Contemporary advancements in perovskite semiconductors are visibly impacting the progress of light conversion applications. These alluring photo absorbers have gained wide consideration owing to their simple processing and striking optoelectronic properties. Although polycrystalline perovskite thin films exhibit phenomenal performance in energy harvesting devices, they suffer from severe instabilities arising from morphological disorder and surface degradation under ambient conditions. Recent progress in perovskite single-crystals, which in theory should outperform their polycrystalline thin-film counterparts, has been demonstrated to surmount these challenges due to the exceptional optoelectronic properties, such as low trap density, high mobility, low intrinsic carrier concentration and long carrier diffusion length.However, most of the growth approaches used for single-crystal syntheses produce very thick crystals and 2 | P a g e subsequently, the related optoelectronic applications are very limited. Given the potential of perovskite single crystals, to break a new path for perovskite optoelectronic devices relies on understanding sustainable issues arising from interfacial/integration losses and developing passivation strategies to achieve performance parity in open ambient. Therefore, the current review provides a comprehensive overview of the advantages, limitations, and challenges associated with growth methods of single-crystals and their chemical stability, device configurations, photophysics, charge carrier dynamics and photovoltaic applications.
TOC GRAPHICSIn recent years, metal halide perovskites (MHP) have captivated the interest of researchers owing to their engrossing properties and phenomenal performances in numerous optoelectronic devices. In the early 1980s, MAPbX3 (MA = CH3NH3, X = Cl¯, Br¯, I¯) and MASnBrxI3-x-based semiconductors were merely considered to be promising for photovoltaics. 1 Nevertheless, their physical and chemical properties have not been meticulously studied. A turning point in the field occurred in 2009 when Miyasaka first reported a thin film-based solar cell with an efficiency of 3.81% and photovoltage of 0.96 V showing external quantum efficiency (EQE) of 65%. 2 Later, many researchers have contributed for the synthesis and device applications of single-crystal perovskite in solar cells and other optoelectronic applications. 3,4 Moreover, 3 | P a g e single-crystal perovskites (SCPs) are a unique class of materials that have been used as solar radiation absorbers. It should be noted that the MAPbX3 (X = Br ─ , I ─ ) perovskite single crystals possess unprecedented long charge carrier diffusion lengths (10 µm) and a striking low trap density (10 9 to 10 10 cm -3 ). 5 More specifically, under 1 sun illumination, the single-crystals of MAPbI3 achieved diffusion lengths of 175 μm and exceeding 3 mm under weak light for both electrons and holes. [6][7] To achieve an efficient device performance, long-range ordered pattern in a perovskite lattice is desirable to significantly...