Photoluminescence Mechanisms of All‐Inorganic Cesium Lead Bromide Perovskites Revealed by Single Particle Spectroscopy

Jiang, Yiqun; Li, Beiye; Zhang, Tianxiang; Shi, Yumeng; Xu, Qing‐Hua

doi:10.1002/cnma.201900690

Cited by 19 publications

(17 citation statements)

References 74 publications

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“…This is very similar to the case of the size‐independent emission observed in Cs 4 PbBr 6 . Although the detailed origin of the emission is still under debate, over the past years of research, it is concluded that the origin of the “CsPbBr 3 ‐like” emission in Cs 4 PbBr 6 is either from trace amount of CsPbBr 3 phase or the structural defect of Cs 4 PbBr 6 [51,52] . In our case, the shift of the UV‐vis is also related to the occurrence of Cs 4 PbCl 6 , although whether it is from trapped CsPbCl 3 or structural defect still requires further investigation.…”

Section: Resultsmentioning

confidence: 64%

Ligand‐Mediated Synthesis of Mixed‐Phase Mn²⁺‐Doped Cesium Lead Chloride Nanocrystals

Liu

2021

ChemNanoMat

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Herein we report a study on the role of alkylamine ligand in tuning the crystal structure and the luminescence of Mn2+‐doped cesium lead chloride (Mn−CPC) nanocrystals. In a typical hot‐injection synthesis of Mn−CPC, oleic acid (OA) and oleylamine (OLA) are used as the capping ligands to mediate the size and surface structure of the nanocrystals. We found that by either increasing the concentration of OLA or substituting OLA with an amine with a shorter chain length (e. g. dodecylamine), the resulted Mn−CPC contains both CsPbCl3 and Cs4PbCl6 phases. The mixed‐phase Mn−CPC exhibit two major photoluminescence emission bands originated from the CsPbCl3 bandgap and the Mn d‐d transition, respectively. Besides, a near‐UV emission from Cs4PbCl6 near‐band‐gap exciton emission also appears and is highly sensitive to the excitation wavelength. The formation mechanism of mixed‐phase Mn−CPC nanocrystals is proposed.

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Section: Resultsmentioning

confidence: 64%

Ligand‐Mediated Synthesis of Mixed‐Phase Mn²⁺‐Doped Cesium Lead Chloride Nanocrystals

Liu

2021

ChemNanoMat

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“…As reported in previous studies, 4,12,26 among all the lead halide perovskite nanoparticles, the bromide perovskite (CsPbBr 3 ) QDs have the most promising properties. The absorption band has been associated with the Pb 2+ (6s)− Pb 2+ (6p) transition.…”

mentioning

confidence: 68%

“…39 One possible explanation of the longer coherence time observed for these perovskite QDs could be due to the presence of allowed dipole moment triplet states in the conduction band. 26,34,40,81,82,88 These states, in fact, present a smaller energy gap fluctuation which can help to preserve the coherent superposition state for longer times.…”

mentioning

confidence: 99%

Enhanced Exciton Quantum Coherence in Single CsPbBr₃ Perovskite Quantum Dots using Femtosecond Two-Photon Near-Field Scanning Optical Microscopy

et al. 2021

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Cesium-halide perovskite quantum dots (QDs) have gained tremendous interest as quantum emitters in quantum information processing applications due to their optical and photophysical properties. However, engineering excitonic states in quantum dots requires a deep knowledge of the coherent dynamics of their excitons at a single-particle level. Here, we use femtosecond timeresolved two-photon near-field scanning optical microscopy (NSOM) to reveal coherences involving a single cesium lead bromide perovskite QD (CsPbBr 3 ) at room temperature. We show that, compared to other nonperovskite nanoparticles, the electronic coherence on a single perovskite QD has a relatively long lifetime of ca. 150 fs, whereas CdSe QDs have exciton coherence times shorter than 75 fs at room temperature. One possible explanation for the longer coherence time observed for the CsPbBr 3 perovskite system is related to the exciton fine structure of these perovskite QDs compared to other nanoparticles. These perovskite QDs exhibit interesting optical properties that differ from those of the traditional QDs including bright triplet exciton states. In fact, due to the small amplitude of the energy gap fluctuations of dipole-allowed triplet states in perovskite QDs, the coherent superposition could be preserved for longer times. Furthermore, single-particle excitation approach implemented in this work allows us to remove effects of heterogeneity that are usually present in ensemble averaging experiments at room temperature. The realization of quantum-mechanical phase-coherence of a charge carrier that can operate at room temperature is an issue of great importance for the potential application of coherent electronic phenomena in electronic and optoelectronic devices. These interesting findings provide further evidence of the great potential of these perovskite QDs as candidates for quantum computing and information processing applications.

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“…[ 33,34 ] Owing to the nanoscale physical size of CsPbBr 3 NPs, the quantum confinement of charge carriers occurs. [ 35 ] Spatial constraint prevents electron and hole separation and induces recombination, resulting in a high PL. In bulk CsPbBr 3 , quantum confinement does not occur, and electrons and holes are easily separated and/or trapped on the surface or in defects, leading to nonradiative recombination and low PL.…”

Section: Resultsmentioning

confidence: 99%

Patterning All‐Inorganic Halide Perovskite with Adjustable Phase for High‐Resolution Color Filter and Photodetector Arrays

Kim

Jeon

et al. 2022

Adv Funct Materials

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Perovskite has been actively studied for optoelectronic applications, such as photodetectors and light-emitting diodes (LEDs), because of its excellent optoelectronic properties. However, ionic bonds of the perovskite structure are vulnerable to chemicals, which makes perovskite incompatible with photolithography processes that use polar solvents. Such incompatibility with photolithography hinders perovskite patterning and device integration. Here, an all-solution based cesium lead halide perovskite (Cs x Pb y Br z ) patterning method is introduced in which PbBr 2 is patterned and then synthesized into Cs x Pb y Br z . Each step of the top-down patterning process (e.g., developing, etching, and rinsing) is designed to be compatible with existing photolithography equipment. Structural, chemical, and optical analyses show that the PbBr 2 pattern of (10 µm) 2 squares is successfully transformed into CsPbBr 3 and Cs 4 PbBr 6 with excellent absorption and emission properties. Highresolution photoconductor arrays and luminescent pattern arrays are fabricated with CsPbBr 3 and Cs 4 PbBr 6 on various substrates, including flexible plastic films, to demonstrate their potential applications in image sensors or displays. The research provides a fundamental understanding of the properties and growth of perovskite and promotes technological advancement by preventing degradation during the photolithography process, enabling the integration of perovskite arrays into image sensors and displays.

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Photoluminescence Mechanisms of All‐Inorganic Cesium Lead Bromide Perovskites Revealed by Single Particle Spectroscopy

Cited by 19 publications

References 74 publications

Ligand‐Mediated Synthesis of Mixed‐Phase Mn²⁺‐Doped Cesium Lead Chloride Nanocrystals

Ligand‐Mediated Synthesis of Mixed‐Phase Mn²⁺‐Doped Cesium Lead Chloride Nanocrystals

Enhanced Exciton Quantum Coherence in Single CsPbBr₃ Perovskite Quantum Dots using Femtosecond Two-Photon Near-Field Scanning Optical Microscopy

Patterning All‐Inorganic Halide Perovskite with Adjustable Phase for High‐Resolution Color Filter and Photodetector Arrays

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Photoluminescence Mechanisms of All‐Inorganic Cesium Lead Bromide Perovskites Revealed by Single Particle Spectroscopy

Cited by 19 publications

References 74 publications

Ligand‐Mediated Synthesis of Mixed‐Phase Mn2+‐Doped Cesium Lead Chloride Nanocrystals

Ligand‐Mediated Synthesis of Mixed‐Phase Mn2+‐Doped Cesium Lead Chloride Nanocrystals

Enhanced Exciton Quantum Coherence in Single CsPbBr3 Perovskite Quantum Dots using Femtosecond Two-Photon Near-Field Scanning Optical Microscopy

Patterning All‐Inorganic Halide Perovskite with Adjustable Phase for High‐Resolution Color Filter and Photodetector Arrays

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Ligand‐Mediated Synthesis of Mixed‐Phase Mn²⁺‐Doped Cesium Lead Chloride Nanocrystals

Ligand‐Mediated Synthesis of Mixed‐Phase Mn²⁺‐Doped Cesium Lead Chloride Nanocrystals

Enhanced Exciton Quantum Coherence in Single CsPbBr₃ Perovskite Quantum Dots using Femtosecond Two-Photon Near-Field Scanning Optical Microscopy