| Autor: |
Pandya, R, Gu, Q, Cheminal, A, Chen, RYS, Booker, EP, Soucek, R, Schott, M, Legrand, L, Mathevet, F, Greenham, NC, Barisien, T, Musser, AJ, Chin, AW, Rao, A |
| Přispěvatelé: |
Pandya, Raj [0000-0003-1108-9322], Greenham, Neil [0000-0002-2155-2432], Rao, Akshay [0000-0003-0320-2962], Apollo - University of Cambridge Repository |
| Rok vydání: |
2020 |
| Předmět: |
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| Popis: |
The S1 (21Ag-) state is an optically dark state of natural and synthetic pi-conjugated materials that can play a critical role in optoelectronic processes such as, energy harvesting, photoprotection and singlet fission. Despite this widespread importance, direct experimental characterisations of the electronic structure of the S1 (21Ag-) wavefunction have remained scarce and uncertain, although advanced theory predicts it to have a rich multi-excitonic character. Here, studying an archetypal polymer, polydiacetylene, and carotenoids, we experimentally demonstrate that S1 (21Ag-) is a superposition state with strong contributions from spin-entangled pairs of triplet excitons (1(TT)). We further show that optical manipulation of the S1 (21Ag-) wavefunction using triplet absorption transitions allows selective projection of the 1(TT) component into a manifold of spatially separated triplet-pairs with lifetimes enhanced by up to one order of magnitude and whose yield is strongly dependent on the level of inter-chromophore coupling. Our results provide a unified picture of 21Ag-states in pi-conjugated materials and open new routes to exploit their dynamics in singlet fission, photobiology and for the generation of entangled (spin-1) particles for molecular quantum technologies. |
| Databáze: |
OpenAIRE |
| Externí odkaz: |
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