We investigate the operational instability of quantum dot (QD)-based light-emitting diodes (QLEDs). Spectroscopic analysis on the QD emissive layer within devices in chorus with the optoelectronic and electrical characteristics of devices discloses that the device efficiency of QLEDs under operation is indeed deteriorated by two main mechanisms. The first is the luminance efficiency drop of the QD emissive layer in the running devices owing to the accumulation of excess electrons in the QDs, which escalates the possibility of nonradiative Auger recombination processes in the QDs. The other is the electron leakage toward hole transport layers (HTLs) that accompanies irreversible physical damage to the HTL by creating nonradiative recombination centers. These processes are distinguishable in terms of the time scale and the reversibility, but both stem from a single origin, the discrepancy between electron versus hole injection rates into QDs. Based on experimental and calculation results, we propose mechanistic models for the operation of QLEDs in individual quantum dot levels and their degradation during operation and offer rational guidelines that promise the realization of high-performance QLEDs with proven operational stability.

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We present multifunctional dendrimer ligands that serve as the charge injection controlling layer as well as the adhesive layer at the interfaces between quantum dots (QDs) and the electron transport layer (ETL) in quantum dot light-emitting diodes (QLEDs). Specifically, we use primary amine-functionalized dendrimer ligands (e.g., a series of poly(amidoamine) dendrimers (PADs, also referred to PAMAM)) that bind to the surface of QDs by replacing the native ligands (oleic acids) and also to the surface of ZnO ETL. PAD ligands control the electron injection rate from ZnO ETL into QDs by altering the electronic energy levels of the surface of ZnO ETL and thereby improve the charge balance within QDs in devices, leading to the enhancement of the device efficiency. As an ultimate achievement, the device efficiency (peak external quantum efficiency) improves by a factor of 3 by replacing the native ligands (3.86%) with PAD ligands (11.36%). In addition, multibranched dendrimer ligands keep the QD emissive layer intact during subsequent solution processing, enabling us to accomplish solution-processed QLEDs. The approach and results in the present study emphasize the importance of controlling the ligands of QDs to enhance QLED performance and also offer simple yet effective chemical mean toward all-solution-processed QLEDs.

Colloidal quantum dots (QDs) are attractive materials for realizing solution-processable laser diodes that could benefit from size-controlled emission wavelengths, low optical-gain thresholds and ease of integration with photonic and electronic circuits1–7. However, the implementation of such devices has been hampered by fast Auger recombination of gain-active multicarrier states1,8, poor stability of QD films at high current densities9,10 and the difficulty to obtain net optical gain in a complex device stack wherein a thin electroluminescent QD layer is combined with optically lossy charge-conducting layers11–13. Here we resolve these challenges and achieve amplified spontaneous emission (ASE) from electrically pumped colloidal QDs. The developed devices use compact, continuously graded QDs with suppressed Auger recombination incorporated into a pulsed, high-current-density charge-injection structure supplemented by a low-loss photonic waveguide. These colloidal QD ASE diodes exhibit strong, broadband optical gain and demonstrate bright edge emission with instantaneous power of up to 170 μW.