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arXiv 2108.01618cond-mat.mtrl-sci
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关于有机polymer聚集体中杂化双激子的稳定性

Concerning the stability of hybrid biexcitons in organic polymer aggregates

Eric R. Bittner, Carlos Silva-Acuna

摘要:

Frenkel激子是有机半导体中的主要光激发,并且最终负责这种材料的光学性质。它们还被预测形成\emph{bound}激子对,称为双激子,这是在广泛的物理过程中的必然中间体。一般来说,我们认为束缚态产生于吸引相互作用。然而,在这里,我们报告我们最近的理论分析预测形成稳定的双激子状态的共轭聚合物材料所产生的吸引力和排斥力的相互作用。我们发现,在J-聚集体系统中,JJ-双激子可以产生从排斥偶极相互作用的能量$E_{JJ}> 2E_J$,而在H-聚集体,HH-双激子态$E_{HH} < 2E_H$对应的吸引偶极激子/激子相互作用。这些预测证实了使用超快双量子相干性光谱的PBTTT材料,表现出J-和H-类激子行为。

英文摘要:

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 \emph{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, JJ-biexcitons can arise from repulsive dipolar interactions with energies $E_{JJ}> 2E_J$ while in H-aggregates, HH-biexciton states $E_{HH} < 2E_H$ corresponding to attractive dipole exciton/exciton interactions. These predictions are corroborated by using ultrafast double-quantum coherence spectroscopy on a PBTTT material that exhibits both J- and H-like excitonic behavior.

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