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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Phys. Chem. Lett. 2020, 11, 19, 8121-8127
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Toward Bright Red-Emissive Carbon Dots through Controlling Interaction among Surface Emission Centers

  • Evgeny V. Kundelev*
    Evgeny V. Kundelev
    Information Optical Technologies Center, ITMO University, St. Petersburg 197101, Russia
    *Email: [email protected]
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    Orcidhttp://orcid.org/0000-0002-7672-1790
  • , 
  • Nikita V. Tepliakov
    Nikita V. Tepliakov
    Information Optical Technologies Center, ITMO University, St. Petersburg 197101, Russia
    Chair of Computational Condensed Matter Physics (C3MP), Institute of Physics, Ecole Polytechnique Federale de Lausanne, CH-1015 Lausanne, Switzerland
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    Orcidhttp://orcid.org/0000-0001-5644-6907
  • , 
  • Mikhail Yu. Leonov
    Mikhail Yu. Leonov
    Information Optical Technologies Center, ITMO University, St. Petersburg 197101, Russia
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  • , 
  • Vladimir G. Maslov
    Vladimir G. Maslov
    Information Optical Technologies Center, ITMO University, St. Petersburg 197101, Russia
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  • , 
  • Alexander V. Baranov
    Alexander V. Baranov
    Information Optical Technologies Center, ITMO University, St. Petersburg 197101, Russia
    More by Alexander V. Baranov
    Orcidhttp://orcid.org/0000-0002-9976-8532
  • , 
  • Anatoly V. Fedorov
    Anatoly V. Fedorov
    Information Optical Technologies Center, ITMO University, St. Petersburg 197101, Russia
    More by Anatoly V. Fedorov
    Orcidhttp://orcid.org/0000-0002-7395-0985
  • , 
  • Ivan D. Rukhlenko
    Ivan D. Rukhlenko
    Information Optical Technologies Center, ITMO University, St. Petersburg 197101, Russia
    Institute of Photonics and Optical Science (IPOS), School of Physics, The University of Sydney, Camperdown 2006, New South Wales, Australia
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    Orcidhttp://orcid.org/0000-0001-5585-4220
  • , and 
  • Andrey L. Rogach
    Andrey L. Rogach
    Information Optical Technologies Center, ITMO University, St. Petersburg 197101, Russia
    Department of Materials Science and Engineering, and Centre for Functional Photonics (CFP), City University of Hong Kong, Hong Kong SAR, China
    More by Andrey L. Rogach
    Orcidhttp://orcid.org/0000-0002-8263-8141
Cite this: J. Phys. Chem. Lett. 2020, 11, 19, 8121–8127
Publication Date (Web):September 6, 2020
https://doi.org/10.1021/acs.jpclett.0c02373
Copyright © 2020 American Chemical Society
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    Abstract

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    Relatively weak red photoluminescence of carbon dots (CDots) is a major challenge on the way to their successful implementation in biological and optoelectronic devices. We present a theoretical analysis of the interaction among the surface emission centers of CDots, showing that it may determine efficiency of the red photoluminescence of CDots. Based on the previous experimental studies, it is assumed that the optical response of the CDots is determined by the molecule-like subunits of polycyclic aromatic hydrocarbons (PAHs) attached to the CDots’ surface. Three characteristic types of coupling of these PAH subunits are considered: non-interacting monomers, noncovalently bound dimers, and covalently bound dimers with two, three, or four carbon linkers. We demonstrate that the CDots’ photoluminescence broadens, redshifts, and weakens by 2 orders of magnitude when the free monomers are substituted by the covalently bridged centers. These and other results of our study show that the realization of CDots with many weakly interacting surface emission centers may constitute an efficient way to achieve their efficient red photoluminescence, which is highly desirable for biological and optoelectronic applications.

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    • Additional data on energies, oscillator strengths, composition, and symmetry of electronic transitions in perylene-based functional subunits of CDots (PDF)

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