Perovskite CH₃NH₃PbI₃(Cl) Single Crystals: Rapid Solution Growth, Unparalleled Crystalline Quality, and Low Trap Density toward 10⁸ cm^–3

Single crystal reflects the intrinsic physical properties of a material, and single crystals with high-crystalline quality are highly desired for the acquisition of high-performance devices. We found that large single crystals of perovskite CH₃NH₃PbI₃(Cl) could be grown rapidly from chlorine-containing solutions. Within 5 days, CH₃NH₃PbI₃(Cl) single crystal as large as 20 mm × 18 mm × 6 mm was harvested. As a most important index to evaluate the crystalline quality, the full width at half-maximum (fwhm) in the high-resolution X-ray rocking curve (HR-XRC) of as-grown CH₃NH₃PbI₃(Cl) single crystal was measured as 20 arcsec, which is far superior to so far reported CH₃NH₃PbI₃ single crystals (∼1338 arcsec). The unparalleled crystalline quality delivered a low trap-state density of down to 7.6 × 10⁸ cm^–3, high carrier mobility of 167 ± 35 cm² V^–1 s^–1, and long transient photovoltaic carrier lifetime of 449 ± 76 μs. The improvement in the crystalline quality, together with the rapid growth rate and excellent carrier transport property, provides state-of-the-art single crystalline hybrid perovskite materials for high-performance optoelectronic devices.