Monocrystalline Methylammonium Lead Halide Perovskite Materials for Photovoltaics

Abstract Lead halide perovskite solar cells have been gaining more and more interest. In only a decade, huge research efforts from interdisciplinary communities enabled enormous scientific advances that rapidly led to energy conversion efficiency near that of record silicon solar cells, at an unprecedented pace. However, while for most materials the best solar cells were achieved with single crystals (SC), for perovskite the best cells have been so far achieved with polycrystalline (PC) thin films, despite the optoelectronic properties of perovskite SC are undoubtedly superior. Here, by taking as example monocrystalline methylammonium lead halide, the authors elaborate the literature from material synthesis and characterization to device fabrication and testing, to provide with plausible explanations for the relatively low efficiency, despite the superior optoelectronics performance. In particular, the authors focus on how solar cell performance is affected by anisotropy, crystal orientation, surface termination, interfaces, and device architecture. It is argued that, to unleash the full potential of monocrystalline perovskite, a holistic approach is needed in the design of next‐generation device architecture. This would unquestionably lead to power conversion efficiency higher than those of PC perovskites and silicon solar cells, with tremendous impact on the swift deployment of renewable energy on a large scale.