Defect Passivation Results in the Stability of Cesium Lead Halide Perovskite Nanocrystals

Nanoheterostructures (NHSs) based on lead halide perovskites (LHPs) and chalcogenide quantum dots have proved to be promising candidates for photovoltaic device applications. However, understanding the defect chemistry at the interfaces of LHPs and chalcogenides is essential to stabilize them and further tune their optoelectronic properties. Here, we demonstrate a route for designing CsPbBr3–PbSe NHSs and other derivatives of LHP-based NHSs using defect-rich MoSe2 nanosheets (NSs) and study the effect of the size of PbSe NPs on their optical properties. In this synthesis route, PbSe nanoparticles (NPs) are formed at an early stage of the reaction through a unique cation displacement reaction, over which CsPbBr3 nanocrystals (NCs) are epitaxially grown. Using this methodology, a nearly 3-fold enhancement in photoluminescence (PL) is achieved, whereas other selenium precursors, which form larger PbSe NPs, result in negligible PL enhancement with respect to the pure CsPbBr3 NCs. Detailed density functional theory (DFT) calculations suggest that the PbSe NPs are responsible for passivating the surface defects that consequently enhance the PL intensity. However, in the case of larger PbSe NPs, the associated valence and conduction bands lie within the band-gap region of CsPbBr3, creating a type-I heterostructure between the two materials, thereby affecting the luminescence properties. Strong passivation of surface defects in CsPbBr3–PbSe NHSs is also evidenced from low-temperature PL studies. Furthermore, the resulting CsPbBr3–PbSe NHSs demonstrate enhanced stability in the presence of water and do not degrade under ambient conditions for several months.