Ionic Liquids Modulating CsPbI₃ Colloidal Quantum Dots Enable Improved Mobility for High-Performance Solar Cells

Colloidal all-inorganic CsPbI3 perovskite quantum dots (PQDs) have shown tremendous potential in photovoltaic applications in recent years due to their outstanding optoelectronic properties that general metal halide perovskites offer, along with the added advantages that originates from size reduction and the quantum confinement effect. However, the issue of low carrier mobility in PQD films caused by insulating organic ligands capped on the PQD surface still remains to be addressed while aiming for high-efficiency PQD solar cells. Herein, we propose a novel strategy that takes benefits of ionic liquids, which can offer the high polarity and the electron donating ability to boost the mobility of PQD films in photovoltaic devices. Specifically, 1-propyl-3-methylimidazolium iodide to modulate the colloidal CsPbI3 PQD surface and couple QDs is demonstrated for the first time. The lone pair electrons on the nitrogen of the imidazole ring within the ionic liquid binds to the empty nonbonding surface orbitals of CsPbI3 PQDs while the long-chain insulating ligands are replaced, which enables not only efficient charge transport but also reduced defect density in the assembled PQD solid films. The resulting CsPbI3 PQD solar cell shows a significant increase in efficiency with suppressed hysteresis, indicating the impressive potential of this strategy for developing highly efficient PQD solar cells.