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Amino Functionalization of Carbon Dots Leads to Red Emission Enhancement

Cite this: J. Phys. Chem. Lett. 2019, 10, 17, 5111–5116
Publication Date (Web):August 8, 2019
https://doi.org/10.1021/acs.jpclett.9b01724
Copyright © 2019 American Chemical Society

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    Abstract

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    The availability of carbon dots (CDots) with bright red photoluminescence (PL) would significantly broaden the range of their biological and optoelectronic applications. We present a theoretical model that predicts that amino functionalization of CDots not only shifts their PL to longer wavelengths but also preserves large oscillator strengths of the fundamental radiative transitions of CDots. The model considers the optical response of amino-functionalized CDots determined by molecule-like subunits of polycyclic aromatic hydrocarbons with one, two, or three −NH2 groups at the CDots’ surface; the excited state of those subunits is characterized by strong charge separation between the amino groups and CDots’ carbon core. Such a separation determines the Stokes shift of the CDots’ emission, which increases with the growing amount of the amino functional groups at the CDot surface. Our model explains the experimentally observed dependence of the PL spectra of CDots on the excitation wavelength, the phenomenon well documented in the literature for nitrogen-containing CDots.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpclett.9b01724.

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

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