Zero-dimensional Cs<sub>4</sub>EuX<sub>6</sub> (X = Br, I) all-inorganic perovskite single crystals for gamma-ray spectroscopy

Wu, Yuntao; Han, Dan; Chakoumakos, Bryan C.; Shi, Hongliang; Chen, Shiyou; Du, Mao‐Hua; Greeley, Ian; Loyd, Matthew; Rutstrom, Daniel; Stand, Luis; Koschan, Merry; Melcher, Charles L.

doi:10.1039/c8tc01458b

Cited by 69 publications

(77 citation statements)

References 49 publications

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“…Bulk crystals of 0D Cs 4 CaI 6 :Eu, Cs 4 SrI 6 :Eu, and Cs 4 EuBr 6 perovskites, isostructural to K 4 CdCl 6 trigonal system, have excellent light yields from 51 800 to 78 000 photons MeV −1 and energy resolutions from 3.3% to 4.3% at 662 keV. [ 9,10 ] However, due to a small Stokes shift of Eu 2+ ions, these materials suffer from strong self‐absorption effect when scaling‐up crystal size. Nanocrystals of 0D CsPbBr 3 /Cs 4 PbBr 6 perovskites show a high light yield of 64 000 photons MeV −1 and a fast decay time of <10 ns.…”

Section: Figurementioning

confidence: 99%

Zero‐Dimensional Cs₃Cu₂I₅ Perovskite Single Crystal as Sensitive X‐Ray and γ‐Ray Scintillator

Cheng

Beitlerová

Kučerková

et al. 2020

Physica Rapid Research Ltrs

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Organic-inorganic hybrid halide perovskites, represented by CH 3 NH 3 PbX 3 (X ¼ Cl, Br, I), have demonstrated excellent optoelectronic and radiation detection properties. [1-3] All-inorganic CsPbX 3 perovskites (X ¼ Cl, Br, I) with better long-term stability are also considered as promising materials for optoelectronic devices and semiconductor γ-ray detectors. [4-6] Recently, there has been a surge of interest in low-dimensional perovskites due to their high photoluminescence quantum yield (PLQY). For example, the crystal structure of Cs 4 PbBr 6 that consist of spatially isolated [PbBr 6 ] 4À octahedra surrounding with Cs þ ions can be regarded as a 0D structure at molecular level, which leads to an intense quantum confinement effect. Excitons are strongly confined at each [PbBr 6 ] 4À octahedron, enabling a high exciton binding energy of 353 meV and a high PLQY of between 42% and 45%. [7,8] Quite a few low-dimensional allinorganic perovskites with remarkable luminescent properties were also reported as sensitive and efficient scintillators. Bulk crystals of 0D Cs 4 CaI 6 :Eu, Cs 4 SrI 6 :Eu, and Cs 4 EuBr 6 perovskites, isostructural to K 4 CdCl 6 trigonal system, have excellent light yields from 51 800 to 78 000 photons MeV À1 and energy resolutions from 3.3% to 4.3% at 662 keV. [9,10] However, due to a small Stokes shift of Eu 2þ ions, these materials suffer from strong self-absorption effect when scaling-up crystal size. Nanocrystals of 0D CsPbBr 3 /Cs 4 PbBr 6 perovskites show a high light yield of 64 000 photons MeV À1 and a fast decay time of <10 ns. [11] Onedimensional materials were also reported as sensitive X-ray scintillators, such as Rb 2 CuBr 3 and Rb 2 CuCl 3. [12,13] In particular, the Rb 2 CuBr 3 , that is self-absorption free and nonhygroscopic, was reported to achieve an ultrahigh scintillation yield of 90 000 photons MeV À1. [12] All-inorganic 0D perovskite Cs 3 Cu 2 I 5 was recently reported as a highly efficient blue-emitting material with a PLQY of 91.2%, and regarded as promising for application in photodetectors, light-emitting diodes, and memristors afterward. [14-17] In 2020, Cs 3 Cu 2 I 5 nanocrystals were developed for X-ray imaging with a light yield of 80 000 photons MeV À1. [18] To the best of our knowledge, the X-ray and γ-ray detection capability of bulk Cs 3 Cu 2 I 5 single crystal has not been reported. Thus, the aim of this work is to study the physical and optical properties and the scintillation performance under X-ray and γ-ray radiation of high-quality Cs 3 Cu 2 I 5 perovskite single crystal grown by the Bridgman method. The 7 mm diameter single crystal of Cs 3 Cu 2 I 5 was grown by the vertical Bridgman method. High-purity powders of CsI (99.99%, Grirem Advanced Materials) and CuI (99.999%, Sigma-Aldrich) were used as raw materials. These starting materials were mixed consistent with stoichiometric ratio and loaded into a quartz ampoule in a glovebox with <0.1 ppm moisture and oxygen. The loaded ampoule was sealed under a vacuum of 10 À6 torr after drying at 180 C for ...

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Section: Figurementioning

confidence: 99%

Zero‐Dimensional Cs₃Cu₂I₅ Perovskite Single Crystal as Sensitive X‐Ray and γ‐Ray Scintillator

Cheng

Beitlerová

Kučerková

et al. 2020

Physica Rapid Research Ltrs

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“…[ 26,27 ] As a comparison, the oxidation potentials of Yb 2+ , Sm 2+ , and Tm 2+ are reported to be −1.18(1) V, −1.50(1) V, and −2.22(5) V, respectively, which are considerably smaller than that of Eu 2+ . Since the emission spectra of Eu 2+ ions are mainly determined by the combined effect of crystal field splitting (ε cfs ) and centroid shift (ε c ), [ 28 ] the coordinating ligands and lattice structure around Eu 2+ ions should be strictly controlled to realize pure blue emission. In CsEuBr 3 , only one Eu 2+ crystallographic site exists in the crystal structure, and the strengths of ε cfs and ε c are suitable to ensure blue emission.…”

Section: Introductionmentioning

confidence: 99%

Efficient Blue Light Emitting Diodes Based On Europium Halide Perovskites

et al. 2021

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Flat panel displays enjoy 100 billion‐dollar markets with significant penetration in daily life, which require efficient, color‐saturated blue, green, and red light‐emitting diodes (LEDs). The recently emerged halide perovskites have demonstrated low‐cost and outstanding performance for potential LED applications. However, the performance of blue perovskite LEDs (PeLEDs) lags far behind red and green cousins, particularly for color coordinates approaching (0.131, 0.046) that fulfill the Rec. 2020 specification for blue emitters. Here, a high‐efficiency, lead‐free perovskite, CsEuBr3, is reported that exhibits bright blue exciton emission centered at 448 nm with a color coordinates of (0.15, 0.04), contributed from Eu‐5d→Eu‐4f/Br‐4p transition with an optical band gap of 2.85 eV. Further optical characterizations reveal its short excited‐state lifetime of 151 ns, excellent exciton diffusion diffusivity of 0.0227 cm2 s−1, and high quantum yield of ≈69%. Inspired by these findings, deep‐blue PeLEDs based on all‐vacuum processing methods, which have been demonstrated as the most successful approach for the organic LED industry, are constructed. The devices show a maximum external quantum efficiency of 6.5% with an operating half‐lifetime of 50 mins at an initial brightness of 15.9 cd m−2. It is anticipated that this work will inspire further research on lanthanide‐based perovskites for next‐generation LED applications.

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“…Therefore, it has been proposed that intrinsic defect states within the band gap may serve as radiative recombination centers for the observed green emission of Cs4PbBr6 materials 3,24 and blue emission of Cs4EuBr6 and Cs4EuI6 single crystals. 25 Strong evidence for the origin of the emissive defect states of Cs4PbBr6 and a detailed theoretical insight on the nature of these defect are thus clearly needed. 26 In this Letter, we systematically study the point defects in inorganic Cs-Pb-Br perovskites (CsPbBr3, CsPb2Br5, and Cs4PbBr6) based on density functional theory (DFT) calculations.…”

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confidence: 99%

Point Defects and Green Emission in Zero-Dimensional Perovskites

Yin

Yang

Song

et al. 2018

J. Phys. Chem. Lett.

146

215

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Zero-dimensional (0D) perovskites have recently opened a new frontier in device engineering for light conversion technologies due to their unprecedented high photoluminescence quantum yield as solids. Although many experimental and theoretical efforts have been made to understand their optical behavior, the origin of their green emission is still opaque. Here, we develop a complete experimental and theoretical picture of point defects in Cs-Pb-Br perovskites and demonstrate that bromide vacancies (V) in prototype 0D perovskite CsPbBr have a low formation energy and a relevant defect level to contribute to the midgap radiative state. Moreover, the state-of-the-art characterizations including atomic-resolution electron imaging not only confirm the purity of the 0D phase of Br-deficient green-emissive CsPbBr nanocrystals (NCs) but also exclude the presence of CsPbBr NCs impurities. Our findings provide robust evidence for defect-induced green luminescence in 0D perovskite NCs, which helps extend the scope of the utility of these bulk 0D quantum materials in optoelectronic applications.

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Zero-dimensional Cs₄EuX₆ (X = Br, I) all-inorganic perovskite single crystals for gamma-ray spectroscopy

Abstract: The zero-dimensional all-inorganic perovskites are self-activated blue emitters with slight hygroscopicity, scalable synthesis, and high radiation detection efficiency.

Cited by 69 publications

References 49 publications

Zero‐Dimensional Cs₃Cu₂I₅ Perovskite Single Crystal as Sensitive X‐Ray and γ‐Ray Scintillator

Zero‐Dimensional Cs₃Cu₂I₅ Perovskite Single Crystal as Sensitive X‐Ray and γ‐Ray Scintillator

Efficient Blue Light Emitting Diodes Based On Europium Halide Perovskites

Point Defects and Green Emission in Zero-Dimensional Perovskites

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Zero-dimensional Cs4EuX6 (X = Br, I) all-inorganic perovskite single crystals for gamma-ray spectroscopy

Abstract: The zero-dimensional all-inorganic perovskites are self-activated blue emitters with slight hygroscopicity, scalable synthesis, and high radiation detection efficiency.

Cited by 69 publications

References 49 publications

Zero‐Dimensional Cs3Cu2I5 Perovskite Single Crystal as Sensitive X‐Ray and γ‐Ray Scintillator

Zero‐Dimensional Cs3Cu2I5 Perovskite Single Crystal as Sensitive X‐Ray and γ‐Ray Scintillator

Efficient Blue Light Emitting Diodes Based On Europium Halide Perovskites

Point Defects and Green Emission in Zero-Dimensional Perovskites

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Product

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Zero-dimensional Cs₄EuX₆ (X = Br, I) all-inorganic perovskite single crystals for gamma-ray spectroscopy

Zero‐Dimensional Cs₃Cu₂I₅ Perovskite Single Crystal as Sensitive X‐Ray and γ‐Ray Scintillator

Zero‐Dimensional Cs₃Cu₂I₅ Perovskite Single Crystal as Sensitive X‐Ray and γ‐Ray Scintillator