Delayed Photoluminescence and Modified Blinking Statistics in Alumina-Encapsulated Zero-Dimensional Inorganic Perovskite Nanocrystals

Guo, Tianle; Bose, Riya; Zhou, Xiaohe; Gartstein, Yuri N.; Yang, Haoze; Kwon, Sunah; Kim, Moon J.; Lutfullin, Marat; Sinatra, Lutfan; Gereige, Issam; AlSaggaf, Ahmed; Bakr, Osman M.; Mohammed, Omar F.; Malko, Anton V.

doi:10.1021/acs.jpclett.9b02594

Cited by 31 publications

(49 citation statements)

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“…[38] The second theory involving a vacancy-assisted PL emission was offered, which regarded the strong PL emission as due to the intrinsic nature of Cs 4 PbBr 6 , in which Br vacancies (in most cases), tribromide and interstitial hydroxyl served as radiative recombination centers. [32,[39][40][41][42][43][44][45] From DFT calculation results, it was found that i) Br vacancies had a small formation energy under Br-deficit conditions; ii) their transition level matched well with the emissive energy; iii) their electronic charge density was highly localized (Figure 3a,b). [29] Therefore, one could obtain Cs 4 PbBr 6 with stronger PL emission if more defects could be induced under extremely Br-poor conditions.…”

Section: D-networked Cs 4 Pbxmentioning

confidence: 99%

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: D-networked Cs 4 Pbxmentioning

confidence: 99%

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

et al. 2020

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“…[56] The blinking behavior in single perovskite QDs was ascribed to random charging/discharging of the quantum dot due to the presence of fast nonradiative Auger recombination driven by photo-assisted ionization, similar to the other semiconductor QDs, e.g., CdSe. [48,53] Using the same techniques of single-molecule spectroscopy and time-resolved spectroscopy, the fluorescence blinking has recently been investigated in MAPbBr 3 QDs, [57][58][59][60] CsPbBr 3 QDs, [61][62][63][64] 0D Cs 4 PbBr 6 , [65] MAPbI 3 QDs. [66] Mandal et al [67] observed blinking in inorganic perovskite CsPbBr 3 QDs.…”

Section: Fluorescence Intermittency In Single Perovskite Quantum Dot mentioning

confidence: 99%

Revealing Dynamic Effects of Mobile Ions in Halide Perovskite Solar Cells Using Time‐Resolved Microspectroscopy

et al. 2020

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Halide perovskites are promising candidate materials for the next generation high-efficiency optoelectronic devices. Since perovskites are electronic-ionic mixed conductors, ion dynamics have a critical impact on the performance and stability of perovskite-based applications. However, comprehensively understanding ionic dynamics is challenging, particularly on nanoscale imaging of ionic dynamics in perovskites. In this review, mobile ion dynamics in halide perovskites investigated via luminescence spectroscopy combined with confocal microscopy are discussed, including mobile ion induced fluorescence quenching, phase segregation in mixed halide hybrid perovskite, and mobile ion accumulation at the interface in perovskite devices. Steady-state and time-resolved luminescence imaging techniques, combined with confocal microscopy, are unique tools for probing ionic dynamics in perovskites, providing invaluable insights on ionic dynamics in nanoscale resolution, along with a wide temporal range from picoseconds to hours. The works in this review are not only for understanding mobile ions to improve the design of perovskite-based devices but also foster the development of microspectroscopic methodologies in a broader solid-state physics context of investigating ionic transports in polycrystalline materials.

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“…The contradictory conclusion may attribute to the loss of surface ligands 88 or the replacement of QDs cations by metal precursor 69 . Thus, fine control of ALD reaction conditions is crucial in determining the performance of QDs 64 . High reaction temperature would strip surface ligands, and thus low temperature is essential to preserve PLQY during ALD processes 65 .…”

Section: (Iii) and (Iv)mentioning

confidence: 99%

Atomic layer deposition for quantum dots based devices

Zhou

Liu

Wen

et al. 2020

Opto-Electronic Advances

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Quantum dots (QDs) are promising candidates for the next-generation optical and electronic devices due to the outstanding photoluminance efficiency, tunable bandgap and facile solution synthesis. Nevertheless, the limited optoelectronic performance and poor lifetime of QDs devices hinder their further applications. As a gas-phase surface treatment method, atomic layer deposition (ALD) has shown the potential in QDs surface modification and device construction owing to the atomic-level control and excellent uniformity/conformality. In this perspective, the attempts to utilize ALD techniques in QDs modification to improve the photoluminance efficiency, stability, carrier mobility, as well as interfacial carrier utilization are introduced. ALD proves to be successful in the photoluminance quantum yield (PLQY) enhancement due to the elimination of QDs surface dangling bonds and defects. The QDs stability and devices lifetime are improved greatly through the introduction of ALD barrier layers. Furthermore, the carrier transport is ameliorated efficiently by infilling interstitial spaces during ALD process. Attributed to the ultra-thin and dense coating on the interface, the improvement on optoelectronic performance is achieved. Finally, the challenges of ALD applications in QDs at present and several prospects including ALD process optimization, in-situ characterization and computational simulations are proposed.

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Delayed Photoluminescence and Modified Blinking Statistics in Alumina-Encapsulated Zero-Dimensional Inorganic Perovskite Nanocrystals

Cited by 31 publications

References 50 publications

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

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

Revealing Dynamic Effects of Mobile Ions in Halide Perovskite Solar Cells Using Time‐Resolved Microspectroscopy

Atomic layer deposition for quantum dots based devices

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