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

Abstract

Vibrational ultrastrong coupling (USC), where the light-matter coupling strength is comparable to the vibrational frequency of molecules, presents new opportunities to probe the interactions of molecules with zero-point fluctuations, harness cavity-enhanced chemical reactions, and develop novel devices in the mid-infrared regime. Here we use epsilon-near-zero nanocavities filled with a model polar medium (SiO${}_2$) to demonstrate USC between phonons and gap plasmons. We present classical and quantum mechanical models to quantitatively describe the observed plasmon-phonon USC phenomena and demonstrate a splitting of up to 50% of the resonant frequency. Our wafer-scale nanocavity platform will enable a broad range of vibrational transitions to be harnessed for USC applications.

45 pages, 12 figures

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• Polaritonic Quantum Matter
• Light propagation and magnon-photon coupling in optically dispersive magnetic media
• Photon and phonon statistics in a qubit-plasmon-phonon ultrastrong coupling system
• Amplification of light scattering in arrays of nanoholes by plasmonic absorption-induced transparency
• Description of ultrastrong light-matter interaction through coupled harmonic oscillator models and their connection with cavity-QED Hamiltonians
• Multimode Phonon-Polaritons in Lead-Halide Perovskites in the Ultrastrong Coupling Regime
• Raman Energy Density (RED) in the Context of Acousto-Plasmonics
• Release of virtual photon and phonon pairs from qubit-plasmon-phonon ultrastrong coupling system
• Polariton-induced Purcell effects via a reduced semiclassical electrodynamics approach
• Behavior of quantum coherence in the ultrastrong and deep strong coupling regimes of light-matter system
• Quantum open system description of a hybrid plasmonic cavity