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Article Dans Une Revue Physical Review Letters Année : 2020

Spin fine-structure reveals bi-exciton geometry in an organic semiconductor

Résumé

In organic semiconductors, bi-exciton states are key intermediates in carrier-multiplication and exciton annihilation. Of particular recent interest is the spin-2 (quintet) bi-exciton. Comprised of two triplet excitons, the bi-exciton can be formed by singlet fission (the formation of two triplet excitons from one singlet state) or by triplet-triplet annihilation (the reverse process). Of interest for photovoltaics and photocatalysis, the wavefunction of these optically dark bi-excitons is difficult to probe and predict. However, the local geometry of the pair-state is imprinted in the fine structure of its spin Hamiltonian. To access the fine structure of the quintet-state we develop and deploy broadband optically detected magnetic resonance (0-9 GHz). Here we correlate the experimentally extracted spin structure with the molecular crystal structure to identify the specific molecular pairings on which the bi-exciton state resides.
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Dates et versions

hal-02403463 , version 1 (11-12-2019)

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K. M. M Yunusova, S. L. L Bayliss, T. Chanelière, V. Derkach, J. E. E Anthony, et al.. Spin fine-structure reveals bi-exciton geometry in an organic semiconductor. Physical Review Letters, 2020, 125 (9), pp.097402. ⟨10.1103/PhysRevLett.125.097402⟩. ⟨hal-02403463⟩
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