Dual‐Functional Quantum Dot Seeding Growth of High‐Quality Air‐Processed CsPbI2Br Film for Carbon‐Based Perovskite Solar Cells

The high‐quality perovskite film is a prerequisite for high‐performance optoelectronic devices. Herein, CdSe colloidal quantum dots (QDs) serve as crystallization seeds for the first time to modulate the nucleation and crystal growth processes simultaneously of the CsPbI 2 Br film in the ambient environment. As additives, CdSe QDs help promote the nucleation process in the initial stage of perovskite formation. In addition, it is revealed that the surface ligands of QDs also have an essential influence on the subsequent crystal growth of the perovskite film. The bifunctional ligands on the surface of QDs are beneficial in delaying the growth process of perovskite due to the free functional groups at the ends. The CsPbI 2 Br film prepared with bifunctional organic ligand‐capped CdSe QD additives shows better crystallinity than that of the inorganic ligand‐based one due to the dual function of these kinds of QDs in not only promoting nucleation but also retarding crystal growth of CsPbI 2 Br crystals. As a result, the high‐quality CsPbI 2 Br film with a low defect state density is prepared in the ambient environment. The optimized efficiency of the assembled hole‐conductor‐free carbon‐based perovskite solar cells (C‐PSCs) is increased from 12.73% to 14.49%, which is one of the best results for all‐inorganic C‐PSCs.