Compared with fluorescence imaging utilizing fluorophores whose lifetimes are in the order of nanoseconds, time-resolved fluorescence microscopy has more advantages in monitoring target fluorescence. In this work, compound DCF-MPYM, which is based on a fluorescein derivative, showed long-lived luminescence (22.11 μs in deaerated ethanol) and was used in time-resolved fluorescence imaging in living cells. Both nanosecond time-resolved transient difference absorption spectra and time-correlated single-photon counting (TCSPC) were employed to explain the long lifetime of the compound, which is rare in pure organic fluorophores without rare earth metals and heavy atoms. A mechanism of thermally activated delayed fluorescence (TADF) that considers the long wavelength fluorescence, large Stokes shift, and long-lived triplet state of DCF-MPYM was proposed. The energy gap (ΔEST) of DCF-MPYM between the singlet and triplet state was determined to be 28.36 meV by the decay rate of DF as a function of temperature. The ΔE(ST) was small enough to allow efficient intersystem crossing (ISC) and reverse ISC, leading to efficient TADF at room temperature. The straightforward synthesis of DCF-MPYM and wide availability of its starting materials contribute to the excellent potential of the compound to replace luminescent lanthanide complexes in future time-resolved imaging technologies.
In recent years, lead halide perovskite nanocrystals (NCs) have attracted significant attention in both fundamental research and commercial applications because of their excellent optical and optoelectrical properties. However, the protective ligands on the surface of the perovskite NCs could be easily removed after the tedious process of centrifugation, separation, and dispersion, which greatly hampers their stability against light, heat, moisture, and oxygen and limits their practical applications. Here, we report a new post-processing free strategy (i.e., without centrifugation, separation, and dispersion process) of using an ultraviolet (UV)-polymerizable acrylic monomer of lauryl methacrylate as the solvent to synthesize CsPbBr3 NCs, and then adding polyester polyurethane acrylate oligomer, monomer (IBOA), and initiator for direct UV polymerization to fabricate NC–polymer composite films. These films exhibited an improved photoluminescence quantum yield (85–90%) than classic NC films (40–50%), which were processed using octadecene (ODE) as the solvent for NC synthesis and postprocessed for UV polymerization. Significantly, the as-fabricated films by post-processing free strategy exhibited excellent photostability against strong Xe lamp illumination; while the other films using classic methods were quickly photodegraded. Meanwhile, these NC–polymer composite films showed good stability against moisture and heating when aging in water at 50 °C for over 200 h. These films, along with K2SiF6:Mn4+ (KSF) phosphor emitters, were used as downconverters for blue light-emitting diodes in liquid-crystal displays with a wide color gamut of 115% in the International Commission on Illumination (CIE) 1931 color space. This work provides a facile and effective strategy for the preparation of ultrastable and bright color-conversion NC films for the development of the next-generation wide color gamut displays.
Lead halide perovskites with well-defined morphology have attracted attention for their unique properties as a promising new class of semiconductor materials in photovoltaics and optoelectronics. However, controlling morphologies and compositions of perovskite nanostructures with improved stability, especially for double cation lead halide perovskite, still remains a challenge. Here, we demonstrate a colloidal synthetic approach for direct synthesis of stable singlecrystal formamidinium (FA) cesium double cation lead halide FA 0.33 Cs 0.67 PbBr 3−x I x (0 ≤ x ≤ 3) perovskite nanostructures with controllable morphology over a wide range of halide compositions, without using a previous anion-exchange process. The presence of FA alloyed in the A site for the pure cesium lead halide perovskite structure can stabilize the nanocrystals while delivering a better balance between structure and composition. On the basis of the FA 0.33 Cs 0.67 PbBr 3−x I x alloy perovskite system, we achieved nanowires and nanosheets with high yield of various halide compositions by tuning the ligand participating in the reaction. These new perovskite nanostructures with well-defined morphology and compositions demonstrated improved stability and fluorescent and optoelectronic properties, which may allow them to find application as replacements for conventional semiconductor nanostructures in nanoscale devices.
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