Sequential addition of cations increases photoluminescence quantum yield of metal nanoclusters near unity
Abstract Photoluminescence is one of the most intriguing properties of metal nanoclusters derived from their molecular-like electronic structure, however, achieving high photoluminescence quantum yield (PLQY) of metal core-dictated fluorescence remains a formidable challenge. Here, we report efficie...
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-55975-y |
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| author | Xue Wang Yuan Zhong Tingting Li Kunyu Wang Weinan Dong Min Lu Yu Zhang Zhennan Wu Aiwei Tang Xue Bai |
| author_facet | Xue Wang Yuan Zhong Tingting Li Kunyu Wang Weinan Dong Min Lu Yu Zhang Zhennan Wu Aiwei Tang Xue Bai |
| author_sort | Xue Wang |
| collection | DOAJ |
| description | Abstract Photoluminescence is one of the most intriguing properties of metal nanoclusters derived from their molecular-like electronic structure, however, achieving high photoluminescence quantum yield (PLQY) of metal core-dictated fluorescence remains a formidable challenge. Here, we report efficient suppression of the total structural vibrations and rotations, and management of the pathways and rates of the electron transfer dynamics to boost a near-unity absolute PLQY, by decorating progressive addition of cations. Specifically, with the sequential addition of Zn2+, Ag+, and Tb3+ into the 3-mercaptopropionic acids capped Au nanoclusters (NCs), the low-frequency vibration of the metal core progressively decreases from 144.0, 55.2 to 40.0 cm−1, and the coupling strength of electrons-high-frequency vibration related to surface motifs gradually diminishes from 40.2, 30.5 to 14.4 meV. Moreover, introducing cation additives significantly reduces electron transfer time from 40, 27 to 12 ps in the pathway from staple motifs to the metal core. This benefits from the shrinkage of the total structure that speeds up the shell-core electron transition, and in particular, the Tb3+ provides a hopping platform for the excited electrons as their intrinsic ladder-like energy level structure. As a result, it allows a remarkable enhancement in PLQY, from 51.2%, 83.4%, up to 99.5%. |
| format | Article |
| id | doaj-art-7bc3ccbed78c42ad8a302c05b5758bce |
| institution | DOAJ |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
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| series | Nature Communications |
| spelling | doaj-art-7bc3ccbed78c42ad8a302c05b5758bce2025-08-20T02:40:35ZengNature PortfolioNature Communications2041-17232025-01-0116111210.1038/s41467-025-55975-ySequential addition of cations increases photoluminescence quantum yield of metal nanoclusters near unityXue Wang0Yuan Zhong1Tingting Li2Kunyu Wang3Weinan Dong4Min Lu5Yu Zhang6Zhennan Wu7Aiwei Tang8Xue Bai9State Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin UniversityState Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin UniversityCollege of Materials Science and Engineering, Jilin Jianzhu UniversityState Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin UniversityState Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin UniversityState Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin UniversityState Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin UniversityState Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin UniversityKey Laboratory of Luminescence and Optical Information, Ministry of Education, School of Physical Science and Engineering, Beijing Jiaotong UniversityState Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin UniversityAbstract Photoluminescence is one of the most intriguing properties of metal nanoclusters derived from their molecular-like electronic structure, however, achieving high photoluminescence quantum yield (PLQY) of metal core-dictated fluorescence remains a formidable challenge. Here, we report efficient suppression of the total structural vibrations and rotations, and management of the pathways and rates of the electron transfer dynamics to boost a near-unity absolute PLQY, by decorating progressive addition of cations. Specifically, with the sequential addition of Zn2+, Ag+, and Tb3+ into the 3-mercaptopropionic acids capped Au nanoclusters (NCs), the low-frequency vibration of the metal core progressively decreases from 144.0, 55.2 to 40.0 cm−1, and the coupling strength of electrons-high-frequency vibration related to surface motifs gradually diminishes from 40.2, 30.5 to 14.4 meV. Moreover, introducing cation additives significantly reduces electron transfer time from 40, 27 to 12 ps in the pathway from staple motifs to the metal core. This benefits from the shrinkage of the total structure that speeds up the shell-core electron transition, and in particular, the Tb3+ provides a hopping platform for the excited electrons as their intrinsic ladder-like energy level structure. As a result, it allows a remarkable enhancement in PLQY, from 51.2%, 83.4%, up to 99.5%.https://doi.org/10.1038/s41467-025-55975-y |
| spellingShingle | Xue Wang Yuan Zhong Tingting Li Kunyu Wang Weinan Dong Min Lu Yu Zhang Zhennan Wu Aiwei Tang Xue Bai Sequential addition of cations increases photoluminescence quantum yield of metal nanoclusters near unity Nature Communications |
| title | Sequential addition of cations increases photoluminescence quantum yield of metal nanoclusters near unity |
| title_full | Sequential addition of cations increases photoluminescence quantum yield of metal nanoclusters near unity |
| title_fullStr | Sequential addition of cations increases photoluminescence quantum yield of metal nanoclusters near unity |
| title_full_unstemmed | Sequential addition of cations increases photoluminescence quantum yield of metal nanoclusters near unity |
| title_short | Sequential addition of cations increases photoluminescence quantum yield of metal nanoclusters near unity |
| title_sort | sequential addition of cations increases photoluminescence quantum yield of metal nanoclusters near unity |
| url | https://doi.org/10.1038/s41467-025-55975-y |
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