Reversible Triple-Mode Photo- and Radioluminescence and Nonlinear Optical Switching in Highly Efficient 0D Hybrid Cuprous Halides

Chemistry of Materials, Journal Year: 2023, Volume and Issue: 35(17), P. 6598 - 6611

Published: Aug. 17, 2023

Multifunctional stimuli-responsive luminescent and optical switching is extremely crucial for wide advanced photonic applications, but it remains a challenging objective halide perovskites. Herein, by performing single-crystal to (SC–SC) transformation as dynamic molecular strategy, we realized reversible triple-mode photoluminescence, radioluminescence (PL RL), nonlinear (NLO) in pair of zero-dimensional (0D) hybrid cuprous halides [ETPP]2Cu4Br6 [ETPP]CuBr2. Specifically, [ETPP]CuBr2 display highly efficient yellow green light emissions under UV excitation with the highest quantum yield up near unity. Simultaneously, identical can also be activated using X-ray RL 57,974 photons MeV–1, surpassing most previously reported halides. Most remarkably, SC–SC between them an ethanol impregnation-heating process, which provides PL/RL transitions two light-emitting states. Additionally, this process accompanied transition centrosymmetric NLO-inactive noncentrosymmetric NLO-active through second harmonic generation (SHG) "silent-active" switching. To best our knowledge, first PL, RL, SHG perovskite chemistry, realize applications data storage, information security, logic gates, etc.

Language: Английский

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High-resolution Tb³⁺-doped Gd-based oxyfluoride glass scintillators for X-ray imaging

Journal of Materials Chemistry C, Journal Year: 2023, Volume and Issue: 11(34), P. 11664 - 11670

Published: Jan. 1, 2023

SiBNaBaGd–5.0Tb glass scintillators with a high spatial resolution of 20 lp mm −1 and XEL intensity are reported.

Language: Английский

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Integrating Full‐Color 2D Optical Waveguide and Heterojunction Engineering in Halide Microsheets for Multichannel Photonic Logical Gates

Advanced Science, Journal Year: 2024, Volume and Issue: 11(17)

Published: Feb. 29, 2024

Ensuring information security has emerged as a paramount concern in contemporary human society. Substantial advancements this regard can be achieved by leveraging photonic signals the primary carriers, utilizing logical gates capable of wavelength tunability across various time and spatial domains. However, challenge remains rational design materials possessing space-time-color multiple-resolution capabilities. In work, facile approach is proposed for crafting metal-organic halides (MOHs) that offer resolution. These MOHs integrate time-resolved room temperature phosphorescence color-resolved excitation dependencies with both space-resolved ex situ optical waveguides heterojunctions. Capitalizing on these multifaceted properties, MOHs-based two-dimensional (2D) heterojunctions exhibit ability to tune full-color emissions spectra from blue red, operating within different temporal scales. Therefore, work introduces an effective methodology engineering resolved MOH microstructures, holding significant promise development high-density devices.

Language: Английский

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Organic Cation Design of Manganese Halide Hybrids Glass toward Low‐Temperature Integrated Efficient, Scaling, and Reproducible X‐Ray Detector

Advanced Optical Materials, Journal Year: 2023, Volume and Issue: 11(13)

Published: April 5, 2023

Abstract Zero‐dimensional (0D) structure‐based manganese metal halides (MHs) are believed to be the most promising candidates for next‐generation X‐ray scintillators due their intense radioluminescence and environmental friendliness. However, low‐temperature (<180 °C), large‐area integration with more efficient detection remains a tremendous challenge. Herein, from perspective of cation (ionic liquids) structure design, basic physical parameters 0D MHs regulated. And calculations experimental results demonstrate larger‐size cations that induce lower melting temperatures, larger exciton‐binding energies, ion migration energy, tunable hardness, which desirable MHscintillators. As result, champion materialHTP 2 MnBr 4 is achieved as glassy transparency wafer by (165 °C) melt‐quenching. Its application imaging features high spatial resolution (17.28 lp mm −1 ), scalability (>30 × 30 cm strong coupling force. Furthermore, HTP glass reproducible properties demonstrates light yield (38 000 photon MeV excellent irradiation stability, low limit (0.13 µGy s ). The authors believe this work will provide guidance MHscintillators further commercial applications.

Language: Английский

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All-inorganic Mn²⁺-doped metal halide perovskite crystals for the late-time detection of X-ray afterglow imaging

Nanoscale, Journal Year: 2023, Volume and Issue: 15(33), P. 13628 - 13634

Published: Jan. 1, 2023

All-inorganic metal halide perovskite (MHP) materials have been widely studied because of their unique optoelectronic properties, whereas there has little research reported on X-ray afterglow imaging properties. Herein, we report the design and synthesis Mn2+-doped hexagonal CsCdCl3 MHP crystals with excellent scintillation induced afterglow. The orange emission from Mn2+ shows a red shift due to strong interaction Mn2+-Mn2+ dimers formed at higher doping concentrations. high-energy X-rays electron filling capacity feed shallow (0.71 eV) deep (0.90-1.08 traps enable long for more than 300 min. can be rejuvenated effectively by 870 nm stimulus or heating even after 72 h decay. Finally, demonstrate proof-of-concept applications fabricated flexible scintillator films real-time online spatial resolution 12.2 lp mm-1, as well time-lapse recorded cell phone, which promise being able do offline late-time detection in future.

Language: Английский

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Zn²⁺ Doping in Organic Manganese(II) Bromide Hybrid Scintillators toward Enhanced Light Yield for X‐Ray Imaging

Advanced Optical Materials, Journal Year: 2023, Volume and Issue: 11(14)

Published: April 23, 2023

Abstract Metal halide scintillators have drawn great interest for X‐ray imaging; however, it remains challenging to simultaneously achieve a high light yield (LY) and highly sensitive detection. Herein, Zn 2+ is successfully introduced into [TPPen] 2 MnBr 4 (TPPMB, TPPen = pentyltriphenylphosphonium) the synthesis of Mn 0.9 0.1 Br (TPPMZB) designed. The LY increases from 43 000 TPPMB 68 photons MeV −1 TPPMZB in virtue atom doping. Additionally, detection limit 204.1 nGy s , showing improvement that with value 696.9 . imaging realized by utilizing large‐scale scintillator film fabricated mixing polydimethylsiloxane or TPPMB, spatial resolution enlarged 4.6 11.2 lp mm after ‐doping. This study provides design principle doping engineering enhancing property metal scintillators.

Language: Английский

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Organic–Inorganic Hybrid Glasses of Atomically Precise Nanoclusters

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(11), P. 7373 - 7385

Published: March 4, 2024

Organic–inorganic atomically precise nanoclusters provide indispensable building blocks for establishing structure–property links in hybrid condensed matter. However, robust glasses of ligand-protected nanocluster solids have yet to be demonstrated. Herein, we show [Cu4I4(PR3)4] cubane coordinated by phosphine ligands (PR3) form melt-quenched air with reversible crystal–liquid–glass transitions. Protective critically influence the glass formation mechanism, modulating glasses' physical properties. A utilizing ethyldiphenylphosphine-based nanoclusters, [Cu4I4(PPh2Et)4], exhibits superb optical properties, including >90% transmission both visible and near-infrared wavelengths, negligible self-absorption, near-unity quantum yield, high light yield. Experimental theoretical analyses demonstrate structural integrity [Cu4I4(PPh2Et)4] nanocluster, i.e., iodine-bridged tetranuclear cubane, has been fully preserved state. The strong internanocluster CH−π interactions found subsequently reduced vibration account its enhanced luminescence Moreover, this highly transparent enables performant X-ray imaging low-loss waveguiding fibers drawn above transition. discovery "nanocluster glass" opens avenues unraveling mechanisms designing novel luminescent well-defined advanced photonics.

Language: Английский

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White emission metal halides for flexible and transparent x-ray scintillators

Applied Physics Reviews, Journal Year: 2024, Volume and Issue: 11(1)

Published: Jan. 24, 2024

Flat-panel x-ray scintillators with a high spatial resolution at low radiation dose rate are desirable for efficient imaging applications in medical diagnostics, security inspection, and nondestructive inspection. To promote the progress of technologies, it is great interest to explore transparent reduced light scattering, yields, uniform radioluminescence. Herein, we design prepare novel lead-free (C12H28N)2Cu2I4 metal halide featuring luminescent efficiency white emission benefiting from double self-trapped exciton mechanism, which enable not only match response semiconductor-based sensors but also enhance yields decrease exposed doses objects. Furthermore, transparent, flexible large areas 20.25 cm2 demonstrate an outstanding scintillation performance including 19.8 lp mm−1 ultralow detection limit 28.39 nGyair s−1, ∼4 times higher 194 lower than typical values imaging, respectively. This work provides new route promising alternatives broadband opportunity develop technology.

Language: Английский

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Capillary Manganese Halide Needle‐Like Array Scintillator with Isolated Light Crosstalk for Micro‐X‐Ray Imaging

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(21)

Published: Feb. 10, 2024

Abstract The exacerbation of inherent light scattering with increasing scintillator thickness poses a major challenge for balancing the thickness‐dependent spatial resolution and scintillation brightness in X‐ray imaging scintillators. Herein, thick pixelated needle‐like array capable micrometer is fabricated via waveguide structure engineering. Specifically, this involves integrating straightforward low‐temperature melting process manganese halide an aluminum‐clad capillary template. In structure, oriented photons propagate along well‐aligned are confined within individual pixels by aluminum reflective cladding, as substantiated from comprehensive analysis including laser diffraction experiments. Consequently, thanks to isolated light‐crosstalk channels robust output due increased thickness, ultrahigh resolutions 60.8 51.7 lp mm −1 at modulation transfer function (MTF) 0.2 achieved on 0.5 even 1 scintillators, respectively, which both exceed pore diameter arrays’ template ( Φ = 10 µm). As far it known, these among highest reported metal scintillators never demonstrated such Here avenue presented demand high‐resolution across diverse scientific practical fields.

Language: Английский

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Multiphase Transformation in Hybrid Copper(I)-Based Halides Enable Improved X-ray Scintillation and Real-Time Imaging

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

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