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Register a new userUltrastrong plasmon-phonon coupling via epsilon-near-zero nanocavities
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Fernando de Le\\'on-P\\'erez
Publication date
2020
fields
Physics
and research's language is
English
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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.
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Ultrafast control of light-matter interactions constitutes a crucial feature in view of new technological frontiers of information processing. However, conventional optical elements are either static or feature switching speeds that are extremely low with respect to the timescales at which it is possible to control light. Here, we exploit high-quality-factor engineered epsilon-near-zero (ENZ) modes of a metal-insulator-metal nanocavity to realize an all-optical ultrafast modulation of the reflectance of light at a tailored wavelength. Our approach is based on the presence of the two, spectrally separated, ENZ absorption resonances of the cavity. Optical pumping of the system at its high energy ENZ mode leads to a strong red-shift of the low energy mode because of the transient increase of the local dielectric function, which leads to a sub-3-ps control of the reflectance at a specific wavelength with a relative modulation depth approaching 120%.
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.
Near-infrared epsilon-near-zero (ENZ) metamaterial slabs based on silver-germanium (Ag-Ge) multilayers are experimentally demonstrated. Transmission, reflection and absorption spectra are characterized and used to determine the complex refractive indices and the effective permittivities of the ENZ metamaterial slabs, which match the results obtained from both the numerical simulations and the optical nonlocalities analysis. A rapid post-annealing process is used to reduce the collision frequency of silver and therefore decrease the optical absorption loss of multilayer metamaterial slabs. Furthermore, multilayer grating structures are studied to enhance the optical transmission and also tune the location of ENZ wavelength. The demonstrated near-infrared ENZ multilayer metamaterial slabs are important for realizing many exotic applications, such as phase front shaping and engineering of photonic density of states.
We observe unique absorption resonances in silver/silica multilayer-based epsilon-near-zero (ENZ) metamaterials that are related to radiative bulk plasmon-polariton states of thin-films originally studied by Ferrell (1958) and Berreman (1963). In the local effective medium, metamaterial descrip- tion, the unique effect of the excitation of these microscopic modes is counterintuitive and captured within the complex propagation constant, not the effective dielectric permittivities. Theoretical anal- ysis of the band structure for our metamaterials shows the existence of multiple Ferrell-Berreman branches with slow light characteristics. The demonstration that the propagation constant reveals subtle microscopic resonances can lead to the design of devices where Ferrell-Berreman modes can be exploited for practical applications ranging from plasmonic sensing to imaging and absorption enhancement.
An optical topological transition is defined as the change in the photonic isofrequency surface around epsilon-near-zero (ENZ) frequencies which can considerably change the spontaneous emission of a quantum emitter placed near a metamaterial slab. Here, we show that due to the strong Kerr nonlinearity at ENZ frequencies, a high power pulse can induce a sudden transition in the topology of the iso-frequency dispersion curve, leading to a significant change in the transmission of propagating as well as evanescent waves through the metamaterial slab. This evanescent wave switch effect allows for the control of spontaneous emission through modulation of the Purcell effect. We develop a theory of the enhanced nonlinear response of ENZ media to s and p polarized inputs and show that this nonlinear effect is stronger for p polarization and is almost independent of the incident angle. We perform finite-difference time-domain (FDTD) simulations to demonstrate the transient response of the metamaterial slab to an ultrafast pulse and fast switching of the Purcell effect at the sub-picosecond scale. The Purcell factor changes at ENZ by almost a factor of three which is an order of magnitude stronger than that away from ENZ. We also show that due to the inhomogeneous spatial field distribution inside the multilayer metal-dielectric super-lattice, a unique spatial topological transition metamaterial can be achieved by the control pulse induced nonlinearity. Our work can lead to ultra-fast control of quantum phenomena in ENZ metamaterials.
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