Indoor photovoltaics (IPVs) are attracting renewed interest because they can provide sustainable energy through the recycling of photon energy from household lighting facilities. Herein, the Shockley–Queisser model is used to calculate the upper limits of the power conversion efficiencies (PCEs) of perovskite solar cells (PeSCs) for two types of artificial light sources: fluorescent tubes (FTs) and white light–emitting diodes (WLEDs). An unusual zone is found in which the dependence of the PCEs on the bandgap (Eg) under illumination from the indoor lighting sources follows trends different from that under solar irradiation. In other words, IPVs exhibiting high performance under solar irradiation may not perform well under indoor lighting conditions. Furthermore, the ideal bandgap energy for harvesting photonic power from these indoor lighting sources is ≈1.9 eV—a value higher than that of common perovskite materials (e.g., for CH3NH3PbI3). Accordingly, Br− ions are added into the perovskite films to increase their values of Eg. A resulting PeSC featuring a wider bandgap exhibits PCEs of 25.94% and 25.12% under illumination from an FT and a WLED, respectively. Additionally, large‐area (4 cm2) devices are prepared for which the PCE reaches ≈18% under indoor lighting conditions.

The synthesis of certain asymmetric perovskite single crystals (SCs)-including CH 3 NH 3 PbI 3 , which is used most commonly-for application in highperformance perovskite solar cells (PeSCs), remains very challenging. Herein, a promising but general method, differential space-limited crystallization (DSLC), is described for synthesizing high-quality perovskite single-crystal micro-plates. The thickness of the perovskite SCs is controlled by the difference between the thicknesses of two sets of polytetrafluoroethylene (PTFE) spacers. Because the DSLC method does not require very thin spacers, it simplifies the procedure of crystal growth. More importantly, the hydrophobicity of the PTFE spacers weakens the attraction between the surfaces of the confined space and the precursor complexes, thereby increasing the rate of diffusion of the precursor ions. Accordingly, the critical nucleation step is not limited by the low rate of diffusion of the ions. This approach is used to prepare mixed-cation lead iodide single-crystalline micro-plates for solar cell applications. The device performance of single-crystal PeSCs improves after introducing formamidinium ions. The stability of the single-crystal devices also improves relative to that of conventional thin-film counterparts. It is anticipated that this DSLC method can also be used to synthesize different types of asymmetrical perovskite SCs for other optoelectronic applications.