No abstract

CsPbX (X = Cl, Br, I) perovskite quantum dots (QDs) are potential emitting materials for illumination and display applications, but toxic Pb is not environment- and user-friendly. In this work, we demonstrate the partial replacement of Pb with Mn through phosphine-free hot-injection preparation of CsPbMnCl QDs in colloidal solution. The Mn substitution ratio is up to 46%, and the as-prepared QDs maintain the tetragonal crystalline structure of the CsPbCl host. Meaningfully, Mn substitution greatly enhances the photoluminescence quantum yields of CsPbCl from 5 to 54%. The enhanced emission is attributed to the energy transfer of photoinduced excitons from the CsPbCl host to the doped Mn, which facilitates exciton recombination via a radiative pathway. The intensity and position of this Mn-related emission are also tunable by altering the experimental parameters, such as reaction temperature and the Pb-to-Mn feed ratio. A light-emitting diode (LED) prototype is further fabricated by employing the as-prepared CsPbMnCl QDs as color conversion materials on a commercially available 365 nm GaN LED chip.

A new type of fluorescent material is presented, which is called non-conjugated polymer dots (NCPDs). The NCPDs only possess sub-fluorophores (which are groups such as C=O, C=N, N=O) instead of typical conjugated fluorophore groups, and thus these materials should not have strong photoluminescence (PL) in the usual sense. Nevertheless, the PL of these sub-fluorophores can be enhanced by chemical crosslinking or physical immobilization of polymer chains, which is named the crosslink-enhanced emission (CEE) effect. The significant advances achieved by us and other groups on both experimental and theoretical aspects are discussed, and the covalent-bond CEE, rigidity-aggregated CEE, or supramolecular CEE in NCPDs is elaborated. Moreover, synthetic strategies, unique optical properties, and the promise of NCPDs in bio-related fields, such as bioimaging and drug delivery, are systematically discussed.

Polymer carbon dots (PCDs) represent a new class of carbon dots (CDs) possessing sub‐fluorophores and unique polymer‐like structures. However, like small molecule dyes and traditional CDs, PCDs often suffer from self‐quenching effect in solid state, limiting their potential applications. Moreover, it is hard to prepare PCDs that have the same chemical structure, exhibiting full‐color emission under one fixed excitation wavelength by only modulating the concentration of the PCDs. Herein, self‐quenching‐resistant solid‐state fluorescent polymer carbon dots (SSFPCDs) are prepared, which exhibit strong red SSF without any other additional solid matrices, while having a large production yield (≈89%) and a considerable quantum yield of 8.50%. When dispersed in water or solid matrices in gradient concentrations, they can exhibit yellow, green, and blue fluorescence, realizing the first SSFPCDs with the same chemical structure emitting in full‐color range by changing the ratio of SSFPCDs to the solid matrices.

A universal route to GQDs is developed based on "solution phase-based scissor" methods. The PL centers of the GQDs are systematically studied and are proved to be the surface state. This is related to the hybridization structure of the edge groups and the connected partial graphene core. Through experiment and analysis, we have preliminarily proved that the efficient edge groups for green emission are mainly carboxyl, carbonyl and amide. This is indicated by the following three factors: firstly, the PL of GQDs is enhanced by UV exposure, during which partial -OH groups are converted into carboxyl groups; secondly, the PL properties of GQDs can be further improved by one-step solvothermal treatment, in which partial carboxyl groups are converted to amide groups and the surface state of the GQDs is enhanced; thirdly, reduced m-GQDs possess more -OH groups compared with reduced GQDs, resulting in more blue PL centers (the carboxyl, carbonyl and amide-based green centers are converted to -OH-based blue centers). The present work highlights a very important direction for the understanding of the PL mechanism of GQDs and other related carbon-based materials.