Over 30% External Quantum Efficiency Light‐Emitting Diodes by Engineering Quantum Dot‐Assisted Energy Level Match for Hole Transport Layer

In the study of hybrid quantum dot light‐emitting diodes (QLEDs), even for state‐of‐the‐art achievement, there still exists a long‐standing charge balance problem, i.e., sufficient electron injection versus inefficient hole injection due to the large valence band offset of quantum dots (QDs) with respect to the adjacent carrier transport layer. Here the dedicated design and synthesis of high luminescence Zn1−x CdxSe/ZnSe/ZnS QDs is reported by precisely controlled shell growth, which have matched energy level with the adjacent hole transport layer in QLEDs. As emitters, such Zn1−xCdxSe‐ based QLEDs exhibit peak external quantum efficiencies (EQE) of up to 30.9%, maximum brightness of over 334 000 cd m−2, very low efficiency roll‐off at high current density (EQE ≈25% @ current density of 150 mA cm−2), and operational lifetime extended to ≈1 800 000 h at 100 cd m−2. These extraordinary performances make this work the best among all solution‐processed QLEDs reported in literature so far by achieving simultaneously high luminescence and balanced charge injection. These major advances are attributed to the combination of an intermediate ZnSe layer with an ultrathin ZnS outer layer as the shell materials and surface modification with 2‐ethylhexane‐1‐thiol, which can dramatically improve hole injection efficiency and thus lead to more balanced charge injection. Light‐emitting diodes with an external quantum efficiency >30% are achieved by exploiting Zn1−xCdxSe core/shell quantum dots with ZnSe as an intermediate layer and ultrathin ZnS as an outer layer to match the energy level of the hole transport layer. The maximum brightness reaches up to 334 000 cd m−2, and the operational lifetime is extended to ≈1 800 000 h at 100 cd m−2.