Novel device architectures for perovskite solar cells

The aim of the work presented in this thesis is to study the opto-electronic properties of semi-conducting perovskite materials when being used in unconventional solar cell device configurations. Being a young technology, perovskites as solar cell materials have seen an unparalleled rise in the research community which has driven the fastest performance inflation to power conversion efficiencies competing with the ones of long established single crystalline technologies. The ability to process perovskites inexpensively makes them the new hope in the fight against climate change. Herein device architectures were developed with a special focus on potential commercial applications. Initially the work in this thesis has been motivated by the interest in crystal growth and morphology of perovskite thin-films, which has led to the study of confined crystal growth within microstructures. Controlling the crystal domain geometry enabled the fabrication of enhanced semi-transparent devices. More efforts were directed into the improvement of specifically neutral colour semi-transparent devices, which could be improved via a simple treatment of selectively attaching shunt-blocking layers. Furthermore, a back-contacted perovskite device design was introduced, which allows not only for the fabrication of a new type of perovskite solar cell, but also represent a great material testing platform to study perovskite and electrode characteristics. This led to the discovery of charge transport distances, that exceed those of other thin-film devices. Finally, perovskite-on-silicon tandem solar cell designs were analysed through a rigorous optical model to estimate the expected real world energy yield from such systems. Important implications include the fact that two terminal tandem solar cells come close to four-terminal configurations and can overall compete, in relative terms, well with established single junction silicon cells.