Resolving the emissive intermediate in singlet fission

Damon de Clercq^a, Jiale Feng^a, Parisa Hosseinabadi^b, Michael Nielsen^b, Matthew Brett^a, Shyamal Prasad^a, Abbas Farahani^a, Hsiu Li^a, Samuel Sanders^c, Jonathon Beves^a, Ned Ekins-Daukes^b, Jared Cole^d, Pall Thordarson^a, Murad Tayebjee^b, Timothy Schmidt^a, Ben Carwithen^a

^aUNSW Sydney, Samuels Building, Kensington, Australia

^bUniversity of New South Wales, Australian Centre for Advanced Photovoltaics, School of Photovoltaic and Renewable Engineering, Sydney 2052, Sydney, Australia

^cRowland Institute at Harvard, Massachusetts, US, Edwin H Land Boulevard, 100, Cambridge, United States

^dRMIT University, Melbourne, Australia

International Conference on Hybrid and Organic Photovoltaics
Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV24)

València, Spain, 2024 May 12th - 15th

Organizer: Bruno Ehrler

Oral, Damon de Clercq, presentation 011
DOI: https://doi.org/10.29363/nanoge.hopv.2024.011
Publication date: 6th February 2024

Singlet fission offers a way to overcome the detailed balance limit in silicon photovoltaics by addressing thermalisation losses.[1] This process, which occurs in adjacent chromophores, describes the splitting of the initial singlet excited state into two low-energy triplet excitons via a triplet pair intermediate ¹(TT). If the triplet state energy is greater than the 1.1 eV bandgap of silicon, the triplet excitons in the organic semiconductor can transfer to silicon. Such a device could realise efficiencies of 45%.[2]

Tetracene was recently shown to undergo triplet transfer to silicon.[3] This demonstration was a major step towards the realisation of a working singlet fission device. However, tetracene is not an ideal chromophore as the singlet fission yield is not unity (c.a. 120% out of 200%) and the triplet energy (1.1 eV) is on the silicon band edge. The field therefore requires new chromophores that have yields closer to unity and greater triplet energies.

To design new chromophores a clear understanding of the role of the excimer and the triplet-pair state in singlet fission is required. This presentation will discuss our recent results in resolving the emissive intermediate state in singlet fission.[4] I will present transient photoluminescence and spectrally resolved magneto-photoluminescence data which identifies an emissive species that is distinct from the excimer state. Our results confirm that the excimer acts as a trap and unites the view that the ¹(TT) state is an emissive intermediate in singlet fission.

References:

[1] Rao, A., Friend, R. Harnessing singlet exciton fission to break the Shockley–Queisser limit. Nat. Rev. Mater. 2017, 2 17063

[2] Tayebjee, M.J.Y., Gray-Weale, A. A., Schmidt, T. W. Thermodynamic Limit of Exciton Fission Solar Cell Efficiency J. Phys. Chem. Lett. 2012, 3, 19, 2749–2754

[3] Einzinger, M., Wu, T., Kompalla, J.F. et al. Sensitization of silicon by singlet exciton fission in tetracene. Nature, 2019 571, 90–94

[4] Feng J*, Hosseinabadi P*, de Clercq D*, Nielsen M, Brett M, Prasad S, et al. Observation of an emissive intermediate in a liquid singlet fission and triplet fusion system at room temperature. ChemRxiv. 2023

Acknowledgements:

This work was supported by the Australian Research Council (Centre of Excellence in Exciton Science CE170100026).

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