltaic measurements while the perovskite crystallizes within this scaffold. The kinetics of crystallization in a solution based 2-step formation process has been analyzed by real-time measurement of the external photon to electron quantum efficiency as well as the photoluminescence emission spectra of the solar cell. With this method it was in particular possible to identify a previously overlooked crystallization stage during the formation of the perovskite absorber layer. This stage has significant influence on the development of the photocurrent, which is attributed to the formation of electrical pathways between the electron and hole contact, enabling efficient charge carrier extraction. We observe that in contrast to previously suggested models, the perovskite layer formation is indeed not complete with the end of crystal growth.

L subcells integrated into a monolithic tandem solar cell is challenging though crucial in order to identify performance limiting loss mechanisms. This method can be used to improve the study of the mutual influence of adjacent subcells in the fully fabricated device, which has been an unfeasible task up to now.

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