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Register a new userAbundance of cavity-free polaritonic states in resonant materials and nanostructures
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Strong coupling between various kinds of material excitations and optical modes has recently shown potential to modify chemical reaction rates in both excited and ground states. The ground-state modification in chemical reaction rates has usually been reported by coupling a vibrational mode of an organic molecule to the vacuum field of an external optical cavity, such as a planar Fabry-Perot microcavity made of two metallic mirrors. However, using an external cavity to form polaritonic states might: (i) limit the scope of possible applications of such systems, and (ii) be unnecessary. Here we highlight the possibility of using optical modes sustained by materials themselves to self-couple to their own electronic or vibrational resonances. By tracing the roots of the corresponding dispersion relations in the complex frequency plane, we show that electronic and vibrational polaritons are natural eigenstates of bulk and nanostructured resonant materials that require no external cavity. Several concrete examples, such as a slab of excitonic material and a spherical water droplet in vacuum are shown to reach the regime of such cavity-free self-strong coupling. The abundance of cavity-free polaritons in simple and natural structures questions their relevance and potential practical importance for the emerging field of polaritonic chemistry, exciton transport, and modified material properties.
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We consider a periodic chain of oscillating dipoles, interacting via long-range dipole-dipole interactions, embedded inside a cuboid cavity waveguide. We show that the mixing between the dipolar excitations and cavity photons into polaritons can lead to the appearance of new states localized at the ends of the dipolar chain, which are reminiscent of Tamm surface states found in electronic systems. A crucial requirement for the formation of polaritonic Tamm states is that the cavity cross-section is above a critical size. Above this threshold, the degree of localization of the Tamm states is highly dependent on the cavity size, since their participation ratio scales linearly with the cavity cross-sectional area. Our findings may be important for quantum confinement effects in one-dimensional systems with strong light-matter coupling.
The functionalities of a wide range of optical and opto-electronic devices are based on resonance effects and active tuning of the amplitude and wavelength response is often essential. Plasmonic nanostructures are an efficient way to create optical resonances, a prominent example is the extraordinary optical transmission (EOT) through arrays of nanoholes patterned in a metallic film. Tuning of resonances by heating, applying electrical or optical signals has proven to be more elusive, due to the lack of materials that can induce modulation over a broad spectral range and/or at high speeds. Here we show that nanopatterned metals combined with phase change materials (PCMs) can overcome this limitation due to the large change in optical constants which can be induced thermally or on an ultrafast timescale. We demonstrate resonance wavelength shifts as large as 385 nm - an order of magnitude higher than previously reported - by combining properly designed Au EOT nanostructures with Ge2Sb2Te5 (GST). Moreover, we show, through pump probe measurements, repeatable and reversible, large amplitude modulations in the resonances, especially at telecommunication wavelengths, over ps time scales and at powers far below those needed to produce a permanent phase transition. Our findings open a pathway to the design of hybrid metal PCM nanostructures with ultrafast and widely tuneable resonance responses, which hold potential impact on active nanophotonic devices such as tuneable optical filters, smart windows, biosensors and reconfigurable memories.
Optical cavities are a cornerstone of photonics. They are indispensable in lasers, optical filters, optical combs and clocks, in quantum physics, and have enabled the detection of gravitational waves. Cavities transmit light only at discrete resonant frequencies, which are well-separated in micro-structures. Despite attempts at the construction of `white-light cavities, the benefits accrued upon optically interacting with a cavity -- such as resonant field buildup -- have remained confined to narrow linewidths. Here, we demonstrate achromatic optical transmission through a planar Fabry-Perot micro-cavity via angularly multiplexed phase-matching that exploits a bio-inspired grating configuration. By correlating each wavelength with an appropriate angle of incidence, a continuous spectrum resonates and the micro-cavity is rendered transparent. The locus of a single-order 0.7-nm-wide resonance is de-slanted in spectral-angular space to become a 60-nm-wide achromatic resonance spanning multiple cavity free-spectral-ranges. This approach severs the link between the resonance bandwidth and the cavity-photon lifetime, thereby promising resonant enhancement of linear and nonlinear optical effects over broad bandwidths in ultrathin devices.
We investigate a geometrically symmetric gold-silicon sphere heterodimer and reveal its extrinsic chiroptical response caused by the interaction with a substrate. The chiroptical response is obtained for oblique incidence owing to the coalescence of extrinsic chirality, heterogeneity and substrate induced break of symmetry. To quantify the chiral response we utilize k-space polarimetry. We elucidate the physics of the involved phenomena by considering scattering properties of the heterodimer in free space and find that incident linearly polarized light is scattered in a spin-split fashion. We corroborate our finding with a coupled dipole model and find that the spin-split behavior originates from the heterogeneity of the structure. This spin-split scattering, combined with the substrate-induced break of symmetry, leads to an extrinsic chiroptical response. Our work sheds new light on the potential and optical properties of heterogeneous nanostructures and paves the way for designing spectrally tunable polarization controlled heterogeneous optical elements.
Hybrid halide perovskites are now considered as low-cost materials for contemporary research in photovoltaics and nanophotonics. In particular, because these materials can be solution processed, they represent a great hope for obtaining low-cost devices. While the potential of 2D layered hybrid perovskites for polaritonic devices operating at room temperature has been demonstrated in the past, the potential of the 3D perovskites has been much less explored for this particular application. Here, we report the strong exciton-photon coupling with 3D bromide hybrid perovskite. Cavity polaritons are experimentallly demonstrated from both reflectivity and photoluminescence experiments, at room temperature, in a 3$lambda$/2 planar microcavity containing a large surface spin-coated $CH_3NH_3PbBr_3$ thin film. A microcavity quality factor of 92 was found and a large Rabi splitting of 70 meV was measured. This result paves the way to low-cost polaritonic devices operating at room temperature, potentially electrically injectable as 3D hybrid perovskites present good transport properties.
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