Tunable plexcitonic nanoparticles: a model system for studying plasmon-exciton interaction from the weak to the ultrastrong coupling regime

Date
2016
Authors
Balci, S.
Kucukoz, B.
Balci, O.
Karatay, A.
Kocabas, C.
Yaglioglu, G.
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Source Title
ACS Photonics
Print ISSN
2330-4022
Electronic ISSN
Publisher
American Chemical Society
Volume
3
Issue
11
Pages
2010 - 2016
Language
English
Type
Article
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Abstract

Controlling the number of dye molecules on metallic nanoparticles, which in turn affects the magnitude of Rabi splitting energy, is crucial for obtaining hybrid metal core–organic shell nanoparticles with tunable optical properties in the visible spectrum since the magnitude of the Rabi splitting energy directly determines the strength of the coupling between plasmonic nanoparticles and dye molecules. In this work, we present a new method for the synthesis of plexcitonic nanoparticles, and thus we are able to control the number of dye molecules self-assembled on Ag nanoprisms (Ag NPs) by adjusting the concentration of dye molecules used in the synthesis. Indeed, individual dye molecules self-assemble into J-aggregates on Ag NPs. Thus, in the finite-element simulations and experimental data of the hybrid metal organic nanoparticles, we observed a transition from weak coupling to the ultrastrong coupling regime. Besides, ultrafast energy transfer between plasmonic nanoparticles and excitonic aggregated dye molecules has been extensively studied as a function of Rabi splitting energy. We observe that the lifetime of the polariton states increases with the coupling strength and the upper polaritons are short-lived, whereas the lower polaritons are long-lived. Hybrid metal–organic nanoparticles presented in this study (i) have tunable Rabi splitting energies, (ii) are easy to prepare in large quantities in aqueous medium, (iii) can be uniformly assembled on solid substrates, (iv) have resonance frequencies in the visible spectrum, and (v) have small mode volume, thus making them an excellent model system for studying light–matter interaction at nanoscale dimensions from the weak to ultrastrong coupling regime.

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Keywords
Eexcitons, J-aggregates, Nanoprisms, Plasmons, Plexcitons, Rabi splitting, Strong coupling, Aggregates, Dielectric waveguides, Energy transfer, Excitons, Finite element method, Metal nanoparticles, Metals, Molecules, Nanoparticles, Nanostructures, Optical properties, Organometallics, Phonons, Photons, Plasmons, Quantum theory, Silver, J aggregates, Nanoprisms, plexcitons, Rabi splitting, Strong coupling, Synthesis (chemical)
Citation
Published Version (Please cite this version)