Large Rabi Splitting Research Articles

Long-Range Ballistic Propagation of 80% Excitonic Fraction Polaritons in a Perovskite Metasurface at Room Temperature.

Exciton-polaritons, hybrid light-matter excitations arising from the strong coupling between excitons in semiconductors and photons in photonic nanostructures, are crucial for exploring the physics of quantum fluids of light and developing all-optical devices. Achieving room temperature propagation of polaritons with a large excitonic fraction is challenging but vital, e.g., for nonlinear light transport. We report on room temperature propagation of exciton-polaritons in a metasurface made from a subwavelength lattice of perovskite pillars. The large Rabi splitting, much greater than the optical phonon energy, decouples the lower polariton band from the phonon bath of the perovskite. These cooled polaritons, in combination with the high group velocity achieved through the metasurface design, enable long-range propagation, exceeding hundreds of micrometers even with an 80% excitonic component. Furthermore, the design of the metasurface introduces an original mechanism for unidirectional propagation through polarization control, suggesting a new avenue for the development of advanced polaritonic devices.

Strong coupling of double excitons with guided mode resonances and quasi-bound states in the continuum in heterogeneous metamaterials.

Heterogeneous metamaterials containing excitonic materials provide an ideal platform for strong exciton-photon coupling. In this Letter, we theoretically demonstrate four strong couplings in a heterogeneous metamaterial consisting of a TiO2 grating standing on a perovskite-WS2-perovskite waveguide layer by tuning the structural sizes. The quasi-bound state in the continuum (qBIC) and the guided mode resonance (GMR) both strongly coupled with the excitons of both perovskite and WS2 under oblique incident illumination, resulting in four large Rabi splittings of 177.32, 187.53, 406.25, and 435.09 meV via a reasonable combination of oscillator strengths of perovskite and WS2. Double strong coupling behaviors are also achieved when the grating period equals 222 nm with an incident light angle of 19.3°. Moreover, double ultrastrong coupling can even be realized by the GMR and qBIC respectively interacting with the exciton of WS2 when its oscillator strength reaches a certain value. Our work paves an effective avenue to realizing strong coupling and even ultrastrong coupling between multiple excitons and multiple optical modes.

Quantized Microcavity Polariton Lasing Based on InGaN Localized Excitons.

Exciton-polaritons, which are bosonic quasiparticles with an extremely low mass, play a key role in understanding macroscopic quantum effects related to Bose-Einstein condensation (BEC) in solid-state systems. The study of trapped polaritons in a potential well provides an ideal platform for manipulating polariton condensates, enabling polariton lasing with specific formation in k-space. Here, we realize quantized microcavity polariton lasing in simple harmonic oscillator (SHO) states based on spatial localized excitons in InGaN/GaN quantum wells (QWs). Benefiting from the high exciton binding energy (90 meV) and large oscillator strength of the localized exciton, room-temperature (RT) polaritons with large Rabi splitting (61 meV) are obtained in a strongly coupled microcavity. The manipulation of polariton condensates is performed through a parabolic potential well created by optical pump control. Under the confinement situation, trapped polaritons are controlled to be distributed in the selected quantized energy sublevels of the SHO state. The maximum energy spacing of 11.3 meV is observed in the SHO sublevels, indicating the robust polariton trapping of the parabolic potential well. Coherent quantized polariton lasing is achieved in the ground state of the SHO state and the coherence property of the lasing is analyzed through the measurements of spatial interference patterns and g(2)(τ). Our results offer a feasible route to explore the manipulation of macroscopic quantum coherent states and to fabricate novel polariton devices towards room-temperature operations.

Deterministic positioning and alignment of a single-molecule exciton in plasmonic nanodimer for strong coupling.

Experimental realization of strong coupling between a single exciton and plasmons remains challenging as it requires deterministic positioning of the single exciton and alignment of its dipole moment with the plasmonic fields. This study aims to combine the host-guest chemistry approach with the cucurbit[7]uril-mediated active self-assembly to precisely integrate a single methylene blue molecule in an Au nanodimer at the deterministic position (gap center of the nanodimer) with the maximum electric field (EFmax) and perfectly align its transition dipole moment with the EFmax, yielding a large spectral Rabi splitting of 116 meV for a single-molecule exciton-matching the analytical model and numerical simulations. Statistical analysis of vibrational spectroscopy and dark-field scattering spectra confirm the realization of the single exciton strong coupling at room temperature. Our work may suggest an approach for achieving the strong coupling between a deterministic single exciton and plasmons, contributing to the development of room-temperature single-qubit quantum devices.

Large Rabi splitting energy in resonant quasi-BIC WSe2 metasurfaces

Strong coupling between excitons in transition metal dichalcogenides and cavities has attracted much attention in recent years, while the Rabi splitting values are usually small, which limits its further applications. In this work, we propose a WSe2 metasurface that supports quasi bound states in the continuous (QBIC) to realize a large Rabi splitting value by adjusting the effective overlap of the exciton with the resonance modes. The designed metasurface consists of composite nanoholes of WSe2. By changing the relative position of the nanoholes and modifying the symmetry of the structure, two QBIC modes are excited, and they mainly localize the electric field inside the device. By tuning the oscillator strength of WSe2, the strong coupling between excitons in WSe2 and QBIC modes is realized, resulting in Rabi splitting energies of 468 meV and 472 meV, respectively. This work provides insights into enhancing light-matter interactions and expands the potential applications of strong coupling.

Room-temperature strong coupling in a single-photon emitter-metasurface system

Solid state single-photon sources with high brightness and long coherence time are promising qubit candidates for modern quantum technology. To prevent decoherence processes and preserve the integrity of the qubits, decoupling the emitters from their surrounding environment is essential. To this end, interfacing single photon emitters (SPEs) with high-finesse cavities is required, especially in the strong coupling regime, when the interaction between emitters can be mediated by cavity fields. However, achieving strong coupling at elevated temperatures is challenging due to competing incoherent processes. Here, we address this long-standing problem by using a quantum system, which comprises a class of SPEs in hexagonal boron nitride and a dielectric cavity based on bound states in the continuum (BIC). We experimentally demonstrate, at room temperature, strong coupling of the system with a large Rabi splitting of ~4 meV thanks to the combination of the narrow linewidth and large oscillator strength of the emitters and the efficient photon trapping of the BIC cavity. Our findings unveil opportunities to advance the fundamental understanding of quantum dynamical system in strong coupling regime and to realise scalable quantum devices capable of operating at room temperature.

Biexcitons-plasmon coupling of Ag@Au hollow nanocube/MoS2 heterostructures based on scattering spectra.

The strong interaction between light and matter is one of the current research hotspots in the field of nanophotonics, and provides a suitable platform for fundamental physics research such as on nanolasers, high-precision sensing in biology, quantum communication and quantum computing. In this study, double Rabi splitting was achieved in a composite structure monolayer MoS2 and a single Ag@Au hollow nanocube (HNC) in room temperature mainly due to the two excitons in monolayer MoS2. Moreover, the tuning of the plasmon resonance peak was realized in the scattering spectrum by adjusting the thickness of the shell to ensure it matches the energy of the two excitons. Two distinct anticrossings are observed at both excitons resonances, and large double Rabi splittings (90 meV and 120 meV) are obtained successfully. The finite-difference time domain (FDTD) method was also used to simulate the scattering spectra of the nanostructures, and the simulation results were in good agreement with the experimental results. Additionally, the local electromagnetic field ability of the Ag@Au hollow HNC was proved to be stronger by calculating and comparing the mode volume of different nanoparticles. Our findings provides a good platform for the realization of strong multi-mode coupling and open up a new way to construct nanoscale photonic devices.

All‐Dielectric SERS Metasurface with Strong Coupling Quasi‐BIC Energized by Transformer‐Based Deep Learning

AbstractResearchers have paid great attention to pursuing metal‐free nanostructures as alternatives to metallic counterparts in the field of surface‐enhanced Raman scattering (SERS) for label‐free sensing. However, these metal‐free investigations are hindered by the tiny enhancement factor of the local near field. Here, the design of all‐dielectric SERS metasurfaces is proposed with quasi‐bound states in the continuum (Q‐BIC), inspired by transformer‐based deep learning. By manipulating the incident angle, the mechanism of strong coupling Q‐BIC is introduced with a large Rabi splitting of ≈105 meV, which opens a bandgap and forms an anti‐crossing behavior. Compared to conventional approaches, the strong coupling Q‐BIC scheme not only boosts an extraordinary SERS enhancement factor of ≈107 but also extends the field‐enhancing scale up to ten‐fold. The theoretical optimization implies overwhelming dominance versus the conventional metallic nanostructure design for SERS. The study denotes an approach to utilize the strong coupling effects of Q‐BIC in all‐dielectric SERS metasurfaces and will provide essential design guides for more powerful sensing applications based on SERS.

Fine-tuning biexcitons-plasmon coherent states in a single nanocavity

Abstract A tunable plexcitonic material that sustains multimode hybridization is highly desirable, which is vital for advanced quantum devices. However, the research about regulations of biexcitons-plasmon coherent states has rarely been reported. Here we apply single-nanoparticle scattering spectroscopy correlative with SEM imaging to identify biexcitons-plasmon interaction in a metal-semiconductor hybrid structure composed of a single Au@Ag nanoparticle, J-aggregates molecules and tungsten disulfide (WS2) monolayer. The mode competition within the localized plasmonic hotspots (∼240 nm3) is revealed by continuously regulating the J-aggregates spacer. Two distinct anticrossings are observed at both excitons resonances, and large double Rabi splittings (137 meV and 124 meV) are obtained successfully. We establish experimentally that J-aggregates and WS2 monolayer are responsible for the middle polariton states, while plasmon rarely contributes. Further calculations show that plasmonic nanocavity enables coherent energy exchange with different excitons by providing a highly enhanced localized E-field. In addition, we find that the multimode coupling strengths can be efficiently tuned by changing the cavity morphology and environment temperature, where the tuning spectral accuracy can reach up to 1 nm. Our findings uncover the distinctive properties of biexcitons-plasmon polaritons, suggest an easily obtainable multiqubit states platform, and open up a new way to construct nanoscale photonic devices.

Strong coupling of multiple optical interface modes with ultra-narrow linewidth in one-dimensional topological photonic heterostructures.

Coherent coupling of optical modes with a high Q-factor underpins realization of efficient light-matter interaction with multi-channels in resonant nanostructures. Here we theoretically studied the strong longitudinal coupling of three topological photonic states (TPSs) in a one-dimensional topological photonic crystal heterostructure embedded with a graphene monolayer in the visible frequencies. It is found that the three TPSs can strongly interplay with one another in the longitudinal direction, enabling a large Rabi splitting (∼ 48 meV) in spectral response. The triple-band perfect absorption and selective longitudinal field confinement have been demonstrated, where the linewidth of hybrid modes can reach 0.2 nm with Q-factor up to 2.6 × 103. Mode hybridization of dual- and triple-TPSs were investigated by calculation of the field profiles and Hopfield coefficients of the hybrid modes. Moreover, simulation results further show that resonant frequencies of the three hybrid TPSs can be actively controlled by simply changing the incident angle or structural parameters, which are nearly polarization independent in this strong coupling system. With the multichannel, narrow-band light trapping and selectively strong field localization in this simple multilayer regime, one can envision new possibilities for developing the practical topological photonic devices for on-chip optical detection, sensing, filtering, and light-emitting.

Room-temperature exciton-polariton and photonic lasing in GaN/InGaN core-shell microrods

Room-temperature exciton-polariton is observed in GaN/InGaN core–shell microrods grown by metal-organic vapor phase epitaxy. We demonstrate a large Rabi splitting in the core–shell microrod structure over 265 meV. Room-temperature lasing in core–shell microrods is confirmed by power-dependent photoluminescence spectra. The lasing in the shell layer results to a modulated lasing wavelength and takes one step further to more stable polariton lasing in MQW core–shell microrods.

Directional Emission from Electrically Injected Exciton–Polaritons in Perovskite Metasurfaces

We present a new approach to achieving strong coupling between electrically injected excitons and photonic bound states in the continuum of a dielectric metasurface. Here a high-finesse metasurface cavity is monolithically patterned in the channel of a perovskite light-emitting transistor to induce a large Rabi splitting of ∼200 meV and more than 50-fold enhancement of the polaritonic emission compared to the intrinsic excitonic emission of the perovskite film. Moreover, the directionality of polaritonic electroluminescence can be dynamically tuned by varying the source-drain bias, which induces an asymmetric distribution of exciton population within the transistor channel. We argue that this approach provides a new platform to study strong light-matter interactions in dispersion engineered photonic cavities under electrical injection and paves the way to solution-processed electrically pumped polariton lasers.

Exploring the resonance absorption of subwavelength-patterned epitaxial-grown group-IV semiconductor composite structures.

We experimentally and theoretically demonstrate a mid-infrared perfect absorber with all group-IV epitaxial layered composite structures. The multispectral narrowband strong absorption (>98%) is attributed to the combined effects of the asymmetric Fabry-Perot (FP) interference and the plasmonic resonance in the subwavelength-patterned metal-dielectric-metal (MDM) stack. The spectral position and intensity of the absorption resonance were analyzed by reflection and transmission. While a localized plasmon resonance in the dual-metal region was found to be modulated by both the horizontal (ribbon width) and vertical (spacer layer thickness) profile, the asymmetric FP modes were modulated merely by the vertical geometric parameters. Semi-empirical calculations show strong coupling between modes with a large Rabi-splitting energy reaching 46% of the mean energy of the plasmonic mode under proper horizontal profile. A wavelength-adjustable all-group-IV-semiconductor plasmonic perfect absorber has potential for photonic-electronic integration.

Strongly coupled Raman scattering enhancement revealed by scattering-type scanning near-field optical microscopy

Abstract Recent advances in near-field technology with an ultrahigh spatial resolution breaking optical diffraction limit, make it possible to further identify surface-enhanced Raman scattering (SERS) enhancement theories, and to monitor the SERS substrates. Here we verify the electromagnetic enhancement mechanism for SERS with a close-up view, using scattering-type scanning near-field optical microscopy. The array of metal-insulator-metal (MIM) subwavelength structures is studied, in which the field enhancement comes from the strong coupling between gap plasmon polariton and surface plasmon polariton modes. The near-field optical measurements reveal that SERS enhancement factor (EF) varies from one MIM subwavelength unit to another in a finite array. Besides the enhancement of isolated unit, the loss exchange phenomenon in strong coupling with a large Rabi splitting can give rise to an additional enhancement of more than 2 orders of magnitude in periodic arrays and close to 3 orders of magnitude in finite arrays. The SERS EF of the array composed of only 5 units is demonstrated to yield the best SERS performance. Our near-field optical measurements show evidence that finite-size structures embodied with strong coupling effect are a key way to develop practical high-performance SERS substrates.

Strong coupling between longitudinal and U-shaped localized surface plasmon modes in rectangular grating-shaped gold nanostructures

Strong couplings between localized surface plasmon resonance (LSPR) modes and single quantum emitters have been intensively investigated recently, and meanwhile the coupling between different LSPR modes inside individual metallic nanoparticle is still rarely researched. Herein, the strong coupling is investigated for different LSPR modes inside individual rectangular-grating-shaped gold nanostructure composed of one main-cuboid and two side-attached subcuboids. Original uncoupled LSPR modes are revealed to be longitudinal and U-shaped LSPRs. For the nanostructure with increased main-cuboid length, the dispersion curves of simulated dual-original LSPR scattering wavelengths and dual-coupled LSPR scattering wavelengths show typical strong coupling patterns featuring anti-crossing and large Rabi splitting of 598.1 meV. The strong coupling is considered to be caused by the overlap of longitudinal and U-shaped LSPR oscillation modes in the gold nanostructure. The extracted coupling strength is found in order of 1013 Hz and it increases with the LSPR overlap length. The spatial mode and time evolution of the coupled LSPR modes are also numerically investigated. The simulated results are well comprehended with the classical strong coupling model of oscillators, further confirming the coupling between the longitudinal and the U-shaped LSPRs. The experimental dark-field scattering spectrum shows the existence of U-shaped LSPR mode in the gold nanostructure.

From weak to strong coupling with enhanced dualband magnetoplasmonic Kerr sensing in the dimer-grating metamaterial

We investigate the evolution of plasmonic spectral features from weak to strong coupling regime, with a large Rabi splitting of 210 meV, in the designed dimer-grating metamaterial. The two-driven coupled oscillator model has been proposed to quantitatively analyze the evolution, where the two oscillators are directly excited by the external driving light wave, demonstrating that the evolution is caused by not only aligning the resonance wavelength of related SP modes, but also low-loss. The proposed metamaterial is of high magnetoplasmonic refractive index sensitivity of 280.05 nm RIU−1 and figure of merit of 3*104 RIU−1, suggesting promising applications in biochemical sensing.

Exciton–polaritons of hBN/WS2 heterostructure in cavity observed at room temperature

The layer-by-layer buildup of a two-dimensional transition metal dichalcogenide monolayer to form a stack is an important development for these materials, which performs many remarkable properties in the light–matter interaction. Herein, we find clear evidence of exciton–polaritons emerging from WS2/hBN/WS2 heterostructures embedded in a dielectric microcavity under optical pumping. A large Rabi splitting of 15 meV is observed at room temperature, which increases to 25 meV at 5 K. An all-dielectric Fabry–Pérot microcavity provides a simple but effective way to study the room temperature strong coupling between cavity photons and excitons. Our results pave the way for room-temperature polaritonic devices based on quantum-well van der Waals heterostructures.

Strong coupling with directional scattering features of metal nanoshells with monolayer WS2 heterostructures

Realizing and manipulating strong light–matter coupling in 2D monolayer semiconductors are of the utmost importance in the development of photonic devices. Hollow nanostructures of noble metals are particularly interesting because of their stronger local electromagnetic field compared with solid nanoparticles, which facilitate the strong coupling of single metal nanostructures. Here, the tunable single nanocavity plasmon–exciton coupling was demonstrated at room temperature in hybrid systems consisting of Ag@Au hollow nanocubes (HNCs) and monolayer WS2 underneath, where a large vacuum Rabi splitting of 131.3 meV was observed. Mode splitting can be clearly observed from the dark-field scattering spectrum of the single hybrid nanocavity, which is ascribed to the strong coupling between the nanocavity mode and the excitonic mode. Then, we used the finite difference time domain method to simulate these hybrid systems. By changing the thickness of the shell of the Ag@Au HNC, we can tune the surface plasmon resonance peak position of HNCs to match the exciton energy of the monolayer WS2. The strong couplings were realized via the calculated scattering spectra. The calculated results were consistent with the experimental results. Furthermore, the mode volume of different nanostructures was discussed, and the mode volume of HNCs is smaller than other solid ones at the same plasmonic resonance wavelength, which also indicates that its ability to restrict an electromagnetic field is stronger. This study provides an ideal platform for the strong coupling of a single nanocavity at room temperature and has broad application prospects in the field of single-photon devices.

Boosting anapole-exciton strong coupling in all-dielectric heterostructures

The light manipulation beyond the diffraction limit plays an invaluable role in modern physics and nanophotonics. In this work, we have demonstrated a strong coupling with a large Rabi splitting of 151 meV between bulk WS 2 excitons and anapole modes in the WS 2 -Si nanodisk heterostructure array with nanoholes as small as 50 nm radius. This result is acquired by introducing anapole modes to suppress radiative losses to confine light into subwavelength volumes and large spatial overlapping between excitons and strong optical fields. Our work shows that anapole modes may serve as a powerful way to enhance the interaction between light and matter at nanoscales, and it should pave an avenue toward high-performance all-dielectric optoelectronic applications.

Effects of disorder on polaritonic and dark states in a cavity using the disordered Tavis-Cummings model.

We consider molecules confined to a microcavity of dimensions such that an excitation of the molecule is nearly resonant with a cavity mode. The molecular excitation energies are assumed to be Gaussianly distributed with mean ϵa and variance σ. We find an asymptotically exact solution for large number density N. Conditions for the existence of the polaritonic states and expressions for their energies are obtained. Polaritonic states are found to be quite stable against disorder. Our results are verified by comparison with simulations. When ϵa is equal to energy of the cavity state ϵc, the Rabi splitting is found to increase by 2σ2N|Ṽ|, where Ṽ is the coupling of a molecular excitation to the cavity state. An analytic expression is found for the disorder-induced width of the polaritonic peak. Results for various densities of states and the absorption spectrum are presented. The dark states turn "gray" in the presence of disorder with their contribution to the absorption increasing with σ. Lifetimes of the cavity and molecular states are found to be important, and for sufficiently large Rabi splitting, the width of the polaritonic peaks is dominated by them. We also give analytical results for the case where the molecular levels follow a uniform distribution. We conclude that the study of the width of the polaritonic peaks as a function of the Rabi splitting can give information on the distribution of molecular energy levels. Finally, the effects of (a) orientational disorder and (b) spatial variation on the cavity field are presented.