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Luminescent Ln3+-based silsesquioxanes with a β-diketonate antenna ligand: toward the design of efficient temperature sensorsстатья
- Авторы: Félix Gautier, Kulakova Alena N., Sene Saad, Khrustalev Victor N., Hernández-Rodríguez Miguel A., Shubina Elena S., Pelluau Tristan, Carlos Luís D., Guari Yannick, Carneiro Neto Albano N., Bilyachenko Alexey N., Larionova Joulia
- Журнал: Frontiers in Chemistry
- Год издания: 2024
- DOI: 10.3389/fchem.2024.1379587
- Аннотация: We report the synthesis and single-crystal X-ray diffraction, magnetic, and luminescence measurements of a novel family of luminescent cage-like tetranuclear silsesquioxanes (PhSiO1.5)8(LnO1.5)4(O)(C5H8O2)6(EtOH)2(CH3CN)2⋅2CH3CN (where Ln = Tb, 1; Tb/Eu, 2; and Gd, 3), featuring seven-coordinated lanthanide ions arranged in a one-capped trigonal prism geometry. Compounds 1 and 2 exhibit characteristic Tb3+ and Tb3+/Eu3+-related emissions, respectively, sensitized by the chelating antenna acetylacetonate (acac) ligands upon excitation in the UV and visible spectral regions. Compound 3 is used to assess the energies of the triplet states of the acac ligand. For compound 1, theoretical calculations on the intramolecular energy transfer and multiphonon rates indicate a thermal balance between the 5D4 Stark components, while the mixed Tb3+/Eu3+ analog 2, with a Tb:Eu ratio of 3:1, showcases intra-cluster Tb3+-to-Eu3+ energy transfer, calculated theoretically as a function of temperature. By utilizing the intensity ratio between the 5D4→7F5 (Tb3+) and 5D0→7F2 (Eu3+) transitions in the range 11–373 K, we demonstrate the realization of a ratiometric luminescent thermometer with compound 2, operating in the range 11–373 K with a maximum relative sensitivity of 2.0% K−1 at 373 K. These findings highlight the potential of cage-like silsesquioxanes as versatile materials for optical sensing-enabled applications.
- Добавил в систему: Астахов Григорий Сергеевич
Прикрепленные файлы
| № | Имя | Описание | Имя файла | Размер | Добавлен |
|---|---|---|---|---|---|
| 1. | Полный текст | fchem-12-1379587.pdf | 2,9 МБ | 3 апреля 2024 [AstakhovGS] | |
| 2. | Акт экспертизы | Front_Chem.pdf | 4,1 МБ | 11 апреля 2024 [BilyachenkoAN] |