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Frenkel excitons are the primary photoexcitations in organic semiconductors and are ultimately responsible for the optical properties of such materials. They are also predicted to form bound exciton pairs, termed biexcitons, which are consequential intermediates in a wide range of photophysical processes. Generally, we think of bound states as arising from an attractive interaction. However, here, we report on our recent theoretical analysis, predicting the formation of stable biexciton states in a conjugated polymer material arising from both attractive and repulsive interactions. We show that in J-aggregate systems, 2J-biexcitons can arise from repulsive dipolar interactions with energies E 2 J > 2 E J , while in H-aggregates, 2H-biexciton states with energies E 2 H < 2 E H can arise corresponding to attractive dipole exciton/exciton interactions. These predictions are corroborated by using ultrafast double-quantum coherence spectroscopy on a [poly(2,5-bis(3-hexadecylthiophene-2-yl)thieno[3,2-b]thiophene)] material that exhibits both J- and H-like excitonic behavior.
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Resonant coupling of molecular excitons and optical anapoles in silicon nanosphere-J-aggregate heterostructures under vector beam illumination
Resonant excitation of high-index dielectric nanostructures and their coupling with molecular excitons provide great opportunities for engineering adaptable platforms for hybrid functional optical devices. Here, we numerically calculate resonance coupling of nonradiating anapole states to molecular excitons within silicon nanosphere-J-aggregate heterostructures under illumination with radially polarized cylindrical vector beams. The results show that the resonance coupling is accompanied by a scattering peak around the exciton transition frequency, and the anapole state splits into a pair of anticrossing eigenmodes with a mode splitting energy of ≈200meV. We also investigate the resonance coupling as a function of the J-aggregate parameters, such as thickness, exciton transition linewidth, and oscillator strength. Resonant coupling of the anapole states and J-aggregate heterostructures could be a promising platform for future nanophotonic applications such as in information processing and sensing.
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- Award ID(s):
- 2208240
- PAR ID:
- 10429995
- Publisher / Repository:
- Optical Society of America
- Date Published:
- Journal Name:
- Applied Optics
- Volume:
- 62
- Issue:
- 20
- ISSN:
- 1559-128X; APOPAI
- Format(s):
- Medium: X Size: Article No. 5487
- Size(s):
- Article No. 5487
- Sponsoring Org:
- National Science Foundation
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