Polariton Dispersion Research Articles

Cylindrical near-field solar thermophotovoltaic system with multilayer absorber/emitter structures: Integrated solar radiation absorption and cooling energy consumption

Near-field radiative heat transfer enhances the intensity of the thermal radiation significantly through evanescent waves, while the combination of selective emitters can effectively improve the output power and system efficiency of solar thermophotovoltaic systems. By calculating the polariton dispersion relation between different layers and combining the energy transmission coefficient of the emitter at different layers, the mechanism by which the emitter enhances near-field radiative heat transfer was analyzed. Concurrently, a comprehensive consideration was given to the conversion of solar radiation to thermal energy, the transformation of thermal radiation into electrical energy, and the impact of the circulating water-cooling system on performance. The analysis indicates that with concentration ratio of > 70 and operating temperatures ranging from 900 K to 1200 K, the output power of near-field solar thermophotovoltaic system can achieve a range of 8905 W/m2 to 52875 W/m2, and the system efficiency can be stably maintained above 20 %.

Visible-frequency hyperbolic plasmon polaritons in a natural van der Waals crystal

Controlling light at subwavelength scales is crucial in nanophotonics. Hyperbolic polaritons, supporting arbitrarily large wavevectors, enable extreme light confinement beyond the diffraction limit. Traditional hyperbolic metamaterials suffer from high losses due to metallic components, while natural low-loss hyperbolic phonon polaritons are limited to the mid-infrared range. Some hyperbolic materials at visible frequencies have been studied, but they are either very lossy or only feature out-of-plane hyperbolicity. Here, we demonstrate the presence of low-loss, in-plane hyperbolic plasmon polaritons in the visible and near-infrared in thin-films of MoOCl2, a natural van der Waals crystal. The polariton dispersion is predicted based on the framework of light propagation in biaxial media and experimentally confirmed by real space nano imaging on exfoliated flakes. MoOCl2 constitutes an ideal material platform for visible range applications leveraging the unboundedness of hyperbolic modes, such as hyperlensing, Purcell factor enhancement, and super-resolution imaging, without the drawbacks of metamaterials.

FMO-LC-TDDFTB method for excited states of large molecular assemblies in the strong light-matter coupling regime.

We present a new methodology to calculate the strong light-matter coupling between photonic modes in microcavities and large molecular aggregates that consist of hundreds of molecular fragments. To this end, we combine our fragment molecular orbital long-range corrected time-dependent density functional tight-binding methodology with a generalized Tavis-Cummings Hamiltonian. We employ an excitonic Hamiltonian, which is built from a quasi-diabatic basis that is constructed from locally excited and charge-transfer states of all molecular fragments. To calculate polaritonic states, we extend our quasi-diabatic basis to include photonic states of a microcavity and derive and implement the couplings between the locally excited states and the cavity states and built a Tavis-Cummings Hamiltonian that incorporates the intermolecular excitonic couplings. Subsequently, we demonstrate the capability of our methodology by simulating the influence of the electric field polarization on the polaritonic spectra for a tetracene aggregate of 125 monomers. Furthermore, we investigate the dependence of the splitting of the upper and lower polaritonic branches on the system size by comparing the spectra of five different tetracene clusters. In addition, we investigate the polariton dispersion of a large tetracene aggregate for electric field polarizations in the x, y, and z directions. Our new methodology can facilitate the future study of exciton dynamics in complex molecular systems, which consist of up to hundreds of molecules that are influenced by strong light-matter coupling to microcavities.

Surface resonance enhanced Goos–Hänchen shifts for different orientations of antiferromagnets in the presence of an applied magnetic field

When reflection takes place off the surface of antiferromagnets, surface resonances, considered as an extension of surface polariton dispersion curves into the reflection region, can enhance the lateral shift of the reflected beam in the presence of an external magnetic field. The effect was earlier studied for both the applied field and the antiferromagnet easy axis perpendicular to the plane of incidence in the case of a small applied field. Here, using MnF2 as the antiferromagnet, we extend the work to look at how increasing the field and changing the antiferromagnet orientation affects the results, which always display nonreciprocity. We find that, when the antiferromagnet easy axis is parallel to the surface within the plane of incidence, leading to spin canting, enhanced shifts in the reflection region occur in much the same way as when the easy axis is along the applied field direction, but an applied field an order of magnitude higher is needed. However, when the easy axis is perpendicular to the surface even higher fields are necessary, and it is difficult to achieve such enhanced shifts.

Linear and nonlinear exciton polariton dispersion in MoS2 nanosheets and its nickel doping dependence

In this paper, we study the influence of Ni-doping on A- and B-exciton polariton dispersion in MoS2 nanosheets. In particular, we have calculated the effect of the Ni-concentration on the energy dispersion and therefore we have deduced the effective masses by adjusting the hopping parameter. The E A , E B -exciton transition energies and the hopping parameter are discerned from the PL of Ni-MoS2 nanosheets. It is shown that the Ni changes considerably the bandgap and as a result the electronic band structure, the effective masses, the optical transition, and the hopping term. We found that the increasing concentration of Ni-dopant can modulate and favors the mixture of A- and B-exciton peaks of MoS2 nanosheets. The diverging Ni-concentration of A- and B-exciton polariton dispersion are also discerned and discussed. Finaly, we can predict that these changes caused by the influence of Ni-doping can be used in most applications involving exciton polariton dispersion for photonics and optoelectronics devices.

Spectroscopic and Interferometric Sum-Frequency Imaging of Strongly Coupled Phonon Polaritons in SiC Metasurfaces.

Phonon polaritons enable waveguiding and localization of infrared light with extreme confinement and low losses. The spatial propagation and spectral resonances of such polaritons are usually probed with complementary techniques such as near-field optical microscopy and far-field reflection spectroscopy. Here, infrared-visible sum-frequency spectro-microscopy is introduced as a tool for spectroscopic imaging of phonon polaritons. The technique simultaneously provides sub-wavelength spatial resolution and highly-resolved spectral resonance information. This is implemented by resonantly exciting polaritons using a tunable infrared laser and wide-field microscopic detection of the upconverted light. The technique is employed to image hybridization and strong coupling of localized and propagating surface phonon polaritons in a metasurface of SiC micropillars. Spectro-microscopy allows to measure the polariton dispersion simultaneously in momentum space by angle-dependent resonance imaging, and in real space by polariton interferometry. Notably, it is possible to directly image how strong coupling affects the spatial localization of polaritons, inaccessible with conventional spectroscopic techniques. The formation of edge states is observed at excitation frequencies where strong coupling prevents polariton propagation into the metasurface. The technique is applicable to the wide range of polaritonic materials with broken inversion symmetry and can be used as a fast and non-perturbative tool to image polariton hybridization andpropagation.

Mesoscale Molecular Simulations of Fabry-Pérot Vibrational Strong Coupling.

Developing theoretical frameworks for vibrational strong coupling (VSC) beyond the single-mode approximation is crucial for a comprehensive understanding of experiments with planar Fabry-Pérot cavities. Herein, a generalized cavity molecular dynamics (CavMD) scheme is developed to simulate VSC of a large ensemble of realistic molecules coupled to an arbitrary 1D or 2D photonic environment. This approach is built upon the Power-Zienau-Woolley Hamiltonian in the normal mode basis and uses a grid representation of the molecular ensembles to reduce the computational cost. When simulating the polariton dispersion relation for a homogeneous distribution of molecules in planar Fabry-Pérot cavities, our data highlight the importance of preserving the in-plane translational symmetry of the molecular distribution. In this homogeneous limit, CavMD yields the consistent polariton dispersion relation as an analytic theory, i.e., incorporating many cavity modes with varying in-plane wave vectors (k∥) produces the same spectrum as the system with a single cavity mode. Furthermore, CavMD reveals that the validity of the single-mode approximation is challenged when nonequilibrium polariton dynamics are considered, as polariton-polariton scattering occurs between modes with the nearest neighbor k∥. The procedure for numerically approaching the macroscopic limit is also demonstrated with CavMD by increasing the system size. Looking forward, our generalized CavMD approach may facilitate understanding vibrational polariton transport and condensation.

Tunable Phonon Polariton Hybridization in a Van der Waals Hetero-Bicrystal.

Phonon polaritons, the hybrid quasiparticles resulting from the coupling of photons and lattice vibrations, have gained significant attention in the field of layered van der Waals heterostructures. Particular interest has been paid to hetero-bicrystals composed of molybdenum oxide (MoO3) and hexagonal boron nitride (hBN), which feature polariton dispersion tailorable via avoided polariton mode crossings. In this work, the polariton eigenmodes in MoO3-hBN hetero-bicrystals self-assembled on ultrasmooth gold are systematically studied using synchrotron infrared nanospectroscopy. It is experimentally demonstrated that the spectral gap in bicrystal dispersion and corresponding regimes of negative refraction can be tuned by material layer thickness, and these results are quantitatively matched with a simple analytic model. Polaritonic cavity modes and polariton propagation along "forbidden" directions are also investigated in microscale bicrystals, which arise from the finite in-plane dimension of the synthesized MoO3 micro-ribbons. The findings shed light on the unique dispersion properties of polaritons in van der Waals heterostructures and pave the way for applications leveraging deeply sub-wavelength mid-infrared light-matter interactions.

Ultra‐Narrow Linewidth Polariton Lasing in Optically Trapped Bose‐Einstein Condensates at Room Temperature

AbstractPolariton lasing via Bose‐Einstein condensation (BEC) provides a peculiar method to achieve low threshold coherent light sources. Until now, the cryogenic operating temperature required for polariton lasers has hampered the development of polaritonics. Here, a novel approach is first reported to realize the ultra‐narrow linewidth polariton lasing under quasi‐3D quantum confinement at room‐temperature (RT). The potential trap landscape is constructed by ring‐shaped optical excitation, wherein the continuum polariton dispersion is modulated into discrete simple harmonic oscillator (SHO) states. The coherent condensation lasing of trapped polaritons occurs beyond the threshold power. Benefiting from the horizontal quantum confinement, the trapped polariton lasing exhibits an ultra‐narrow linewidth (0.7 meV) and excellent quality factor (Q = 3510). Moreover, the second‐order quantum coherence properties of trapped polariton condensation are determined to reveal the quantum phase transition of Bosonic system. The results offer a feasible route for realizing a low‐threshold ultra‐narrow linewidth polariton laser at RT, which significantly facilitates the fabrication of polariton laser and switches on opportunities for future applications.

Exciton polariton condensation from bound states in the continuum at room temperature

Exciton–polaritons (polaritons) resulting from the strong exciton–photon interaction stimulates the development of novel low-threshold coherent light sources to circumvent the ever-increasing energy demands of optical communications1–3. Polaritons from bound states in the continuum (BICs) are promising for Bose–Einstein condensation owing to their theoretically infinite quality factors, which provide prolonged lifetimes and benefit the polariton accumulations4–7. However, BIC polariton condensation remains limited to cryogenic temperatures ascribed to the small exciton binding energies of conventional material platforms. Herein, we demonstrated room-temperature BIC polariton condensation in perovskite photonic crystal lattices. BIC polariton condensation was demonstrated at the vicinity of the saddle point of polariton dispersion that generates directional vortex beam emission with long-range coherence. We also explore the peculiar switching effect among the miniaturized BIC polariton modes through effective polariton−polariton scattering. Our work paves the way for the practical implementation of BIC polariton condensates for integrated photonic and topological circuits.

Multiplication of the orbital angular momentum of phonon polaritons via sublinear dispersion

Optical vortices (OVs) promise to greatly enhance optical information capacity via orbital angular momentum multiplexing. The need for the on-chip integration of orbital angular momentum technologies has prompted research into subwavelength-confined polaritonic OVs. However, the topological order imprinted by the structure used for transduction from free-space beams to surface polaritons is inherently fixed after fabrication. Here we overcome this limitation via dispersion-driven topological charge multiplication. We switch the OV topological charge within a small frequency range (~3%) by leveraging the strong sublinear dispersion of low-loss surface phonon polaritons on silicon carbide membranes. Applying the Huygens principle, we quantitatively evaluate the topological order of experimental OVs detected by near-field imaging. We further explore the deuterogenic effect, which predicts the coexistence of multiple topological charges in higher-order polaritonic OVs. Our work demonstrates a viable method to manipulate the topological charge of polaritonic OVs, paving the way for the exploration of novel orbital-angular-momentum-enabled light–matter interactions at mid-infrared frequencies.

Van der Waals quaternary oxides for tunable low-loss anisotropic polaritonics.

The discovery of ultraconfined polaritons with extreme anisotropy in a number of van der Waals (vdW) materials has unlocked new prospects for nanophotonic and optoelectronic applications. However, the range of suitable materials for specific applications remains limited. Here we introduce tellurite molybdenum quaternary oxides-which possess non-centrosymmetric crystal structures and extraordinary nonlinear optical properties-as a highly promising vdW family of materials for tunable low-loss anisotropic polaritonics. By employing chemical flux growth and exfoliation techniques, we successfully fabricate high-quality vdW layers of various compounds, including MgTeMoO6, ZnTeMoO6, MnTeMoO6 and CdTeMoO6. We show that these quaternary vdW oxides possess two distinct types of in-plane anisotropic polaritons: slab-confined and edge-confined modes. By leveraging metal cation substitutions, we establish a systematic strategy to finely tune the in-plane polariton propagation, resulting in the selective emergence of circular, elliptical or hyperbolic polariton dispersion, accompanied by ultraslow group velocities (0.0003c) and long lifetimes (5 ps). Moreover, Reststrahlen bands of these quaternary oxides naturally overlap that of α-MoO3, providing opportunities for integration. As an example, we demonstrate that combining α-MoO3 (an in-plane hyperbolic material) with CdTeMoO6 (an in-plane isotropic material) in a heterostructure facilitates collimated, diffractionless polariton propagation. Quaternary oxides expand the family of anisotropic vdW polaritons considerably, and with it, the range of nanophotonics applications that can be envisioned.

Coherent transient exciton transport in disordered polaritonic wires.

Excitation energy transport can be significantly enhanced by strong light-matter interactions. In the present work, we explore intriguing features of coherent transient exciton wave packet dynamics on a lossless disordered polaritonic wire. Our main results can be understood in terms of the effective exciton group velocity, a new quantity we obtain from the polariton dispersion. Under weak and moderate disorder, we find that the early wave packet spread velocity is controlled by the overlap of the initial exciton momentum distribution and its effective group velocity. Conversely, when disorder is stronger, the initial state is nearly irrelevant, and red-shifted cavities support excitons with greater mobility. Our findings provide guiding principles for optimizing ultrafast coherent exciton transport based on the magnitude of disorder and the polariton dispersion. The presented perspectives may be valuable for understanding and designing new polaritonic platforms for enhanced exciton energy transport.

Accelerated Nano-Optical Imaging through Sparse Sampling.

The integration time and signal-to-noise ratio are inextricably linked when performing scanning probe microscopy based on raster scanning. This often yields a large lower bound on the measurement time, for example, in nano-optical imaging experiments performed using a scanning near-field optical microscope (SNOM). Here, we utilize sparse scanning augmented with Gaussian process regression to bypass the time constraint. We apply this approach to image charge-transfer polaritons in graphene residing on ruthenium trichloride (α-RuCl3) and obtain key features such as polariton damping and dispersion. Critically, nano-optical SNOM imaging data obtained via sparse sampling are in good agreement with those extracted from traditional raster scans but require 11 times fewer sampled points. As a result, Gaussian process-aided sparse spiral scans offer a major decrease in scanning time.

Polariton Microfluidics for Nonreciprocal Dragging and Reconfigurable Shaping of Polaritons.

Dielectric environment engineering is an efficient and general approach to manipulating polaritons. Liquids serving as the surrounding media of polaritons have been used to shift polariton dispersions and tailor polariton wavefronts. However, those liquid-based methods have so far been limited to their static states, not fully unleashing the promise offered by the mobility of liquids. Here, we propose a microfluidic strategy for polariton manipulation by merging polaritonics with microfluidics. The diffusion of fluids causes gradient refractive indices over microchannels, which breaks the symmetry of polariton dispersions and realizes the microfluidic analogue to nonreciprocal polariton dragging. Based on polariton microfluidics, we also designed a set of on-chip polaritonic elements to actively shape polaritons, including planar lenses, off-axis lenses, Janus lenses, bends, and splitters. Our strategy expands the toolkit for the manipulation of polaritons at the subwavelength scale and possesses potential in the fields of polariton biochemistry and molecular sensing.

Anomalous Dispersion in Reflection and Emission of Dye Molecules Strongly Coupled to Surface Plasmon Polaritons.

We have studied dispersion of surface plasmon polaritons (SPPs) in the Kretschmann geometry (prism/Ag/dye-doped polymer) in weak, intermediate, and ultra-strong exciton-plasmon coupling regimes. The dispersion curves obtained in the reflection experiment were in good agreement with the simple model predictions at small concentrations of dye (Rhodamine 590, Rh590) in the polymer (Poly(methyl methacrylate), PMMA). At the same time, highly unusual multi-segment "staircase-like" dispersion curves were observed at extra-large dye concentrations, also in agreement with the simple theoretical model predicting large, small, and negative group velocities featured by different polariton branches. In a separate experiment, we measured angular dependent emission of Rh590 dye and obtained the dispersion curves consisting of two branches, one nearly resembling the SPP dispersion found in reflection and the second one almost horizontal. The results of our study pave the road to unparalleled fundamental science and future applications of weak and strong light-matter interactions.

Direct observation of split-mode exciton-polaritons in a single MoS2 nanotube.

A single nanotube synthesized from a transition metal dichalcogenide (TMDC) exhibits strong exciton resonances and, in addition, can support optical whispering gallery modes. This combination is promising for observing exciton-polaritons without an external cavity. However, traditional energy-momentum-resolved detection methods are unsuitable for this tiny object. Instead, we propose to use split optical modes in a twisted nanotube with the flattened cross-section, where a gradually decreasing gap between the opposite walls leads to a change in mode energy, similar to the effect of the barrier width on the eigenenergies in the double-well potential. Using micro-reflectance spectroscopy, we investigated the rich pattern of polariton branches in single MoS2 tubes with both variable and constant gaps. Observed Rabi splitting in the 40-60 meV range is comparable to that for a MoS2 monolayer in a microcavity. Our results, based on the polariton dispersion measurements and polariton dynamics analysis, present a single TMDC nanotube as a perfect polaritonic structure for nanophotonics.

Polariton Condensation in Gap-Confined States of Photonic Crystal Waveguides.

The development of patterned multiquantum well heterostructures in GaAs/AlGaAs waveguides has recently made it possible to achieve exciton-polariton condensation in a topologically protected bound state in the continuum (BIC). Polariton condensation was shown to occur above a saddle point of the two-dimensional polariton dispersion in a one-dimensional photonic crystal waveguide. A rigorous analysis of the condensation phenomenon in these systems, as well as the role of the BIC, is still missing. In the present Letter, we theoretically and experimentally fill this gap by showing that polariton confinement resulting from the negative effective mass and the photonic energy gap in the dispersion play a key role in enhancing the relaxation toward the condensed state. In fact, our results show that low-threshold polariton condensation is achieved within the effective trap created by the exciting laser spot, regardless of whether the resulting confined mode is long-lived (polariton BIC) or short-lived (lossy mode). In both cases, the spatial quantization of the polariton condensate and the threshold differences associated to the corresponding state lifetime are measured and characterized. For a given negative mass, a slightly lower condensation threshold from the polariton BIC mode is found and associated to its reduced radiative losses, as compared to the lossy one.

Hyperbolic Polaritonic Rulers Based on van der Waals α-MoO3 Waveguides and Resonators.

Low-dimensional, strongly anisotropic nanomaterials can support hyperbolic phonon polaritons, which feature strong light-matter interactions that can enhance their capabilities in sensing and metrology tasks. In this work, we report hyperbolic polaritonic rulers, based on microscale α-phase molybdenum trioxide (α-MoO3) waveguides and resonators suspended over an ultraflat gold substrate, which exhibit near-field polaritonic characteristics that are exceptionally sensitive to device geometry. Using scanning near-field optical microscopy, we show that these systems support strongly confined image polariton modes that exhibit ideal antisymmetric gap polariton dispersion, which is highly sensitive to air gap dimensions and can be described and predicted using a simple analytic model. Dielectric constants used for modeling are accurately extracted using near-field optical measurements of α-MoO3 waveguides in contact with the gold substrate. We also find that for nanoscale resonators supporting in-plane Fabry-Perot modes, the mode order strongly depends on the air gap dimension in a manner that enables a simple readout of the gap dimension with nanometer precision.

Terahertz Plasmon Polaritons in Large Area Bi2Se3 Topological Insulators

AbstractAssessing the nature of topological quantum materials, and in particular probing the existence of topological surface states, is a very challenging task. Terahertz (THz) frequency scattering near‐field optical microscopy has emerged as an effective technique to investigate the presence of massless surface carriers by locally probing collective surface excitations, i.e., plasmon polaritons, whose dispersion critically depends on the density and nature of surface carriers. Here, thin (14–19 nm) films of Bi2Se3 are experimentally investigated through a combination of x‐ray diffraction, Hall‐bar magneto‐transport, and near‐field detectorless optical holography at THz frequencies, from 2 to 4.3 THz. The dispersion of surface plasmon polaritons are determined for different Bi2Se3 film thicknesses, proving the presence of massless surface carriers. The results open intriguing opportunities in THz nano‐plasmonics and topological nano‐photonics including the development of superlenses and metasurfaces, making use of plasmon polaritons.