Green Emitting Single-Crystalline Bulk Assembly of Metal Halide Clusters with Near-Unity Photoluminescence Quantum Efficiency

Zhou, Chenkun; Lin, Haoran; Neu, Jennifer; Zhou, Yan; Chaaban, Maya; Lee, Sujin; Worku, Michael; Chen, Banghao; Clark, Ronald J.; Cheng, Wen‐Hao; Guan, Jingjiao; Djurovich, Peter I.; Zhang, Dongzhou; Lu, Xiaofeng; Bullock, James D.; Pak, Chongin; Shatruk, Michael; Du, Mao‐Hua; Siegrist, T.; Ma, Biwu

doi:10.1021/acsenergylett.9b00991

Cited by 121 publications

(139 citation statements)

References 30 publications

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“…Such broadband, large Stokes shift combined with long lifetimes suggest that the PL emission of Cs 3 Cu 2 I 5 NCs is likely originated from the STEs as those of low dimensional metal halides. [ 28,40–42 ]…”

Section: Resultsmentioning

confidence: 99%

Efficient and Reabsorption‐Free Radioluminescence in Cs₃Cu₂I₅ Nanocrystals with Self‐Trapped Excitons

et al. 2020

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Radioluminescent materials (scintillators) are widely applied in medical imaging, nondestructive testing, security inspection, nuclear and radiation industries, and scientific research. Recently, all‐inorganic lead halide perovskite nanocrystal (NC) scintillators have attracted great attention due to their facile solution processability and ultrasensitive X‐ray detection, which allows for large area and flexible X‐ray imaging. However, the light yield of these perovskite NCs is relatively low because of the strong self‐absorption that reduces the light out‐coupling efficiency. Here, NCs with self‐trapped excitons emission are demonstrated to be sensitive, reabsorption‐free scintillators. Highly luminescent and stable Cs3Cu2I5 NCs with a photoluminescence quantum yields of 73.7%, which is a new record for blue emission lead‐free perovskite or perovskite‐like NCs, is produced with the assistance of InI3. The PL peak of the Cs3Cu2I5 NCs locates at 445 nm that matches with the response peak of a silicon photomultiplier. Thus, Cs3Cu2I5 NCs are demonstrated as efficient scintillators with zero self‐absorption and extremely high light yield (≈79 279 photons per MeV). Both Cs3Cu2I5 NC colloidal solution and film exhibit strong radioluminescence under X‐ray irradiation. The potential application of Cs3Cu2I5 NCs as reabsorption‐free, low cost, large area, and flexible scintillators is demonstrated by a prototype X‐ray imaging with a high spatial resolution.

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Section: Resultsmentioning

confidence: 99%

Efficient and Reabsorption‐Free Radioluminescence in Cs₃Cu₂I₅ Nanocrystals with Self‐Trapped Excitons

et al. 2020

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“…Problems, such as toxicity, expensive vacuum‐based processing, high defect density faced by conventional LEDs, e.g., organic LEDs [ 1 ] and quantum dot LEDs [ 2 ] pose a challenge to cost‐effective large‐scale commercial application, urging people to explore new emissive species for the next‐generation light‐emitting diodes. During the past few years, lead halide perovskites have received considerable attention as a promising candidate owing to their remarkably high photoluminescence quantum efficiencies (near‐unity for blue, green, and red light‐emission), [ 3–5 ] low defect density as well as potential to be made at low cost via facile solution processing. [ 6–10 ] So far, the record of the external quantum efficiency of green LEDs based on lead halide perovskites has surpassed 20%, [ 11 ] approaching the performance of organic LEDs.…”

Section: Introductionmentioning

confidence: 99%

A Lead‐Free All‐Inorganic Metal Halide with Near‐Unity Green Luminescence

Zhang

Mao

Zheng

et al. 2020

Laser & Photonics Reviews

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As the increasing demand of lighting display technology, environmentallyfriendly, economic light-emitting materials with high performance are required. Herein, a novel solution-processed, highly emissive copper chloride compound -Cs 3 Cu 2 Cl 5 is reported. The crystal structure determined by the Rietveld refinement of the powder X-ray diffraction patterns shows that the corner-sharing tetrahedral Cu-Cl chains are surrounded by Cs + cations, yielding a one-dimensional structure at molecular level. The all-inorganic compound shows excellent photostability, and is thermally stable up to 550°C. Excitingly, it exhibits room-temperature photoluminescence in the green region with near-unity quantum yield. Currently, this appears to be the most efficient lead-free all-inorganic green-light emitting metal halides reported.

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“…This temperature-dependent dual emissions indicate that there may be two excited structures on the triplet excited-state potential energy surface. [3,18] During the warming process (from 80 to 260 K), the emission of A band gradually increases, while that of B band gradually weakens and disappears. This phenomenon shows that when the temperature rises, the self-trapped excitons can gain enough thermal energy to overcome the energy barrier between two emitting triplet excited states.…”

mentioning

confidence: 99%

Doped Zero‐Dimensional Cesium Zinc Halides for High‐Efficiency Blue Light Emission

Cheng

Liu

et al. 2020

Angewandte Chemie

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All-inorganic zero-dimensional (0D) metal halides have recently received increasing attention due to their excellent photoluminescence (PL) performance and high stability. Herein, we present the successful doping of copper(I) into 0D Cs 2 ZnBr 4. The incorporating of Cu + cations enables the originally weakly luminescent Cs 2 ZnBr 4 to exhibit an efficient blue emission centered at around 465 nm, with a high photoluminescence quantum yield (PLQY) of 65.3 %. Detailed spectral characterizations, including ultrafast transient absorption (TA) techniques, were carried out to investigate the effect of Cu + dopants and the origin of blue emission in Cs 2 ZnBr 4 :Cu. To further study the role of the A-site cation and halogen, A 2 ZnCl 4 :Cu (A = Cs, Rb) were also synthesized and found to generate intense sky-blue emission (PLQY % 73.1 %). This work represents an effective strategy for the development of environmentally friendly, low-cost and high-efficiency blueemitting 0D all-inorganic metal halides. Low-dimensional metal halides have been widely studied as optoelectronic materials in the past two decades. [1] Zerodimensional (0D) metal halides have recently attracted intense interest due to their high photoluminescence quantum yields (PLQYs) and color tunability. [2] In terms of the 0D structure, various metal halide species, including tetrahedral BX 4 , pyramidal BX 5 , and octahedral BX 6 , have been reported to form highly crystalline materials. [3] Inspiringly, green, yellow and red luminescent 0D metal halides with high PLQYs have been realized in Cu-, Sn-, Sb-and In-based halide single crystals. [4] Nevertheless, blue-emitting 0D metal halides with high efficiency and stability remain challenging. Recently, several lead-free all-inorganic 0D metal halides with high efficient deep-blue emission in short wavelength blue light region (< 460 nm) have been reported. [5] However, all-inorganic 0D metal halides with intense emission in pureblue spectral region (460-480 nm), [6] which are more desirable for display and solid-state lighting, [7] remain largely unexplored. Therefore, it is of great significance to develop environmentally friendly, stable and high-efficiency 0D metal halides with PL peaks located at pure-blue region. Recent studies have demonstrated that doping is an effective strategy for the preparation of highly luminescent and stable metal halides. [8] Among the various alternatives, first row transition metals are of great interest as the majority are inexpensive, earth abundant, relatively nontoxic, and tend to form low-dimensional metal halides. [9] In this work, we chose Cs 2 ZnBr 4 as host and Cu + as the dopant for the 0D all-inorganic, stable, and efficient blueemitting metal halides. By introduction Cu + into the weakly luminescent Cs 2 ZnBr 4 (PLQY % 3.6 %, PL peak % 465 nm), an unprecedented improvement of PLQY (% 65.3 %) was realized without affecting the emission peak position. Detailed spectral characterizations including ultrafast transient absorption (TA) techniques reveal that the bright...

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Green Emitting Single-Crystalline Bulk Assembly of Metal Halide Clusters with Near-Unity Photoluminescence Quantum Efficiency

Cited by 121 publications

References 30 publications

Efficient and Reabsorption‐Free Radioluminescence in Cs₃Cu₂I₅ Nanocrystals with Self‐Trapped Excitons

Efficient and Reabsorption‐Free Radioluminescence in Cs₃Cu₂I₅ Nanocrystals with Self‐Trapped Excitons

A Lead‐Free All‐Inorganic Metal Halide with Near‐Unity Green Luminescence

Doped Zero‐Dimensional Cesium Zinc Halides for High‐Efficiency Blue Light Emission

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Green Emitting Single-Crystalline Bulk Assembly of Metal Halide Clusters with Near-Unity Photoluminescence Quantum Efficiency

Cited by 121 publications

References 30 publications

Efficient and Reabsorption‐Free Radioluminescence in Cs3Cu2I5 Nanocrystals with Self‐Trapped Excitons

Efficient and Reabsorption‐Free Radioluminescence in Cs3Cu2I5 Nanocrystals with Self‐Trapped Excitons

A Lead‐Free All‐Inorganic Metal Halide with Near‐Unity Green Luminescence

Doped Zero‐Dimensional Cesium Zinc Halides for High‐Efficiency Blue Light Emission

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Product

Resources

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Efficient and Reabsorption‐Free Radioluminescence in Cs₃Cu₂I₅ Nanocrystals with Self‐Trapped Excitons

Efficient and Reabsorption‐Free Radioluminescence in Cs₃Cu₂I₅ Nanocrystals with Self‐Trapped Excitons