Quantifying Efficiency Roll-Off Factors in Quantum-Dot Light-Emitting Diodes

The application of quantum-dot light-emitting diodes (QLEDs) is hindered by efficiency roll-off at high current densities. Factors contributing to this roll-off include Auger recombination, electric field-induced quenching, Joule heating, and electron leakage into the hole transport layer. However, a method to quantitatively attribute the contribution of each factor to roll-off has not yet been available, leaving the primary cause of roll-off unidentified. This work addresses this gap using electrically pumped transient absorption spectroscopy, which measures the accumulated electrons and electric field in quantum dots (QDs). This study also introduces a method to quantify electron leakage in QLEDs using this spectroscopic technique. Based on the spectroscopic experimental results, the contribution of each factor to roll-off is quantified. A green QLED with a peak external quantum efficiency (EQE) of 26.8% is studied as an example. The EQE declines to 20.5% at a current density of 354 mA cm^-2, where field-induced quenching accounts for 5% of the efficiency roll-off, and electron leakage contributes 95%. Contributions from Auger recombination and heat-induced quenching are negligible. This work demonstrates strong correlations between roll-off and electron leakage amplitude using statistical data obtained in multiple QLEDs, confirming that electron leakage is the primary factor in EQE roll-off.