Understanding the Origin of Ultrasharp Sub-bandgap Luminescence from Zero-Dimensional Inorganic Perovskite Cs<sub>4</sub>PbBr<sub>6</sub>

Shin, Mingue; Nam, Sung-Wook; Sadhanala, Aditya; Shivanna, Ravichandran; Anaya, Miguel; Jiménez‐Solano, Alberto; Yoon, Hyewon; Jeon, Seungwon; Stranks, Samuel D.; Hoye, Robert L. Z.; Shin, Byungha

doi:10.1021/acsaem.9b02214

Cited by 38 publications

(53 citation statements)

References 51 publications

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“…Some researchers believed that the embedded CsPbBr 3 should be responsible for the highly bright green emission from Cs 4 PbBr 6 . [ 21,33–37 ] This argument was supported by the direct observation of CsPbBr 3 in Cs 4 PbBr 6 . For example, Raman spectroscopy, [ 21 ] temperature‐dependent PL spectroscopy [ 34 ] and cathodoluminescence spectral mapping [ 36 ] were employed to confirm the presence of CsPbBr 3 in Cs 4 PbBr 6 .…”

Section: Properties and Emission Originsmentioning

confidence: 79%

“…This method was employed in the preparation of lead halide perovskites and its related films. [35,79,[116][117][118][119][120] In a typical process, PbBr 2 in DMF solution (1 m) was spin-coated onto a substrate to form a solid PbBr 2 layers, then CsBr in ethanol (0.07 m) was further coated for different cycles (Figure 7d). [121] The morphology of the obtained films is shown in Figure 7e.…”

Section: Solution-processed Depositionmentioning

confidence: 99%

“…Published by John Wiley & Sons Austrialia, Ltd on behalf of UESTC. [200] CsPbBr 3 in Cs 4 PbBr 6 NCs ITO/PEDOT:PSS/poly-TPD/EL/TPBi/LiF/Al 514 3.5 × 10 −3 850 -2017 [180] CsPb 2 I 5 film ITO/PEDOT:PSS/EL/TPBi/LiF/Al 693 0.14 --2017 [96] CsPb 2 Br 5 film ITO/PEDOT:PSS/EL/TPBi/LiF/Al 520 1.1 7317 -2017 [96] PEA 2 Cs n−1 Pb n Br 3n+1 /Cs 4 PbBr 6 film ITO/PEDOT:PSS:PFI/EL/TPBi/LiF/Al 500 4.51 3259 2.8 2018 [206] CsPbBr 3 /CsPb 2 Br 5 NCs ITO/poly-TPD/PVK/EL/PO-T2T/LiF/Al 518 0.6 8383 2.5 2018 [203] CsPbBr 3 /Cs 4 PbBr 6 film ITO/PEDOT:PSS/EL/TPBi/LiF/Al 525 0.36 --2019 [35] PEA 2 Csn −1 Pb n Br 3n+1 /CsPbBr 3 film ITO/PVK/EL/TPBi/LiF/Al 512 12.7 8457 -2019 [207] PEA 2 Cs n−1 Pb n Br 3n+1 /Cs 4 PbBr 6 film ITO/PVK/EL/TPBi/LiF/Al 484 0.13 45 -2019 [207] CsPbBr 3 /Cs 4 PbBr 6 film ITO/PEDOT:PSS/EL/TPBi/LiF/Al 519 2.5 55 000 2.86 2019 [175] CsPbBr 3 /Cs 4 PbBr 6 film ITO/PEDOT:PSS/EL/TPBi/NiO x /Al 516 3.26 9442 4.2 2019 [117] Cs 4 PbBr 6 NCs ITO/PEDOT:PSS/EL/TPBi/LiF/Al 520 1.21 1942 -2019 [146] CsPbBr 3 in CsPb 2 Br 5 NCs ITO/PVK/EL/TPBi/LiF/Al 525 0.3 904 -2019 [161] ITO/PEDOT:PSS/CsPb 2 Br 5 /TPBi/LiF/Al structure. No significant energy barrier at the PEDOT:PSS/CsPb 2 Br 5 and CsPb 2 Br 5 / TPBi interfaces could be observed, suggesting the possibility of hole and electron injection into CsPb 2 Br 5 .…”

Section: Ledsmentioning

confidence: 99%

“…The element distribution in Cs 4 PbBr 6 film (prepared by thermal evaporation) was found to be nonuniform as well. [ 35 ] Local fluctuation of the compositions could be observed, suggesting the local inclusion of CsPbBr 3 with CsBr‐deficit formula in the dominative Cs 4 PbBr 6 film. Not restricted to widely acknowledged 3D CsPbBr 3 , a 2D Cs 2 PbBr 4 inclusion was claimed to be a potential origin of the fluorescence as well.…”

Section: Properties and Emission Originsmentioning

confidence: 99%

“…In some cases, low‐dimensional‐networked perovskites exhibited strong emission and high PLQY. Benefitting from the excellent optical properties, researchers fabricated high‐efficiency LEDs from Cs 4 PbBr 6 [ 35,40,213,214 ] and CsPb 2 Br 5 [ 64,96,215,216 ] emitting layers. For instance, a pure CsPb 2 Br 5 film [ 96 ] was employed as the active layer in an electroluminescent LED with ITO/PEDOT:PSS/CsPb 2 Br 5 /TPBi/LiF/Al structure.…”

Section: Applicationsmentioning

confidence: 99%

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Low‐Dimensional‐Networked Cesium Lead Halide Perovskites: Properties, Fabrication, and Applications

et al. 2020

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resistance against thermal-treatment compared to organic-inorganic hybrid lead halide perovskites (MAPbX 3 and FAPbX 3), due to the high thermal decomposition temperature of inorganic cations, thus drawing much attention. Owing to their impressive features, all-inorganic lead halide perovskites have been greatly useful in photovoltaic and optoelectronic applications, including solar cells, light-emitting diodes (LEDs), lasers, photodetectors and photocatalysis. [5-17] The conspicuous achievements in CsPbX 3 provoke the rapid development of its derivatives, Cs 4 PbX 6 and CsPb 2 X 5. These Cs x Pb y X z materials are composed of the same element compositions and [PbX 6 ] 4− unit cells. However, they possess completely different connectivity characters of [PbX 6 ] 4− octahedrons. CsPbX 3 is classified as a type of 3D perovskite, because [PbX 6 ] 4− octahedra are corner-shared along all three axes, while CsPb 2 X 5 has a sandwich-like arrangement with Cs + cations in between PbX 2 crystallographic planes, which can be regarded as a 2D phase. In Cs 4 PbX 6 , disconnected [PbBr 6 ] 4− octahedra are completely decoupled by Cs + cations. Among these three structures, CsPb 2 X 5 and Cs 4 PbX 6 , with dimensional-network less than 3 are referred to as lowdimensional-networked cesium lead halide perovskites. Besides the connectivity, these structures can be understood from a confinement perspective. CsPbX 3 is not confined in any dimension such that it can be considered as a 3D networked semiconductor. CsPb 2 X 5 and Cs 4 PbX 6 are confined in one dimension and all three dimensions, hence the name 2D and 0D structures, respectively. [18,19] In CsPb 2 X 5 and Cs 4 PbX 6 , the excitons cannot dissociate easily within all dimensions; instead, they are confined in the PbX 2 planes and individual [PbX 6 ] 4− units, respectively, resulting in larger bandgaps compared to the traditional ABX 3 phase. Figure 1 illustrates these three structures with different dimensions. Until now, comprehensive accounts of these Cs x Pb y X z materials have been made. However, most recent research focuses on CsPbX 3 , which has excellent optical properties and promising potential in various applications. Its derivatives, CsPb 2 X 5 and Cs 4 PbX 6 have achieved tremendous progress but are still far behind that of CsPbX 3. Many problems still seriously limit the rapid development of these low-dimensional-networked perovskites, a typical one being the debate on the origin of their luminescence. In this Review article, we focus on Cs 4 PbX 6 and CsPb 2 X 5 , and attempt to unveil their features, potential in All-inorganic cesium lead halide perovskites have emerged as promising optoelectronic materials with excellent photophysical properties and great potential in a variety of applications. In parallel with the most investigated CsPbX 3 , its derivates, Cs 4 PbX 6 and CsPb 2 X 5 , with low-dimensional-networked structures have also attracted great attention. In this review, recent advancements on the low-dimensional-networked cesium lead halide perovs...

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Section: Properties and Emission Originsmentioning

confidence: 79%

Section: Solution-processed Depositionmentioning

confidence: 99%

Section: Ledsmentioning

confidence: 99%

Section: Properties and Emission Originsmentioning

confidence: 99%

Section: Applicationsmentioning

confidence: 99%

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Low‐Dimensional‐Networked Cesium Lead Halide Perovskites: Properties, Fabrication, and Applications

et al. 2020

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Synthesis of 0D Manganese‐Based Organic–Inorganic Hybrid Perovskite and Its Application in Lead‐Free Red Light‐Emitting Diode

Yan

Tian

Chen

et al. 2021

Adv Funct Materials

106

101

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Lead‐based perovskite light‐emitting diodes (PeLEDs) have exhibited excellent purity, high efficiency, and good brightness. In order to develop nontoxic, highly luminescent metal halide perovskite materials, tin, copper, germanium, zinc, bismuth, and other lead‐free perovskites have been developed. Here, a novel 0D manganese‐based (Mn‐based) organic–inorganic hybrid perovskite with the red emission located at 629 nm, high photoluminescence quantum yield of 80%, and millisecond level triplet lifetime is reported. When applied as the emissive layer in the PeLEDs, the maximum recording brightness of devices after optimization is 4700 cd m−2, and the peak external quantum efficiency is 9.8%. The half‐life of the device reaches 5.5 h at 5 V. The performance and stability of Mn‐based PeLEDs are one order of magnitude higher than those of other lead‐free PeLEDs. This work clearly shows that the Mn‐based perovskite will provide another route to fabricate stable and high‐performance lead‐free PeLEDs.

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Effects of Quantum and Dielectric Confinement on the Emission of Cs‐Pb‐Br Composites

Caicedo‐Dávila

Caprioglio

Lehmann

et al. 2023

Adv Funct Materials

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The halide perovskite CsPbBr3 belongs to the Cs‐Pb‐Br material system, which features two additional thermodynamically stable ternary phases, Cs4PbBr6 and CsPb2Br5. The coexistence of these phases and their reportedly similar photoluminescence (PL) have resulted in a debate on the nature of the emission in these systems. Herein, optical and microscopic characterizations are combined with an effective mass, correlated electron–hole model of excitons in confined systems, to investigate the emission properties of the ternary phases in the Cs‐Pb‐Br system. It is found that all Cs‐Pb‐Br phases exhibit green emission and the non‐perovskite phases exhibit PL quantum yields orders of magnitude larger than CsPbBr3. In particular, blue‐ and red‐shifted emission for the Cs‐ and Pb‐rich phases, respectively, are measured, stemming from embedded CsPbBr3 nanocrystals (NCs). This model reveals that the difference in emission shift is caused by the combined effects of NC size and different band mismatch. Furthermore, the importance of including the dielectric mismatch in the calculation of the emission energy for Cs‐Pb‐Br composites is demonstrated. The results explain the reportedly limited blue shift in CsPbBr3@Cs4PbBr6 composites and rationalize some of its differences with CsPb2Br5.

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Understanding the Origin of Ultrasharp Sub-bandgap Luminescence from Zero-Dimensional Inorganic Perovskite Cs₄PbBr₆

Cited by 38 publications

References 51 publications

Low‐Dimensional‐Networked Cesium Lead Halide Perovskites: Properties, Fabrication, and Applications

Low‐Dimensional‐Networked Cesium Lead Halide Perovskites: Properties, Fabrication, and Applications

Synthesis of 0D Manganese‐Based Organic–Inorganic Hybrid Perovskite and Its Application in Lead‐Free Red Light‐Emitting Diode

Effects of Quantum and Dielectric Confinement on the Emission of Cs‐Pb‐Br Composites

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Understanding the Origin of Ultrasharp Sub-bandgap Luminescence from Zero-Dimensional Inorganic Perovskite Cs4PbBr6

Cited by 38 publications

References 51 publications

Low‐Dimensional‐Networked Cesium Lead Halide Perovskites: Properties, Fabrication, and Applications

Low‐Dimensional‐Networked Cesium Lead Halide Perovskites: Properties, Fabrication, and Applications

Synthesis of 0D Manganese‐Based Organic–Inorganic Hybrid Perovskite and Its Application in Lead‐Free Red Light‐Emitting Diode

Effects of Quantum and Dielectric Confinement on the Emission of Cs‐Pb‐Br Composites

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Understanding the Origin of Ultrasharp Sub-bandgap Luminescence from Zero-Dimensional Inorganic Perovskite Cs₄PbBr₆