arXivDaily arXiv每日学术速递 周一至周五更新
arXiv 2006.11295cond-mat.mtrl-sciphysics.chem-phphysics.comp-ph
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聚二乙炔链中激子-极化激元的第一性原理模拟

First principles modeling of exciton-polaritons in polydiacetylene chains

Antonios M. Alvertis, Raj Pandya, Claudio Quarti, Laurent Legrand, Thierry Barisien, Bartomeu Monserrat, Andrew J. Musser, Akshay Rao, Alex W. Chin, David Beljonne

摘要:

有机材料中的激子-极化激元是由光子和这些材料所承载的束缚激子的强相互作用产生的混合状态。有机极化激元对光电应用有很大的兴趣,然而由于缺乏量化这些系统中光-物质相互作用的第一性原理方法,并且这将允许分子设计规则的制定,因此这一目标的进展受到阻碍。在这里,我们开发了这样的第一原理方法,量化光-物质相互作用。我们通过研究共轭聚合物聚丁二炔的变体来验证我们的方法,并且我们表明,大的聚合物共轭长度对强激子-光子耦合是至关重要的,因此没有静态无序的纯结构的重要性。通过比较我们的实验反射率测量,我们表明,激子振动的耦合,表现为声子边带的吸收,在一定的频率范围内的光-物质耦合的幅度有很大的影响。我们的方法开辟了更深入地了解有机材料中的极化激元的道路,我们强调,激子-光子相互作用的定量准确计算将需要自洽地考虑所有无序源。

英文摘要:

Exciton-polaritons in organic materials are hybrid states that result from the strong interaction of photons and the bound excitons that these materials host. Organic polaritons hold great interest for optoelectronic applications, however progress towards this end has been impeded by the lack of a first principles approach that quantifies light-matter interactions in these systems, and which would allow the formulation of molecular design rules. Here we develop such a first principles approach, quantifying light-matter interactions. We exemplify our approach by studying variants of the conjugated polymer polydiacetylene, and we show that a large polymer conjugation length is critical towards strong exciton-photon coupling, hence underlying the importance of pure structures without static disorder. By comparing to our experimental reflectivity measurements, we show that the coupling of excitons to vibrations, manifested by phonon side bands in the absorption, has a strong impact on the magnitude of light-matter coupling over a range of frequencies. Our approach opens the way towards a deeper understanding of polaritons in organic materials, and we highlight that a quantitatively accurate calculation of the exciton-photon interaction would require accounting for all sources of disorder self-consistently.

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