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Register a new userMicrocavity phonon polaritons from weak to ultrastrong phonon-photon coupling
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Strong coupling between molecular vibrations and microcavity modes has been demonstrated to modify physical and chemical properties of the molecular material. Here, we study the much less explored coupling between lattice vibrations (phonons) and microcavity modes. Embedding thin layers of hexagonal boron nitride (hBN) into classical microcavities, we demonstrate the evolution from weak to ultrastrong phonon-photon coupling when the hBN thickness is increased from a few nanometers to a fully filled cavity. Remarkably, strong coupling is achieved for hBN layers as thin as 10 nm. Further, the ultrastrong coupling in fully filled cavities yields a cavity polariton dispersion matching that of phonon polaritons in bulk hBN, highlighting that the maximum light-matter coupling in microcavities is limited to the coupling strength between photons and the bulk material. The tunable cavity phonon polaritons could become a versatile platform for studying how the coupling strength between photons and phonons may modify the properties of polar crystals.
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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.
In recent years there has been significant fundamental research into phonon polaritons, owing to their ability to compress light to extremely small dimensions, low-losses, and ability to support anisotropic propagation. In this perspective, after briefly reviewing the present state of mid-infrared optoelectronics, we will assess the potential of phonon-polariton based nanophotonics for infrared (3-100$mathrm{mu}$m) light sources, detectors and modulators. These will operate in the Reststrahlen region where conventional semiconductor light sources become ineffective. Drawing on the results from the past few years, we will sketch some promising paths to create such devices and we will evaluate their practical advantages and disadvantages when compared to other approaches to infrared optoelectronics.
We present the numerical solution of the renormalization group (RG) equations derived in Ref. [1], for the problem of superconductivity in the presence of both electron-electron and electron-phonon coupling at zero temperature. We study the instability of a Fermi liquid to a superconductor and the RG flow of the couplings in presence of retardation effects and the crossover from weak to strong coupling. We show that our numerical results provide an ansatz for the analytic solution of the problem in the asymptotic limits of weak and strong coupling.
Phonon polaritons (PPs) in van der Waals (vdW) materials can strongly enhance light-matter interactions at mid-infrared frequencies, owing to their extreme infrared field confinement and long lifetimes. PPs thus bear potential for achieving vibrational strong coupling (VSC) with molecules. Although the onset of VSC has recently been observed spectroscopically with PP nanoresonators, no experiments so far have resolved VSC in real space and with propagating modes in unstructured layers. Here, we demonstrate by real-space nanoimaging that VSC can be achieved between propagating PPs in thin vdW crystals (specifically h-BN) and molecular vibrations in adjacent thin molecular layers. To that end, we performed near-field polariton interferometry, showing that VSC leads to the formation of a propagating hybrid mode with a pronounced anti-crossing region in its dispersion, in which propagation with negative group velocity is found. Numerical calculations predict VSC for nanometer-thin molecular layers and PPs in few-layer vdW materials, which could make propagating PPs a promising platform for ultra-sensitive on-chip spectroscopy and strong coupling experiments.
Plasmonic dimer cavities can induce extreme electric-field hot spots that allow one to access ultrastrong coupling regimes using Raman-type spectroscopy on single vibrating molecules. Using a generalized master equation, we study resonant Raman scattering in the strong coupling regime of cavity-QED, when also in the vibrational ultrastrong coupling regime, leading to phonon-dressed polaritons. The master equation rigorously includes spectral baths for the cavity and vibrational degrees of freedom, as well as a pure dephasing bath for the resonant two-level system, which play a significant role. Employing realistic parameters for gold dimer cavity modes, we investigate the emission spectra in several characteristic strong-coupling regimes, leading to extremely rich spectral resonances due to an interplay of phonon-modified polariton states and bath-induced resonances. We also show explicitly the failure of the standard master equation in these quantum nonlinear regimes.
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