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Journal ArticleDOI: 10.1038/S41566-021-00769-Z

Composite fast scintillators based on high-Z fluorescent metal–organic framework nanocrystals

04 Mar 2021-Nature Photonics (Nature Publishing Group)-Vol. 15, Iss: 5, pp 393-400
Abstract: Scintillators, materials that produce light pulses upon interaction with ionizing radiation, are widely employed in radiation detectors. In advanced medical-imaging technologies, fast scintillators enabling a time resolution of tens of picoseconds are required to achieve high-resolution imaging at the millimetre length scale. Here we demonstrate that composite materials based on fluorescent metal–organic framework (MOF) nanocrystals can work as fast scintillators. We present a prototype scintillator fabricated by embedding MOF nanocrystals in a polymer. The MOF comprises zirconium oxo-hydroxy clusters, high-Z linking nodes interacting with the ionizing radiation, arranged in an orderly fashion at a nanometric distance from 9,10-diphenylanthracene ligand emitters. Their incorporation in the framework enables fast sensitization of the ligand fluorescence, thus avoiding issues typically arising from the intimate mixing of complementary elements. This proof-of-concept prototype device shows an ultrafast scintillation rise time of ~50 ps, thus supporting the development of new scintillators based on engineered fluorescent MOF nanocrystals. Composites of fluorescent metal–organic framework nanocrystals in a polymer are exploited to create fast scintillators with a rise time of about 50 ps.

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8 results found


Open accessDOI: 10.1016/J.MATT.2021.11.012
02 Dec 2021-
Abstract: Summary In this work, we describe a highly efficient and reabsorption-free X-ray-harvesting system using luminescent metal-organic framework (MOF)-fluorescence chromophore composite films. The ultrafast time-resolved experiments and density functional theory calculations demonstrate that a nearly 100% energy transfer from a luminescent MOF with a high atomic number to an organic chromophore with thermally activated delayed fluorescence (TADF) character can be achieved. Such an unprecedented efficiency of interfacial energy transfer and the direct harnessing of singlet and triplet excitons of the TADF chromophore led to remarkable enhancement of radioluminescence upon X-ray radiation. A low detection limit of 256 nGy/s of the fabricated X-ray imaging scintillator was achieved, about 60 times lower than the MOF and 7 times lower than the organic chromophore counterparts. More importantly, this detection limit is about 22 times lower than the standard dosage for a medical examination, making it an excellent candidate for X-ray radiography.

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Topics: Chromophore (55%), Radioluminescence (51%)

1 Citations


Open accessJournal ArticleDOI: 10.3390/APP11157073
30 Jul 2021-Applied Sciences
Abstract: Nanomedicine is emerging as promising approach for the implementation of oncological methods. In this review, we describe the most recent methods exploiting heavy nanoparticles and hybrid nanomaterials aiming at improving the traditional X-rays-based treatments. High-Z nanoparticles are proposed as radiosensitizers due to their ability to stop the ionizing radiation and to increase the locally delivered therapeutic dose. Other nanoparticles working as catalysts can generate reactive oxygen species upon X-rays exposure. Thanks to their high toxicity and reactivity, these species promote DNA cancer cells damage and apoptosis. Hybrid nanoparticles, composed by scintillators coupled to organic molecules, are suitable in X-rays activated photodynamic therapy. This work highlights the roles played by the diverse nanoparticles, upon ionizing radiation irradiation, according to their physico-chemical properties, surface functionalization, and targeting strategies. The description of nanoparticle qualities demanded by the oncological nanomedicine is presented in relation to the processes occurring in biological medium when X-ray radiation interacts with heavy nanoparticles, including the scintillation mechanisms, the stopping power amplification, and the disputed modeling of the effective deposit of energy within nanomaterials. The comprehension of these issues in nanomedicine drives the strategies of nanoparticles engineering and paves the way for the development of advanced medical therapies.

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Topics: Nanomedicine (60%)

Journal ArticleDOI: 10.1002/SMLL.202103516
Jianxin Ma1, Jianxin Ma2, Tong Shu3, Tong Shu1  +6 moreInstitutions (3)
03 Oct 2021-Small
Abstract: Luminescent covalent organic frameworks (LCOFs) have attracted significant attention due to their tunability of structures and photophysical properties at molecular level. LCOFs are built to highly ordered and periodic 2D or 3D framework structures through covalently assembling with various luminophore building blocks. Recently, the advantages of LCOFs including predesigned properties of structure, unique photoluminescence, hypotoxicity and good biocompatibility and tumor penetration, broaden their applications in biorelated fields, such as biosensing, bioimaging, and drug delivery. A specific review that analyses the advances of LCOFs in the field of biosensing and bioimaging is thus urged to emerge. Here the construction of LCOFs is reviewed first. The synthetic chemistry of LCOFs highlights the key role of chemical linkages, which not only concrete the building blocks but also affect the optical properties and even can act as the responsive sites for potential sensing applications. How to brighten LCOFs are clarified through description of structure managements. The ability to utilize the luminescence of LCOFs for applications in biosensing and bioimaging is discussed using state-of-the-art examples of varied practical goals. A prospect finally addresses opportunities and challenges the development of LCOFs facing from chemistry, physics to the applications, according to their current progress.

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Open accessJournal ArticleDOI: 10.1016/J.JLUMIN.2021.118589
Xiaofeng Chen1, Xiaokun Li1, Xiaoling Chen1, Zhijian Yang1  +9 moreInstitutions (2)
Abstract: : Colloidal nanocrystal scintillators hold great potential in fabricating large-area, flexible X-ray detectors for high-resolution X-ray imaging of highly curved, irregularly shaped objects. The synthesis of high-efficiency, high-stability nanoscintillators is of great importance for the development of X-ray imaging detectors. In this study, we develop a class of cerium (Ce3+)-sensitized core-shell nanoscintillators that are suitable for achieving flexible X-ray luminescence imaging. We demonstrate that an epitaxial growth of NaGdF4:Ce(60%) on the surface of NaGdF4:Eu(15%) nanoscintillators as a sensitization layer allows for enhancing X-ray-induced radioluminescence. We reveal that the enhancement of X-ray luminescence in nanoscintillators could be attributed to the synergistic effect of high-Z composition-induced X-ray absorption, Ce3+ sensitization, and surface passivation to relieve energy quenching. By incorporating the nanoscintillators into a flexible elastomer of polydimethylsiloxane (PDMS), we demonstrate its utility in high-resolution flexible X-ray luminescence imaging.

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Topics: Energy quenching (52%), Luminescence (50%)

Journal ArticleDOI: 10.1002/ANIE.202109802
Chaomin Dong1, Xiao Wang2, Wenqi Gong1, Wenbo Ma3  +15 moreInstitutions (4)
17 Sep 2021-Angewandte Chemie
Abstract: There are few reports about purely organic phosphorescence scintillators, and the relationship between molecular structures and radioluminescence in organic scintillators is still unclear. Here, we presented isomerism strategy to study the effect of molecular structures on radioluminescence. The isomers can achieve phosphorescence efficiency of up to 22.8 % by ultraviolet irradiation. Under X-ray irradiation, both m-BA and p-BA show excellent radioluminescence, while o-BA has almost no radioluminescence. Through experimental and theoretical investigation, we found that radioluminescence was not only affected by non-radiation in emissive process, but also highly depended on the material conductivity caused by the different molecular packing. This study not only allows us to clearly understand the relationship between the molecular structures and radioluminescence, but also provides a guidance to rationally design new organic scintillators.

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Topics: Radioluminescence (69%)

References
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52 results found


Journal ArticleDOI: 10.1002/ANIE.200300610
26 Apr 2004-Angewandte Chemie
Abstract: The chemistry of the coordination polymers has in recent years advanced extensively, affording various architectures, which are constructed from a variety of molecular building blocks with different interactions between them. The next challenge is the chemical and physical functionalization of these architectures, through the porous properties of the frameworks. This review concentrates on three aspects of coordination polymers: 1). the use of crystal engineering to construct porous frameworks from connectors and linkers ("nanospace engineering"), 2). characterizing and cataloging the porous properties by functions for storage, exchange, separation, etc., and 3). the next generation of porous functions based on dynamic crystal transformations caused by guest molecules or physical stimuli. Our aim is to present the state of the art chemistry and physics of and in the micropores of porous coordination polymers.

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Topics: Metal-organic framework (52%)

9,050 Citations


Open accessJournal ArticleDOI: 10.1038/NATURE01650
Omar M. Yaghi1, Michael O'Keeffe2, Nathan W. Ockwig1, Hee K. Chae3  +3 moreInstitutions (3)
12 Jun 2003-Nature
Abstract: The long-standing challenge of designing and constructing new crystalline solid-state materials from molecular building blocks is just beginning to be addressed with success. A conceptual approach that requires the use of secondary building units to direct the assembly of ordered frameworks epitomizes this process: we call this approach reticular synthesis. This chemistry has yielded materials designed to have predetermined structures, compositions and properties. In particular, highly porous frameworks held together by strong metal-oxygen-carbon bonds and with exceptionally large surface area and capacity for gas storage have been prepared and their pore metrics systematically varied and functionalized.

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7,384 Citations


Journal ArticleDOI: 10.1039/B618320B
Gerard Ferey1Institutions (1)
Abstract: This critical review will be of interest to the experts in porous solids (including catalysis), but also solid state chemists and physicists. It presents the state-of-the-art on hybrid porous solids, their advantages, their new routes of synthesis, the structural concepts useful for their ‘design’, aiming at reaching very large pores. Their dynamic properties and the possibility of predicting their structure are described. The large tunability of the pore size leads to unprecedented properties and applications. They concern adsorption of species, storage and delivery and the physical properties of the dense phases. (323 references)

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4,877 Citations


Journal ArticleDOI: 10.1021/CR200101D
08 Feb 2012-Chemical Reviews
Topics: Luminescent Measurements (67%)

4,507 Citations


Open accessBook
02 Dec 1999-
Abstract: The first edition of Pope and Swenberg's Electronic Processes of Organic Crystals, published in 1982, became the classic reference in the field. It provides a tutorial on the experimental and related theoretical properties of aromatic hydrocarbon crystals and includes emerging work on polymers and superconductivity. This new edition has been expanded to cover the major theoretical and experimental advances over the last fifteen years. It contains a unified description of what is known in almost every aspect of the field. The basic phenomena covered in the first edition included fluorescence, exciton and charge carrier generation, transport, recombination, and photoemission; the new edition adds solitons, polarons, bipolarons, spin waves, and charge density waves. It provides in-depth coverage of such model polymers such as polyacetylene, polydiacetylene, poly (phenylene-vinylene), polyanilines, polysilanes, and fullerenes. It also provides detailed treatments of the expanding areas of electroluminescence, non-linear optics, organic magnets, organic superconductors, and Langmuir-Blodgett films. In addition, it contains a chapter on major applications, including LED's, photocopiers, photoconductors, batteries, transistors, liquid crystals, photorefractive devices, and sensors. As in the first volume, the authors take informed positions in controversial areas. This book will be an essential reference for organic material scientists, whether they are experienced researchers or just entering the field. It will also be a reliable guide to anyone interested in this rapidly growing field

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1,706 Citations


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20217