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Abstract 0D organic metal halide hybrids (OMHHs) have recently emerged as a new generation of scintillation materials, due to their high luminescence quantum efficiency, sensitivity, stability, and cost‐effectiveness. While numerous 0D OMHH scintillators have been developed to date, most of them are based on solution grown single crystals that require time‐consuming synthesis and are limited in size. Here, high‐performance X‐ray scintillators based on facile solution processed 0D OMHH amorphous films are reported for the first time. By reacting triphenyl(9‐phenyl‐9H‐carbazol‐3‐yl) phosphonium bromide (TPPcarzBr) with manganese bromide (MnBr2), 0D (TPPcarz)₂MnBr₄ amorphous films can be prepared via solution processing with mild thermal annealing, which exhibits green photoluminescence with an emission maximum ≈517 nm and a photoluminescence quantum efficiency of ≈87%. The X‐ray scintillation of 0D (TPPcarz)₂MnBr₄ amorphous films is characterized to exhibit a light yield of 44600 photon MeV−1and an outstanding linearity with a low limit of detection of 32.42 nGyairs−1over a wide range of X‐ray dose rates. The versatile processability of 0D (TPPcarz)₂MnBr₄ is illustrated with remarkable recyclability, high cost‐effectiveness, and scalability for large‐scale production. By taking advantage of the amorphous nature of newly designed OMHHs, the approach opens up new opportunities for developing high‐performance, solution‐processable scintillators.
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Solution‐Processed Amorphous Zero‐Dimensional Organic Metal Halide Hybrid Films for Direct X‐Ray Detectors
Zero‐dimensional (0D) organic metal halide hybrids (OMHHs) are emerging materials with significant potential for optoelectronic applications, including direct X‐ray detectors. While 0D OMHH single crystals exhibit excellent X‐ray detection properties, their scalability remains a significant challenge due to the time‐intensive growth process and difficulty in producing large single crystals exceeding a few centimeters. This limitation hinders their practicality for large‐area detector applications. Here, we report for the first time the development of amorphous 0D OMHH films via solution processing for efficient direct X‐ray detection. By reacting a non‐crystalline organic halide, triphenyl(9‐phenyl‐9H‐carbazol‐3‐yl)phosphonium bromide (TPPCarzBr), with zinc bromide (ZnBr2), we have successfully produced amorphous 0D (TPPCarz)2ZnBr4films with controlled thickness via facile solution processing. The organic cations (TPPCarz⁺) feature a lower bandgap than the ZnBr42−anions, enabling efficient molecular sensitization, where ZnBr42−anions serve as X‐ray absorbers and TPPCarz⁺ cations as charge transporters. Direct X‐ray detectors based on 0D (TPPCarz)2ZnBr4films demonstrate outstanding performance, achieving a stable X‐ray detection sensitivity of 2,165 µC Gyair⁻1cm⁻2at 20 V mm⁻¹ and a detection limit of 6.01 nGyair s⁻¹. The amorphous nature of these films enhances their processability, allowing for fabrication in various sizes and shapes, and making them highly adaptable for scalable detector applications.
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- Award ID(s):
- 2204466
- PAR ID:
- 10644889
- Publisher / Repository:
- Wiley-VCH GmbH
- Date Published:
- Journal Name:
- Angewandte Chemie International Edition
- Volume:
- 64
- Issue:
- 35
- ISSN:
- 1433-7851
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript
- Journal Article:
- https://doi.org/10.1002/anie.202509589
