Diffusion-Free Intramolecular Triplet-Triplet Annihilation in Engineered Conjugated Chromophores for Sensitized Photon Upconversion

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Abstract

The photon upconversion based on sensitized triplet-triplet annihilation (sTTA-UC) is a spin-flip mechanism exploited to recover the energy stored on dark triplet states in conjugated systems. In this process, a high-energy fluorescent singlet is created through the collision and fusion of two low-energy triplets belonging to different diffusing molecules. Its high yield in solution under low excitation intensity and noncoherent light highlighted the huge potential of sTTA-UC to provide a breakthrough in solar technologies. However, its diffusion-limited nature restrains its efficiency in the solid state. To overcome this issue, we propose a single-molecule system that is able to host simultaneously more than one triplet, thus enabling a diffusion-free intramolecular TTA. We obtain the first direct demonstration of intramolecular triplet fusion by tailored photoluminescence spectroscopy experiments, thus opening the way to realize a new family of single-molecule upconverters with huge potential in solar and lighting technologies by accessing the natural triplets' energy reservoir.

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Mattiello, S., Mecca, S., Ronchi, A., Calascibetta, A., Mattioli, G., Pallini, F., … Monguzzi, A. (2022). Diffusion-Free Intramolecular Triplet-Triplet Annihilation in Engineered Conjugated Chromophores for Sensitized Photon Upconversion. ACS Energy Letters, 7(8), 2435–2442. https://doi.org/10.1021/acsenergylett.2c01224

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