Controlling CH3NH3PbI(3-x)Cl(x) Film Morphology with Two-Step Annealing Method for Efficient Hybrid Perovskite Solar Cells.

The methylammonium lead halide perovskite solar cells have become very attractive because they can be prepared with low-cost solution-processable technology and their power conversion efficiency have been increasing from 3.9% to 20% in recent years. However, the high performance of perovskite photovoltaic devices are dependent on the complicated process to prepare compact perovskite films with large grain size. Herein, a new method is developed to achieve excellent CH3NH3PbI3-xClx film with fine morphology and crystallization based on one step deposition and two-step annealing process. This method include the spin coating deposition of the perovskite films with the precursor solution of PbI2, PbCl2, and CH3NH3I at the molar ratio 1:1:4 in dimethylformamide (DMF) and the post two-step annealing (TSA). The first annealing is achieved by solvent-induced process in DMF to promote migration and interdiffusion of the solvent-assisted precursor ions and molecules and realize large size grain growth. The second annealing is conducted by thermal-induced process to further improve morphology and crystallization of films. The compact perovskite films are successfully prepared with grain size up to 1.1 μm according to SEM observation. The PL decay lifetime, and the optic energy gap for the film with two-step annealing are 460 ns and 1.575 eV, respectively, while they are 307 and 327 ns and 1.577 and 1.582 eV for the films annealed in one-step thermal and one-step solvent process. On the basis of the TSA process, the photovoltaic devices exhibit the best efficiency of 14% under AM 1.5G irradiation (100 mW·cm(-2)).