Perovskite solar cells prepared via spray-deposition of the active layer have been realized, advancing this promising technology towards roll-to-roll compatible processing methods.
Strongly coupled optical microcavities containing different exciton states permit the creation of hybrid-polariton modes that can be described in terms of a linear admixture of cavity-photon and the constituent excitons. Such hybrid states have been predicted to have optical properties that are different from their constituent parts, making them a test bed for the exploration of light-matter coupling. Here, we use strong coupling in an optical microcavity to mix the electronic transitions of two J-aggregated molecular dyes and use both non-resonant photoluminescence emission and photoluminescence excitation spectroscopy to show that hybrid-polariton states act as an efficient and ultrafast energy-transfer pathway between the two exciton states. We argue that this type of structure may act as a model system to study energy-transfer processes in biological light-harvesting complexes.
We have measured the temperature-dependent photoluminescence quantum yields
(PLQYs) of poly(9, 9-dioctylfluorene) (PFO) films with four morphologies,
namely as-spin-coated (SC) glass, quenched nematic glass, crystalline, and
vapour-treated SC glass containing a fraction of 21 helix conformation (β-phase)
chains. We find that the room temperature PLQYs of the as-SC,
crystalline, and quenched films all increase as the temperature
is reduced. However, the PLQY of the film containing β-phase chains
decreases at temperatures below 150 K. Via temperature-dependent photoinduced
absorption measurements, we show that the polaron population in films containing β-phase
PFO chains grows as the temperature is reduced, and is significantly larger than in films
with any of the other morphologies. Because of the smaller HOMO–LUMO (highest
occupied molecular orbital–lowest unoccupied molecular orbital) energy gap of the β-phase
chains compared to chains in the surrounding glassy PFO matrix, they
act as recombination sites for excitons, and as traps for polarons. Hence
at low temperatures, the polarons become strongly localized on these
chains, where they quench the singlet excitons and reduce the PLQY.
Coherent excitations of intricate assemblies of molecules play an important role in natural photosynthesis. Microcavities are wavelength-dimension artificial structures in which excitations can be made to couple through their mutual interactions with confined photon modes. Results for microcavities containing two spatially separated cyanine dyes are presented here, where simultaneous strong coupling of the excitations of the individual dyes to a single cavity mode leads to new eigenmodes, described as admixtures of all three states. These "hybrid" exciton-photon structures are of potential interest as model systems in which to study energy capture, storage, and transfer among coherently coupled molecular excitations.
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