Optical projection and spatial separation of spin entangled triplet-pairs from the S1 (21Ag-) state of pi-conjugated systems

• URL: http://arxiv.org/abs/2002.12465v2
• Date: Wed, 6 Jan 2021 13:55:26 GMT
• Title: Optical projection and spatial separation of spin entangled triplet-pairs from the S1 (21Ag-) state of pi-conjugated systems
• Authors: Raj Pandya, Qifei Gu, Alexandre Cheminal, Richard Y. S. Chen, Edward P. Booker, Richard Soucek, Michel Schott, Laurent Legrand, Fabrice Mathevet, Neil C. Greenham, Thierry Barisien, Andrew J. Musser, Alex W. Chin and Akshay Rao
• Abstract summary: We experimentally demonstrate that S1 (21Ag-) is a superposition state with strong contributions from spin-entangled pairs of triplet excitons (1(TT)) We 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. 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
• Score: 40.96261204117952
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: 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.

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