Antisolvent diffusion-induced growth, equilibrium behaviours in aqueous solution and optical properties of CH3NH3PbI3 single crystals for photovoltaic applications

Crystallization and decomposition of organolead trihalide perovskites (OTPs) are very sensitive to the presence of water in precursor or in ambient conditions. Thus, understanding equilibrium behaviours (crystallization and decomposition) of OTPs in aqueous solution is very critical for OTP solar cells fabricated with water-based precursor solutions. Here, equilibrium behaviours in an aqueous solution of CH3NH3PbI3 (MAPbI3) single crystals (MSCs) were studied. Diethyl ether, as an antisolvent, effectively diffused and induced MSC growth by screening different solvents (diethyl ether, tetrahydrofuran, dichloromethane, and chloroform). The structure transforms from the initial PbI2 to intermediate (HxPbI2+x·xH2O) and finally MSCs were observed by X-ray diffraction. Decomposition of MSCs in aqueous solution was significantly enhanced by potassium iodide coordination and inhibited by CH3NH3I (MAI) addition. We ascribed this inhibition behaviour to suppressing MAI migration from the MSC crystal structure. Finally, the optical properties of MSC were studied.