Heterocyclic Modification Leading to Luminescent 0D Metal Organochalcogenide with Stable X-ray Scintillating Properties
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Kastner_ACSCatal_2025.pdf
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Accepted version
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Author(s)
Khamlue, Rattapon
Sakurada, Tomoaki
Cho, Yeongsu
Lee, Woo Seok
Leangtanom, Pimpan
Taylor, Michael G
Naewthong, Worakit
Sripetch, Pongsakun
Na Ranong, Busayakorn
Autila, Tossawat
Date Issued
May 7, 2024
Journal
Chemistry of Materials
Publisher
American Chemical Society
Citation
Khamlue, Rattapon, Sakurada, Tomoaki, Cho, Yeongsu, Lee, Woo Seok, Leangtanom, Pimpan et al. 2024. "Heterocyclic Modification Leading to Luminescent 0D Metal Organochalcogenide with Stable X-ray Scintillating Properties." Chemistry of Materials, 36 (10).
Version
Author's final manuscript
Abstract
Metal organochalcogenides (MOCs) are an emerging class of luminescent hybrid organic–inorganic semiconductors, whose structures and properties can be tuned by organic functionalization and substitutions of their metal and chalcogen elements. Herein, we present a new design strategy by heterocyclic modification, resulting in the transformation of prototypical two-dimensional (2D) silver phenylselenide (AgSePh) to a zero-dimensional (0D) silver pyridinylselenide (AgSePy) via the formation of Ag–N bonds. At room temperature, AgSePy shows strong and broad orange photoluminescence (PL; λmax = 636 nm, full-width-at-half-maximum = 111 nm, quantum yield = 64%) with a large 259 nm Stoke’s shift and a 3.4 μs lifetime. Using steady-state and time-resolved PL spectroscopy under varying temperature and oxygen conditions, we found AgSePy to exhibit air-stable luminescence and maintain a high PL quantum yield and a single exponential PL lifetime down to 4 K. Furthermore, AgSePy shows excellent thermal stability up to ∼250 °C and chemical stability against polar, nonpolar, and aqueous solvents at pH 3–14. Density functional theory calculations further confirm the 0D electronic structure. Finally, we successfully demonstrated the performance of AgSePy as an X-ray scintillator with an estimated light yield of ∼8,000 phe/MeV and a spatial resolution down to 0.080 ± 0.005 mm. Overall, this work provides a novel tactic to modify the structures and properties of MOCs, highlighting their structural richness and structure–property relationship, and introduces their new use as X-ray scintillators, encouraging further development in radiation detection and medical imaging.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Biological Engineering
Massachusetts Institute of Technology. Department of Chemistry
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DOI of Published Version
10.1021/acs.chemmater.4c00653
