Concentration Dependent Modulation in Optoelectronic Traits of Self‐Collated CsPbBr₃ Perovskites

Self-collation of perovskite nanocrystals into superstructures of larger length scales has been growing in research interest due to their dramatically enhanced performance in various nano-devices, modulating their optical and electrical traits. Herein, the unique concentration-dependent self-assembly of phenethylamine (PEA)-capped CsPbBr₃ (PCPB) perovskites spanning a size range of nano to micron level without structural phase alteration is infered. By optimizing various synthetic parameters like PEA amount, and solvents, the self-coalescence in PCPB crystal growth is controlled. Furthermore, the highest-concentrated PCPB (C5) has improved the charge transfer (CT) efficiency to 1,4-Napthoquinone (NPQ), corroborated with stronger binding between C5 and NPQ, compared to the lowest-concentrated PCPB (C1). Incorporating NPQ into such concentration-dependent PCPB enhances their local conductance unveiling the CT-induced current rise, while the detrimental insulating property of PEA molecules reduces the conductance in C5 compared to C1. These outcomes offer a foundation for tailoring the properties of self-assembled perovskites for optoelectronic devices and energy conversion technologies.