Realizing Near-Unity Quantum Efficiency of Zero-Dimensional Antimony Halides through Metal Halide Structural Modulation DOI

Linyuan Lian,

Peng Zhang, Xiuwen Zhang

et al.

ACS Applied Materials & Interfaces, Journal Year: 2021, Volume and Issue: 13(49), P. 58908 - 58915

Published: Dec. 3, 2021

Zero-dimensional (0D) organic metal halides have attracted significant attention because of their exceptional structure tunability and excellent optical characteristics. However, controllable synthesis a desirable configuration halide species in rational way remains formidable challenge, how the unique crystal structures affect photophysical properties are not yet well understood. Here, reasonable structural modulation strategy is proposed to realize near-unity photoluminescence quantum efficiency (PLQE) 0D antimony halides. By carefully controlling reaction conditions, both (C12H28N)2SbCl5 (C12H28N)SbCl4 with different configurations can be prepared. pyramid-shaped [SbCl5]2- exhibits yellow emission PLQE 96.8%, while seesaw-shaped [SbCl4]- emissive at room temperature. Theoretical calculations indicate that these two crystals attributed symmetries structures. adopts triclinic P-1 symmetry, possesses monoclinic P21/c which has an inversion center, thus transitions between band-edge states give minimal dipole intensity similar parity character. In addition, we also successfully synthesized nanocrystals for first time, particularly appealing solution processibility properties. Furthermore, flexible composite film shows bright under β-ray excitation, suggesting strong potential detection.

Language: Английский

Ceramic Wafer Scintillation Screen by Utilizing Near‐Unity Blue‐Emitting Lead‐Free Metal Halide (C8H20N)2Cu2Br4 DOI
Binbin Su, Jiance Jin, Kai Han

et al.

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 33(5)

Published: Nov. 18, 2022

Abstract Scintillators with high light yield, low detection limit, large X‐ray attenuation efficiency as well stable and nontoxic compositions are of great importance for radiation applications. Here, 0D (C 8 H 20 N) 2 Cu Br 4 single crystals obtained show blue emission peaking at 468 nm a near‐unity photoluminescence quantum yield 99.7%, Stokes shift 148 (i.e., negligible self‐absorption), good environmental stability along strong absorption capability. Moreover, up to ≈ 91 300 photons/MeV limit 52.1 nGy air s −1 realized, which is more than one hundred times lower the dose rate 5.5 µGy required medical diagnostics. ceramic wafer scintillation screen fabricated by cold pressing sintering process, clear contrast images opaque metal box electronic component spatial resolution 9.54 lp mm realized. This study not only designs new lead‐free halide scintillator, but also develops universal strategy preparation large‐sized scintillator in nondestructive imaging.

Language: Английский

Citations

106

Chiral Hybrid Copper(I) Halides for High Efficiency Second Harmonic Generation with a Broadband Transparency Window DOI
Fei Ge, Bohan Li,

Puxin Cheng

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(10)

Published: Jan. 10, 2022

Chiral hybrid organic-inorganic metal halides (HOMHs) with intrinsic noncentrosymmetry have shown great promise for applications in second-order nonlinear optics (NLO). However, established chiral HOMHs often suffer from their relatively small band gaps, which lead to negative impacts on transparent window and laser-induced damage thresholds (LDT). Here, we synthesized two based CuI halides, namely (R-/S-MBA)CuBr2 , feature well-balanced NLO performances a highly efficient SHG response, outstanding optical transparency, high LDT. The effective coefficient of (R-MBA)CuBr2 has been determined be ≈24.7 pm V-1 is orders magnitude higher than that CuII counterparts. This work shows the promising potential -based photonic wide wavelength regions.

Language: Английский

Citations

76

Zero‐Dimensional Organic Copper(I) Iodide Hybrid with High Anti‐Water Stability for Blue‐Light‐Excitable Solid‐State Lighting DOI
Binbin Su, Jiance Jin,

Yin-Hui Peng

et al.

Advanced Optical Materials, Journal Year: 2022, Volume and Issue: 10(12)

Published: April 21, 2022

Abstract The discovery of rare‐earth free luminescent materials with blue‐light‐excitable characteristic is great importance for solid‐sate lighting applications. Herein, a Cu(I)‐based 0D hybrid ( 1,3‐dppH 2 ) Cu 4 I 8 ∙H O synthesized by facile solution method, and it shows the orange‐red emission peaking at 625 nm upon 460 excitation. structure‐related luminescence mechanism has been elaborated experimental theoretical investigations. Moreover, intensity remains unchanged even after continuous water treatment 60 days due to improved structural stability originating from intermolecular π–π interaction between organic cations. A warm white light‐emitting diode (LED) device color rendering index 91.4% fabricated combining 440 LED chip, green‐emitting Lu 3 Al 5 12 :Ce 3+ , O. This work provides new design route towards cuprous halide will initiate more exploration their intrinsic mechanism.

Language: Английский

Citations

71

Moisture-Induced reversible structure conversion of Zero-Dimensional organic cuprous bromide hybrids for multiple photoluminescent anti-Counterfeiting, information encryption and rewritable luminescent paper DOI Creative Commons
Ye Tian, Hui Peng, Qilin Wei

et al.

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 458, P. 141436 - 141436

Published: Jan. 13, 2023

Language: Английский

Citations

62

2D Perovskite Mn2+‐Doped Cs2CdBr2Cl2 Scintillator for Low‐Dose High‐Resolution X‐ray Imaging DOI Open Access

Haiping Xu,

Wenqing Liang, Zhizhuan Zhang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(26)

Published: March 27, 2023

High-performance X-ray scintillators with low detection limits and high light yield are of great importance a challenge for low-dose imaging in medical diagnosis industrial detection. In this work, the synthesis new 2D perovskite, Cs2 CdBr2 Cl2 , via hydrothermal reaction is reported. By doping Mn2+ into yellow emission located at 593 nm obtained, photoluminescence quantum (PLQY) :5%Mn2+ perovskite reaches highest value 98.52%. The near-unity PLQY negligible self-absorption enable excellent scintillation performance 64 950 photons MeV-1 limit 17.82 nGyair s-1 . Moreover, combining poly(dimethylsiloxane) to fabricate flexible scintillator screen achieves resolution 12.3 line pairs (lp) mm-1 results suggest that promising candidate high-resolution imaging. study presents approach designing high-performance through metal-ion doping.

Language: Английский

Citations

57

Photophysical studies for Cu(i)-based halides: broad excitation bands and highly efficient single-component warm white-light-emitting diodes DOI Creative Commons

Shuigen Zhou,

Yihao Chen,

Kailei Li

et al.

Chemical Science, Journal Year: 2023, Volume and Issue: 14(20), P. 5415 - 5424

Published: Jan. 1, 2023

Designing and synthesizing cuprous halide phosphors unifying efficient low-energy emission a broad excitation band is still great challenge. Herein, by rational component design, three novel Cu(i)-based metal halides, DPCu4X6 [DP = (C6H10N2)4(H2PO2)6; X Cl, Br, I], were synthesized reacting p-phenylenediamine with (CuX), they show similar structures, consisting of isolated [Cu4X6]2- units separated organic layers. Photophysical studies uncover that the highly localized excitons rigid environment give rise to yellow-orange photoluminescence in all compounds spanning from 240 450 nm. The bright PL (X Br) originates self-trapped due strong electron-phonon coupling. Intriguingly, DPCu4I6 features dual-band emissive characteristic, attributed synergistic effect halide/metal-to-ligand charge-transfer (X/MLCT) triplet cluster-centered (3CC) excited states. Benefiting broadband excitation, high-performance white-light emitting diode (WLED) high color rendering index 85.1 was achieved using single-component phosphor. This work not only unveils role halogens photophysical processes but also provides new design principles for WLEDs.

Language: Английский

Citations

49

Multiphase Transformation in Hybrid Copper(I)-Based Halides Enable Improved X-ray Scintillation and Real-Time Imaging DOI
Bohan Li, Jiance Jin, Xia Liu

et al.

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 6(4), P. 1542 - 1548

Published: March 19, 2024

Crystal-glass phase transformation and glass recrystallization in zero-dimensional (0D) hybrid metal halides make them thriving X-ray scintillators with the advantages of large-area fabrication improved performance. Herein, we report three 0D copper(I) composed identical organic cations versatile self-assembly copper-iodide anions find that volumes inorganic groups are related to their lattice energies, which conformationally governed thermodynamics formation through destabilization. A subsequent heating counterparts allows bulk glass-ceramic via recrystallization, exhibiting outstanding scintillation performances (with a light yield 64 000 ph MeV–1 detection limit 72.6 nGy s–1) high stability for real-time imaging (spatial resolution above 20 lp mm–1). This multiphase strategy luminescence halide opens an exploratory way structural design engineering scintillator screens imaging.

Language: Английский

Citations

21

Highly Efficient Light‐Emitting Diodes Based on an Organic Antimony(III) Halide Hybrid DOI

Jin‐Long Li,

Y.L. Sang,

Liang‐Jin Xu

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 61(6)

Published: Nov. 16, 2021

As low-dimensional lead-free hybrids with higher stability and lower toxicity than those of three-dimensional lead perovskites, organic antimony(III) halides show great application potential in opt-electronic field owing to diverse topologies along exceptional optical properties. We report herein an hybrid (MePPh3 )2 SbCl5 a zero-dimensional (0D) structure, which exhibits brilliant orange emission peaked at 593 nm near-unity photoluminescent quantum yield (99.4 %). The characterization photophysical properties demonstrates that the broadband microsecond lifetime (3.24 μs) arises from self-trapped (STE). Electrically driven light-emitting diodes (OLEDs) based on neat doped films were fabricated. devices significant improvement comparison non-doped OLEDs. Owing much improved surface morphology balanced carrier transport layers devices, peak luminance, current efficiency (CE) external (EQE) are boosted 82 cd m-2 3500 , 1.1 A-1 6.8 0.7 % 3.1 relative respectively.

Language: Английский

Citations

95

Bright Cyan‐Emissive Copper(I)‐Halide Single Crystals for Multi‐Functional Applications DOI

Jun‐Hua Wei,

Yong‐Wei Yu,

Jianbin Luo

et al.

Advanced Optical Materials, Journal Year: 2022, Volume and Issue: 10(16)

Published: May 29, 2022

Abstract Anti‐counterfeiting has become a serious issue around the global world; fluorescence‐based tags are praised for low‐cost and facile decryption process. However, high‐level anti‐counterfeiting application requires incorporating multifunctional luminescent materials with response to different excitation sources. Herein, dimeric Cu(I)‐halide‐clusters‐assembled single‐crystal (AEP) 2 Cu I 6 ·2I·2H O (AEP = N ‐aminoethylpiperazinium) concerning high down‐conversion photoluminescence quantum yield (PLQY) value of near unity is reported (λ ex 305 nm), which can also be activated by near‐infrared light X‐ray. The ultrafast spectroscopy density functional theory calculations reveal that broad‐band emission originates from recombination self‐trapped excitons. Remarkably, PLQY excellent attenuation capability X‐ray confers an outstanding 55 650 photons MeV −1 O, 5.25 times higher than standard bismuth germaniumoxide scintillator. Such multi‐light‐stimulus endows great potential in anti‐counterfeiting, solid‐state lighting devices, digital radiography.

Language: Английский

Citations

69

Promoting Single Channel Photon Emission in Copper(I) Halide Clusters for X‐Ray Detection DOI
Kai Han, Jiance Jin, Binbin Su

et al.

Advanced Optical Materials, Journal Year: 2022, Volume and Issue: 10(20)

Published: July 15, 2022

Abstract Metal clusters with color‐tunable radioluminescence have attracted growing attention as X‐ray detection materials. However, they are generally less scintillation‐efficient due to the coexistence of multiple exciton recombination centers. Herein, two new zero‐dimensional copper(I)‐based (DIET) 3 Cu X (DIET = 1,3‐Diethyl‐2‐thiourea, Cl, Br) designed, which support single channel photon emission (Cu cluster centered, CC) enhance scintillation performance. Those DIET ligands (L) anchoring copper(I) ions not only generate direct CuL bonds, but also form a disorder [Cu ] cluster, results in intense absorption. Br low halogen electronegativity further weakens halogen‐to‐ligand charge transfer (XLCT) emission, enabling enhanced quantum efficiency (≈69%) and performance comparable commercially available Lu Al 5 O 12 :Ce. Moreover, flexible thin film counterpart demonstrates legible imaging high spatial resolution 11.71 lp mm −1 . This study provides feasible design principle discover metal cluster‐based scintillators expand their radiation applications.

Language: Английский

Citations

68