A two-step ligand-exchange strategy is developed, in which the long-carbon- chain ligands on all-inorganic perovskite (CsPbX , X = Br, Cl) quantum dots (QDs) are replaced with halide-ion-pair ligands. Green and blue light-emitting diodes made from the halide-ion-pair-capped quantum dots exhibit high external quantum efficiencies compared with the untreated QDs.
Although halide perovskite nanocrystals (NCs) are promising materials for optoelectronic devices, they suffer severely from chemical and phase instabilities. Moreover, the common capping ligands like oleic acid and oleylamine that encapsulate the NCs will form an insulating layer, precluding their utility in optoelectronic devices. To overcome these limitations, we develop a postsynthesis passivation process for CsPbI NCs by using a bidentate ligand, namely 2,2'-iminodibenzoic acid. Our passivated NCs exhibit narrow red photoluminescence with exceptional quantum yield (close to unity) and substantially improved stability. The passivated NCs enabled us to realize red light-emitting diodes (LEDs) with 5.02% external quantum efficiency and 748 cd/m luminance, surpassing by far LEDs made from the nonpassivated NCs.
Colloidal quantum dots (CQDs) offer promise in flexible electronics, light sensing and energy conversion. These applications rely on rectifying junctions that require the creation of high-quality CQD solids that are controllably n-type (electron-rich) or p-type (hole-rich). Unfortunately, n-type semiconductors made using soft matter are notoriously prone to oxidation within minutes of air exposure. Here we report high-performance, air-stable n-type CQD solids. Using density functional theory we identify inorganic passivants that bind strongly to the CQD surface and repel oxidative attack. A materials processing strategy that wards off strong protic attack by polar solvents enabled the synthesis of an air-stable n-type PbS CQD solid. This material was used to build an air-processed inverted quantum junction device, which shows the highest current density from any CQD solar cell and a solar power conversion efficiency as high as 8%. We also feature the n-type CQD solid in the rapid, sensitive, and specific detection of atmospheric NO2. This work paves the way for new families of electronic devices that leverage air-stable quantum-tuned materials.
So-called zero-dimensional perovskites, such as Cs 4 PbBr 6 , promise outstanding emissive properties. However, Cs 4 PbBr 6 is mostly prepared by melting of precursors that usually leads to a coformation of undesired phases. Here, we report a simple low-temperature solution-processed synthesis of pure Cs 4 PbBr 6 with remarkable emission properties. We found that pure Cs 4 PbBr 6 in solid form exhibits a 45% photoluminescence quantum yield (PLQY), in contrast to its three-dimensional counterpart, CsPbBr 3 , which exhibits more than 2 orders of magnitude lower PLQY. Such a PLQY of Cs 4 PbBr 6 is significantly higher than that of other solid forms of lower-dimensional metal halide perovskite derivatives and perovskite nanocrystals. We attribute this dramatic increase in PL to the high exciton binding energy, which we estimate to be ∼353 meV, likely induced by the unique Bergerhoff−Schmitz−Dumont-type crystal structure of Cs 4 PbBr 6 , in which metal-halide-comprised octahedra are spatially confined. Our findings bring this class of perovskite derivatives to the forefront of color-converting and light-emitting applications.
Organo-metal halide perovskites are a promising platform for optoelectronic applications in view of their excellent charge transport and bandgap tunability. However, their low photoluminescence quantum efficiencies, especially in low excitation regimes, limit their efficiency for light emission. Consequently, perovskite light emitting devices are operated under high injection, a regime under which the materials have so far been unstable. Here we show that, by concentrating photoexcited states into a small subpopulation of radiative domains, one can achieve a high quantum yield even at low excitation intensities. We tailor the composition of quasi-2D perovskites to direct energy transfer into the lowest-bandgap
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