1D Silver Organochalcogenide Semiconductors: Color Tunable Luminescence, Polarized Emission, and Long-Range Exciton Diffusion
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1d-silver-organochalcogenide-semiconductors-color-tunable-luminescence-polarized-emission-and-long-range-exciton.pdf
Description
Published version
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11.31 MB
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Checksum (MD5)
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Author(s)
Sakurada, Tomoaki
Pathoor, Nithin
Matsumoto, Takuma
Khamlue, Rattapon
Chatsiri, Petcharaphorn
Valenta, Jan
Kawamoto, Tadashi
Omagari, Shun
Tisdale, William A
Paritmongkol, Watcharaphol
Date Issued
October 14, 2025
Journal
Journal of the American Chemical Society
Publisher
American Chemical Society
Citation
Tomoaki Sakurada, Nithin Pathoor, Takuma Matsumoto, Rattapon Khamlue, Petcharaphorn Chatsiri, Jan Valenta, Tadashi Kawamoto, Shun Omagari, William A. Tisdale, Watcharaphol Paritmongkol, Yeongsu Cho, and Martin Vacha. Journal of the American Chemical Society 2025 147 (43), 39516-39526.
Version
Final published version
Abstract
Metal organochalcogenides (MOCs) represent a promising class of organic-inorganic hybrid semiconductors with unique light-matter interactions. Their hybrid nature enables extensive structural and optoelectronic tunability via ligand engineering. In this study, we systematically modulated the electronic properties of ligands using Cl and Me functional groups, achieving precise control over the optoelectronic properties of Ag-based MOCs. Structural analysis revealed that these MOCs adopt a one-dimensional (1D) chain structure with organic ligands surrounding a Ag-chalcogen core. Density functional theory (DFT) calculations demonstrated that MOCs exhibit characteristics of 1D semiconductors with strongly dispersive conduction and valence bands aligned along the crystal rod directions. Experimentally, the MOCs displayed bright luminescence, with peaks centered between 560 and 690 nm. The substitution of Cl with Me groups in the benzene ligands induced a red shift in both absorption and photoluminescence, corroborated by experimental and theoretical analyses. Further optical measurements indicated that the emission from the MOCs is strongly polarized along the chain directions. Notably, Se-based MOCs exhibited enhanced exciton diffusivity along the chain axis with a diffusion length of 130 nm, which is among the highest reported for covalent systems. The observed trend in carrier diffusivity among individual compounds is attributed to differences in the effective masses of the carriers, as determined by DFT calculations. Our findings offer valuable insights into the systematic structural and property tuning of hybrid semiconductors and highlight the unique characteristics of the 1D MOC family.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
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DOI of Published Version
10.1021/jacs.5c12551
