Ni2+-Doped CsPbI3 Perovskite Nanocrystals with Near-Unity Photoluminescence Quantum Yield and Superior Structure Stability for Red Light-Emitting Devices

Abstract Room temperature phase instability of cubic CsPbI3 perovskite nanocrystals is one of the notorious limitations for practical applications in optoelectronic fields. Herein, the incorporation of Ni2+ ions into CsPbI3 lattice was successfully achieved by a modified hot-injection method using nickel acetate as doping precursor. The as-prepared Ni2+ (3.3 mol%): CsPbI3 nanocrystals exhibited an improved, near-unity (95%∼100%) photoluminescence quantum yield owing to the enhanced radiative decay rate and the decreased non-radiative decay rate. Additionally, Ni-doping was demonstrated to stabilize CsPbI3 lattice and the Ni2+: CsPbI3 film and colloidal solution can retain their red luminescence up to 15 days and 7 months in atmosphere, respectively. First-principle calculations verified that the significantly improved optical performance and stability of Ni2+: CsPbI3 nanocrystals arose primarily from the increased formation energy due to the successful doping of Ni2+ in CsPbI3. Benefiting from such an effective doping strategy, the as-prepared Ni2+-doped CsPbI3 perovskite nanocrystals can function well as efficient red-light emitter toward the fabrication of high-performance perovskite LED with a peak external quantum efficiency of ∼7%.