Ultrastable CsPbBr3 Perovskite Quantum Dot and Their Enhanced Amplified Spontaneous Emission by Surface Ligand Modification

Abstract

The poor stability and aggregation problem of CsPbBr₃ quantum dots (QDs) in air are great challenges for their future practical application. Herein, a simple and effective ligand-modification strategy is proposed by introducing 2-hexyldecanoic acid (DA) with two short branched chains to replace oleic acid (OA) with long chains during the synthesis process. These two short branched chains not only maintain their colloidal stability but also contribute to efficient radiative recombination. The calculations show that CsPbBr₃ QDs with DA modification (CsPbBr₃ -DA QDs) have larger binding energy than CsPbBr₃ QDs with OA (CsPbBr₃ -OA QDs), resulting in significantly enhanced stability. Due to the strong binding energy between DA ligands and QDs, CsPbBr₃ -DA QDs exhibit no aggregation phenomenon even after stored in air for more than 70 d, and CsPbBr₃ -DA QDs films can maintain 94.3% of initial PL intensity after 28 d, while in CsPbBr₃ -OA QDs films occurs a rapid degradation of PL intensity. Besides, the enhanced amplified spontaneous emission (ASE) performance of CsPbBr₃ -DA QDs films has been demonstrated under both one- and two-photon laser excitation. The ASE threshold of CsPbBr₃ -DA QDs films is reduced by more than 50% and their ASE photostability is also improved, in comparison to CsPbBr₃ -OA QDs films.

Keywords: CsPbBr3 quantum dots; amplified spontaneous emission; density functional theory; ligand modification; stability.