Highly Efficient Stable Luminescent Radical-Based X-ray Scintillator

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(49), С. 27095 - 27102

Опубликована: Ноя. 28, 2023

Stable luminescent radicals are open-shell emitters with unique doublet emission characteristics. This feature makes stable exhibit widespread application prospects in constructing optical, electrical, and magnetic materials. In this work, a radical-based X-ray scintillator of AuPP-1.0 was prepared, which exhibited high excited luminescence (XEL) efficiency as well excellent stability. A mechanism study showed that the heavy atom Au endowed it effective absorption X-rays, characteristics significantly increased its exciton utilization rate radioluminescence process. Moreover, has good processability to fabricate flexible screen for high-quality imaging, whose resolution can reach 20 LP mm-1. work demonstrates is beneficial improving radioluminescence, providing brand-new strategy construction high-performance scintillators.

Язык: Английский

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High-Efficiency Circularly Polarized Light-Emitting Diodes Based on Chiral Metal Nanoclusters

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(6), С. 4144 - 4152

Опубликована: Фев. 5, 2024

Circularly polarized light-emitting diodes (CP-LEDs) are critical for next-generation optical technologies, ranging from holography to quantum information processing. Currently deployed chiral luminescent materials, with their intricate synthesis and processing limited efficiency, the main bottleneck CP-LEDs. Chiral metal nanoclusters (MNCs) potential CP-LED given ease of processability as well diverse structures excited states. However, films usually plagued by inferior electronic quality aggregation-caused photoluminescence quenching, necessitating incorporation into host materials; without such a scheme, MNC-based LEDs exhibit external efficiencies (EQEs) < 10%. Herein, we achieve an efficiency leap both CP-LEDs cluster-based using novel MNCs aggregation-induced emission enhancement. enantiopure MNC attain EQEs up 23.5%. Furthermore, incorporating devices yield record 36.5% LEDs, along electroluminescence dissymmetry factors (|gEL|) around 1.0 × 10–3. These findings open new avenue advancing light sources optoelectronics.

Язык: 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, Год журнала: 2024, Номер 6(4), С. 1542 - 1548

Опубликована: Март 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.

Язык: Английский

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Isostructural Nanocluster Manipulation Reveals Pivotal Role of One Surface Atom in Click Chemistry

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(37)

Опубликована: Июль 20, 2023

Elucidating single-atom effects on the fundamental properties of nanoparticles is challenging because modifications are typically accompanied by appreciable changes to overall particle's structure. Herein, we report synthesis a [Cu58 H20 PET36 (PPh3 )4 ]2+ (Cu58 ; PET: phenylethanethiolate; PPh3 : triphenylphosphine) nanocluster-an atomically precise nanoparticle-that can be transformed into surface-defective analog [Cu57 ]+ (Cu57 ). Both nanoclusters virtually identical, with five concentric metal shells, save for one missing surface copper atom in Cu57 . Remarkably, loss this single drastically alters reactivity nanocluster. In contrast Cu58 , shows promising activity click chemistry, particularly photoinduced [3+2] azide-alkyne cycloaddition (AAC), which attributed active catalytic site after removal atom. Our study not only presents unique system uncovering effect single-surface modification nanoparticle but also showcases as powerful means designing catalysts.

Язык: Английский

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High‐Confidentiality X‐Ray Imaging Encryption Using Prolonged Imperceptible Radioluminescence Memory Scintillators

Advanced Materials, Год журнала: 2023, Номер 35(52)

Опубликована: Ноя. 11, 2023

X-ray imaging plays an increasingly crucial role in clinical radiography, industrial inspection, and military applications. However, current technologies have difficulty protecting against information leakage caused by brute force attacks via trial-and-error. Here high-confidentiality encryption fabricating ultralong radioluminescence memory films composed of lanthanide-activated nanoscintillators (NaLuF4 : Gd3+ or Ce3+ ) with imperceptible purely-ultraviolet (UV) emission is reported. Mechanistic investigations unveil that attributed to the long-lived trapping thermalized charge carriers within Frenkel defect states subsequent slow release form radioluminescence. The encrypted can be securely stored film for more than 7 days optically decoded perovskite nanocrystal. Importantly, this strategy protect trial-and-error through perception lifetime change persistent It further demonstrated as-fabricated flexible enables achieving 3D curved objects a high spatial resolution 20 lp/mm excellent recyclability. This study provides valuable insights into fundamental understanding X-ray-to-UV conversion nanocrystal lattices opens up new avenue toward development high-confidential technologies.

Язык: Английский

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Hybrid Thermally Activated Nanocluster Fluorophores for X-ray Scintillators

ACS Energy Letters, Год журнала: 2023, Номер 8(12), С. 5088 - 5097

Опубликована: Ноя. 9, 2023

Thermally activated delayed fluorescence (TADF) X-ray scintillators have attracted increasing attention because of their theoretical ability to utilize 100% radiation-induced excitons. However, scintillation performance is severely hampered by typically low attenuation efficiencies or mechanochromic properties. Here, we demonstrate hybrid organic–inorganic TADF with remarkably high absorption cross sections based on non-mechanochromic Cu2X2 (X = Cl, Br, I) nanoclusters. The nanoclusters display radioluminescence light yields as 175 000 photons MeV–1, attributable self-absorption and spatially separated HOMO LUMO orbitals. Furthermore, properties, these can be formed into scintillating screens excellent radiation humidity stability via soft-pressing. fabricated a imaging efficiency, benefiting from spatial resolutions (∼30 lp mm–1). This work highlights the promise nanocluster-based in meeting demanding requirements cutting-edge imaging.

Язык: Английский

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Anchoring the AIEgen by Zr clusters in metal-organic gel for efficient X-ray detection and imaging

Chem, Год журнала: 2024, Номер 10(4), С. 1268 - 1278

Опубликована: Фев. 21, 2024

Язык: Английский

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Fluorescence resonance energy transfer in atomically precise metal nanoclusters by cocrystallization-induced spatial confinement

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Июнь 24, 2024

Abstract Understanding the fluorescence resonance energy transfer (FRET) of metal nanoparticles at atomic level has long been a challenge due to lack accurate systems with definite distance and orientation molecules. Here we present realization achieving FRET between two atomically precise copper nanoclusters through cocrystallization-induced spatial confinement. In this study, demonstrate establishment in cocrystallized Cu 8 ( p -MBT) (PPh 3 ) 4 @Cu 10 system by exploiting overlapping spectra excitation cluster emission cluster, combined control over confined space nanoclusters. Density functional theory is employed provide deeper insights into role dipole orientations molecules illustrate procedure electronic structure level.

Язык: Английский

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Thermally Activated Delayed Fluorescent Ag(I) Complexes for Highly Efficient Scintillation and High‐Resolution X‐Ray Imaging

Advanced Functional Materials, Год журнала: 2024, Номер 34(33)

Опубликована: Март 25, 2024

Abstract Organic thermally activated delayed fluorescent (TADF) scintillators hold promising potential for applications in medical radiography and security detection, but the poor X‐ray absorption ability inferior radioluminescence (RL) hampered their progression. Herein, study has pioneered development of high‐performance TADF Ag(I)‐based from M 2 X (dppb) (M = Ag, Cu; Cl, Br, I) complexes with 1,2‐Bis(diphenylphosphino)benzene ligand. In comparison Cu(I) complexes, Ag(I) series generally exhibited superior scintillation performance. Notably, Ag Cl (Ag1) stands out exceptionally high RL intensity (≈125% higher than that CsI:Tl) a low detection limit 59.8 nGy s −1 . The outstanding performance Ag1 is primarily attributed to synergistic effect exciton utilization efficiency origin small singlet‐triplet energy gap, enhanced capacity by heavy atoms, photoluminescence quantum yield (76.47% ambient atmosphere). By fabricating flexible film constructed submicron crystalline powders, spatial resolution 25.0 lp mm imaging obtained. It offers new opportunities utilizing metal–organic highly efficient imaging.

Язык: Английский

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Triplet–triplet annihilation-based photon upconversion using nanoparticles and nanoclusters

Materials Horizons, Год журнала: 2024, Номер 11(10), С. 2304 - 2322

Опубликована: Янв. 1, 2024

The phenomenon of photon upconversion (UC), generating high-energy photons from low-energy photons, has attracted significant attention. In particular, triplet-triplet annihilation-based UC (TTA-UC) been achieved by combining the excitation states two types molecules, called sensitizer and emitter (or annihilator). With TTA-UC, it is possible to convert weak, incoherent near-infrared (NIR) light, which constitutes half solar radiation intensity, into ultraviolet visible light that are suitable for operation light-responsive functional materials or devices such as cells photocatalysts. Research on TTA-UC being conducted worldwide, often employing with high intersystem crossing rates, metal porphyrins, sensitizers. This review summarizes recent research trends in triplet energy transfer semiconductor nanoparticles nanocrystals diameters nanometer range, also known quantum dots, ligand-protected nanoclusters, have even smaller well-defined sub-nanostructures. Concerning nanoparticles, transmitter ligands applied surface efficiently excitons formed inside emitters. Applications expanding solid-state NIR light. Additionally, there active development sensitizers using more cost-effective environmentally friendly elements. Regarding methods established evaluation excited states, deepening understanding luminescent properties relaxation processes.

Язык: Английский

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