Energy/Charge Transfer Modulation with Spacer Ligands for Highly Emissive Quantum Dot–Polymer Blend

A blend of perovskite quantum dots (QDs) and a hole transport layer (HTL) is a feasible candidate to solve the long-standing issues in light-emitting diodes (LEDs) such as charge injection, energy state matching, and defect passivation. However, QD:HTL blend structures for QD-based LEDs suffer from fast charge and energy transfers due to an inhomogeneous distribution of QDs and the HTL matrix. Here we report new cross-linkable spacer ligands between QDs and TFB that result in a highly emissive QD:TFB-blended LED device. We synthesize three representative spacer ligands to control the charge and energy transfers between QDs and the HTL. The first spacer ligand is used for controlling the molecular distance between QDs and TFB, and the second spacer ligand is designed to investigate how molecular interaction between QDs and the spacer ligand affects the optical property of the QD:TFB blend. Subsequently, the best spacer ligand, a 10-((2-benzoylbenzoyl)oxy)decanoic acid, is designed to anchor TFB (via a benzophenone group) and simultaneously bond to QDs (with a carboxylic acid functional group). The carboxylic acid group strongly interacts with QDs, dramatically improving the cross-linking rate between QDs and TFB. Due to the direct interaction between QDs and TFB, hole carriers can be effectively injected to perovskite QDs through the conductive backbone of TFB, resulting in the highest luminance values of 10917 cd/m 2 at 7.4 V due to carrier injection balance. This is at least 10 times better LED performance compared with a pristine QD device.