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学者姓名：林梅金
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Abstract ：
The architectural design and fabrication of low-cost, high-performance organic scintillators are critical for medical imaging and material/device analysis. However, achieving large-area and high-transparency organic scintillators in a low-cost and easy-to-implement method remains a challenge. Herein, a new design strategy for regulating the side chain length of maleimide derivatives is demonstrated to develop organic scintillators for achieving low-cost, large-area, and high spatial resolution in X-ray imaging. The effective intermolecular interactions and relatively twisted molecular structure endow PAM-M4 molecule with outstanding scintillator properties. More importantly, as demonstrated for the first time, pure organic glassy films with a diameter over 10 cm and high optical transparency can be prepared by the developed melt-quenched method using PAM-M4 crystal powder as a raw material. This glassy film exhibits excellent X-ray imaging ability with a spatial resolution as high as 27.0 lp mm-1 at MTF = 0.20, which is one of the best results among reported organic scintillators. The results of this work not only develop a new design strategy for high-performance organic scintillators but also demonstrate a reliable approach to fabricating large area screens with superior spatial resolution for medical or industrial X-ray imaging applications. A maleimide-based scintillator can be easily synthesized and exhibits a fast scintillation decay time of 12.38 ns, a high PLQY of 87.6%, and a low detection limit of 0.14 mu Gy s-1. By using the melt-quenched method, PAM-M4 crystal can turn into a large-area glassy film. This glassy film exhibits a transmittance of over 90%, along with a resolution of 27.0 lp mm-1 for X-ray imaging, which represents the state-of-the-art performance for organic scintillators. image
Keyword ：
fluorescence fluorescence maleimide derivatives maleimide derivatives organic glassy scintillators organic glassy scintillators X-ray imaging X-ray imaging
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| GB/T 7714 | Quan, Xin , Zhang, Guo-Zhen , Zhang, Yang et al. Low-Cost, Large-Area, and Highly Transparent Organic Glassy Scintillators for High Resolution X-Ray Imaging [J]. | ADVANCED OPTICAL MATERIALS , 2024 , 12 (18) . |
| MLA | Quan, Xin et al. "Low-Cost, Large-Area, and Highly Transparent Organic Glassy Scintillators for High Resolution X-Ray Imaging" . | ADVANCED OPTICAL MATERIALS 12 . 18 (2024) . |
| APA | Quan, Xin , Zhang, Guo-Zhen , Zhang, Yang , Liao, Qing , Chen, Hong-Ming , Lin, Mei-Jin . Low-Cost, Large-Area, and Highly Transparent Organic Glassy Scintillators for High Resolution X-Ray Imaging . | ADVANCED OPTICAL MATERIALS , 2024 , 12 (18) . |
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Cuprous complex scintillators show promise for X-ray detection with abundant raw materials, diverse luminescent mechanisms, and adjustable structures. However, their synthesis typically requires a significant amount of organic solvents, which conflict with green chemistry principles. Herein, we present the synthesis of two high-performance cuprous complex scintillators using a simple mechanochemical method for the first time, namely [CuI(PPh3)(2)R] (R = 4-phenylpyridine hydroiodide (PH, Cu-1) and 4-(4-bromophenyl)pyridine hydroiodide (PH-Br, Cu-2). Both materials demonstrated remarkable scintillation performances, exhibiting radioluminescence (RL) intensities 1.52 times (Cu-1) and 2.52 times (Cu-2) greater than those of Bi4Ge3O12 (BGO), respectively. Compared to Cu-1, the enhanced RL performance of Cu-2 can be ascribed to its elevated quantum yield of 51.54%, significantly surpassing that of Cu-1 at 37.75%. This excellent luminescent performance is derived from the introduction of PH-Br, providing a more diverse array of intermolecular interactions that effectively constrain molecular vibration and rotation, further suppressing the nonradiative transition process. Furthermore, Cu-2 powder can be prepared into scintillator film with excellent X-ray imaging capabilities. This work establishes a pathway for the rapid, eco-friendly, and cost-effective synthesis of high-performance cuprous complex scintillators.
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| GB/T 7714 | Chen, Yue-Chen , Yuan, Si-Qi , Zhang, Guo-Zhen et al. Mechanochemical Synthesis of Cuprous Complexes for X-ray Scintillation and Imaging [J]. | INORGANIC CHEMISTRY , 2024 , 63 (7) : 3572-3577 . |
| MLA | Chen, Yue-Chen et al. "Mechanochemical Synthesis of Cuprous Complexes for X-ray Scintillation and Imaging" . | INORGANIC CHEMISTRY 63 . 7 (2024) : 3572-3577 . |
| APA | Chen, Yue-Chen , Yuan, Si-Qi , Zhang, Guo-Zhen , Di, Yi-Ming , Qiu, Qiang-Wen , Yang, Xi et al. Mechanochemical Synthesis of Cuprous Complexes for X-ray Scintillation and Imaging . | INORGANIC CHEMISTRY , 2024 , 63 (7) , 3572-3577 . |
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Correction for 'Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging' by Yu-Hua Chen et al., Chem. Sci., 2024, https://doi.org/10.1039/d4sc00735b.
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| GB/T 7714 | Chen, Yu-Hua , Zhang, Guo-Zhen , Chen, Fu-Hai et al. Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging (20 Apr, 10.1039/d4sc00735b, 2024) [J]. | CHEMICAL SCIENCE , 2024 , 15 (21) : 8249-8249 . |
| MLA | Chen, Yu-Hua et al. "Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging (20 Apr, 10.1039/d4sc00735b, 2024)" . | CHEMICAL SCIENCE 15 . 21 (2024) : 8249-8249 . |
| APA | Chen, Yu-Hua , Zhang, Guo-Zhen , Chen, Fu-Hai , Zhang, Shu-Quan , Fang, Xin , Chen, Hong-Ming et al. Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging (20 Apr, 10.1039/d4sc00735b, 2024) . | CHEMICAL SCIENCE , 2024 , 15 (21) , 8249-8249 . |
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Phosphates are ideal candidates in the search for deep ultraviolet (DUV) nonlinear optical (NLO) materials due to their wide DUV transmission. However, the small optical anisotropy of the highly symmetric [PO4](3-) tetrahedron hinders phase matching (PM) in the DUV wavelength range. In this work, the polar tetrahedron [PO2(NHCONH2)(2)](-), which combines the pi-conjugated urea unit and the non-pi-conjugated [PO4](3-) unit via covalent bonds, is proposed as a new DUV NLO-active unit. [PO2(NHCONH2)(2)](-) tetrahedron exhibits greatly improved polarizability, anisotropy, and hyperpolarizability while maintaining a large highest occupied molecular orbital-lowest unoccupied molecular orbital gap. Accordingly, two DUV transparent alkali metal N, N-bis(aminocarbonyl)-phosphorodiamidates [A[PO2(NHCONH2)(2)] (A = K, Rb)] are screened out, and their nonlinear properties are systematically evaluated by first-principles methods. The results show that K[PO2(NHCONH2)(2)] (KPOU) achieves significant enhancements in multiple properties compared to the existing phosphate DUV NLO materials, including a strong SHG effect (3.44 x KDP) and the largest birefringence (0.088@532 nm) for DUV PM. Moreover, the shortest PM wavelength (lambda(PM)) of KPOU is 196 nm, making it a promising DUV NLO candidate for practical applications. This work proposes an excellent NLO-active unit and offers a new direction for exploring novel high-performance DUV NLO materials.
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| GB/T 7714 | Chen, Fuhai , Mo, Fuxiang , Chen, Hongming et al. KPO2(NHCONH2)2: A Promising Deep-Ultraviolet Nonlinear Optical Phosphate Containing Polar [PO2(NHCONH2)2]- Tetrahedra [J]. | CHEMISTRY OF MATERIALS , 2024 , 36 (6) : 2985-2992 . |
| MLA | Chen, Fuhai et al. "KPO2(NHCONH2)2: A Promising Deep-Ultraviolet Nonlinear Optical Phosphate Containing Polar [PO2(NHCONH2)2]- Tetrahedra" . | CHEMISTRY OF MATERIALS 36 . 6 (2024) : 2985-2992 . |
| APA | Chen, Fuhai , Mo, Fuxiang , Chen, Hongming , Lin, Mei-Jin , Chen, Yong . KPO2(NHCONH2)2: A Promising Deep-Ultraviolet Nonlinear Optical Phosphate Containing Polar [PO2(NHCONH2)2]- Tetrahedra . | CHEMISTRY OF MATERIALS , 2024 , 36 (6) , 2985-2992 . |
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Surface defects induce non-radiative charge recombination and reduce the photovoltaic performance of perovskite solar cells (PSCs). To realize highly efficient and stable PSCs, surface passivation is an effective strategy to reduce defects in mixed halide perovskite films. Organic iodides have emerged as valuable candidates for perovskite surface passivation owing to their facile preparation, optimal lattice matching with perovskites, and robust defect passivation capability. Here, a novel phthalimide N-alkylammonium iodide (PAE-I) is introduced as a passivating agent for the defects on the surface of FAPbI(3) perovskite films. The incorporated PAE-I layer effectively passivates interface traps and reduces non-radiative recombination, improving carrier extraction and transfer. As a result, the power conversion efficiency (PCE) of PSCs increases from 19.76% to 21.30%. Furthermore, the PAE-I-passivated PSCs without encapsulation exhibit excellent long-term stability, retaining 80% of the initial efficiency after 2400 hours under an ambient atmosphere. This work provides deep insights into the reduction of non-radiative recombination and the enhancement of device performance through the application of phthalimide as a superior and promising passivator.
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| GB/T 7714 | Wang, Yao , Chen, Shan-Ci , Tai, Shuya et al. Improving the performance and stability of perovskite solar cells via surface passivation of phthalimide N-alkylammonium iodides [J]. | JOURNAL OF MATERIALS CHEMISTRY C , 2024 , 12 (18) : 6540-6547 . |
| MLA | Wang, Yao et al. "Improving the performance and stability of perovskite solar cells via surface passivation of phthalimide N-alkylammonium iodides" . | JOURNAL OF MATERIALS CHEMISTRY C 12 . 18 (2024) : 6540-6547 . |
| APA | Wang, Yao , Chen, Shan-Ci , Tai, Shuya , Wang, Di , Ma, Yunlong , Wu, Jishan et al. Improving the performance and stability of perovskite solar cells via surface passivation of phthalimide N-alkylammonium iodides . | JOURNAL OF MATERIALS CHEMISTRY C , 2024 , 12 (18) , 6540-6547 . |
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Organic scintillators, pivotal in security and medical applications, face challenges due to limited X-ray absorption and exciton utilization. Herein, a novel class of organic scintillators is introduced, named guest-induced thermally activated delayed fluorescence (TADF) within supramolecular macrocycles via host-guest through-space charge transfer (TSCT). Four co-crystals are obtained through orthogonal crystallizations involving calix[3]acridan (C[3]A) and calix[3]phenothiazine (C[3]P) macrocycles as hosts, along with 1,2-dicyanobenzene (DCB) and 4-bromo-1,2-benzenedicarbonitrile (BrDCB) as guests. Interestingly, DCB@C[3]A and BrDCB@C[3]A co-crystals exhibit strong host-guest TSCT with reduced single-triplet energy gap for efficient TADF emission, which leads to enhanced exciton utilization and X-ray absorption, yielding radioluminescence intensities over 29 and 25 times higher than C[3]A. Similarly, substituting C[3]A with C[3]P, the obtained TADF co-crystals also outperform C[3]P in scintillation performance. Additionally, the scintillation color of co-crystals can be adjusted by varying the electron-donating abilities of macrocycles and the electron-accepting abilities of guests, offering a simpler color-tuning mechanism than covalent-bonded scintillators. Furthermore, the flexible film based on DCB@C[3]A exhibits promising application in X-ray radiography, showcasing a high spatial resolution of 20 lp mm-1 @MTF = 0.77. The innovative strategy of fabricating organic scintillators via reversible non-covalent interactions presents a novel solution for designing color-tunable and high-performance scintillators. The Table of Contents (TOC) image illustrates that novel organic supramolcular macrocycle scintillators with guest-induced TADF emission via host-guest through-space charge transfers, enabling efficient and color-tunable X-ray luminescence, as well as high-resolution imaging of 20 lp mm-1 in devices. image
Keyword ：
organic scintillators organic scintillators supramolecular macrocycles supramolecular macrocycles thermally activated delayed fluorescence thermally activated delayed fluorescence through-space charge transfers through-space charge transfers X-ray imaging X-ray imaging
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| GB/T 7714 | Zhang, Guozhen , Chen, Fuhai , Di, Yiming et al. Guest-Induced Thermally Activated Delayed Fluorescence Organic Supramolcular Macrocycle Scintillators for High-Resolution X-Ray Imaging [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (41) . |
| MLA | Zhang, Guozhen et al. "Guest-Induced Thermally Activated Delayed Fluorescence Organic Supramolcular Macrocycle Scintillators for High-Resolution X-Ray Imaging" . | ADVANCED FUNCTIONAL MATERIALS 34 . 41 (2024) . |
| APA | Zhang, Guozhen , Chen, Fuhai , Di, Yiming , Yuan, Siqi , Zhang, Yang , Quan, Xin et al. Guest-Induced Thermally Activated Delayed Fluorescence Organic Supramolcular Macrocycle Scintillators for High-Resolution X-Ray Imaging . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (41) . |
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As an emerging class of hybrid complexes, donor-acceptor (D-A) hybrid heterostructures, which combine the advantages of both organic and inorganic photoactive components, provide excellent platforms for the fabrication of photochromic materials with enhanced photo-responsive performances. Herein, four novel hybrid heterostructures, namely H3TPT(PW12O40)2NMP (1), (H1.5TPT)(2)(PW12O40) (2), (H3TPT)(2)(SiW12O40)2Cl2MeCN (3), and H3TPT(HPMo12O40)Cl3NMP (4) (TPT is tri(4-pyridyl)-s-triazine, NMP is N-methylpyrrolidone), have been synthesized and characterized. Benefitting from the strong interactions (anion-pi interactions) and matching electron energy levels between the donors and acceptors, some of them exhibited ultrafast photochromic behaviour even up to 1 second. Furthermore, based on experimental and theoretical calculations, the plausible PIET process and structure-activity relationship have been discussed in detail.
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| GB/T 7714 | Chen, Yue-Chen , Di, Yi-Ming , Zhang, Shu-Quan et al. Polyoxometalate/s-triazine hybrid heterostructures with ultrafast photochromic properties [J]. | DALTON TRANSACTIONS , 2024 , 53 (7) : 3215-3223 . |
| MLA | Chen, Yue-Chen et al. "Polyoxometalate/s-triazine hybrid heterostructures with ultrafast photochromic properties" . | DALTON TRANSACTIONS 53 . 7 (2024) : 3215-3223 . |
| APA | Chen, Yue-Chen , Di, Yi-Ming , Zhang, Shu-Quan , Lin, Mei-Jin . Polyoxometalate/s-triazine hybrid heterostructures with ultrafast photochromic properties . | DALTON TRANSACTIONS , 2024 , 53 (7) , 3215-3223 . |
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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 and inferior radioluminescence (RL) hampered their progression. Herein, the study has pioneered the development of high-performance TADF Ag(I)-based scintillators from M2X2(dppb)2 (M = Ag, Cu; X = Cl, Br, I) complexes with 1,2-Bis(diphenylphosphino)benzene (dppb) ligand. In comparison with Cu(I) complexes, the Ag(I) series generally exhibited superior scintillation performance. Notably, Ag2Cl2(dppb)2 (Ag1) stands out with exceptionally high RL intensity (approximate to 125% higher than that of CsI:Tl) and a low detection limit of 59.8 nGy s-1. The outstanding scintillation performance of Ag1 is primarily attributed to the synergistic effect of the high exciton utilization efficiency origin from a small singlet-triplet energy gap, enhanced X-ray absorption capacity by heavy atoms, and the high photoluminescence quantum yield (76.47% in ambient atmosphere). By fabricating a flexible film constructed with Ag1 submicron crystalline powders, a high spatial resolution of 25.0 lp mm-1 for X-ray imaging is obtained. It offers new opportunities for utilizing TADF metal-organic complexes for highly efficient X-ray scintillation and imaging. Scintillators with good radioluminescence performance are prepared by combining the TADF mechanism to optimize the utilization of triplet excitons, coupled with increased X-ray absorption through heavy atoms, verifying the advantages of Ag(I)-halide complexes on radioluminescence. Besides, the influence of halogens on photoluminescence and radioluminescence are investigated. As a practical application, Ag2Cl2(dppb)2 is applied to fabricate flexible scintillator films, achieving high-resolution imaging of 25 lp mm-1. image
Keyword ：
scintillators scintillators silver-based complexes silver-based complexes thermally activated delayed fluorescence thermally activated delayed fluorescence X-ray imaging X-ray imaging
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| GB/T 7714 | Yuan, Siqi , Zhang, Guozhen , Chen, Fuhai et al. Thermally Activated Delayed Fluorescent Ag(I) Complexes for Highly Efficient Scintillation and High-Resolution X-Ray Imaging [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (33) . |
| MLA | Yuan, Siqi et al. "Thermally Activated Delayed Fluorescent Ag(I) Complexes for Highly Efficient Scintillation and High-Resolution X-Ray Imaging" . | ADVANCED FUNCTIONAL MATERIALS 34 . 33 (2024) . |
| APA | Yuan, Siqi , Zhang, Guozhen , Chen, Fuhai , Chen, Jingru , Zhang, Yang , Di, Yiming et al. Thermally Activated Delayed Fluorescent Ag(I) Complexes for Highly Efficient Scintillation and High-Resolution X-Ray Imaging . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (33) . |
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The construction of molecular crystal materials with physical properties that can be dynamically controllable through various stimuli such as light and electricity is of extraordinary significance, while this remains a tremendous challenge. In this context, we demonstrate two novel 2-D multi-function viologen complexes, {[Ln (bcbp)(BDC)(CH3OH)(H2O)2]center dot Cl center dot CH3OH center dot H2O}n (1-Eu, and 2-Dy; H2bcbp center dot 2Cl = 1,1 '-bis(4-carboxyphenyl)-(4,4 ' bipyridinium) dichloride; BDC = p-phthalic acid, and Ln = Eu, Dy). Due to the strong 7c-7c interaction between viologen and BDC in the interlocked structure, both compounds exhibit rapid and reversible responses under the stimuli of UV light and electricity. Furthermore, accompanying the photochromic process, photo-modulated luminescent and photomagnetic behavior have been observed. Considering the excellent photochromic performance, the function filter paper and smart organic glass were successfully prepared and used for ink-free printing and UV light filtering.
Keyword ：
Electrochromism Electrochromism Inkless printing Inkless printing Photochromism Photochromism Photomagnetism Photomagnetism Viologen complex Viologen complex
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| GB/T 7714 | Zhao, Jia-Li , Chen, Fu-Hai , Ruan, Zheng et al. Interlocking viologen-based lanthanide complexes for multifunctionality: Photochromism, electrochromism, photoluminescence, photomagnetism, and inkless printing and UV shielding applications [J]. | DYES AND PIGMENTS , 2024 , 225 . |
| MLA | Zhao, Jia-Li et al. "Interlocking viologen-based lanthanide complexes for multifunctionality: Photochromism, electrochromism, photoluminescence, photomagnetism, and inkless printing and UV shielding applications" . | DYES AND PIGMENTS 225 (2024) . |
| APA | Zhao, Jia-Li , Chen, Fu-Hai , Ruan, Zheng , Cao, Zhi-Wei , Xu, Yuan-Qing , Cao, Zhong-Yan et al. Interlocking viologen-based lanthanide complexes for multifunctionality: Photochromism, electrochromism, photoluminescence, photomagnetism, and inkless printing and UV shielding applications . | DYES AND PIGMENTS , 2024 , 225 . |
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The development of high-quality organic scintillators encounters challenges primarily associated with the weak X-ray absorption ability resulting from the presence of low atomic number elements. An effective strategy involves the incorporation of halogen-containing molecules into the system through co-crystal engineering. Herein, we synthesized a highly fluorescent dye, 2,5-di(4-pyridyl)thiazolo[5,4-d]thiazole (Py2TTz), with a fluorescence quantum yield of 12.09%. Subsequently, Py2TTz was co-crystallized with 1,4-diiodotetrafluorobenzene (I2F4B) and 1,3,5-trifluoro-2,4,6-triiodobenzene (I3F3B) obtaining Py2TTz-I2F4 and Py2TTz-I3F3. Among them, Py2TTz-I2F4 exhibited exceptional scintillation properties, including an ultrafast decay time (1.426 ns), a significant radiation luminescence intensity (146% higher than Bi3Ge4O12), and a low detection limit (70.49 nGy s-1), equivalent to 1/78th of the detection limit for medical applications (5.5 mu Gy s-1). This outstanding scintillation performance can be attributed to the formation of halogen-bonding between I2F4B and Py2TTz. Theoretical calculations and single-crystal structures demonstrate the formation of halogen-bond-induced rather than pi-pi-induced charge-transfer cocrystals, which not only enhances the X-ray absorption ability and material conductivity under X-ray exposure, but also constrains molecular vibration and rotation, and thereby reducing non-radiative transition rate and sharply increasing its fluorescence quantum yields. Based on this, the flexible X-ray film prepared based on Py2TTz-I2F4 achieved an ultrahigh spatial resolution of 26.8 lp per mm, underscoring the superiority of this strategy in developing high-performance organic scintillators. Two organic halogen co-crystal scintillators with strong halogen-bond-induced charge-transfer interactions enable a fast response, low detection limit and ultra-high-resolution imaging.
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| GB/T 7714 | Chen, Yu-Hua , Zhang, Guo-Zhen , Chen, Fu-Hai et al. Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging [J]. | CHEMICAL SCIENCE , 2024 , 15 (20) : 7659-7666 . |
| MLA | Chen, Yu-Hua et al. "Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging" . | CHEMICAL SCIENCE 15 . 20 (2024) : 7659-7666 . |
| APA | Chen, Yu-Hua , Zhang, Guo-Zhen , Chen, Fu-Hai , Zhang, Shu-Quan , Fang, Xin , Chen, Hong-Ming et al. Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging . | CHEMICAL SCIENCE , 2024 , 15 (20) , 7659-7666 . |
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