Metal halide perovskite nanocrystals (NCs) have emerged as highly promising light emitting materials for various applications, ranging from perovskite light‐emitting diodes (PeLEDs) to lasers and radiation detectors. While remarkable progress has been achieved in highly efficient and stable green, red, and infrared perovskite NCs, obtaining efficient and stable blue‐emitting perovskite NCs remains a great challenge. Here, a facile synthetic approach for the preparation of blue emitting CsPbBr3nanoplatelets (NPLs) with treatment by an organic sulfate is reported, 2,2‐(ethylenedioxy) bis(ethylammonium) sulfate (EDBESO4), which exhibit remarkably enhanced photoluminescence quantum efficiency (PLQE) and stability as compared to pristine CsPbBr3NPLs coated with oleylamines. The PLQE is improved from ≈28% for pristine CsPbBr3NPLs to 85% for EDBESO4treated CsPbBr3NPLs. Detailed structural characterizations reveal that EDBESO4treatment leads to surface passivation of CsPbBr3NPLs by both EDBE2+and SO42–ions, which helps to prevent the coalescence of NPLs and suppress the degradation of NPLs. A simple proof‐of‐concept device with emission peaked at 462 nm exhibits an external quantum efficiency of 1.77% with a luminance of 691 cd m−2and a half‐lifetime of 20 min, which represents one of the brightest pure blue PeLEDs based on NPLs reported to date.
Lead halide perovskites are promising materials for a range of applications owing to their unique crystal structure and optoelectronic properties. Understanding the relationship between the atomic/mesostructures and the associated properties of perovskite materials is crucial to their application performances. Herein, the detailed pressure processing of CsPbBr3perovskite nanocube superlattices (NC‐SLs) is reported for the first time. By using in situ synchrotron‐based small/wide angle X‐ray scattering and photoluminescence (PL) probes, the NC‐SL structural transformations are correlated at both atomic and mesoscale levels with the band‐gap evolution through a pressure cycle of 0 ↔ 17.5 GPa. After the pressurization, the individual CsPbBr3NCs fuse into 2D nanoplatelets (NPLs) with a uniform thickness. The pressure‐synthesized perovskite NPLs exhibit a single cubic crystal structure, a 1.6‐fold enhanced photoluminescence quantum yield, and a longer emission lifetime than the starting NCs. This study demonstrates that pressure processing can serve as a novel approach for the rapid conversion of lead halide perovskites into structures with enhanced properties.
more » « less- NSF-PAR ID:
- 10034886
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 29
- Issue:
- 18
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract All‐inorganic lead halide perovskite nanocrystals (NCs) have great optoelectronic properties with promising applications in light‐emitting diodes (LEDs), lasers, photodetectors, solar cells, and photocatalysis. However, the intrinsic toxicity of Pb and instability of the NCs impede their broad applications. Shell‐coating is an effective method for enhanced environmental stability while reducing toxicity by choosing non‐toxic shell materials such as metal oxides, polymers, silica, etc. However, multiple perovskite NCs can be encapsulated within the shell material and a uniform epitaxial‐type shell growth of well‐isolated NCs is still challenging. In this work, lead‐free vacancy‐ordered double perovskite Cs2SnX6(X = Cl, Br, and I) shells are epitaxially grown on the surface of CsPbX3NCs by a hot‐injection method. The effectiveness of the non‐toxic double perovskite shell protection is demonstrated by the enhanced environmental and phase stability against UV illumination and water. In addition, the photoluminescence quantum yields (PL QYs) increase for the CsPbCl3and CsPbBr3NCs after shelling because of the type I band alignment of the core/shell materials, while enhanced charge transport properties obtained from CsPbI3/Cs2SnI6core/shell NCs are due to the efficient charge separation in the type II core/shell band alignment.
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Metal halide perovskite nanocrystals (NCs) have emerged as new-generation light-emitting materials with narrow emissions and high photoluminescence quantum efficiencies (PLQEs). Various types of perovskite NCs, e.g., platelets, wires, and cubes, have been discovered to exhibit tunable emissions across the whole visible spectrum. Despite remarkable advances in the field of perovskite NCs, many nanostructures in inorganic NCs have not yet been realized in metal halide perovskites, and producing highly efficient blue-emitting perovskite NCs remains challenging and of great interest. Here, we report the discovery of highly efficient blue-emitting cesium lead bromide (CsPbBr 3 ) perovskite hollow NCs. By facile solution processing of CsPbBr 3 precursor solution containing ethylenediammonium bromide and sodium bromide, in situ formation of hollow CsPbBr 3 NCs with controlled particle and pore sizes is realized. Synthetic control of hollow nanostructures with quantum confinement effect results in color tuning of CsPbBr 3 NCs from green to blue, with high PLQEs of up to 81%.more » « less
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All-inorganic halide perovskite nanocrystals (NCs) offer impressive optoelectronic properties for light harvesting, energy conversion, and photoredox applications, with two-dimensional (2D) perovskite NCs further increasing these prospects due to their improved photoluminescence (PL) tuneability, impressive color purity, high in-plane charge transport, and large lateral dimensions which is advantageous for device integration. However, the synthesis of 2D perovskites is still challenging, especially toward large-scale applications. In this study, through the control of surface ligand composition and concentration of a mixture of short (octanoic acid and octylamine, 8-carbon chain) and long (oleic acid and oleylamine, 18-carbon chain) ligands, we have developed an extremely facile ligand-mediated synthesis of 2D CsPbX 3 (X = Cl, Br, or mixture thereof) nanoplatelets (NPLs) at room temperature in an open vessel. In addition, the developed method is highly versatile and can be applied to synthesize Mn-doped CsPbX 3 NPLs, showing a systematic increase in the total PL quantum yield (QY) and the Mn-dopant emission around 600 nm with increasing Mn and Cl concentrations. The reaction occurs in toluene by the introduction of CsX, PbX 2 , and MnX 2 precursors under ambient conditions, which requires no harsh acids, avoids excessive lead waste, little thermal energy input, and is potentially scalable toward industrial applications.more » « less
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Abstract Perovskite photovoltaic ABX3systems are being studied due to their high energy‐conversion efficiencies with current emphasis placed on pure inorganic systems. In this work, synchrotron single‐crystal diffraction measurements combined with second harmonic generation measurements reveal the absence of inversion symmetry below room temperature in CsPbBr3. Local structural analysis by pair distribution function and X‐ray absorption fine structure methods are performed to ascertain the local ordering, atomic pair correlations, and phase evolution in a broad range of temperatures. The currently accepted space group assignments for CsPbBr3are found to be incorrect in a manner that profoundly impacts physical properties. New assignments are obtained for the bulk structure: (above ≈410 K),
P 21/m (between ≈300 K and ≈410 K), and the polar groupPm (below ≈300 K), respectively. The newly observed structural distortions exist in the bulk structure consistent with the expectation of previous photoluminescence and Raman measurements. High‐pressure measurements reveal multiple low‐pressure phases, one of which exists as a metastable phase at ambient pressure. This work should help guide research in the perovskite photovoltaic community to better control the structure under operational conditions and further improve transport and optical properties.
