Low-Temperature Cross-Linkable Hole Transport Materials for Solution-Processed Quantum Dot and Organic Light-Emitting Diodes with High Efficiency and Color Purity

Cross-linkable hole transport materials (HTMs) are ideal for improving the performance of solution-processed quantum dot light-emitting diodes (QLEDs) and phosphorescent light-emitting diodes (OLEDs). However, previously developed cross-linkable HTMs possessed poor hole transport properties, high cross-linking temperatures, and long curing times. To achieve efficient cross-linkable HTMs with high mobility, low cross-linking temperature, and short curing time, we designed and synthesized a series of low-temperature cross-linkable HTMs comprising dibenzofuran (DBF) and 4-divinyltriphenylamine (TPA) segments for highly efficient solution-processed QLEDs and OLEDs. The introduction of divinyl-functionalized TPA in various positions of the DBF core remarkably affected their chemical, physical, and electrochemical properties. In particular, cross-linked 4-(dibenzo[b,d]furan-3-yl)-N,N-bis(4-vinylphenyl)aniline (3-CDTPA) exhibited a deep highest occupied molecular orbital energy level (5.50 eV), high hole mobility (2.44 × 10-4 cm2 V-1 s-1), low cross-linking temperature (150 °C), and short curing time (30 min). Furthermore, a green QLED with 3-CDTPA as the hole transport layer (HTL) exhibited a notable maximum external quantum efficiency (EQEmax) of 18.59% with a remarkable maximum current efficiency (CEmax) of 78.48 cd A-1. In addition, solution-processed green OLEDs with 3-CDTPA showed excellent device performance with an EQEmax of 15.61%, a CEmax of 52.51 cd A-1, and outstanding CIE(x, y) color coordinates of (0.29, 0.61). This is one of the highest reported EQEs and CEs with high color purity for green solution-processed QLEDs and OLEDs using a divinyl-functionalized cross-linked HTM as the HTL. We believe that this study provides a new strategy for designing and synthesizing practical cross-linakable HTMs with enhanced performance for highly efficient solution-processed QLEDs and OLEDs.