Persistence of Spin Coherence in a Crystalline Environment

Curran, Gerald; Rex, Zachary; Xallan Wilson, Casper; Weaver, Luke J.; Biaggio, Ivan

doi:10.1103/PhysRevLett.133.056901

Persistence of Spin Coherence in a Crystalline Environment

Journal Article · Mon Jul 29 00:00:00 EDT 2024 · Physical Review Letters

DOI:https://doi.org/10.1103/PhysRevLett.133.056901· OSTI ID:2967036

^[1]; Rex, Zachary ^[1]; ^[1]; ^[1]; ^[1]

Lehigh Univ., Bethlehem, PA (United States)

Here, 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 wave function 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.

View Accepted Manuscript (DOE)

Research Organization:: Lehigh Univ., Bethlehem, PA (United States); Lehigh University, Bethlehem, PA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: SC0020981

OSTI ID:: 2967036

Alternate ID(s):: OSTI ID: 2377662
OSTI ID: 2406961
OSTI ID: 2473790

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 5 Vol. 133; ISSN 1079-7114; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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