TY - JOUR
T1 - Bulk-state and single-particle imaging are central to understanding carbon dot photo-physics and elucidating the effects of precursor composition and reaction temperature
AU - Fathi, Parinaz
AU - Khamo, John S.
AU - Huang, Xuedong
AU - Srivastava, Indrajit
AU - Esch, Mandy B.
AU - Zhang, Kai
AU - Pan, Dipanjan
N1 - Funding Information:
We gratefully acknowledge Richard Haasch (UIUC Materials Research Laboratory) for his assistance with collecting XPS spectra, and Santosh K. Misra for his valuable scientific input. This project was funded through grants from National Institute of Health, Department of Defense, and University of Illinois (KZ). P. Fathi was funded by the National Physical Science Consortium and the National Institute of Standards & Technology through an NPSC graduate fellowship, and by the Nadine Barrie Smith Memorial Fellowship from the Beckman Institute. J. Khamo was supported by the Westcott fellowship in the Department of Biochemistry at UIUC. Research reported in this publication was supported by the National Institute of Biomedical Imaging And Bioengineering of the National Institutes of Health under Award Number T32EB019944. The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health. This work was carried out in part in the Frederick Seitz Materials Research Laboratory Central Research Facilities, University of Illinois. Any mention of commercial products within this work is for information only; it does not imply recommendation or endorsement by NIST.
Funding Information:
We gratefully acknowledge Richard Haasch (UIUC Materials Research Laboratory) for his assistance with collecting XPS spectra, and Santosh K. Misra for his valuable scientific input. This project was funded through grants from National Institute of Health , Department of Defense , and University of Illinois (KZ). P. Fathi was funded by the National Physical Science Consortium and the National Institute of Standards & Technology through an NPSC graduate fellowship, and by the Nadine Barrie Smith Memorial Fellowship from the Beckman Institute . J. Khamo was supported by the Westcott fellowship in the Department of Biochemistry at UIUC. Research reported in this publication was supported by the National Institute of Biomedical Imaging And Bioengineering of the National Institutes of Health under Award Number T32EB019944 . The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health. This work was carried out in part in the Frederick Seitz Materials Research Laboratory Central Research Facilities, University of Illinois. Any mention of commercial products within this work is for information only; it does not imply recommendation or endorsement by NIST.
Publisher Copyright:
© 2019 Elsevier Ltd
PY - 2019/4
Y1 - 2019/4
N2 - Carbon dots have garnered attention for their strong multi-color luminescence properties and unprecedented biocompatibility. Despite significant progress in the recent past, a fundamental understanding of their photoluminescence and structure-properties relationships, especially at the bulk vs. single-particle level, has not been well established. Here we present a comparative study of bulk- and single-particle properties as a function of precursor composition and reaction temperature. The synthesis and characterization of multicolored inherently functionalized carbon dots were achieved from a variety of carbon sources, and at synthesis temperatures of 150 °C and 200 °C. Solvothermal synthesis at 200 °C led to quantum yields as high as 86%, smaller particle sizes, and a narrowed fluorescence emission, while synthesis at 150 °C resulted in a greater UV–visible absorbance, increase in nanoparticle stability, red-shifted fluorescence, and a greater resistance to bulk photobleaching. These results suggest the potential for synthesis temperature to be utilized as a simple tool for modulating carbon dot photophysical properties. Single-particle imaging resolved that particle brightness was determined by both the instantaneous intensity and the on-time duty cycle. Increasing the synthesis temperature caused an enhancement in blinking frequency, which led to an increase in on-time duty cycle in three out of four precursors.
AB - Carbon dots have garnered attention for their strong multi-color luminescence properties and unprecedented biocompatibility. Despite significant progress in the recent past, a fundamental understanding of their photoluminescence and structure-properties relationships, especially at the bulk vs. single-particle level, has not been well established. Here we present a comparative study of bulk- and single-particle properties as a function of precursor composition and reaction temperature. The synthesis and characterization of multicolored inherently functionalized carbon dots were achieved from a variety of carbon sources, and at synthesis temperatures of 150 °C and 200 °C. Solvothermal synthesis at 200 °C led to quantum yields as high as 86%, smaller particle sizes, and a narrowed fluorescence emission, while synthesis at 150 °C resulted in a greater UV–visible absorbance, increase in nanoparticle stability, red-shifted fluorescence, and a greater resistance to bulk photobleaching. These results suggest the potential for synthesis temperature to be utilized as a simple tool for modulating carbon dot photophysical properties. Single-particle imaging resolved that particle brightness was determined by both the instantaneous intensity and the on-time duty cycle. Increasing the synthesis temperature caused an enhancement in blinking frequency, which led to an increase in on-time duty cycle in three out of four precursors.
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U2 - 10.1016/j.carbon.2018.12.105
DO - 10.1016/j.carbon.2018.12.105
M3 - Article
AN - SCOPUS:85060912315
SN - 0008-6223
VL - 145
SP - 572
EP - 585
JO - Carbon
JF - Carbon
ER -