A generic, facile, and waterborne strategy is introduced to fabricate flexible, low‐cost nanocomposite films with room‐temperature phosphorescence (RTP) by incorporating waterborne RTP polymers into self‐assembled bioinspired polymer/nanoclay nanocomposites. The excellent oxygen barrier of the lamellar nanoclay structure suppresses the quenching effect from ambient oxygen (kq) and broadens the choice of polymer matrices towards lower glass transition temperature (Tg), while providing better mechanical properties and processability. Moreover, the oxygen permeation and diffusion inside the films can be fine‐tuned by varying the polymer/nanoclay ratio, enabling programmable retention times of the RTP signals, which is exploited for transient information storage and anti‐counterfeiting materials. Additionally, anti‐interception materials are showcased by tracing the interception‐induced oxygen history that interferes with the preset self‐erasing time. Merging bioinspired nanocomposite design with RTP materials contributes to overcoming the inherent limitations of molecular design of organic RTP compounds, and allows programmable temporal features to be added into RTP materials by controlled mesostructures. This will assist in paving the way for practical applications of RTP materials as novel anti‐counterfeiting materials.
Fast emission and high color purity are essential characteristics of modern opto-electronic devices, such as organic light emitting diodes (OLEDs). These properties are currently not met by the latest generation of thermally activated delayed fluorescence (TADF) emitters. Here, we present an approach, called “hot exciplexes” that enables access to both attributes at the same time. Hot exciplexes are produced by coupling facing donor and acceptor moieties to an anthracene bridge, yielding an exciplex with large T1 to T2 spacing. The hot exciplex model is investigated using optical spectroscopy and quantum chemical simulations. Reverse intersystem crossing is found to occur preferentially from the T3 to the S1 state within only a few nanoseconds. Application and practicality of the model are shown by fabrication of organic light-emitting diodes with up to 32 % hot exciplex contribution and low efficiency roll-off.
The transition toward future sustainable societies largely depends on disruptive innovations in biobased materials to substitute nonsustainable advanced functional materials. In the field of optics, advanced devices (e.g., lasers or metamaterial devices) are typically manufactured using top‐down engineering and synthetic materials. This work breaks with such concepts and switchable lasers self‐assembled from plant‐based cellulose nanocrystals and fluorescent polymers at room temperature and from water are shown. Controlled structure formation allows laser‐grade cholesteric photonic bandgap materials, in which the photonic bandgap is matched to the fluorescence emission to function as an efficient resonator for low threshold multimode lasing. The lasers can be switched on and off using humidity, and can be printed into pixelated arrays. Additionally, the materials exhibit stiffness above typical thermoplastic polymers and biodegradability in soil. The concept showcases that highly advanced functions can be encoded into biobased materials, and opens the design space for future sustainable optical devices of unprecedented function.
Here, we present a hybrid organic/inorganic photonic composite, which generates laser emission from the organic material after pumping the inorganic component. The composite consists of a methylammonium lead-halide perovskite matrix CH 3 NH 3 Pb(Br x Cl (1−x) ) 3 and monodisperse poly(fluorene-co-divinylbenzene) particles, which have excellent optical feedback and gain. Micrometer-sized conjugated polymer particles (CPPs) are deposited together with the perovskite precursor from solution using a single-step vertical deposition method. The particles self-assemble into a photonic crystal and the perovskite forms an inorganic matrix in the interstitial space. Energy transfer to the polymer particles after optically pumping the metal-halide perovskite is studied in two systems with different halide ratios in the perovskite (Br to Cl: 1/9 and 4/6) to control the overlap of the perovskite emission energy with the absorption of the particles. From time-resolved photoluminescence experiments, we observe nonradiative energy transfer from the perovskite to the particle in both coassemblies; however, increased spectral overlap of perovskite emission and particle absorption enhances energy transfer efficiency by 37%. Because of the ordered assembly of the CPPs, we observe laser emission after energy transfer from the Cl-rich perovskite matrix at fluences of 13 mJ/cm 2 . Our report of a hybrid material system that combines the excellent optoelectronic properties of metal-halide perovskites with the outstanding optical properties of conjugated polymers represents a new approach and progress in the pursuit of electrically pumped polymer lasers.
Step-growth dispersion polymerization is a powerful method to produce uniform and monodisperse particles of π-conjugated polymers with tunable sizes. While the growth period in such step-growth dispersion polymerizations is well understood, it remains unknown whether or not the nucleation process comprises an aggregation or coalescence step. Only a complete understanding of the entire mechanism of particle formation during step-growth dispersion polymerization will provide information about the morphology inside of the polymer particles and enable design of synthesis strategies to give access to more sophisticated particle architectures, such as core–shell or patchy particles. We employ spectroscopic and light scattering analysis to shed light on the nucleation event in a Heck-type C–C cross-coupling dispersion polymerization. In contrast to the typical mechanism, our dispersion polymerization of conjugated polymer particles does not feature the aggregation step.
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