Triplet-triplet annihilation photon upconversion (TTA-UC) combines the energy of two photons to provide one of higher energy that can be used to drive photochemical or photophysical processes. TTA-UC proceeds at high efficiencies in dilute solution, but in solid state the efficiency drastically reduces. This is because exciton diffusion, compared to molecular diffusion in solid annihilator films, suffers concentration induced quenching, undermining efficient emission.
View Article and Find Full Text PDFWe report the formation of polariton condensates from strongly coupled molecules to bound states in the continuum with quadrupolar character in a metasurface of silicon nanoparticles. Our experiments demonstrate a strong dependence of the condensation threshold on the excitation spot size. The condensation threshold decreases as the excitation spot size increases, achieving thresholds below 3 μm cm for spot sizes of around 1 mm and condensate lifetimes exceeding 20 ps.
View Article and Find Full Text PDFThe short exciton diffusion length in organic semiconductors results in a strong dependence of the conversion efficiency of organic photovoltaic (OPV) cells on the morphology of the donor-acceptor bulk-heterojunction blend. Strong light-matter coupling provides a way to circumvent this dependence by combining the favorable properties of light and matter via the formation of hybrid exciton-polaritons. By strongly coupling excitons in P3HT-C OPV cells to Fabry-Perot optical cavity modes, exciton-polaritons are formed with increased propagation lengths.
View Article and Find Full Text PDFH-type supramolecular polymers with preferred helicity and highly efficient emission have been prepared from the self-assembly of chiral tetraphenylene-based monomers. Implementation of the one-dimensional fibers into dielectric nanoparticle arrays allows for a significant reshaping of fluorescence due to weak light-matter coupling.
View Article and Find Full Text PDFEfficient energy transport over long distances is essential for optoelectronic and light-harvesting devices. Although self-assembled nanofibers of organic molecules are shown to exhibit long exciton diffusion lengths, alignment of these nanofibers into films with large, organized domains with similar properties remains a challenge. Here, it is shown how the functionalization of C -symmetric carbonyl-bridged triarylamine trisamide (CBT) with oligodimethylsiloxane (oDMS) side chains of discrete length leads to fully covered surfaces with aligned domains up to 125 × 70 µm in which long-range exciton transport takes place.
View Article and Find Full Text PDFExciton transport in most organic materials is based on an incoherent hopping process between neighboring molecules. This process is very slow, setting a limit to the performance of organic optoelectronic devices. In this Article, we overcome the incoherent exciton transport by strongly coupling localized singlet excitations in a tetracene crystal to confined light modes in an array of plasmonic nanoparticles.
View Article and Find Full Text PDFUsing diffraction-limited ultrafast imaging techniques, we investigate the propagation of singlet and triplet excitons in single-crystal tetracene. Instead of an expected broadening, the distribution of singlet excitons narrows on a nanosecond time scale after photoexcitation. This narrowing results in an effective negative diffusion in which singlet excitons migrate toward the high-density region, eventually leading to a singlet exciton distribution that is smaller than the laser excitation spot.
View Article and Find Full Text PDFMaterials based on the laminar ordering of self-assembled molecules have a unique potential for applications requiring efficient energy migration through densely packed chromophores. Here, employing molecular assemblies of coil-rod-coil block molecules for triplet-triplet annihilation upconversion (TTA-UC) based on triplet energy migration with linearly polarized emission is reported. By covalently attaching discrete-length oligodimethylsiloxane (oDMS) to 9,10-diphenylanthracene (DPA), highly ordered 2D crystalline DPA sheets separated by oDMS layers are obtained.
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