The power conversion efficiencies (PCEs) of polycrystalline perovskite solar cells (PC-PSCs) have now reached a plateau after a decade of rapid development, leaving a distinct gap from their Shockley-Queisser limit. To continuously mitigate the PCE deficit, nonradiative carrier losses resulting from defects should be further optimized. Single-crystal perovskites are considered an ideal platform to study the efficiency limit of perovskite solar cells due to their intrinsically low defect density, as demonstrated in bulk single crystals. However, current single-crystal perovskite solar cells (SC-PSCs) based on single-crystal thin film (SCTF) suffer from severe nonradiative carrier losses at the interface and in the bulk simultaneously due to the immature SCTF growth techniques. In this study, we show that the SC-PSCs can outperform state-of-the-art PC-PSCs, with MAPbI3 as an example, by suppressing carrier losses at the interface and in the bulk in device-compatible SCTFs through precisely controlling their growth.
Keywords: interfacial engineering; nonradiative carrier losses; perovskite solar cells; single-crystal perovskite; solvent engineering.