Carbon dots keep attracting attention in multidisciplinary fields, motivating the development of new compounds. Phenylenediamine C 6 H 4 (NH 2 ) 2 dots are known to exhibit colorful emission, which depends on size, composition, and the functional surface groups, forming those structures. While quite a few fabrication protocols have been developed, the quantum yield of phenylenediamine dots still does not exceed 50% owing to undesired fragment formation during carbonization. Here, we demonstrate that an ethylene glycol-based environment allows obtaining multicolor high-quantum-yield phenylenediamine carbon dots. In particular, a kinetic realization of solvothermal synthesis in acidic environments enhances carbonization reaction yield for meta phenylenediamine compounds and leads to quantum yields, exciting 60%. Reaction yield after the product’s purification approaches 90%. Furthermore, proximity of metal ions (Nd 3+ , Co 3+ , La 3+ ) can either enhance or quench the emission, depending on the concentration. Optical monitoring of the solution allows performing an accurate detection of ions at picomolar concentrations. An atomistic model of carbon dots was developed to confirm that the functional surface group positioning within the molecular structure has a major impact on dots’ physicochemical properties. The high performance of new carbon dots paves the way toward their integration in numerous applications, including imaging, sensing, and therapeutics.
Local environment of fluorescent dyes could strongly affects emission dynamics of the latter. In particular, both signal intensities and emission lifetimes are highly sensitive to solvent temperatures. Here, temperature-dependent behavior Rhodamine B fluorescence in water and ethanol solutions was experimentally investigated. Phase transition point between liquid water and ice was shown to have a dramatic impact on both in intensity (30-fold drop) and in lifetime (from 2.68 ns down to 0.13 ns) of the dye luminescence along with the shift of spectral maxima from 590 to 625 nm. At the same time, use of ethanol as solvent does not lead to any similar behavior. The reported results and approaches enable further investigations of dye-solvent interactions and studies of physical properties at phase transition points.
Organic crystals with unique nonlinear optical properties have been attracting attention owing to their capability to outperform their conventional nonorganic counterparts. Since nonlinear material responses are linked to a crystal’s internal microscopic structure, molecular engineering of maximally unharmonic quantum potentials can boost macromolecular susceptibilities. Here, large-scale kainic acid (kainate) single crystals were synthesized, and their linear and nonlinear optical properties were studied in a broad spectral range, spanning the visible to THz spectral regions. The non-centrosymmetric zwitterionic crystallization, molecular structure, and intermolecular arrangement were found to act as additive donor–acceptor domains, enhancing the efficiency of the intrinsic second-order optical nonlinearity of this pure enantiomeric crystal. Molecular simulations and experimental analysis were performed to retrieve the crystals’ properties. The crystals were predicted and found to have good transparency in a broad spectral range from the UV to the infrared (0.2–20 μm). Second-harmonic generation was measured for ultrashort pumping wavelengths between 800 and 2400 nm, showing an enhanced response around 600 nm. Broadband THz generation was demonstrated with a detection limited bandwidth of >8 THz along with emission efficiencies comparable to and prevailing those of commercial ZnTe crystals. The broadband nonlinear response and high transparency make kainate crystals extremely attractive for realizing a range of nonlinear optical devices.
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