Carbon dots (CDs) with tunable photoluminescence (PL) and a quantum yield of up to 35% in water were hydrothermally synthesized in one pot and separated via silica column chromatography. These separated CDs emitted bright and stable luminescence in gradient colors from blue to red under a single-wavelength UV light. They exhibited high optical uniformity; that is, every sample showed only one peak in the PL excitation spectrum, only one peak in the excitation-independent PL emission spectrum, and similar monoexponential fluorescence lifetimes. Although these samples had similar distributions of particle size and graphite structure in their carbon cores, the surface state gradually varied among the samples, especially the degree of oxidation. Therefore, the observed red shift in their emission peaks from 440 to 625 nm was ascribed to a gradual reduction in their band gaps with the increasing incorporation of oxygen species into their surface structures. These energy bands were found to depend on the surface groups and structures but not on the particle size, not as in traditional semiconductor quantum dots. In addition, because of their excellent PL properties and low cytotoxicity, these CDs could be used to image cells in different colors under a single-wavelength light source, and the red-emitting CDs could be used to image live mice because of the strong penetration capability of their fluorescence.
Sulfur-doped carbon dots (S-CDs) with a quantum yield (QY) of 5.5% and nitrogen, sulfur co-doped carbon dots (N,S-CDs) with a QY of 54.4% were synthesized, respectively, via the same hydrothermal route using α-lipoic acid as the carbon source. The obtained S-CDs and N,S-CDs had similar sizes but different optical features. The QY of N,S-CDs was gradually enhanced when extending the reaction time to increase the nitrogen content. After careful characterization of these CDs, the doped nitrogen element was believed to be in the form of C=N and C-N bonds which enhanced the fluorescence efficiency significantly. Meanwhile, the co-doped sulfur element was found to be synergistic for nitrogen doping in N,S-CDs. The optimal N,S-CDs were successfully employed as good multicolor cell imaging probes due to their fine dispersion in water, excitation-dependent emission, excellent fluorescence stability and low toxicity. Besides, such N,S-CDs showed a wide detection range and excellent accuracy as fluorescent sensors for Fe(3+) ions.
Carbon dots (CDs) have tremendous potential applications in bioimaging, biomedicine, and optoelectronics. By far, it is still difficult to produce photoluminescence (PL) tunable CDs with high quantum yield (QY) across the entire visible spectrum and narrow the emission peak widths of CDs close to those of typical quantum dots. In this work, a series of CDs with tunable emission from 443 to 745 nm, quantum yield within 13-54%, and narrowed full width at half maximum (FWHM) from 108 to 55 nm, are obtained by only adjusting the reaction solvents in a one-pot solvothermal route. The distinct optical features of these CDs are based on their differences in the particle size, and the content of graphitic nitrogen and oxygen-containing functional groups, which can be modulated by controlling the dehydration and carbonization processes during solvothermal reactions. Blue, green, yellow, red, and even pure white light emitting films (Commission Internationale de L'Eclairage (CIE)= 0.33, 0.33, QY = 39%) are prepared by dispersing one or three kinds of CDs into polyvinyl alcohol with appropriate ratios. The near-infrared emissive CDs are excellent fluorescent probes for both in vitro and in vivo bioimaging because of their high QY in water, long-term stability, and low cytotoxicity.
Carbon dots (CDs) are a new class of photoluminescent (PL), biocompatible, environment-friendly, and low-cost carbon nanomaterials. Synthesis of highly efficient red-emitting carbon dots (R-CDs) on a gram scale is a great challenge at present, which heavily restricts the wide applications of CDs in the bioimaging field. Herein, R-CDs with a high quantum yield (QY) of 53% are produced on a gram scale by heating a formamide solution of citric acid and ethylenediamine. The as-prepared R-CDs have an average size of 4.1 nm and a nitrogen content of about 30%, with an excitation-independent emission at 627 nm. After detailed characterizations, such strong red fluorescence is ascribed to the contribution from the nitrogen- and oxygen-related surface states and the nitrogen-derived structures in the R-CD cores. Our R-CDs show good photostability and low cytotoxicity, and thus they are excellent red fluorescence probes for bioimaging both in vitro and in vivo.
Brightly red fluorescent carbon dots are synthesized hydrothermally and dissolved in diluted hydrochloric acid solution. Such carbon dots exhibit excitation-independent emission at about 620 nm with quantum yield over 10%, which is visible in daylight. After the carbon dots solution is sprayed to the fingerprints on various solid substrates and dried in air, clear fingerprints can be seen under an ultraviolet lamp and stay stable for 1 day. Detailed characterizations suggest that during the drying process, the coffee-ring effect and the electrostatic interactions between the carbon dots and the fingerprint residues prevent the typical aggregation-induced fluorescence quenching of carbon dots.
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