Abstract

Strong light-matter interactions in both the single-emitter and collective strong coupling regimes attract significant attention due to emerging applications in quantum and nonlinear optics as well as opportunities for modifying material-related properties. Exploration of these phenomena is theoretically demanding, as polaritons exist at the intersection between quantum optics, solid state physics, and quantum chemistry. Fortunately, nanoscale polaritons can be realized in small plasmon-molecule systems, enabling treatment with ab initio methods. Here, we show that time-dependent density-functional theory calculations access the physics of nanoscale plasmon-molecule hybrids and predict vacuum Rabi splitting. By considering a system comprising a few-hundred-atom aluminum nanoparticle interacting with benzene molecules, we show that cavity quantum electrodynamics holds down to resonators of a few cubic nanometers in size, yielding a single-molecule coupling strength exceeding 200 meV due to a massive vacuum field of 4.5 V · nm−1. In a broader perspective, ab initio methods enable parameter-free in-depth studies of polaritonic systems for emerging applications.

Details

Title
Strong plasmon-molecule coupling at the nanoscale revealed by first-principles modeling
Author
Rossi, Tuomas P 1   VIAFID ORCID Logo  ; Shegai, Timur 1   VIAFID ORCID Logo  ; Erhart, Paul 1   VIAFID ORCID Logo  ; Antosiewicz, Tomasz J 2   VIAFID ORCID Logo 

 Department of Physics, Chalmers University of Technology, Gothenburg, Sweden 
 Department of Physics, Chalmers University of Technology, Gothenburg, Sweden; Faculty of Physics, University of Warsaw, Warsaw, Poland 
Pages
1-7
Publication year
2019
Publication date
Jul 2019
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
2264592130
Copyright
© 2019. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.