Inorganic perovskite CsPbBr nanocrystals (NCs) are emerging, highly attractive light emitters with high color purity and good thermal stability for light-emitting diodes (LEDs). Their high photo/electroluminescence efficiencies are very important for fabricating efficient LEDs. Here, we propose a novel strategy to enhance the photo/electroluminescence efficiency of CsPbBr NCs through doping of heterovalent Ce ions via a facile hot-injection method. The Ce cation was chosen as the dopant for CsPbBr NCs by virtue of its similar ion radius and formation of higher energy level of conduction band with bromine in comparison with the Pb cation to maintain the integrity of perovskite structure without introducing additional trap states. It was found that by increasing the doping amount of Ce in CsPbBr NCs to 2.88% (atomic percentage of Ce compared to Pb) the photoluminescence quantum yield (PLQY) of CsPbBr NCs reached up to 89%, a factor of 2 increase in comparison with the native, undoped ones. The ultrafast transient absorption and time-resolved photoluminescence (PL) spectroscopy revealed that Ce-doping can significantly modulate the PL kinetics to enhance the PL efficiency of doped CsPbBr NCs. As a result, the LED device fabricated by adopting Ce-doped CsPbBr NCs as the emitting layers exhibited a pronounced improvement of electroluminescence with external quantum efficiency (EQE) from 1.6 to 4.4% via Ce-doping.
All-inorganic lead halide perovskite nanocrystals (NCs) are potential candidates for fabricating high-performance light-emitting diodes (LEDs) owing to their precisely tunable bandgaps, high photoluminescence (PL) efficiency, and excellent color purities. However, the performance of pure red (630−640 nm) all-inorganic perovskite LEDs is still limited by the halide segregation-induced instability of the electroluminescence (EL) of mixed halide CsPbI 3-x Br x NCs. Herein, we report an effective approach to improving the EL stability of pure red all-inorganic CsPbI 3-x Br x NC-based LEDs via the passivation of potassium bromide on NCs. By adding potassium oleate to the reaction system, we obtained potassium bromide surfacepassivated (KBr-passivated) CsPbI 3-x Br x NCs with pure red PL emission and a photoluminescence quantum yield (PLQY) exceeding 90%. We determine that most potassium ions present on the surface of NCs bind with bromide ions and thus demonstrate that potassium bromide surface passivation of NCs can both improve the PL stability and inhibit the halide segregation of NCs. Using KBr-passivated CsPbI 3-x Br x NCs as an emitting layer, we fabricated stable and pure red perovskite LEDs with emission at 637 nm, showing a maximum brightness of 2671 cd m −2 , maximum external quantum efficiency of 3.55%, and good EL stability. The proposed KBrpassivated NC strategy will open a new avenue for fabricating efficient, stable, and tunable pure color perovskite NC LEDs.
Cubic phase CsPbI3 quantum dots (α-CsPbI3 QDs) as a newly emerging type of semiconducting QDs hold tremendous promise for fundamental research and optoelectronic device applications. However, stable and sub-5 nm-sized α-CsPbI3 QDs have rarely been demonstrated so far due to their highly labile ionic structure and low phase stability. Here, we report a novel strontium-substitution along with iodide passivation strategy to stabilize the cubic phase of CsPbI3, achieving the facile synthesis of α-CsPbI3 QDs with a series of controllable sizes down to sub-5 nm. We demonstrate that the incorporation of strontium ions can significantly increase the formation energies of α-CsPbI3 QDs and hence reduce the structure distortion to stabilize the cubic phase at the few-nanometer size. The size ranging from 15 down to sub-5 nm of as-prepared stable α-CsPbI3 QDs allowed us to investigate their unique size-dependent optical properties. Strikingly, the few-nanometer-sized α-CsPbI3 QDs turned out to retain high photoluminescence and highly close packing in solid state thin films, and the fabricated red light emitting diodes exhibited high brightness (1250 cd m–2 at 9.2 V) and good operational stability (L50 > 2 h driven by 6 V). The developed cation-substitution strategy will provide an alternative method to prepare uniform and finely size-controlled colloidal lead halide perovskite QDs for various optoelectronic applications.
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