Optical probes of the quantum-entangled triplet-triplet state in a heteroacene dimer

Souratosh Khan, Sumitendra Mazumdar

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

The nature and extent of the spin-entanglement in the triplet-triplet biexciton with total spin zero in correlated-electron π-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.

Original languageEnglish (US)
Article number165202
JournalPhysical Review B
Volume98
Issue number16
DOIs
StatePublished - Oct 10 2018

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Dimers
atomic energy levels
dimers
Excited states
Excitons
probes
Electrons
excitons
Electronic structure
Absorption spectra
excitation
fission
Wavelength
electrons
electronic structure
absorption spectra
predictions
Experiments
wavelengths
LDS 751

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics

Cite this

Optical probes of the quantum-entangled triplet-triplet state in a heteroacene dimer. / Khan, Souratosh; Mazumdar, Sumitendra.

In: Physical Review B, Vol. 98, No. 16, 165202, 10.10.2018.

Research output: Contribution to journalArticle

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