Impact of Bifunctional Ligands on Charge Transfer Kinetics in CsPbBr-CdSe/CdS/ZnS Nanohybrids.

Mixed dimensional nanohybrids (MDNHs) between zero-dimensional (0D) perovskites and two-dimensional (2D) II-VI semiconductors hold great potential for photonic device applications. An in-depth study to understand the shuttling of charge carriers is carried out utilizing bifunctional ligands such as 4-aminothiophenol (4-ATP), -aminobenzoic acid, and 6-amino-2-naphthoic acid in the synthesis of MDNHs of CsPbBr nanocrystals (NCs) and CdSe/CdS/ZnS core/shell/shell (CSS) nanoplatelets (NPLs). These MDNHs form donor-bridge-acceptor systems, where the electronic interaction is greatly influenced by the nature of ligands. The smaller size and stronger binding affinity of 4-ATP to CSS NPLs lead to a faster rate of charge transfer as compared to other linkers. Electronic structure calculations under the framework of density functional theory (DFT) confirms that in 4-ATP capped CSS NPLs, stronger electronic overlap occurs between CSS NPLs and 4-ATP at the valence band maxima (VBM). Furthermore, Poisson distribution modeling proposes that in 4-ATP linked MDNHs, the number of CSS NPLs around CsPbBr NCs is highest.