The persistence of spin coherence in a crystalline environment

Fuente: arXiv
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Auteurs principaux: Curran III, Gerald, Rex, Zachary, Wilson, Casper X., Weaver, Luke J., Biaggio, Ivan
Format: Preprint
Publié: 2024
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author Curran III, Gerald
Rex, Zachary
Wilson, Casper X.
Weaver, Luke J.
Biaggio, Ivan
author_facet Curran III, Gerald
Rex, Zachary
Wilson, Casper X.
Weaver, Luke J.
Biaggio, Ivan
contents We analyze quantum interference in the triplet-exciton pair generated by singlet exciton fission in a molecular crystal, and introduce transport-induced dephasing (TID) as a key effect that can suppress the expected fluorescence quantum beats when the triplet-exciton wavefunction can localize on inequivalent sites. TID depends on the triplet-exciton hopping rate between inequivalent sites and on the energy-shifts among the stationary states of the entangled triplet pair in different spatial configurations. The theoretical model is confirmed by experiments in rubrene single crystals, where triplet pairs remain entangled for more than 50 ns but quantum beats are suppressed by TID within a few nanoseconds when the magnetic field is misaligned by just a few degrees from specific symmetric directions. Our experiments deliver the zero-field parameters for the rubrene molecule in its orthorhombic lattice and information on triplet-exciton transport, in particular the triplet-exciton hopping rate between inequivalent sites, which we evaluate to be of the order of 150 ps in rubrene.
format Preprint
id arxiv_https___arxiv_org_abs_2406_02703
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle The persistence of spin coherence in a crystalline environment
Curran III, Gerald
Rex, Zachary
Wilson, Casper X.
Weaver, Luke J.
Biaggio, Ivan
Mesoscale and Nanoscale Physics
Optics
Quantum Physics
We analyze quantum interference in the triplet-exciton pair generated by singlet exciton fission in a molecular crystal, and introduce transport-induced dephasing (TID) as a key effect that can suppress the expected fluorescence quantum beats when the triplet-exciton wavefunction can localize on inequivalent sites. TID depends on the triplet-exciton hopping rate between inequivalent sites and on the energy-shifts among the stationary states of the entangled triplet pair in different spatial configurations. The theoretical model is confirmed by experiments in rubrene single crystals, where triplet pairs remain entangled for more than 50 ns but quantum beats are suppressed by TID within a few nanoseconds when the magnetic field is misaligned by just a few degrees from specific symmetric directions. Our experiments deliver the zero-field parameters for the rubrene molecule in its orthorhombic lattice and information on triplet-exciton transport, in particular the triplet-exciton hopping rate between inequivalent sites, which we evaluate to be of the order of 150 ps in rubrene.
title The persistence of spin coherence in a crystalline environment
topic Mesoscale and Nanoscale Physics
Optics
Quantum Physics
url https://arxiv.org/abs/2406.02703