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Progress in Chemistry 2021, Vol. 33 Issue (7): 1059-1073 DOI: 10.7536/PC200715   Next Articles

• Review •

Photoluminescence Mechanisms of Carbon Quantum Dots

Xingchen Wu1, Wenhui Liang1,2, Chenxin Cai1,*()   

  1. 1 College of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China
    2 College of Life Science and Chemistry, Jiangsu Second Normal University, Nanjing 210023, China
  • Received: Revised: Online: Published:
  • Contact: Chenxin Cai
  • About author:
    * Corresponding author e-mail:
  • Supported by:
    National Natural Science Foundation of China(21675088)
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Carbon quantum dots (CQDs) generally refer to zero-dimensional carbon materials with a particle size of less than 10 nm. Due to their excellent optical properties, they have been used extensively in the fields of bioimaging, optical devices, biocomposite materials, biosensing, etc., and can be expected to become one of the most widely used carbon material in the future. The optical properties of CQDs are affected by particle size, surface functional groups, synthesis temperature, type of solvent, and pH. In order to precisely control their optical properties and further expand their scope of application, their photoluminescence (PL) mechanisms need to be elucidated in details, however, the PL mechanism of CQDs is currently not complete clear. At present, the proposed PL mechanism includes quantum confinement effect, surface states emission, molecular fluorophores and carbogenic core, polycyclic aromatic hydrocarbon molecular emission, self-trapped exciton emission, surface dipole emission center, aggregate emission center, multiple emission center, slowed solvent relaxation and solvatochromic shift etc. But each mechanism can only explain part of the PL phenomenon of CQDs to a certain extent. No mechanism can explain all the PL phenomena of CQDs, which seriously restricts the regulation of the optical properties of CQDs. This review classifies and summarizes the different PL mechanisms of CQDs, its purpose is to provide a reference for further elucidating its PL mechanism and achieving controllable adjustment of the optical characteristics of CQDs.

Contents

1 Introduction

2 Optical characteristics of CQDs

2.1 UV-Vis absorption characteristics

2.2 Fluorescence characteristics (photoluminescence characteristics)

2.3 Electroluminescence characteristics

2.4 Up-converted luminescence

3 PL mechanism of CQDs

3.1 Quantum confinement effect

3.2 Surface states emission

3.3 Molecular fluorophores and carbogenic core

3.4 Polycyclic aromatic hydrocarbon molecular emission

3.5 Self-trapped exciton emission

3.6 Surface dipole emission center

3.7 Aggregate emission center

3.8 Multiple emission center

3.9 Slowed solvent relaxation and solvatochromic shift

4 Conclusion and outlook

Key words: carbon quantum dots, synthesis, optical characteristics, photoluminescence mechanism
Fig. 1 (a) Absorption spectra of CQDs prepared under different conditions[55]; (b) solvent-induced absorption peak redshift for CQDs[49]; (c) aggregation-induced absorption in the long-wavelength region[55]; (d) modification group-induced absorption of CQDs in the long-wavelength region[23]
Fig. 2 (a) Formal process of photoluminescence: electrons transition and back to lower energy levels, releasing energy in the form of photons; (b) PL emission spectra of the CQDs under excitation wavelengths from 300 to 470 nm[23]
Fig. 3 (a)ECL responses of Pt electrodes (a’) with and (b’) without CQDs at its surface in 0.1 mol/L phosphate buffer solution[59]. (b) Electroluminescence(EL) spectra and photographs of multicolor emissions[63]
Fig. 4 Excitation-dependent up-conversion fluorescence spectra of CQDs[66]
Fig. 5 The mechanism of up-and down-conversion fluorescence: single-photon absorption, release less energy, and produce down-conversion fluorescence. Multiphoton absorption releases more energy and produces up-converted fluorescence
Fig. 6 (a) Absorption spectra of CQDs with different particle sizes[68]. (b) Normalized PL spectra of CQDs with different particle sizes[68]. (c)Calculated emission wavelength with diameter of graphene quantum dots[73]. (d) Energy gap of π-π * transitions calculated based on DFT as a function of the number of fused aromatic rings[74]
Fig. 7 (a) Fluorescence photographs of CQDs with different color under 365 nm UV excitation[75]. (b) Schematic diagram of the band gap of four selected CQDs (average particle size is about 2.6 nm)[75]. (c) Schematic diagram of PL emission affected by the surface state[76]
Fig. 8 (a) Schematic representation of the emission characteristics of three photoactive species produced from the thermal treatment of mixture of CA and EA[81]. (b) Schematic illustration of the CQDs obtained at different hydrothermal temperatures[82]
Fig. 9 (a) Absorption spectra of CQDs, anthracene, perylene, pyrene. (b) PL spectra of CQDs, anthracene, perylene, pyrene under 337 nm excitation wavelength. (c) Absorption spectra of CQDs and PAH-film. (d) Schematic diagram of PAH-induced luminescence[87]
Fig.10 Changes in the content of fluorophores and aromatic domain structures with different reaction times[88]
Fig.11 (a) Emission anisotropy and degree of linear polarization of CQDs. (b) Electric-field modulation of CQDs emission. (c) Power-dependent PL intensity. (d) Electronic structure of self-trapped excitons, which contribute to carbon dots emission[91]
Fig.12 (a) HRTEM images of individual CQDs possessing various crystal structures. (b) Consecutive images of the same sample area recorded by using an azimuthally polarized laser beam (scanning direction up-down). Each double-lobe pattern corresponds to the same CQDs. (c) Single CQDs spectra under 467 nm. (d) PL spectra of single CQDs under 467 and 488 nm laser[95]
Fig.13 (a) Absorption, excitation and fluorescence spectra of CQDs at 300 K. (b) CQDs aggregation structure model and its distortion process. (c) Aggregation structure-induced band gap reduction[97]
Fig.14 (a) Proposed fluorescent mechanism of the ternary fluorescent centers of CQDs[103]. (b) Schematic diagram of one-pot synthesis and purification of CQDs. Changes in particle size and defect content lead to shift in PL emission wavelength[104]
Fig.15 (a) Photograph of the CQDs excited by different wavelength lights in solvents of CCl4, toluene, CHCl3, acetone, DMF, and H2O[109]. (b) Illustration of the possible emission processes of the CQDs in different solvents[109]. (c) Illustration of the combination of solvent and molecule to generate new energy level[109]. (d) Photographs of CQDs, DA-CQDs, and PFDA-CQDs in chloroform and methanol under white light, 365 nm UV light, and 302 nm UV light[111]
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