Carbon dots (CDs) are light-emitting nanoparticles that show great promise for applications in biology and medicine due to the ease of fabrication, biocompatibility, and attractive optical properties. Optical chirality, on the other hand, is an intrinsic feature inherent in many objects in nature, and it can play an important role in the formation of artificial complexes based on CDs that are implemented for enantiomer recognition, site-specific bonding, etc. We employed a one-step hydrothermal synthesis to produce chiral CDs from the commonly used precursors citric acid and ethylenediamine together with a set of different chiral precursors, namely, L-isomers of cysteine, glutathione, phenylglycine, and tryptophan. The resulting CDs consisted of O,N-doped (and also S-doped, in some cases) carbonized cores with surfaces rich in amide and hydroxyl groups; they exhibited high photoluminescence quantum yields reaching 57%, chiral optical signals in the UV and visible spectral regions, and two-photon absorption. Chiral signals of CDs were rather complex and originated from a combination of the chiral precursors attached to the CD surface, hybridization of lower-energy levels of chiral chromophores formed within CDs, and intrinsic chirality of the CD cores. Using DFT analysis, we showed how incorporation of the chiral precursors at the optical centers induced a strong response in their circular dichroism spectra. The optical characteristics of these CDs, which can easily be dispersed in solvents of different polarities, remained stable during pH changes in the environment and after UV exposure for more than 400 min, which opens a wide range of bio-applications.
Today, the development of nanomaterials with sensing properties attracts much scientific interest because of the demand for low-cost nontoxic colloidal nanoprobes with high sensitivity and selectivity for various biomedical and environment-related applications. Carbon dots (CDs) are promising candidates for these applications as they demonstrate unique optical properties with intense emissions, biocompatibility, and ease of fabrication. Herein, we developed synthesis protocols to obtain CDs based on o-phenylenediamine with a variety of optical responses depending on additional precursors and changes in the reaction media. The obtained CDs are N-doped (N,S-doped in case of thiourea addition) less than 10 nm spherical particles with emissions observed in the 300–600 nm spectral region depending on their chemical composition. These CDs may act simultaneously as absorptive/fluorescent sensing probes for solvent polarity with ∆S/∆ENT up to 85, for ∆ENT from 0.099 to 1.0 and for pH values in the range of 3.0–8.0, thus opening an opportunity to check the pH in non-pure water or a mixture of solvents. Moreover, CDs preserve their optical properties when embedded in cellulose strips that can be used as sensing probes for fast and easy pH checks. We believe that the resulting dual-purpose sensing nano probes based on CDs will have high demand in various sensing applications.
Photovoltaic devices based on organic–inorganic hybrid perovskites have engaged tremendous attention due to the enormous increase in power conversion efficiency (PCE). However, defect states formed at grain boundaries and interfaces hinder the achievement of PCE. A prospective strategy to both reduce interfacial defects and control perovskite growth is the passivation of interfaces. The passivation of the electron-transporting layer/perovskite interface with ultrasmall carbon dots (CDs) with suitable chemical composition and functional groups on their surface may simultaneously affect the morphology of a perovskite layer, facilitate charge carriers extraction, and suppress interfacial recombination. Here, we show that CDs synthesized from diamine precursors may be used as an interlayer at the SnO2/FACsPbI3 interface. Ultrasmall CDs form a smooth, thin layer, providing better perovskite layer morphology. CD interlayers result in an increased average perovskite grain size, suppress the formation of small grains, and improve charge carriers’ extraction. As a result, photovoltaic devices with CD interlayers demonstrate a higher PCE due to the increased short-circuit current density and fill factor. These findings provide further insight into the construction of interfaces based on carbon nanomaterials.
Carbon dots can be used for the fabrication of colloidal multi-purpose complexes for sensing and bio-visualization due to their easy and scalable synthesis, control of their spectral responses over a wide spectral range, and possibility of surface functionalization to meet the application task. Here, we developed a chemical protocol of colloidal complex formation via covalent bonding between carbon dots and plasmonic metal nanoparticles in order to influence and improve their fluorescence. We demonstrate how interactions between carbon dots and metal nanoparticles in the formed complexes, and thus their optical responses, depend on the type of bonds between particles, the architecture of the complexes, and the degree of overlapping of absorption and emission of carbon dots with the plasmon resonance of metals. For the most optimized architecture, emission enhancement reaching up to 5.4- and 4.9-fold for complexes with silver and gold nanoparticles has been achieved, respectively. Our study expands the toolkit of functional materials based on carbon dots for applications in photonics and biomedicine to photonics.
In recent years, carbon dots have attracted much scientific attention due to their unique properties, which can find applications in many fields. We have developed synthesis protocols of carbon dots with different structure and optical properties using o-phenylenediamine. The change in absorption and luminescence spectra of carbon dots were studied in detail. The obtained samples show intensive luminescence at 350 nm and 450 or 550 nm dependent on synthesis parameters.
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