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The original version of this Article contained an error in the spelling of the author Dan Credgington, which was incorrectly given as Dan Credington. This has now been corrected in both the PDF and HTML versions of the Article.
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Two-dimensional (2D) lead halide perovskites with long-chain ammonium halides display high photoluminescence quantum yields (PLQYs), because of their size and dielectric confinement, which hold promise for a high-efficiency and low-cost light-emitting diode (LED). However, the presence of an insulating organic long-chain spacer cation (L) dramatically deteriorates the charge transport properties along the out-of-plane nanoplatelet direction or adjacent nanocrystals, which would limit the device performance of the LED. To overcome this issue, we successfully incorporate small alkaline ions such as sodium (Na+) to replace the long organic molecule. Grazing incidence X-ray diffraction measurements verify 2D layer formation with a preferred crystallite orientation. In addition, the incorporated sodium salt also generates amorphous sodium lead bromide (NaPbBr3) in perovskite as spacers to form a nanocrystal-like halide perovskite film. The PLQY is dramatically improved in the sodium-incorporated film because of its enhanced photoluminescence lifetime. Upon incorporation of a low concentration of an organic additive, this two-dimensional-three-dimensional (2D-3D) perovskite can achieve a compact and uniform film. Therefore, a 2D-3D perovskite achieves a high external quantum efficiency of 15.9% with good operational stability. We develop a type of 2D-3D halide perovskite with various inorganic ions as spacers for promising high-performance optoelectronic devices.
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Organometal halide perovskites (OHP) are promising materials for low-cost, high-efficiency light-emitting diodes. In films with a distribution of two-dimensional OHP nanosheets and small three-dimensional nanocrystals, an energy funnel can be realized that concentrates the excitations in highly efficient radiative recombination centers. However, this energy funnel is likely to contain inefficient pathways as the size distribution of nanocrystals, the phase separation between the OHP and the organic phase. Here, we demonstrate that the OHP crystallite distribution and phase separation can be precisely controlled by adding a molecule that suppresses crystallization of the organic phase. We use these improved material properties to achieve OHP light-emitting diodes with an external quantum efficiency of 15.5%. Our results demonstrate that through the addition of judiciously selected molecular additives, sufficient carrier confinement with first-order recombination characteristics, and efficient suppression of non-radiative recombination can be achieved while retaining efficient charge transport characteristics.
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All inorganic perovskite nanocrystals (NCs) of CsPbX3 (X = Cl, Br, I, or their mixture) are regarded as promising candidates for high-performance light-emitting diode (LED) owing to their high photoluminescence (PL) quantum yield (QY) and easy synthetic process. However, CsPbX3 NCs synthesized by the existing methods, where oleic acid (OA) and oleylamine (OLA) are generally used as surface-chelating ligands, suffer from poor stability due to the ligand loss, which drastically deteriorates their PL QY, as well as dispersibility in solvents. Herein, the OA/OLA ligands are replaced with octylphosphonic acid (OPA), which dramatically enhances the CsPbX3 stability. Owing to a strong interaction between OPA and lead atoms, the OPA-capped CsPbX3 (OPA-CsPbX3) NCs not only preserve their high PL QY (>90%) but also achieve a high-quality dispersion in solvents after multiple purification processes. Moreover, the organic residue in purified OPA-CsPbBr3 is only â¼4.6%, which is much lower than â¼29.7% in OA/OLA-CsPbBr3. Thereby, a uniform and compact OPA-CsPbBr3 film is obtained for LED application. A green LED with a current efficiency of 18.13 cd A-1, corresponding to an external quantum efficiency of 6.5%, is obtained. Our research provides a path to prepare high-quality perovskite NCs for high-performance optoelectronic devices.
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Solution-processed perovskite light-emitting diodes (LEDs) have attracted wide attention in the past several years. However, the overall efficiency and stability of perovskite-based LEDs remain inferior to those of organic or quantum dot LEDs. Nonradiative charge recombination and the unbalanced charge injection are two critical factors that limit the device efficiency and operational stability of perovskite LEDs. Here, we develop a strategy to modify the interface between the hole transport layer and the perovskite emissive layer with an amphiphilic conjugated polymer of poly[(9,9-bis(3'-( N, N-dimethylamino)propyl)-2,7-fluorene)- alt-2,7-(9,9-dioctylfluorene)] (PFN). We show evidences that PFN improves the quality of the perovskite film, which effectively suppresses nonradiative recombination. By further improving the charge injection balance rate, a green perovskite LED with a champion current efficiency of 45.2 cd/A, corresponding to an external quantum efficiency of 14.4%, is achieved. In addition, the device based on the PFN layer exhibits improved operational lifetime. Our work paves a facile way for the development of efficient and stable perovskite LEDs.
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Film morphologies of functional layers in all-solution-processed quantum dot light-emitting diodes (QLEDs) play a crucial role in device performance. Solvents for adjacent layers should be strictly orthogonal to prevent the preceding layer being redissolved by the processing solvent of the next layer. Herein, we use a photochemical crosslinking method to obtain solvent-resistant hole transport layers (HTLs) with photoinitiator bifunctional bis-benzophenone (BP-BP). With this method, ultra-smooth quantum dot (QD) layers can be fabricated using toluene as solvent, which is known to be a nonorthogonal solvent in common non-crosslinked HTLs. A green QLED device based on crosslinked HTLs exhibits a high external quantum efficiency of 8.93%, which is 1.9-fold higher than that of the non-crosslinked device. The improved device performance is ascribed to the well preserved film morphology of crosslinked HTLs and the prevention of QDs intermixing with HTLs during the QD deposition in toluene. This crosslinking strategy avoids high-temperature annealing, allowing the fabrication of flexible devices on plastic substrates. Moreover, it broadens the range of applicable solvents for solution-processed multilayer optoelectronic devices because non-orthogonal solvents can be used after crosslinking preceding layers.