Electron–phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dots
Abstract Due to the complex core–shell structure and variety of surface functional groups, the photoluminescence (PL) mechanism of carbon dots (CDs) remain unclear. o-Phenylenediamine (oPD), as one of the most common precursors for preparing red emissive CDs, has been extensively studied. Interestin...
| Main Authors: | , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Nature Publishing Group
2022-06-01
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| Series: | Light: Science & Applications |
| Online Access: | https://doi.org/10.1038/s41377-022-00865-x |
| _version_ | 1817975388495675392 |
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| author | Boyang Wang Zhihong Wei Laizhi Sui Jingkun Yu Baowei Zhang Xiaoyong Wang Shengnan Feng Haoqiang Song Xue Yong Yuxi Tian Bai Yang Siyu Lu |
| author_facet | Boyang Wang Zhihong Wei Laizhi Sui Jingkun Yu Baowei Zhang Xiaoyong Wang Shengnan Feng Haoqiang Song Xue Yong Yuxi Tian Bai Yang Siyu Lu |
| author_sort | Boyang Wang |
| collection | DOAJ |
| description | Abstract Due to the complex core–shell structure and variety of surface functional groups, the photoluminescence (PL) mechanism of carbon dots (CDs) remain unclear. o-Phenylenediamine (oPD), as one of the most common precursors for preparing red emissive CDs, has been extensively studied. Interestingly, most of the red emission CDs based on oPD have similar PL emission characteristics. Herein, we prepared six different oPD-based CDs and found that they had almost the same PL emission and absorption spectra after purification. Structural and spectral characterization indicated that they had similar carbon core structures but different surface polymer shells. Furthermore, single-molecule PL spectroscopy confirmed that the multi-modal emission of those CDs originated from the transitions of different vibrational energy levels of the same PL center in the carbon core. In addition, the phenomenon of “spectral splitting” of single-particle CDs was observed at low temperature, which confirmed these oPD-based CDs were unique materials with properties of both organic molecules and quantum dots. Finally, theoretical calculations revealed their potential polymerization mode and carbon core structure. Moreover, we proposed the PL mechanism of red-emitting CDs based on oPD precursors; that is, the carbon core regulates the PL emission, and the polymer shell regulates the PL intensity. Our work resolves the controversy on the PL mechanism of oPD-based red CDs. These findings provide a general guide for the mechanism exploration and structural analysis of other types of CDs. |
| first_indexed | 2024-04-13T21:49:18Z |
| format | Article |
| id | doaj.art-afe8b32c9edb42e48a631cdc4b27d9b2 |
| institution | Directory Open Access Journal |
| issn | 2047-7538 |
| language | English |
| last_indexed | 2024-04-13T21:49:18Z |
| publishDate | 2022-06-01 |
| publisher | Nature Publishing Group |
| record_format | Article |
| series | Light: Science & Applications |
| spelling | doaj.art-afe8b32c9edb42e48a631cdc4b27d9b22022-12-22T02:28:28ZengNature Publishing GroupLight: Science & Applications2047-75382022-06-0111111410.1038/s41377-022-00865-xElectron–phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dotsBoyang Wang0Zhihong Wei1Laizhi Sui2Jingkun Yu3Baowei Zhang4Xiaoyong Wang5Shengnan Feng6Haoqiang Song7Xue Yong8Yuxi Tian9Bai Yang10Siyu Lu11Green Catalysis Center, and College of Chemistry, Zhengzhou UniversityKey Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Jiangsu Key Laboratory of Vehicle Emissions Control, Nanjing UniversityState Key Lab of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of SciencesGreen Catalysis Center, and College of Chemistry, Zhengzhou UniversityNanochemistry Department, Istituto Italiano di Tecnologia (IIT)School of Physics, National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing UniversitySchool of Physics, National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing UniversityGreen Catalysis Center, and College of Chemistry, Zhengzhou UniversityDepartment of Chemistry, University of SheffieldKey Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Jiangsu Key Laboratory of Vehicle Emissions Control, Nanjing UniversityState Key Lab of Supramolecular Structure and Materials, College of Chemistry, Jilin UniversityGreen Catalysis Center, and College of Chemistry, Zhengzhou UniversityAbstract Due to the complex core–shell structure and variety of surface functional groups, the photoluminescence (PL) mechanism of carbon dots (CDs) remain unclear. o-Phenylenediamine (oPD), as one of the most common precursors for preparing red emissive CDs, has been extensively studied. Interestingly, most of the red emission CDs based on oPD have similar PL emission characteristics. Herein, we prepared six different oPD-based CDs and found that they had almost the same PL emission and absorption spectra after purification. Structural and spectral characterization indicated that they had similar carbon core structures but different surface polymer shells. Furthermore, single-molecule PL spectroscopy confirmed that the multi-modal emission of those CDs originated from the transitions of different vibrational energy levels of the same PL center in the carbon core. In addition, the phenomenon of “spectral splitting” of single-particle CDs was observed at low temperature, which confirmed these oPD-based CDs were unique materials with properties of both organic molecules and quantum dots. Finally, theoretical calculations revealed their potential polymerization mode and carbon core structure. Moreover, we proposed the PL mechanism of red-emitting CDs based on oPD precursors; that is, the carbon core regulates the PL emission, and the polymer shell regulates the PL intensity. Our work resolves the controversy on the PL mechanism of oPD-based red CDs. These findings provide a general guide for the mechanism exploration and structural analysis of other types of CDs.https://doi.org/10.1038/s41377-022-00865-x |
| spellingShingle | Boyang Wang Zhihong Wei Laizhi Sui Jingkun Yu Baowei Zhang Xiaoyong Wang Shengnan Feng Haoqiang Song Xue Yong Yuxi Tian Bai Yang Siyu Lu Electron–phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dots Light: Science & Applications |
| title | Electron–phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dots |
| title_full | Electron–phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dots |
| title_fullStr | Electron–phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dots |
| title_full_unstemmed | Electron–phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dots |
| title_short | Electron–phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dots |
| title_sort | electron phonon coupling assisted universal red luminescence of o phenylenediamine based carbon dots |
| url | https://doi.org/10.1038/s41377-022-00865-x |
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