Rabi Splitting Research Articles

Ultrastrong coupling between molecular vibrations in water and surface lattice resonances.

We investigate the vibrational ultrastrong coupling between molecular vibrations of water molecules and surface lattice resonances (SLRs) sustained by extended arrays of plasmonic microparticles. We design and fabricate an array of gold bowties, which sustain a very high field enhancement, with its SLR resonated with the OH stretching modes of water. We measure a Rabi splitting of 567 cm-1 in the strongly coupled system, whose coupling strength is 8% of the OH vibrational energy, at the onset of the ultrastrong coupling regime (10%). These results introduce metallic microparticle arrays as a platform for the investigation of ultrastrong coupling, which could be used in polaritonic chemistry to modify the dynamics of chemical reactions that require high coupling strengths.

Tailoring Second Harmonic Generation via Strong Coupling in a One‐Dimensional Photonic Crystal Heterostructure

Controlling harmonic generation is crucial for nonlinear optics and nanophotonic devices. Herein, a 1D photonic crystal heterostructure is theoretically proposed comprising a metal film, a lithium niobate layer, and a distributed Bragg reflector with a defect layer. The Tamm state and the defect state for dual‐band second‐harmonic generation (SHG) enhancement simultaneously are numerically investigated. Finite‐element method simulations indicate that SHG efficiencies based on Tamm plasmons and the defect state are 6.85 × 10−6 and 3.28 × 10−4, respectively. Intriguingly, the strong coupling between the defect state and Tamm plasmons enables spatial energy exchange, leading to the SHG switching between them. In the strong coupling region with Rabi splitting energy up to 5.5 meV, the SHG conversion efficiency reaching 5 × 10−5 is observed for both two new hybridized states. During the entire anticrossing Rabi splitting process, the SHG efficiency difference between two resonances can be modulated by up to two orders of magnitude. The coupling strength between two resonances is adjusted by varying the position of the defect layer. Simulation results are consistent with the coupled oscillator model. This work not only offers a platform for studying nonlinear frequency conversion but also establishes a new method of using strong coupling to tailor SHG.

Probing plexciton emission from 2D materials on gold nanotrenches

Probing strongly coupled quasiparticle excitations at their intrinsic length scales offers unique insights into their properties and facilitates the design of devices with novel functionalities. In this work, we investigate the formation and emission characteristics of plexcitons, arising from the interaction between surface plasmons in narrow gold nanotrenches and excitons in monolayer WSe2. We study this strong plasmon–exciton coupling in both the far-field and the near-field. Specifically, we observe a Rabi splitting in the far-field reflection spectra of about 80 meV under ambient conditions, consistent with our theoretical modeling. Using a custom-designed near-field probe, we find that plexciton emission originates predominantly from the lower-frequency branch, which we can directly probe and map its local field distribution. We precisely determine the plexcitonʼs spatial extension, similar to the trench width, with nanometric precision by collecting spectra at controlled probe locations. Our work opens exciting prospects for nanoscale mapping and engineering of plexcitons in complex nanostructures with potential applications in nanophotonic devices, optoelectronics, and quantum electrodynamics in nanoscale cavities.

Direct Microwave Spectroscopy of Andreev Bound States in Planar Ge Josephson Junctions

We demonstrate microwave measurements of the Andreev-bound-state (ABS) spectrum in planar Josephson junctions (JJs) defined in Ge high-mobility two-dimensional hole gases contacted by superconducting platinum germanosilicide (PtSiGe). The JJs and readout circuitry are located on separate chips and inductively coupled via flip-chip bonding. For a device with 350-nm junction length, the spectroscopic signatures were consistent with the short-junction limit, with an induced superconducting gap Δ∗≈48μeV and transmission τ≈0.94. The interaction between the highest-transmission ABS and the resonator was well described by a Jaynes-Cummings model with a vacuum Rabi splitting of approximately 6 MHz. A device with a junction length of 1μm showed an ABS spectrum consistent with a long-junction model. Time-resolved monitoring of the readout resonator in the dispersive regime revealed gate-voltage tunable-junction parity fluctuations on the time scale of seconds. Our work indicates a viable path toward hybrid quantum devices based on planar Ge. Published by the American Physical Society 2024

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.

Analyte-dependent Rabi splitting in solid-state plexcitonic sensors based on plasmonic nanoislands strongly coupled to J-aggregates

A key challenge in the field of plexcitonic quantum devices is the fabrication of solid-state, device-friendly plexcitonic nanostructures using inexpensive and scalable techniques. Lithography-free, bottom-up nanofabrication methods have remained relatively unexplored within the context of plexcitonic coupling. In this work, a plexcitonic system consisting of thermally dewetted plasmonic gold nanoislands (AuNI) coated with a thin film of J-aggregates was investigated. Control over nanoisland size and morphology allowed for a range of plasmon resonances with variable detuning from the exciton. The extinction spectra of the hybrid AuNI/J-aggregate films display clear splitting into upper and lower hybrid resonances, while the dispersion curve shows anti-crossing behavior with an estimated Rabi splitting of 180 eV at zero detuning. As a proof of concept for quantum sensing, the AuNI/J-aggregate hybrid was demonstrated to behave as a plexcitonic sensor for hydrochloric acid vapor analyte. This work highlights the possibility of using thermally dewetted nanoparticles as a platform for high-quality, tunable, cost-effective, and scalable plexcitonic nanostructures for sensing devices and beyond.

Effect of magnetic field on the Bose–Einstein condensation of quantum well exciton–polaritons

We theoretically investigate the nonlinear effects of a magnetic field on the relaxation process of exciton–polaritons toward Bose–Einstein condensation in GaAs quantum wells. Our study reveals that the modification of the exciton’s effective mass, Rabi splitting, and dispersion significantly alters the relaxation rate of polaritons as they approach condensation. By employing a quasi-stationary pump, we clarify the dynamics of the total and condensed polariton populations in response to varying magnetic field strengths. Notably, we demonstrate that under low-energy pumping conditions, the presence of a magnetic field significantly suppresses condensation. This suppression is attributed to the decreased scattering rate between energy levels, which is a consequence of the reduced steepness in the high-energy dispersion. Conversely, increasing both the pump energy and the magnetic field can enhance relaxation efficiency, leading to a substantially larger number of condensed polaritons.

Unraveling abnormal collective effects via the non-monotonic number dependence of electron transfer in confined electromagnetic fields.

Strong light-matter coupling within an optical cavity leverages the collective interactions of molecules and confined electromagnetic fields, giving rise to the possibilities of modifying chemical reactivity and molecular properties. While collective optical responses, such as enhanced Rabi splitting, are often observed, the overall effect of the cavity on molecular systems remains ambiguous for a large number of molecules. In this paper, we investigate the non-adiabatic electron transfer process in electron donor-acceptor pairs influenced by collective excitation and local molecular dynamics. Using the timescale difference between reorganization and thermal fluctuations, we derive analytical formulas for the electron transfer rate constant and the polariton relaxation rate. These formulas apply to any number of molecules (N) and account for the collective effect as induced by cavity photon coupling. Our findings reveal a non-monotonic dependence of the rate constant on N, which can be understood by the interplay between electron transfer and polariton relaxation. As a result, the cavity-induced quantum yield increases linearly with N for small N (as predicted by a simple Dicke model) but shows a turnover and suppression for large N. We also interrelate the thermal bath frequency and the number of molecules, suggesting the optimal number for maximizing enhancement. The analysis provides an analytical insight for understanding the collective excitation of light and electron transfer, helping to predict the optimal condition for effective cavity-controlled chemical reactivity.

Strongly coupled plasmon-exciton polaritons for photobleaching suppression

Abstract Strong light–matter interactions have received a lot of attention, for example in the pursuit of plasmonic-excitonic structures as coherent light sources with low-power threshold. In this study, we investigate the influence of room temperature strong coupling between surface plasmon polaritons (SPP) and excitons on fluorescence lifetimes and photobleaching effects. Our plasmonic-photonic structure, comprising of thin silver (Ag) and gold (Au) layers with a Rhodamine 6G (R6G) dye layer, shows a clear shift in the plasmon resonance and R6G absorption lines with varying incident angles, indicative of strong coupling, with a measured Rabi splitting of approximately 90 meV. Fluorescence lifetime imaging microscopy (FLIM) was then employed to assess photobleaching, revealing a significant reduction in photobleaching effect for in strongly coupled plasmonic-excitonic structures compared to single Rhodamine R6G layers. Our findings indicate the pivotal role of strong light–matter interactions in reducing photobleaching effects and stabilizing fluorescence intensities, offering promising avenues for developing quantum multiparticle nanophotonic devices with enhanced stability and performance.

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.

Robust consistent single quantum dot strong coupling in plasmonic nanocavities

Strong coupling between a single quantum emitter and an optical cavity (at rate Ω) accesses fundamental quantum optics and provides an essential building block for photonic quantum technologies. However, the minimum mode volume of conventional dielectric cavities restricts their operation to cryogenic temperature for strong coupling. Here we harness surface self-assembly to make deterministic strong coupling at room temperature using CdSe/CdS quantum dots (QDs) in nanoparticle-on-mirror (NPoM) plasmonic nanocavities. We achieve a fabrication yield of ~70% for single QD strong coupling by optimizing their size and nano-assembly. A clear and reliable Rabi splitting is observed both in the scattering of each nanocavity and their photoluminescence, which are however not equal. Integrating these quantum elements with electrical pumping allows demonstration of strong coupling in their electroluminescence. This advance provides a straightforward way to achieve practical quantum devices at room temperature, and opens up exploration of their nonlinear, electrical, and quantum correlation properties.

Coherent coupling of localized surface plasmons and surface plasmons in borophene-based metamaterial

The strong coherent coupling in different electromagnetic modes can control the light-matter interaction more conveniently. Here, we theoretically researched the hybridization between the borophene surface plasmon (BSP) mode and the borophene localized surface plasmon (BLSP) mode in borophene grating structure. This coupling effect leads to the emergence of multiple hybrid modes. The absorption spectra of the system are investigated through finite difference time domain (FDTD) simulation and coupled oscillator model (COM). Results show that the coherent coupling of BSP and BLSP can be achieved by adjusting the carrier density of the borophene gratings. A Rabi splitting effect with frequency of 21.6 THz can be observed. Furthermore, we investigated the effects of geometric structural parameters, incident angle, and relaxation time on the correlated coupling spectra. Our work may deepen the understanding of light–matter interactions and provide a reference for borophene-based active photonic devices in the near-infrared region.

Multimodal competition shapes enzymatic ATP hydrolysis: Deciphering microscale confinement by vibrational strong coupling

Confinement effect at microscale level is ubiquitous in biosystems and microreactors, but its mechanism remains debated. Herein we discovered that the multimode competition of molecular vibrational strong coupling (VSC) with optical resonators can well account for the confinement effects as reflected by the efficacy of enzymatic ATP hydrolysis. As O-H stretching vibration coupling with 6th cavity mode, the VSC effect on ATP hydrolysis shows significant enhancement, while VSC with higher cavity modes will gradually reduce such effect due to the multimodal competition. The higher the cavity mode coupled with, the closer to the outside of Fabry-Pérot cavity. Moreover, the underlying mechanism of VSC effect on ATP hydrolysis could be originated from the Rabi splitting of hydrogen bond landscape, mainly altering the binding affinity between Ca2+ and ATPase. This research deepens our understanding of the microscale confinement effect on reactions from the aspect of quantum mechanism, which can guide the rational design of microreactors.

Dynamic Ultrastrong Coupling in a 2 nm Gap Plasmonic Cavity at the Sub-Picosecond Scale.

Localized surface plasmon resonances (LSPRs) can enhance the electromagnetic fields on metallic nanostructures upon light illumination, providing an approach for manipulating light-matter interactions at the sub-wavelength scale. However, currently, there is no thorough investigation of the physical mechanism in the dynamic formation of the strongly coupled LSPRs on sub-5 nm plasmonic cavities at the sub-picosecond scale. In this work, through femtosecond broadband transient absorption spectroscopy, we reveal the dynamic ultrastrong coupling processes in a nanoparticle-in-trench (NPiT) structure containing 2 nm gap cavities, and demonstrate a coherent motional coupling between vibrating AuNPs and the nanogaps. We achieve a maximum Rabi splitting energy of ∼660 meV in the sub-picosecond hot-electron relaxation time scale under the resonant excitation of the nanogap cavity's LSPR, reaching the ultrastrong coupling regime. This leads to a change of global vibration modes for the 2 nm gap cavity, potentially related to the dynamical Casimir effect with nanogap resonators.

Plasmon-Exciton Interaction at the Nanoscale: Silver Is More "Precious" than Gold!

Predictive understanding of factors affecting plasmon-exciton coupling is crucial for the successful realization of the exciting potentials of plexcitonic nanostructures. Here, we systematically investigate the role of plasmonic metals in controlling the plasmon-exciton coupling strength. We use gold and silver nanoprisms, having identical LSPR maxima, as the plasmonic components and form two plexciton hybrids with the J-aggregates of a cyanine dye. Single-particle spectroscopy is employed to study and compare the abilities of gold and silver in influencing plasmon-exciton interaction at the nanoscale. Despite much faster plasmon dephasing than its gold counterpart, the silver nanoprism exhibits greater Rabi splitting. We reveal that the smaller plasmon mode-volume despite having larger physical volume, superior local electric-field enhancement, and smaller Ohmic losses compared to gold, enables the silver nanoprism to defy the pronounced plasmon decoherence effects and to show stronger plasmon-exciton coupling. These findings suggest that silver nanostructures should be the unequivocal choice over gold when "strong coupling" is desired for any application.

Giant strong coupling in a Q-BICs' tetramer metasurface.

Due to their ultrahigh Q-factor and small mode volume, bound states in the continuum (BICs) are intriguing for the fundamental study of the strong coupling regime. However, the strong coupling generated by BICs in one metasurface is not always strong enough, which highly limits its efficiency in applications. In this work, we realize a giant strong coupling of at most 60 meV in a quasi-BICs' (Q-BICs) tetramer metasurface composed of four Si cylinders with two different sets of diagonal lengths. The Q-BICs are induced from two types of electric quadrupole (EQ), for which detuning can be flexibly controlled by manipulating the C4v symmetry breaking Δd. The giant Rabi splitting in our proposed metasurface performs more than 15 times of the previous works, which provides more possibilities for important nonlinear and quantum applications, such as nanolaser and quantum optics.

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.

Room-temperature strong coupling between CdSe nanoplatelets and a metal-DBR Fabry-Pérot cavity.

The generation of exciton-polaritons through strong light-matter interactions represents an emerging platform for exploring quantum phenomena. A significant challenge in colloidal nanocrystal-based polaritonic systems is the ability to operate at room temperature with high fidelity. Here, we demonstrate the generation of room-temperature exciton-polaritons through the coupling of CdSe nanoplatelets (NPLs) with a Fabry-Pérot optical cavity, leading to a Rabi splitting of 74.6meV. Quantum-classical calculations accurately predict the complex dynamics between the many dark state excitons and the optically allowed polariton states, including the experimentally observed lower polariton photoluminescence emission, and the concentration of photoluminescence intensities at higher in-plane momenta as the cavity becomes more negatively detuned. The Rabi splitting measured at 5K is similar to that at 300K, validating the feasibility of the temperature-independent operation of this polaritonic system. Overall, these results show that CdSe NPLs are an excellent material to facilitate the development of room-temperature quantum technologies.

Multiple micro-cavity vibro-polaritons formation with different vibrational bands of the methylene group

We present an experimental technique to accurately predict the formation of vibro-polaritons from a molecular polymeric film embedded in a resonant mid-infrared cavity. Using simple Fourier-transform reflectance measurement, we extract the complex dielectric function of a polyethylene film using Kramers-Kronig relations. The fitted dielectric function can be plugged into a numerical code to predict the strength and dispersion of the strong light-matter coupling regime between the quantized electromagnetic modes of a microcavity and the vibrational bands of the molecules. As a demonstration, we experimentally resolve the simultaneous formation of multiple vibro-polariton modes issued from the strong coupling of some vibrational bands of the methylene group (CH2) in a 2.5-μm-thick polyethylene film embedded in a microcavity. We measure a Rabi splitting of 6.3 THz for the stretching doublet around 87.5 THz and a Rabi splitting of 1.1 THz for the scissoring doublet around 43.7 THz, in excellent agreement with numerical predictions.

Polarization dependent exciton-plasmon coupling in PEA2PbI4/Al and its application to perovskite solar cell.

This paper reports the strong coupling between Al nanostructure and two-dimensional (2D) layered perovskite PEA2PbI4 (PEPI) films. The high exciton binding energy of 118 meV and long carrier lifetime of 216 ps are characterized from the 2D PEA2PbI4 film, which indicates that the excitons in perovskite are robust and can couple to metal plasmons. The ordinary and extraordinary optical dispersions are revealed from the anisotropic 2D perovskite. The transmission spectra of PEA2PbI4/Al nanoparticle arrays are simulated under different polarization excitations, and the typical anti-crossing behaviors originating from exciton-plasmon strong coupling are demonstrated. We found that compared with transverse magnetic (TM) polarization, transverse electric (TE) polarization excitation is more conducive to the realization of exciton-plasmon coupling with a larger Rabi splitting. Furthermore, the PEA2PbI4/Al nanoparticle arrays are proposed, which present polarization-dependent local electrical field enhancement due to the exciton-local surface plasmon polariton coupling. Additionally, it is noticed that the proposed plasmonic structure increases the photo-generation rate inside the active material with improved current density. Therefore, the 2D proposed plasmonic design increases the power conversion efficiency (PCE) with an enhancement of 3.3% and 1.3% relative to the planar structures for TE and TM polarizations, respectively. This study provides a deeper understanding of polarized exciton-plasmon coupling properties, promoting the development of the field of plasmon and providing guidance for the design and preparation of efficient optoelectronic devices.