We report on strong coupling between surface plasmon polaritons (SPP) and Rhodamine 6G (R6G) molecules, with double vacuum Rabi splitting energies up to 230 and 110 meV. In addition, we demonstrate the emission of all three energy branches of the strongly coupled SPP-exciton hybrid system, revealing features of system dynamics that are not visible in conventional reflectometry. Finally, in analogy to tunable-Q microcavities, we show that the Rabi splitting can be controlled by adjusting the interaction time between waveguided SPPs and R6G deposited on top of the waveguide. The interaction time can be controlled with sub-fs precision by adjusting the length of the R6G area with standard lithography methods.
In this letter we show the inclusion of Rhodamine B molecules (RhB) inside a dielectric-loaded surface plasmon waveguide enables for a precise determination of its optical characteristics. The principle relies on the coupling of the fluorescence emission of the dye to plasmonic waveguided modes allowed in of the structure. Using leakage radiation microscopy in real and reciprocal spaces, we measure the propagation constant of the mode and as well as their attenuation length.
Angle-resolved reflection and emission spectra of metal gratings consisting of sub-wavelength grooves and immersed into rhodamine B and rhodamine 19 solutions are presented. The measured reflection and emission dispersion diagrams reveal the surface plasmon polaritons positions and strong plasmon mediated emission enhancement, respectively. The same grating could be easily re-used for the characterization of different dye-molecules.
We study the use of exciton-polaritons in semiconductor microcavities to generate radiation spanning the infrared to terahertz regions of the spectrum by exploiting transitions between upper and lower polariton branches. The process, which is analogous to difference-frequency generation (DFG), relies on the use of semiconductors with a nonvanishing second-order susceptibility. For an organic microcavity composed of a nonlinear optical polymer, we predict a DFG irradiance enhancement of $2.8\cdot10^2$, as compared to a bare nonlinear polymer film, when triple resonance with the fundamental cavi…
Two-dimensional (2D) semiconducting microcavity, where exciton-polaritons can be formed, constitues a promising setup for exploring and manipulating various regimes of light-matter interaction. Here, the coupling between 2D excitons and metallic cavity photons is studied by using first-principles propagator technique. The strength of exciton-photon coupling is characterised by its Rabi splitting to two exciton-polaritons, which can be tuned by cavity thickness. Maximum splitting of 128 meV is achieved in phosporene cavity, while remarkable value of about 440 meV is predicted in monolayer hBN d…
We propose theoretically and demonstrate experimentally a generation of light pulses whose polarization varies temporally to cover selected areas of the Poincaré sphere with tunable swirling speed and total duration (1 ps and 10 ps respectively in our implementation). The effect relies on the Rabi oscillations of two polarized fields in the strong coupling regime, excited by two counter-polarized and delayed pulses. The interferences of the oscillating fields result in the precession of the Stokes vector of the emitted light while polariton lifetime imbalance results in its drift from a circle…
We experimentally resolve the dispersion of multiple vibro-polariton modes issued from the strong coupling of different vibrational bands of the methylene group (CH2) in a 2.56$μ$m thick polyethylene film with the confined modes of a mid-infrared Fabry-Perot micro-cavity. We measure a Rabi frequency of 111 cm$^{-1}$ for the stretching doublet around 2950 cm$^{-1}$ and a Rabi frequency of 29 cm$^{-1}$ for the scissoring doublet around 1460 cm$^{-1}$. This simple experimental approach offers the possibility to accurately fit the measured molecular film dielectric function. We show that the polar…
Strongly-coupled quantum fields, such as multi-component atomic condensates, optical fields and polaritons, are remarkable systems where the simple dynamics of coupled oscillators can meet the intricate phenomenology of quantum fluids. When the coupling between the components is coherent, not only the particles number, but also their phase texture that maps the linear and angular momentum, can be exchanged. Here, on a system of exciton-polaritons, we have realized a so-called full-Bloch beam: a configuration in which all superpositions of the upper and the lower polariton -- all quantum states…
Semiconductor nanoparticles and nanostructures in the strong coupling regime exhibit an intriguing energy scale in the optical frequencies, which is specified by the Rabi splitting between the upper and lower exciton-polariton states. Technically, exciton-polaritons are part-light, part-matter quasiparticles that arise from the strong interaction of excitonic substances and photonic platforms. In this work, using full-wave numerical and theoretical studies, we showed the emergence of strong light-matter coupling between the nonradiating anapole states from an individual semiconductor nanodisk …
Two-dimensional transition metal dichalcogenides exhibit strong optical transitions with significant potential for optoelectronic devices. In particular they are suited for cavity quantum electrodynamics in which strong coupling leads to polariton formation as a root to realisation of inversionless lasing, polariton condensationand superfluidity. Demonstrations of such strongly correlated phenomena to date have often relied on cryogenic temperatures, high excitation densities and were frequently impaired by strong material disorder. At room-temperature, experiments approaching the strong coupl…
Electronic resonances can significantly enhance the photon-phonon coupling in cavity optomechanics, but are normally avoided due to absorption losses and dephasing by inhomogeneous broadening. We experimentally demonstrate that exciton-polaritons in semiconductor microcavities enable GHz optomechanics with single-particle resonant couplings reaching record values in the 10s of MHz range. Moreover, this resonant enhancement is protected from inhomogeneous broadening by the Rabi gap. Single-polariton non-linearities and the optomechanical strong-coupling regime become accessible in this platform…
Enhancement of light-matter interactions is of great importance for many nanophotonic devices, and one way to achieve it is to feed energy perfectly to the strongly coupled system. Here, we propose gap-perturbed dimerized gratings based on bulk WS2 for flexible control of the strong coupling between quasi-bound state in the continuum (quasi-BIC) and exciton. The simulation results show that when a gap perturbation is introduced into the system resulting in the Brillouin zone folding, BIC transforms into quasi-BIC whose quality factor (Q-factor) is related to the value of gap perturbation. The …
We propose a hybrid quantum system where the strong coupling regime can be achieved between a Rydberg atomic ensemble and propagating surface phonon polaritons on a piezoelectric superlattice. By exploiting the large electric dipole moment and long lifetime of Rydberg atoms as well as tightly confined surface phonon polariton modes, it is possible to achieve a coupling constant far exceeding the relevant decay rates. The frequency of the surface mode can be selected so it is resonant with a Rydberg transition by engineering the piezoelectric superlattice. We describe a way to observe the Rabi …
The strong coupling of an IR-active molecular transition with an optical mode of the cavity results in vibrational polaritons, which opens a new way to control chemical reactivity via confined electromagnetic fields of the cavity. In this study, we design a voltage-tunable open microcavity and we show the formation of multiple vibrational polaritons in methyl salicylate. A Rabi splitting and polariton anticrossing behaviour is observed when the cavity mode hybridizes with the C=O stretching vibration of methyl salicylate. As this vibration contributes to the reaction coordinate of the photoind…
Coherent light-matter interaction at the single photon and electronic qubit level promises the remarkable potential for nonclassical information processing. Against the efforts of improving the figure of merit of the cavities, here we demonstrate strong anharmonicity in the polariton dressed states via dark state resonances in a highly dissipative cavity. It is shown that vacuum Rabi oscillation occurs for a single quantum emitter inside a cavity even with bosonic decay-to-interaction rate ratio exceeding $10^{2}$, when the photon field is coupled to an auxiliary high-$Q$ cavity. Moreover, pho…
Plasmonic structures are known to support the modes with subwavelength volumes in which the field matter interactions are greatly enhanced. Coupling between the molecular excitations and plasmons leading to formation of plexcitons has been investigated for a number of organic molecules. However, plasmon-exciton coupling in metal semiconductor structures have not experienced the same degree of attention. In this work we show that the very strong coupling regime in which the Rabi energy exceeds the exciton binding energy is attainable in semiconductor cladded plasmonic nanoparticles and leads to…
Two dimensional (2D) semiconductor materials of transition-metal dichalcogenides (TMDCs) manifest many peculiar physical phenomena in the light-matter interaction. Due to their ultrathin property, strong interaction with light and the robust excitons at room temperature, they provide a perfect platform for studying the physics of strong coupling in low dimension and at room temperature. Here we report the strong coupling between 2D semiconductor excitons and Tamm plasmon polaritons (TPPs). We observe a Rabi splitting of about 54 meV at room temperature by measuring the angle resolved different…
Polaritons are compositional light-matter quasiparticles that have recently enabled remarkable breakthroughs in quantum and nonlinear optics, as well as in material science. Despite the enormous progress, however, a direct nanometer-scale visualization of polaritons has remained an open challenge. Here, we demonstrate that plasmon-exciton polaritons, or plexcitons, generated by a hybrid system composed of an individual silver nanoparticle and a few-layer transition metal dichalcogenide can be spectroscopically mapped with nanometer spatial resolution using electron energy loss spectroscopy in …
Cavity quantum electrodynamics advances the coherent control of a single quantum emitter with a quantized radiation field mode, typically piecewise engineered for the highest finesse and confinement in the cavity field. This enables the possibility of strong coupling for chip-scale quantum processing, but till now is limited to few research groups that can achieve the precision and deterministic requirements for these polariton states. Here we observe for the first time coherent polariton states of strong coupled single quantum dot excitons in inherently disordered one-dimensional localized mo…
Depending on the relative rates of coupling and dissipation, a light-matter coupled system is either in the weak- or strong-coupling regime. Here, we present a unique system where the coupling rate continuously increases with an externally applied magnetic field while the dissipation rate remains constant, allowing us to monitor a weak-to-strong coupling transition as a function of magnetic field. We observed a Rabi splitting of a terahertz magnon mode in yttrium orthoferrite above a threshold magnetic field of ~14 T. Based on a microscopic theoretical model, we show that with increasing magne…
Light-matter coupling in van der Waal's materials holds significant promise in realizing Bosonic condensation and superfluidity. The underlying semiconductor's crystal asymmetry, if any, can be utilized to form anisotropic half-light half-matter quasiparticles. We demonstrate generation of such highly anisotropic exciton-polaritons at the interface of a biaxial layered semiconductor, stacked on top of a distributed Bragg reflector. The spatially confined photonic mode in this geometry couples with polarized excitons and their Rydberg states, creating a system of highly anisotropic polariton ma…
Achieving electrical injection of exciton-polaritons, half-light, half-matter quasiparticles arising from the strong coupling between photonic and excitonic resonances, is a crucial milestone to scale up polaritonic devices such as optical computers, quantum simulators and inversionless lasers. Here we present a new approach to achieve strong coupling between electrically injected excitons and photonic bound states in the continuum of a dielectric metasurface monolithically patterned in the channel of a light-emitting transistor. Exciton-polaritons are generated by coupling electrically inject…
A theoretical variation between the two distinct light-matter coupling regimes, namely weak and strong coupling, becomes uniquely feasible in open optical Fabry-Pérot microcavities with low mode volume, as discussed here. In combination with monolayers of transition-metal dichalcogenides (TMDCs) such as WS2, which exhibits a large exciton oscillator strength and binding energy, the room-temperature observation of hybrid bosonic quasiparticles, referred to as exciton-polaritons and characterized by a Rabi splitting, comes into reach. In this context, our simulations using the transfer-matrix me…
Exciton-polaritons in semiconductor microcavities generate fascinating effects such as long-range spatial coherence and Bose-Einstein Condensation (BEC), which are attractive for their potential use in low threshold lasers, vortices and slowing light, etc. However, currently most of exciton-polariton effects either occur at cryogenic temperature or rely on expensive cavity fabrication procedures. Further exploring new semiconductor microcavities with stronger exciton photon interaction strength is extensively needed. Herein, we demonstrate room temperature photon exciton strong coupling in hyb…
Formation of dressed light-matter states in optical structures, manifested as Rabi splitting of the eigen energies of a coupled system, is one of the key effects in quantum optics. In pursuing this regime with semiconductors, light is usually made to interact with excitons $-$ electrically neutral quasiparticles of semiconductors, meanwhile interactions with charged three-particle states $-$ trions $-$ have received little attention. Here, we report on strong interaction between plasmons in silver nanoprisms and charged excitons $-$ trions $-$ in monolayer tungsten disulphide (WS$_{2}$). We sh…
We consider a high-Q microresonator with $χ^{(2)}$ nonlinearity under conditions when the coupling rates between the sidebands around the pump and second harmonic exceed the damping rates, implying the strong coupling regime (SC). Using the dressed-resonator approach we demonstrate that this regime leads to the dominance of the Hermitian part of the operator driving the side-band dynamics over its non-Hermitian part responsible for the parametric gain. This has allowed us to introduce and apply the cross-area concept of the polariton quasi-particles and define their effective masses in the con…
A laser threshold is determined by the gain condition, which has been progressively reduced by the use of heterostructures and of quantum confinement. The polariton laser is the ultimate step of this evolution: coherent emission is obtained from the spontaneous decay of an exciton-polariton condensate, without the achievement of any gain condition. ZnO, with its unique excitonic properties, is the best choice for a blue/UV-emitting polariton laser device. We report on the fabrication of a new family of fully hybrid microcavities that combine the best-quality ZnO material available (bulk substr…
We demonstrate Resonant Tunneling Diodes, embedded in double metal cavities, strongly coupled to the cavity field, while maintaining their electronic properties. We measure the polariton dispersion and find a relative vacuum Rabi splitting of 16%, which explicitly qualifies for the strong-coupling regime. Additionally we show that electronic transport has a significant influence on the polaritons by modulating the coupling strength. The merge between electronic transport and polaritonic physics in our devices opens up a new aspect of cavity quantum electro-dynamics and integrated photonics.
We present experimental observations of a non-resonant dynamic Stark shift in strongly coupled microcavity quantum well exciton-polaritons - a system which provides a rich variety of solid-state collective phenomena. The Stark effect is demonstrated in a GaAs/AlGaAs system at 10K by femtosecond pump-probe measurements, with the blue shift approaching the meV scale for a pump fluence of 2 mJcm^-2 and 50 meV red detuning, in good agreement with theory. The energy level structure of the strongly coupled polariton Rabi-doublet remains unaffected by the blue shift. The demonstrated effect should al…
Semiconductor-microcavity polaritons are composite quasiparticles of excitons and photons, emerging in the strong coupling regime. As quantum superpositions of matter and light, polaritons have much stronger interparticle interactions compared with photons, enabling rapid equilibration and Bose-Einstein condensation (BEC). Current realizations based on 1D photonic structures, such as Fabry-Pérot microcavities, have limited light-trapping ability resulting in picosecond polariton lifetime. We demonstrate, theoretically, above-room-temperature (up to 590 K) BEC of long-lived polaritons in MoSe$_…
We investigate second harmonic generation (SHG) from hexagonal periodic arrays of triangular nano-holes of aluminum using a self-consistent methodology based on the hydrodynamics-Maxwell-Bloch approach. It is shown that angular polarization patterns of the far-field second harmonic response abide to three-fold symmetry constraints on tensors. When a molecular layer is added to the system and its parameters are adjusted to achieve the strong coupling regime between a localized plasmon mode and molecular excitons, Rabi splitting is observed from occurrence of both single- and two-photon transiti…
Solid state cavity quantum electrodynamics is a rapidly advancing field which explores the frontiers of light-matter coupling. Plasmonic approaches are of particular interest in this field, since they carry the potential to squeeze optical modes to spaces significantly below the diffraction limit1,2, enhancing light-matter coupling. They further serve as an architecture to design ultra-fast, non-linear integrated circuits with smallest footprints3. Transition metal dichalcogenides are ideally suited as the active material in such circuits as they interact strongly with light at the ultimate mo…
The realization and control of polaritons is of paramount importance in the prospect of novel photonic devices. Here, we investigate the emergence of plasmon-exciton polaritons in hybrid structures consisting of a two-dimensional (2D) transition metal dichalcogenide (TMDC) deposited onto a metal substrate or coating a metallic thin-film. We determine the polaritonic spectrum and show that, in the former case, the addition of a top dielectric layer, and, in the latter, the thickness of the metal film,can be used to tune and promote plasmon-exciton interactions well within the strong coupling re…
We investigate the optical response of a system consisting of periodic silver V-grooves interacting with quantum emitters. Two surface plasmon-polariton resonances are identified in the reflection spectrum of bare silver grooves, with the intensity of one resonance being localized near the bottom of the groove and that of the other resonance being distributed throughout the entire groove. The linear response of the hybrid silver-emitter system is thoroughly analyzed by considering the coupling between surface plasmon polaritons and emitters as the geometry of the grooves and the spatial distri…
Polaritonic self-hybridized critical coupling by Brillouin zone folding induced quasi-bound states in the continuum in bulk WS2 metasurfaces
Key Laboratory for Physical Electronics and Devices of the Ministry of Education and Shaanxi Key Lab of Information Photonic Technique, School of Electronic Science and Engineering, Xi’an Jiaotong University（教育部电子科学与技术重点实验室和陕西信息光子技术重点实验室，西安交通大学电子科学与工程学院）
We simulate vibrational strong (VSC) and ultrastrong coupling (V-USC) for liquid water with classical molecular dynamics simulations. When the cavity modes are resonantly coupled to the O-H stretch mode of liquid water, the infrared spectrum shows asymmetric Rabi splitting. The lower polariton (LP) may be suppressed or enhanced relative to the upper polariton (UP) depending on the frequency of the cavity mode. Moreover, although the static properties and the translational diffusion of water are not changed under VSC or V-USC, we do find the modification of the orientational autocorrelation fun…
The ability to feed energy into a system, or - equivalently - to drive that system with an external input is a fundamental aspect of light-matter interaction. The key concept in many photonic applications is the "critical coupling" condition: at criticality, all the energy fed to the system via an input channel is dissipated within the system itself. Although this idea was crucial to enhance the efficiency of many devices, it was never considered in the context of systems operating in a non-perturbative regime. In this so-called strong coupling regime, the matter and light degrees of freedom a…
