TY - JOUR AU - Daehan Yoo AU - Fernando de León-Pérez AU - Matthew Pelton AU - In-Ho Lee AU - Daniel Mohr AU - Markus Raschke AU - Joshua Caldwell AU - Luis Martín-Moreno AU - Sang-Hyun Oh AB - 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. BT - Nature Photonics DA - 2020-12 DO - 10.1038/s41566-020-00731-5 N2 - 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. PY - 2020 SN - 1749-4893 EP - 125–130 T2 - Nature Photonics TI - Ultrastrong plasmon–phonon coupling via epsilon-near-zero nanocavities UR - https://doi.org/10.1038/s41566-020-00731-5 VL - 15 ER -