sp2-sp3-Hybridized Atomic Domains Determine Optical Features of Carbon Dots

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review

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Author(s)

  • Nikita V. Tepliakov
  • Evgeny V. Kundelev
  • Pavel D. Khavlyuk
  • Mikhail Yu. Leonov
  • Weiren Zhu
  • Alexander V. Baranov
  • Anatoly V. Fedorov
  • Ivan D. Rukhlenko

Detail(s)

Original languageEnglish
Pages (from-to)10737-10744
Journal / PublicationACS Nano
Volume13
Issue number9
Online published14 Aug 2019
Publication statusPublished - 24 Sep 2019

Abstract

Carbon dots (CDots) are a promising biocompatible nanoscale source of light, yet the origin of their emission remains under debate. Here, we show that all the distinctive optical properties of CDots, including the giant Stokes shift of photoluminescence and the strong dependence of emission color on excitation wavelength, can be explained by the linear optical response of the partially sp2-hybridized carbon domains located on the surface of the CDots' sp3-hybridized amorphous cores. Using a simple quantum chemical approach, we show that the domain hybridization factor determines the localization of electrons and the electronic bandgap inside the domains and analyze how the distribution of this factor affects the emission properties of CDots. Our calculation data fully agree with the experimental optical properties of CDots, confirming the overall theoretical picture underlying the model. It is also demonstrated that fabrication of CDots with large hybridization factors of carbon domains shifts their emission to the red side of the visible spectrum, without a need to modify the size or shape of the CDots. Our theoretical model provides a useful tool for experimentalists and may lead to extending the applications of CDots in biophysics, optoelectronics, and photovoltaics.

Research Area(s)

  • absorption, carbon domains, extended Hückel method, hybridization, photoluminescence, quantum chemistry

Citation Format(s)

sp2-sp3-Hybridized Atomic Domains Determine Optical Features of Carbon Dots. / Tepliakov, Nikita V.; Kundelev, Evgeny V.; Khavlyuk, Pavel D.; Xiong, Yuan; Leonov, Mikhail Yu.; Zhu, Weiren; Baranov, Alexander V.; Fedorov, Anatoly V.; Rogach, Andrey L.; Rukhlenko, Ivan D.

In: ACS Nano, Vol. 13, No. 9, 24.09.2019, p. 10737-10744.

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review