Despite its benefits for facilitating device fabrication, utilization of a polymeric hole transport layer (HTL) in inverted quantum dots (QDs) light-emitting devices (IQLEDs) often leads to poor device performance. In this work, we find that the poor performance arises primarily from electron leakage, inefficient charge injection, and significant exciton quenching at the HTL interface in the inverted architecture and not due to solvent damage effects as is widely believed. We also find that using a layer of wider band gap QDs as an interlayer (IL) in between the HTL and the main QDs' emission material layer (EML) can facilitate hole injection, suppress electron leakage, and reduce exciton quenching, effectively mitigating the poor interface effects and resulting in high electroluminescence performance. Using an IL in IQLEDs with a solution-processed poly(9,9-dioctylfluorene-alt-N-(4-sec-butylphenyl)-diphenylamine) (TFB), HTL improves the efficiency by 2.85× (from 3 to 8.56%) and prolongs the lifetime by 9.4× (from 1266 to 11,950 h at 100 cd/m 2 ), which, to the best of our knowledge, is the longest lifetime for an R-IQLED with a solution-coated HTL. Measurements on single-carrier devices reveal that while electron injection becomes easier as the band gap of the QDs decreases, hole injection surprisingly becomes more difficult, indicating that EMLs of QLEDs are more electron-rich in the case of red devices and more hole-rich in the case of blue devices. Ultraviolet photoelectron spectroscopy measurements verify that blue QDs have a shallower valence band energy than their red counterparts, corroborating these conclusions. The findings in this work, therefore, provide not only a simple approach for achieving high performance in IQLEDs with solution-coated HTLs but also novel insights into charge injection and its dependence on QDs' band gap as well as into different HTL interface properties of the inverted versus upright architecture.

Poly[(9,9-dioctylfluorenyl-2,7-diyl)-alt-(4,4′-(N-(4-butylphenyl))-diphenylamine)] (TFB) is commonly used as the organic hole transport layer (HTL) in high-efficiency Cd-based quantum-dot light-emitting devices (QDLEDs). Despite its good hole transport performance, limitations with its cross-linking properties often result in susceptibility to solvent damage when coating subsequent layers. Here, we investigate the use of a robust thermally cross-linked polymer, 9,9-bis[4-[(4-ethenylphenyl)methoxy]phenyl]-N2,N7-di-1-naphthalenyl-N2,N7-diphenyl-9H-fluorene-2,7-diamine (VB-FNPD), as an HTL for QDLEDs. The results show that using VB-FNPD instead of TFB can double the electroluminescence half-life (LT50) of the devices, leading to an LT50 of 10,100 h versus only 4900 h for the TFB device at an initial luminance (L 0) of 1000 cd m–2. Atomic force microscopy surface scans show that VB-FNPD HTLs have smoother and more uniform morphologies when compared to TFB, which may help improve the quality of the HTL/QD interface and QD film uniformity, both of which are important for long-lived QDLEDs. Steady-state photoluminescence studies on hole-only devices suggest that VB-FNPD is also more stable under hole current flow. Further investigations using capacitance versus voltage on the devices show that replacing TFB by VB-FNPD reduces charge accumulation in the devices, which is likely another factor in the stability improvement.

Encapsulating blue quantum dot light-emitting devices (QLEDs) using an ultraviolet curable resin is known to lead to a significant increase in their efficiency. Some of this efficiency increase occurs immediately, whereas some of it proceeds over a period of time, typically over several tens of hours following the encapsulation, a behavior commonly referred to as positive aging. The root causes of this positive aging, especially in blue QLEDs, remain not well understood. Here, it is revealed that contrary to the expectation, the significant improvement in device efficiency during positive aging arises primarily from an improvement in electron injection across the QD/ZnMgO interface and not due to the inhibition of interface exciton quenching as is widely believed. The underlying changes are investigated by XPS measurements. Results show that the enhancement in device performance arises primarily from the reduction in O-related defects in both the QDs and ZnMgO at the QD/ZnMgO interface. After 51.5 h, the blue QLEDs reach the optimal performance, exhibiting an EQEmax of 12.58%, which is more than sevenfold higher than that in the control device without encapsulation. This work provides design principles for realizing high efficiency in blue QLEDs with oxide electron-transporting layers (ETLs) and provides a new understanding of the mechanisms underlying positive aging in these devices and thus offers a new starting point for both fundamental investigations and practical applications.