Petoukhoff Christopher E, Dani Keshav M, O'Carroll Deirdre M
Femtosecond Spectroscopy Unit, Okinawa Institute of Science and Technology Graduate University, Onna, Okinawa 904-0495, Japan.
Department of Materials Science and Engineering, Rutgers University, 607 Taylor Rd., Piscataway, NJ 08854, USA.
Polymers (Basel). 2020 Sep 19;12(9):2141. doi: 10.3390/polym12092141.
Strong plasmon-exciton coupling between tightly-bound excitons in organic molecular semiconductors and surface plasmons in metal nanostructures has been studied extensively for a number of technical applications, including low-threshold lasing and room-temperature Bose-Einstein condensates. Typically, excitons with narrow resonances, such as -aggregates, are employed to achieve strong plasmon-exciton coupling. However, -aggregates have limited applications for optoelectronic devices compared with organic conjugated polymers. Here, using numerical and analytical calculations, we demonstrate that strong plasmon-exciton coupling can be achieved for Ag-conjugated polymer core-shell nanostructures, despite the broad spectral linewidth of conjugated polymers. We show that strong plasmon-exciton coupling can be achieved through the use of thick shells, large oscillator strengths, and multiple vibronic resonances characteristic of typical conjugated polymers, and that Rabi splitting energies of over 1000 meV can be obtained using realistic material dispersive relative permittivity parameters. The results presented herein give insight into the mechanisms of plasmon-exciton coupling when broadband excitonic materials featuring strong vibrational-electronic coupling are employed and are relevant to organic optoelectronic devices and hybrid metal-organic photonic nanostructures.
有机分子半导体中紧密束缚的激子与金属纳米结构中的表面等离子体激元之间的强等离子体激元 - 激子耦合已针对许多技术应用进行了广泛研究,包括低阈值激光发射和室温玻色 - 爱因斯坦凝聚。通常,具有窄共振的激子,如 - 聚集体,被用于实现强等离子体激元 - 激子耦合。然而,与有机共轭聚合物相比, - 聚集体在光电器件中的应用有限。在此,通过数值和解析计算,我们证明了对于银 - 共轭聚合物核壳纳米结构,尽管共轭聚合物的光谱线宽较宽,但仍可实现强等离子体激元 - 激子耦合。我们表明,通过使用厚壳、大的振子强度以及典型共轭聚合物特有的多个振动电子共振,可以实现强等离子体激元 - 激子耦合,并且使用实际的材料色散相对介电常数参数可以获得超过1000 meV的拉比分裂能。本文给出的结果深入了解了使用具有强振动 - 电子耦合的宽带激子材料时等离子体激元 - 激子耦合的机制,并且与有机光电器件和混合金属 - 有机光子纳米结构相关。