Cascade of multi-exciton states generated by singlet fission

Fuente: arXiv
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Autori principali: Sun, Yan, Monteverde, M., Derkach, V., Anthony, J. E., Chepelianskii, A. D.
Natura: Preprint
Pubblicazione: 2024
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author Sun, Yan
Monteverde, M.
Derkach, V.
Anthony, J. E.
Chepelianskii, A. D.
author_facet Sun, Yan
Monteverde, M.
Derkach, V.
Anthony, J. E.
Chepelianskii, A. D.
contents Identifying multi-exciton states generated from singlet fission is key to understanding the carrier multiplication process, which presents a strategy for improving the efficiency of photovoltaics and bio-imaging. Broadband optically detected magnetic resonance is a sensitive technique to detect multi-exciton states. Here we report a dominant species emerging under intense light excitation corresponding to a weakly exchange coupled triplet pair located on adjacent molecules oriented by nearly 90 degrees, contrasting to the pi-stacked triplet pair under low excitation intensity. The weakly coupled species model precisely reproduces the intricate spin transitions in the Hilbert space of the triplet pair. Combining the magneto photoluminescence and high-magnetic field ODMR, we also identify a strongly exchange-coupled state of three triplet excitons formed by photoexcited V2, which manifests through the magnetic field induced level crossings between its quintet and triplet manifolds. The excellent agreement between the experimental Zeeman fan and the two-triplet spin Hamiltonian highlights the potential of multi-exciton states for quantum information processing.
format Preprint
id arxiv_https___arxiv_org_abs_2406_09268
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Cascade of multi-exciton states generated by singlet fission
Sun, Yan
Monteverde, M.
Derkach, V.
Anthony, J. E.
Chepelianskii, A. D.
Mesoscale and Nanoscale Physics
Identifying multi-exciton states generated from singlet fission is key to understanding the carrier multiplication process, which presents a strategy for improving the efficiency of photovoltaics and bio-imaging. Broadband optically detected magnetic resonance is a sensitive technique to detect multi-exciton states. Here we report a dominant species emerging under intense light excitation corresponding to a weakly exchange coupled triplet pair located on adjacent molecules oriented by nearly 90 degrees, contrasting to the pi-stacked triplet pair under low excitation intensity. The weakly coupled species model precisely reproduces the intricate spin transitions in the Hilbert space of the triplet pair. Combining the magneto photoluminescence and high-magnetic field ODMR, we also identify a strongly exchange-coupled state of three triplet excitons formed by photoexcited V2, which manifests through the magnetic field induced level crossings between its quintet and triplet manifolds. The excellent agreement between the experimental Zeeman fan and the two-triplet spin Hamiltonian highlights the potential of multi-exciton states for quantum information processing.
title Cascade of multi-exciton states generated by singlet fission
topic Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2406.09268