Distinguishing crystallization stages and their influence on quantum efficiency during perovskite solar cell formation in real-time.

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.

Novel Low-Temperature Process for Perovskite Solar Cells with a Mesoporous TiO2 Scaffold.

The most efficient organic-inorganic perovskite solar cells (PSCs) contain the conventional n-i-p mesoscopic device architecture using a semiconducting TiO2 scaffold combined with a compact TiO2 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 TiO2-based PSCs; instead, other device architectures have been promoted for low-temperature processing. In this paper the compatibility of the conventional mesoscopic TiO2 device architecture with low-temperature processing is presented for the first time with the combination of electron beam evaporation for the compact TiO2 and UV treatment for the mesoporous TiO2 layer. Vacuum evaporation is introduced as an excellent deposition technique of uniform compact TiO2 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 TiO2 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.