We report a full series of blue, green and red quantum-dot-based light-emitting devices (QD-LEDs), all with high external quantum efficiencies over 10%. We show that the fine nanostructure of quantum dots-especially the composition of the graded intermediate shell and the thickness of the outer shell-plays a very important role in determining QD-LED device performance due to its effects on charge injection, transport and recombination. These simple devices have maximum current and external quantum efficiencies of 63 cd A −1 and 14.5% for green QD-LEDs, 15 cd A −1 and 12.0% for red devices, and 4.4 cd A −1 and 10.7% for blue devices, all of which are well maintained over a wide range of luminances from 10 2 to 10 4 cd m −2 . All the QD-LEDs are solution-processed for ease of mass production, and have low turn-on voltages and saturated pure colours. The green and red devices exhibit lifetimes of more than 90,000 and 300,000 h, respectively. Since their inception about three decades ago 1-3 , semiconductor quantum dots have been intensively investigated because of their unique optical properties, including size-controlled tunable emission wavelength (known as the 'quantum confinement effect'), narrow emission spectra, high luminescent efficiency and colloidal-based synthesis process 4-7 . All these attractive characteristics make quantum dots excellent candidates for the development of next-generation display technologies. Quantum dot-based lightemitting diodes (QD-LEDs) have been demonstrated recently, and may offer many advantages over conventional LED and organic LED (OLEDs) technologies in terms of colour purity, stability and production cost, while still achieving similar levels of efficiency. To date, however, the electroluminescence efficiencies of QD-LEDs have remained significantly below those of OLEDs, despite steady progress in recent years [8][9][10][11][12][13][14][15][16][17] . Recently, an efficient deep-blue QD-LED has been reported that makes use of solutionprocessed poly(3,4-ethylenedioxythiophene):polystyrene sulphonate (PEDOT:PSS) and poly(N-vinyl carbazole) (PVK) as its hole injection and transport layers (HIL and HTL), respectively, and ZnO nanoparticles as its electron transport layer (ETL), and achieves a maximum external quantum efficiency (η EQE ) of 7.1% (ref. 15). The same device structure was also used to achieve a green QD-LED with an η EQE of 12.6% (ref. 17). Highly efficient red QD-LEDs with η EQE = 18-20% have been realized using an inverted device structure containing a vacuum-deposited HIL and HTL 16 , and also in another arrangement using a thin insulating layer to obtain an enhanced charge balance 18 . These are the first times that the performances of QD-LEDs have been comparable to those of state-of-the-art phosphorescent OLEDs 19-21 .It is noted that although high efficiencies have been achieved with blue (B), green (G) and red (R) QD-LEDs, these singlecolour QD-LEDs, developed by different research groups, commonly involve very different quantum dot preparation procedures (fo...
We report high-efficiency blue-violet quantum-dot-based light-emitting diodes (QD-LEDs) by using high quantum yield ZnCdS/ZnS graded core-shell QDs with proper surface ligands. Replacing the oleic acid ligands on the as-synthesized QDs with shorter 1-octanethiol ligands is found to cause a 2-fold increase in the electron mobility within the QD film. Such a ligand exchange also results in an even greater increase in hole injection into the QD layer, thus improving the overall charge balance in the LEDs and yielding a 70% increase in quantum efficiency. Using 1-octanethiol capped QDs, we have obtained a maximum luminance (L) of 7600 cd/m(2) and a maximum external quantum efficiency (ηEQE) of (10.3 ± 0.9)% (with the highest at 12.2%) for QD-LEDs devices with an electroluminescence peak at 443 nm. Similar quantum efficiencies are also obtained for other blue/violet QD-LEDs with peak emission at 455 and 433 nm. To the best of our knowledge, this is the first report of blue QD-LEDs with ηEQE > 10%. Combined with the low turn-on voltage of ∼2.6 V, these blue-violet ZnCdS/ZnS QD-LEDs show great promise for use in next-generation full-color displays.
For the state-of-the-art quantum dot light-emitting diodes, while the ZnO nanoparticle layers can provide effective electron injections into quantum dots layers, the hole transporting materials usually cannot guarantee sufficient hole injection owing to the deep valence band of quantum dots. Developing proper hole transporting materials to match energy levels with quantum dots remains a great challenge to further improve the device efficiency and operation lifetime. Here we demonstrate high-performance quantum dot light-emitting diodes with much extended operation lifetime using quantum dots with tailored energy band structures that are favorable for hole injections. These devices show a T95 operation lifetime of more than 2300 h with an initial brightness of 1000 cd m−2, and an equivalent T50 lifetime at 100 cd m−2 of more than 2,200,000 h, which meets the industrial requirement for display applications.
The operating lifetime of blue quantum-dot light-emitting diodes (QLED) is currently a short slab for this emerging display technology. To pinpoint the origin of device degradation, here we apply multiple techniques to monitor the electric-field distribution and space-charge accumulation across the multilayered structure before and after lifetime tests. Evident by charge-modulated electro-absorption and capacitance-voltage characteristics, the excited electrons in blue quantum dots (QD) are prone to cross the type II junction between the QD emission layer and the electron-transporting layer (ETL) due to the offset of conduction band minimum, leading to space-charge accumulation and operating-voltage rise in the ETL. Therefore, unlike those very stable red devices, of which the lifetime is primarily limited by the slow degradation of hole-transporting layer, the poor lifetime of blue QLED originates from the fast degradation at the QD-ETL junction. Materials engineering for efficient electron injection is prerequisite for the boost of operating lifetime.
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