Highly efficient green InP-based quantum dot light-emitting diodes regulated by inner alloyed shell component

InP-based quantum dot light-emitting diodes (QLEDs), as less toxic than Cd-free and Pb-free optoelectronic devices, have become the most promising benign alternatives for the next generation lighting and display. However, the development of green-emitting InP-based QLEDs still remains a great challenge to the environmental preparation of InP quantum dots (QDs) and superior device performance. Herein, we reported the highly efficient green-emitting InP-based QLEDs regulated by the inner alloyed shell components. Based on the environmental phosphorus tris(dimethylamino)phosphine ((DMA)₃P), we obtained highly efficient InP-based QDs with the narrowest full width at half maximum (~35 nm) and highest quantum yield (~97%) by inserting the gradient inner shell layer ZnSe_xS_1-x without further post-treatment. More importantly, we concretely discussed the effect and physical mechanism of ZnSe_xS_1-x layer on the performance of QDs and QLEDs through the characterization of structure, luminescence, femtosecond transient absorption, and ultraviolet photoelectron spectroscopy. We demonstrated that the insert inner alloyed shell ZnSe_xS_1-x provided bifunctionality, which diminished the interface defects upon balancing the lattice mismatch and tailored the energy levels of InP-based QDs which could promote the balanced carrier injection. The resulting QLEDs applying the InP/ZnSe_0.7S_0.3/ZnS QDs as an emitter layer exhibited a maximum external quantum efficiency of 15.2% with the electroluminescence peak of 532 nm, which was almost the highest record of InP-based pure green-emitting QLEDs. These results demonstrated the applicability and processability of inner shell component engineering in the preparation of high-quality InP-based QLEDs.