Ultrastrong Electron-Phonon Coupling in Uranium-Organic Frameworks Leading to Inverse Luminescence Temperature Dependence
© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH..
Electron-phonon interactions, crucial in condensed matter, are rarely seen in Metal-Organic Frameworks (MOFs). Detecting these interactions typically involves analyzing luminescence in lanthanide- or actinide-based compounds. Prior studies on Ln- and Ac-based MOFs at high temperatures revealed additional peaks, but these were too faint for thorough analysis. In our research, we fabricated a high-quality, crystalline uranium-based MOF (KIT-U-1) thin film using a layer-by-layer method. Under UV light, this film showed two distinct "hot bands," indicating a strong electron-phonon interaction. At 77 K, these bands were absent, but at 300 K, a new emission band appeared with half the intensity of the main luminescence. Surprisingly, a second hot band emerged above 320 K, deviating from previous findings in rare-earth compounds. We conducted a detailed ab-initio analysis employing time-dependent density functional theory to understand this unusual behaviour and to identify the lattice vibration responsible for the strong electron-phonon coupling. The KIT-U-1 film's hot-band emission was then utilized to create a highly sensitive, single-compound optical thermometer. This underscores the potential of high-quality MOF thin films in exploiting the unique luminescence of lanthanides and actinides for advanced applications.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:63 |
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| Enthalten in: |
Angewandte Chemie (International ed. in English) - 63(2024), 11 vom: 11. März, Seite e202318559 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Chen, Dong-Hui [VerfasserIn] |
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| Links: |
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| Themen: |
DFT Calculation |
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| Anmerkungen: |
Date Revised 04.03.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1002/anie.202318559 |
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| 520 | |a Electron-phonon interactions, crucial in condensed matter, are rarely seen in Metal-Organic Frameworks (MOFs). Detecting these interactions typically involves analyzing luminescence in lanthanide- or actinide-based compounds. Prior studies on Ln- and Ac-based MOFs at high temperatures revealed additional peaks, but these were too faint for thorough analysis. In our research, we fabricated a high-quality, crystalline uranium-based MOF (KIT-U-1) thin film using a layer-by-layer method. Under UV light, this film showed two distinct "hot bands," indicating a strong electron-phonon interaction. At 77 K, these bands were absent, but at 300 K, a new emission band appeared with half the intensity of the main luminescence. Surprisingly, a second hot band emerged above 320 K, deviating from previous findings in rare-earth compounds. We conducted a detailed ab-initio analysis employing time-dependent density functional theory to understand this unusual behaviour and to identify the lattice vibration responsible for the strong electron-phonon coupling. The KIT-U-1 film's hot-band emission was then utilized to create a highly sensitive, single-compound optical thermometer. This underscores the potential of high-quality MOF thin films in exploiting the unique luminescence of lanthanides and actinides for advanced applications | ||
| 650 | 4 | |a Journal Article | |
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| 650 | 4 | |a Electron-Phonon Coupling | |
| 650 | 4 | |a Single-Metal Ratiometric Thermometer | |
| 650 | 4 | |a Thin Film | |
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| 700 | 1 | |a Vankova, Nina |e verfasserin |4 aut | |
| 700 | 1 | |a Jha, Gautam |e verfasserin |4 aut | |
| 700 | 1 | |a Yu, Xiaojuan |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Yuemin |e verfasserin |4 aut | |
| 700 | 1 | |a Lin, Ling |e verfasserin |4 aut | |
| 700 | 1 | |a Kirschhöfer, Frank |e verfasserin |4 aut | |
| 700 | 1 | |a Greifenstein, Raphael |e verfasserin |4 aut | |
| 700 | 1 | |a Redel, Engelbert |e verfasserin |4 aut | |
| 700 | 1 | |a Heine, Thomas |e verfasserin |4 aut | |
| 700 | 1 | |a Wöll, Christof |e verfasserin |4 aut | |
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