Inverted Solution-Processed Quantum Dot Light-Emitting Devices with Wide Band Gap Quantum Dot Interlayers

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/m²), 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.