Probing the Structural Degradation of CsPbBr3 Perovskite Nanocrystals in the Presence of H2O and H2S: How Weak Interactions and HSAB Matter

Structural degradation of all inorganic CsPbBr3 in the presence of moisture is considered as one of its major limitations to use as an active component in various light-harvesting and light-emitting devices. Herein, we used two similar molecules, H2O and H2S, with similar structures, to follow the decomposition mechanism of CsPbBr3 perovskite nanocrystals. Interestingly, H2O acts as a catalyst for the decomposition of CsPbBr3, which is in contrast to H2S. Our experimental observations followed by density functional theory (DFT) calculations showed that the water molecule is intercalated in the CsPbBr3 perovskite whereas H2S is adsorbed in the (100) planes of CsPbBr3 by a weak electrostatic interaction. According to Pearson’s hard–soft acid–base theory, both cations present in CsPbBr3 prefer soft/intermediate bases. In the case of the water molecule, it lacks a soft base and thus it is not directly involved in the reaction whereas H2S can provide a soft base and thus it gets involved in the reaction. Understanding the mechanistic aspects of decomposition can give different methodologies for preventing such unwanted reactions.