Surface Chemistry Routes to Modulate the Photoluminescence of Graphene Quantum Dots: From Fluorescence Mechanism to Up-Conversion Bioimaging Applications

The bandgap in graphene‐based materials can be tuned from 0 eV to that of benzene by changing size and/or surface chemistry, making it a rising carbon‐based fluorescent material. Here, the surface chemistry of small size graphene (graphene quantum dots, GQDs) is tuned programmably through modificati...

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Published inAdvanced functional materials Vol. 22; no. 22; pp. 4732 - 4740
Main Authors Zhu, Shoujun, Zhang, Junhu, Tang, Shijia, Qiao, Chunyan, Wang, Lei, Wang, Haiyu, Liu, Xue, Li, Bo, Li, Yunfeng, Yu, Weili, Wang, Xingfeng, Sun, Hongchen, Yang, Bai
Format Journal Article
LanguageEnglish
Published Weinheim WILEY-VCH Verlag 21.11.2012
WILEY‐VCH Verlag
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Online AccessGet full text
ISSN1616-301X
1616-3028
DOI10.1002/adfm.201201499

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Abstract The bandgap in graphene‐based materials can be tuned from 0 eV to that of benzene by changing size and/or surface chemistry, making it a rising carbon‐based fluorescent material. Here, the surface chemistry of small size graphene (graphene quantum dots, GQDs) is tuned programmably through modification or reduction and green luminescent GQDs are changed to blue luminescent GQDs. Several tools are employed to characterize the composition and morphology of resultants. More importantly, using this system, the luminescence mechanism (the competition between both the defect state emission and intrinsic state emission) is explored in detail. Experiments demonstrate that the chemical structure changes during modification or reduction suppresses non‐radiative recombination of localized electron‐hole pairs and/or enhances the integrity of surface π electron network. Therefore the intrinsic state emission plays a leading role, as opposed to defect state emission in GQDs. The results of time‐resolved measurements are consistent with the suggested PL mechanism. Up‐conversion PL of GQDs is successfully applied in near‐IR excitation for bioimaging. The preparation of controllable fluorescent graphene quantum dots (GQDs) using a new surface chemistry tuning method is reported. The photoluminescence (PL) mechanism is investigated and the competition between both the defect state emission and intrinsic state emission are analyzed in detail. Moreover, the up‐conversion PL of GQDs is successfully used in multiphoton luminescent biolabeling under near‐IR excitation.
AbstractList The bandgap in graphene‐based materials can be tuned from 0 eV to that of benzene by changing size and/or surface chemistry, making it a rising carbon‐based fluorescent material. Here, the surface chemistry of small size graphene (graphene quantum dots, GQDs) is tuned programmably through modification or reduction and green luminescent GQDs are changed to blue luminescent GQDs. Several tools are employed to characterize the composition and morphology of resultants. More importantly, using this system, the luminescence mechanism (the competition between both the defect state emission and intrinsic state emission) is explored in detail. Experiments demonstrate that the chemical structure changes during modification or reduction suppresses non‐radiative recombination of localized electron‐hole pairs and/or enhances the integrity of surface π electron network. Therefore the intrinsic state emission plays a leading role, as opposed to defect state emission in GQDs. The results of time‐resolved measurements are consistent with the suggested PL mechanism. Up‐conversion PL of GQDs is successfully applied in near‐IR excitation for bioimaging. The preparation of controllable fluorescent graphene quantum dots (GQDs) using a new surface chemistry tuning method is reported. The photoluminescence (PL) mechanism is investigated and the competition between both the defect state emission and intrinsic state emission are analyzed in detail. Moreover, the up‐conversion PL of GQDs is successfully used in multiphoton luminescent biolabeling under near‐IR excitation.
The bandgap in graphene‐based materials can be tuned from 0 eV to that of benzene by changing size and/or surface chemistry, making it a rising carbon‐based fluorescent material. Here, the surface chemistry of small size graphene (graphene quantum dots, GQDs) is tuned programmably through modification or reduction and green luminescent GQDs are changed to blue luminescent GQDs. Several tools are employed to characterize the composition and morphology of resultants. More importantly, using this system, the luminescence mechanism (the competition between both the defect state emission and intrinsic state emission) is explored in detail. Experiments demonstrate that the chemical structure changes during modification or reduction suppresses non‐radiative recombination of localized electron‐hole pairs and/or enhances the integrity of surface π electron network. Therefore the intrinsic state emission plays a leading role, as opposed to defect state emission in GQDs. The results of time‐resolved measurements are consistent with the suggested PL mechanism. Up‐conversion PL of GQDs is successfully applied in near‐IR excitation for bioimaging.
Author Li, Yunfeng
Wang, Xingfeng
Zhu, Shoujun
Wang, Haiyu
Li, Bo
Yu, Weili
Qiao, Chunyan
Liu, Xue
Zhang, Junhu
Tang, Shijia
Wang, Lei
Sun, Hongchen
Yang, Bai
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  givenname: Shoujun
  surname: Zhu
  fullname: Zhu, Shoujun
  organization: State Key Laboratory of Supramolecular, Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, P. R. China
– sequence: 2
  givenname: Junhu
  surname: Zhang
  fullname: Zhang, Junhu
  organization: State Key Laboratory of Supramolecular, Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, P. R. China
– sequence: 3
  givenname: Shijia
  surname: Tang
  fullname: Tang, Shijia
  organization: State Key Laboratory of Supramolecular, Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, P. R. China
– sequence: 4
  givenname: Chunyan
  surname: Qiao
  fullname: Qiao, Chunyan
  organization: School of Stomatology, Jilin University, Changchun, 130041, P. R. China
– sequence: 5
  givenname: Lei
  surname: Wang
  fullname: Wang, Lei
  organization: State Key Laboratory on Integrated Optoelectronics, College of Electronic Science & Engineering, Jilin University, Changchun, 130012, P. R. China
– sequence: 6
  givenname: Haiyu
  surname: Wang
  fullname: Wang, Haiyu
  organization: State Key Laboratory on Integrated Optoelectronics, College of Electronic Science & Engineering, Jilin University, Changchun, 130012, P. R. China
– sequence: 7
  givenname: Xue
  surname: Liu
  fullname: Liu, Xue
  organization: State Key Laboratory of Supramolecular, Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, P. R. China
– sequence: 8
  givenname: Bo
  surname: Li
  fullname: Li, Bo
  organization: State Key Laboratory of Supramolecular, Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, P. R. China
– sequence: 9
  givenname: Yunfeng
  surname: Li
  fullname: Li, Yunfeng
  organization: State Key Laboratory of Supramolecular, Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, P. R. China
– sequence: 10
  givenname: Weili
  surname: Yu
  fullname: Yu, Weili
  organization: State Key Laboratory of Supramolecular, Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, P. R. China
– sequence: 11
  givenname: Xingfeng
  surname: Wang
  fullname: Wang, Xingfeng
  organization: State Key Laboratory of Supramolecular, Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, P. R. China
– sequence: 12
  givenname: Hongchen
  surname: Sun
  fullname: Sun, Hongchen
  organization: School of Stomatology, Jilin University, Changchun, 130041, P. R. China
– sequence: 13
  givenname: Bai
  surname: Yang
  fullname: Yang, Bai
  email: byangchem@jlu.edu.cn
  organization: State Key Laboratory of Supramolecular, Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, P. R. China
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2010; 10
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2010; 132
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2010; 150
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Snippet The bandgap in graphene‐based materials can be tuned from 0 eV to that of benzene by changing size and/or surface chemistry, making it a rising carbon‐based...
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wiley
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SubjectTerms graphene quantum dots
photoluminescence mechanisms
tunable fluorescence
up-conversion bioimaging
Title Surface Chemistry Routes to Modulate the Photoluminescence of Graphene Quantum Dots: From Fluorescence Mechanism to Up-Conversion Bioimaging Applications
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