Ultrastrong plasmon–phonon coupling via epsilon-near-zero nanocavities

Vibrational ultrastrong coupling, where the light–matter coupling strength is comparable to the vibrational frequency of molecules, presents new opportunities to probe the interactions between molecules and zero-point fluctuations, harness cavity-modified chemical reactions and develop novel devices...

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Bibliographic Details
Authors: Yoo, Daehan, León Pérez, Fernando de, Pelton, Matthew, Lee, In-Ho, Mohr, Daniel A., Raschke, Markus B., Caldwell, Joshua D., Martín-Moreno, Luis, Oh, Sang-Hyun
Format: article
Status:Versión aceptada para publicación
Publication Date:2021
Country:España
Institution:Universidad de Zaragoza
Repository:Zaguán. Repositorio Digital de la Universidad de Zaragoza
OAI Identifier:oai:zaguan.unizar.es:106156
Online Access:http://zaguan.unizar.es/record/106156
Access Level:Open access
Description
Summary:Vibrational ultrastrong coupling, where the light–matter coupling strength is comparable to the vibrational frequency of molecules, presents new opportunities to probe the interactions between molecules and zero-point fluctuations, harness cavity-modified chemical reactions and develop novel devices in the mid-infrared spectral range. Here we use epsilon-near-zero nanocavities filled with a model polar medium (SiO2) to demonstrate ultrastrong coupling between phonons and gap plasmons. We present classical and quantum-mechanical models to quantitatively describe the observed plasmon–phonon ultrastrong coupling phenomena and demonstrate a modal splitting of up to 50% of the resonant frequency (normalized coupling strength η > 0.25). Our wafer-scale nanocavity platform will enable a broad range of vibrational transitions to be harnessed for ultrastrong coupling applications