Optical probes of the quantum-entangled triplet-triplet state in a heteroacene dimer
AffiliationUniv Arizona, Dept Phys
Univ Arizona, Dept Chem & Biochem
Univ Arizona, Coll Opt Sci
MetadataShow full item record
PublisherAMER PHYSICAL SOC
CitationKhan, S., & Mazumdar, S. (2018). Optical probes of the quantum-entangled triplet-triplet state in a heteroacene dimer. Physical Review B, 98(16), 165202.
JournalPHYSICAL REVIEW B
Rights© 2018 American Physical Society.
Collection InformationThis item from the UA Faculty Publications collection is made available by the University of Arizona with support from the University of Arizona Libraries. If you have questions, please contact us at email@example.com.
AbstractThe nature and extent of the spin-entanglement in the triplet-triplet biexciton with total spin zero in correlated-electron pi-conjugated systems continues to be an enigma. Differences in the ultrafast transient absorption spectra of free triplets versus the triplet-triplet can give a measure of the entanglement. This, however, requires theoretical understandings of transient absorptions from the optical spin-singlet, the lowest spin-triplet exciton, as well as from the triplet-triplet state, whose spectra are often overlapping and hence difficult to distinguish. We present a many-electron theory of the electronic structure of the triplet-triplet, and of complete wavelength-dependent excited state absorptions (ESAs) from all three states in a heteroacene dimer of interest in the field of intramolecular singlet fission. The theory allows direct comparisons of ESAs with existing experiments as well as experimental predictions, and gives physical understandings of transient absorptions within a pictorial exciton basis that can be carried over to other experimental systems.
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