CH₃NH₃PbBr_3–xI_x Quantum Dots Enhance Bulk Crystallization and Interface Charge Transfer for Efficient and Stable Perovskite Solar Cells

Obtaining a perovskite light-absorbing layer with good crystallization, low defect concentration, good stability, and well-matched energy levels is critical to obtaining high-efficiency perovskite solar cells (PSCs). Here, a hybrid PSC with a graded band gap is explored using MAPbBr3 (MA = CH3NH3) and MAPbBr0.9I2.1 quantum dots (QDs) as component cells. We have creatively designed a solar cell device with a double-QD structure [indium tin oxide (ITO)/SnO2/perovskite:MAPbBr3 QDs/MAPbBr0.9I2.1 QDs/Spiro-OMeTAD/Au]. A better crystal film of the perovskite absorption layer can be obtained because the MAPbBr3 QDs are doped in an antisolvent, which induces nucleation and growth in the polycrystalline perovskite. In addition, we expect that digestive ripening occurred in the crystallization, and the oleic acid ligands on the surface of the QDs disintegrate during the doping process and transfer to the surface of the perovskite absorption layer finally; it follows that the hydrophobicity and stability of the perovskite film are greatly enhanced. Moreover, a thin film of MAPbBr0.9I2.1 QDs is introduced between the perovskite absorption layer and the hole layer, acting as an energy-level ladder, which leads to well-matched energy levels, an increase in fill factor (FF), and an enhanced hole transport capability. In particular, the mechanism of the crystallization process involving the effect of oleic acid ligands on the interior and surface of the perovskite film is fully discussed here. The final research results from the PSCs show that both high efficiency and long-term stability are achieved successfully by this design strategy.