Sensitized triplet–triplet-annihilation-based photon upconversion (TTA-UC) permits the conversion of light into radiation of higher energy and involves a sequence of photophysical processes between two dyes. In contrast to other upconversion schemes, TTA-UC allows the frequency shifting of low-intensity light, which makes it particularly suitable for solar-energy harvesting technologies. High upconversion yields can be observed for low viscosity solutions of dyes; but, in solid materials, which are better suited for integration in devices, the process is usually less efficient. Here, it is shown that this problem can be solved by using transparent nanodroplet-containing polymers that consist of a continuous polymer matrix and a dispersed liquid phase containing the upconverting dyes. These materials can be accessed by a simple one-step procedure that involves the free-radical polymerization of a microemulsion of hydrophilic monomers, a lipophilic solvent, the upconverting dyes, and a surfactant. Several glassy and rubbery materials are explored and a range of dyes that enable TTA-UC in different spectral regions are utilized. The materials display upconversion efficiencies of up to ≈15%, approaching the performance of optimized oxygen-free reference solutions. The data suggest that the matrix not only serves as mechanically coherent carrier for the upconverting liquid phase, but also provides good protection from atmospheric oxygen.
High yields of triplet–triplet-annihilation-based photon upconversion can be observed for solutions of dyes; but, in solid materials, which are better suited for integration in devices, this process is usually less efficient. It is shown that new, easily accessible nanodroplet-containing polymers consisting of a continuous polymer matrix and a dispersed liquid phase doped with dyes approach the performance of oxygen-free reference solutions.
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