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Abstract:

Cesium lead halide perovskite nanocrystals (PNCs) exhibit promising prospects for application in optoelectronic devices. However, electroactivated near-infrared (NIR) PNC light-emitting diodes (LEDs) with emission peaks over 800 nm have not been achieved. Herein, we demonstrate the electroactivated NIR PNC LEDs based on Yb³⁺-doped CsPb(Cl_1-xBr_x)₃ PNCs with extraordinary high NIR photoluminescence quantum yields over 170%. The fabricated NIR LEDs possess an irradiance of 584.7 μW cm^-2, an EQE of 1.2%, and a turn-on voltage of 3.1 V. The ultrafast quantum cutting process from the PNC host to Yb³⁺ has been revealed as the main mechanism of electroluminescence (EL)-activated Yb³⁺ for the first time via exploring how the trend between the EL intensity of PNC and Yb³⁺ varies with different voltages along with the tendency of temperature- and doping-concentration-dependent PL and EL spectra. This work will extend the application of PNCs to optical communication, night-vision devices, and biomedical imaging.

Abstract:

AbstractThe dimension is a leading parameter in customization of unique optoelectronic properties of halide perovskite, while it is still challenging to achieve dimension control beyond the well‐developed composition regulation‐based strategy considering their intrinsic feature of ionic crystal. In this paper, ligands‐directed confinement effect is emphasized in rendering the reduced‐dimensional engineering of halide perovskite, and quasi‐2D (OAm)2CsPb2Br7 (n = 2) nanosheets are obtained by introducing a large amount of metal ions. As a representation, with Mg2+ participation, the initial adsorption of organic ligands (i.e., OA and OAm) to inorganic components (i.e., [PbBr6]4−) is promoted, conferring a ligands‐directed surface reconstruction to form the lamellar structure composed of alternate organic and inorganic layers. Namely, the inorganic–organic lamellar ensemble will play as a soft template, which effectively restricts the growth of [PbBr6]4− in the c‐axis direction even after the Cs‐OA injection, thus producing the anisotropic layered perovskite of (OAm)2CsPb2Br7 from CsPbBr3 scenario. Notably, such reduced‐dimensional engineering enables a remarkable luminescence tailoring, of which the deep blue emission centered at 439 nm is achieved. In addition, benefiting from such universal strategy, the luminescence is also dependent on the species of introduced metal ions (e.g., Ca2+, Co2+, Sr2+, and Mn2+).

Abstract:

AbstractAlthough light‐emitting devices (LEDs) based on metal halide perovskite nanocrystals (PNCs) developed rapidly in recent years, the luminance of pure red LEDs with the Rec. 2020 standard Commission Internationale de l'Eclairage 1931 color coordinates of (0.708, 0.292) cannot meet the requirement of outdoor display. Herein, a facile in situ modification strategy is proposed to prepare the efficiently luminescent CsPb(Br/I)3 PNCs, where metal bromides are used to create a halide‐rich environment and inhibit the formation of nonradiative surface defects. Synchronously, appropriately increased surface ligands improved the effective exciton confinement. Hence, the modified CsPb(Br/I)3 PNCs exhibited a high photoluminescence quantum yield of 92.0%. Additionally, the electrical conductivity is improved due to the increased hole mobility, and the Auger process is inhibited caused by balanced carrier mobilities. Consequently, LEDs based on the modified CsPb(Br/I)3 PNCs exhibited a maximum luminance of 11233 cd m−2 with the pure red color coordinate (0.704, 0.292) and a peak external quantum efficiency value of 13.2%. Furthermore, the luminance reached 5198 cd m−2 under the driving voltage of 4.4 V. This is the first study to realize a pure red PNC LED with high luminance under low bias, which can meet the requirement of outdoor display.

Abstract:

Oleylamine and oleic acid are common organic capping ligands used in the hot injection preparation of perovskite quantum dots (QDs). Their labile nature is responsible for the poor colloidal stability and conductivity that affect the performance of perovskite QD light-emitting diodes (LEDs). We introduced 4-trifluoro phenethylammonium iodide (CF₃PEAI) directly in the synthesis and found that CF₃PEAI efficiently modified the I^- vacancy defects on the QD surface and partially substituted the surface capping ligand oleylamine. The strong electron pulling ability of F in CF₃PEAI results in a more positive -NH₃⁺ terminal compared to that of PEAI, which promotes tight bonding of CF₃PEAI on the surface of CsPbI₃ QDs. As a result, we achieved bright QDs with a photoluminescence quantum yield of 92% and efficient red LEDs. The maximal luminance was improved to 4550 cd m^-2 for 685 nm red light, which was nearly 4.6-fold of the LEDs with plain CsPbI₃ QDs. Additionally, the peak external quantum efficiency reached 12.5%.