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.

Mattiello, S., Mecca, S., Ronchi, A., Calascibetta, A., Mattioli, G., Pallini, F., et al. (2022). Diffusion-Free Intramolecular Triplet–Triplet Annihilation in Engineered Conjugated Chromophores for Sensitized Photon Upconversion. ACS ENERGY LETTERS, 2022(7), 2435-2442 [10.1021/acsenergylett.2c01224].

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

Mattiello, Sara;Mecca, Sara;Ronchi, Alessandra;Calascibetta, Adiel;Pallini, Francesca;Meinardi, Francesco
;
Beverina, Luca
;
Monguzzi, Angelo
2022

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.
Articolo in rivista - Articolo scientifico
Scientifica
excitons, triplets, upconversion, conjugated systems, fluorescence, photon managing;
English
Mattiello, S., Mecca, S., Ronchi, A., Calascibetta, A., Mattioli, G., Pallini, F., et al. (2022). Diffusion-Free Intramolecular Triplet–Triplet Annihilation in Engineered Conjugated Chromophores for Sensitized Photon Upconversion. ACS ENERGY LETTERS, 2022(7), 2435-2442 [10.1021/acsenergylett.2c01224].
Mattiello, S; Mecca, S; Ronchi, A; Calascibetta, A; Mattioli, G; Pallini, F; Meinardi, F; Beverina, L; Monguzzi, A
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/10281/386925
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