Rabi Splitting Research Articles

Background-free imaging of cold atoms in optical traps

Optical traps, including those used in atomic physics, cold chemistry, and quantum science, are widely used in the research on cold atoms and molecules. Owing to their microscopic structure and excellent operational capability, optical traps have been proposed for cold atom experiments involving complex physical systems, which generally induce violent background scattering. In this study, using a background-free imaging scheme in cavity quantum electrodynamics systems, a cold atomic ensemble was accurately prepared below a fiber cavity and loaded into an optical trap for transfer into the cavity. By satisfying the demanding requirements for the background-free imaging scheme in optical traps, cold atoms in an optical trap were detected with a high signal-to-noise ratio while maintaining atomic loading. The cold atoms were then transferred into the fiber cavity using an optical trap, and the vacuum Rabi splitting was measured, facilitating relevant research on cavity quantum electrodynamics. This method can be extended to related experiments involving cold atoms and molecules in complex physical systems using optical traps.

Tunable Near-Infrared Transparent Bands Based on Cascaded Fabry–Perot Cavities Containing Phase Change Materials

In this paper, we construct a near-infrared Fabry–Perot cavity composed of two sodium (Na) layers and an antimony trisulfide (Sb2S3) layer. By cascading two Fabry–Perot cavities, the transmittance peak splits into two transmittance peaks due to the coupling between two Fabry–Perot modes. We utilize a coupled oscillator model to describe the mode coupling and obtain a Rabi splitting of 60.0 meV. By cascading four Fabry–Perot cavities, the transmittance peak splits into four transmittance peaks, leading to a near-infrared transparent band. The near-infrared transparent band can be flexibly tuned by the crystalline fraction of the Sb2S3 layers. In addition, the effects of the layer thickness and incident angle on the near-infrared transparent band and the mode coupling are investigated. As the thickness of the Na layer increases, the coupling strength between the Fabry–Perot modes becomes weaker, leading to a narrower transparent band. As the thickness of the Sb2S3 layer increases, the round-trip propagating of the Sb2S3 layer increases, leading to the redshift of the transparent band. As the incident angle increases, the round-trip propagating of the Sb2S3 layer decreases, leading to the blueshift of the transparent band. This work not only provides a viable route to achieving tunable near-infrared transparent bands, but also possesses potential applications in high-performance display, filtering, and sensing.

Hybrid architectures for terahertz molecular polaritonics

Atoms and their different arrangements into molecules are nature’s building blocks. In a regime of strong coupling, matter hybridizes with light to modify physical and chemical properties, hence creating new building blocks that can be used for avant-garde technologies. However, this regime relies on the strong confinement of the optical field, which is technically challenging to achieve, especially at terahertz frequencies in the far-infrared region. Here we demonstrate several schemes of electromagnetic field confinement aimed at facilitating the collective coupling of a localized terahertz photonic mode to molecular vibrations. We observe an enhanced vacuum Rabi splitting of 200 GHz from a hybrid cavity architecture consisting of a plasmonic metasurface, coupled to glucose, and interfaced with a planar mirror. This enhanced light-matter interaction is found to emerge from the modified intracavity field of the cavity, leading to an enhanced zero-point electric field amplitude. Our study provides key insight into the design of polaritonic platforms with organic molecules to harvest the unique properties of hybrid light-matter states.

Molecular strong coupling: evaluating dipole oscillator and cavity field parameters

In this report we use material parameters to calculate the strength of the expected Rabi splitting for a molecular resonance. As an example we focus on the molecular resonance associated with the C=O bond in a polymer host, specifically the stretch resonance at ∼1730 cm−1. Two related approaches to modelling the anticipated extent of the coupling are examined, and the results compared with data from experiments available in the literature. The approaches adopted here indicate how material parameters may be used to assess the potential of a material to exhibit strong coupling, and also enable other useful parameters to be derived, including the molecular dipole moment and the vacuum cavity field strength.

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.

Strong coupling between plasmonic nanocavity gold nanorods and quantum dots emitter

The discovery of hybrid states in strong coupling interaction has gained growing attention in cavity-quantum electrodynamics research owing to its fundamental directives and potential in advanced optical applications. The ultra-confined mode volume of plasmonic cavity gold nanorods (AuNRs), particularly at the nanorod tip “hotspot” provides a large coupling strength, a prerequisite for a coherent energy exchange in the strong coupling regime. Here, we reported a remarkable Rabi splitting of ∼231 meV between gold nanorods longitudinal localized surface plasmon resonance (LLSPR) mode and quantum dots (QDs) at ambient conditions, monitored by dielectric medium tuning. Numerical simulations confirmed the result, displaying absorption spectral splitting.

Quasi-bound states in the continuum for electromagnetic induced transparency and strong excitonic coupling

Advancing on previous reports, we utilize quasi-bound states in the continuum (q-BICs) supported by a metasurface of TiO2 meta-atoms with broken inversion symmetry on an SiO2 substrate, for two possible applications. Firstly, we demonstrate that by tuning the metasurface's asymmetric parameter, a spectral overlap between a broad q-BIC and a narrow magnetic dipole resonance is achieved, yielding an electromagnetic induced transparency analogue with a 50 μs group delay. Secondly, we have found that, due to the strong coupling between the q-BIC and WS2 exciton at room temperature and normal incidence, by integrating a single layer of WS2 to the metasurface, a 37.9 meV Rabi splitting in the absorptance spectrum with 50% absorption efficiency is obtained. These findings promise feasible two-port devices for visible range slow-light characteristics or nanoscale excitonic coupling.

Topologically protected subradiant cavity polaritons through linewidth narrowing enabled by dissipationless edge states

Cavity polaritons derived from strong light–matter interaction provide a basis for efficient manipulation of quantum states via cavity field. Polaritons with narrow linewidth and long lifetime are appealing in applications, such as quantum sensing and storage. Here, we propose a prototypical arrangement to implement a whispering-gallery-mode resonator with one-dimensional topological atom mirror, which allows to boost the lifetime of cavity polaritons over an order of magnitude. This considerable enhancement attributes to the coupling of polaritonic states to dissipationless edge states protected by the topological bandgap of atom mirror that suppresses the leakage of cavity modes. When exceeding the width of Rabi splitting, topological bandgap can further reduce the dissipation from polaritonic states to bulk states, giving arise to subradiant cavity polaritons with extremely sharp linewidth. The resultant Rabi oscillation experiences decay rate lower than the free-space decay of a single quantum emitter. Inheriting from the topologically protected properties of edge states, the subradiance of cavity polaritons can be preserved in disordered atom mirror with moderate perturbations involving the atomic frequency, interaction strengths and location fluctuations. Our work opens up a new paradigm of topology-engineered quantum states with robust quantum coherence for future applications in quantum computing and network.

Strong coupling between colloidal quantum dots and dielectric cavity investigated by both photoluminescence spectrum and reflection spectrum at room temperature

In this study, the angle-resolved photoluminescence spectra and reflection spectra from colloidal quantum dots on SiO2/Si material were investigated at room temperature. The strong coupling between quantum dots and F-P cavity was verified by both the photoluminescence spectral splitting and reflection dispersion. A Rabi splitting was obtained from both angle-resolved photoluminescence spectra and reflection spectra. The Hopfield coefficient of exciton and photon for polariton branches were calculated and analyzed. The relationship between Rabi frequency and excitation power for colloidal quantum dots was also studied. A method was proposed and used to characterize the cavity mode and the reflection dispersion by using open-aperture and close-aperture reflection spectra.

The Mechanism of Manipulating Chirality and Chiral Sensing Based on Chiral Plexcitons in a Strong-Coupling Regime.

Manipulating plasmonic chirality has shown promising applications in nanophotonics, stereochemistry, chirality sensing, and biomedicine. However, to reconfigure plasmonic chirality, the strategy of constructing chiral plasmonic systems with a tunable morphology is cumbersome and complicated to apply for integrated devices. Here, we present a simple and effective method that can also manipulate chirality and control chiral light-matter interactions only via strong coupling between chiral plasmonic nanoparticles and excitons. This paper presents a chiral plexcitonic system consisting of L-shaped nanorod dimers and achiral molecule excitons. The circular dichroism (CD) spectra in our strong-coupling system can be calculated by finite element method simulations. We found that the formation of the chiral plexcitons can significantly modulate the CD spectra, including the appearance of new hybridized peaks, double Rabi splitting, and bisignate anti-crossing behaviors. This phenomenon can be explained by our extended coupled-mode theory. Moreover, we explored the applications of this method in enantiomer ratio sensing by using the properties of the CD spectra. We found a strong linear dependence of the CD spectra on the enantiomer ratio. Our work provides a facile and efficient method to modulate the chirality of nanosystems, deepens our understanding of chiral plexcitons in nanosystems, and facilitates the development of chiral devices and chiral sensing.

Strong coupling in molecular systems: a simple predictor employing routine optical measurements.

We provide a simple method that enables readily acquired experimental data to be used to predict whether or not a candidate molecular material may exhibit strong coupling. Specifically, we explore the relationship between the hybrid molecular/photonic (polaritonic) states and the bulk optical response of the molecular material. For a given material, this approach enables a prediction of the maximum extent of strong coupling (vacuum Rabi splitting), irrespective of the nature of the confined light field. We provide formulae for the upper limit of the splitting in terms of the molar absorption coefficient, the attenuation coefficient, the extinction coefficient (imaginary part of the refractive index) and the absorbance. To illustrate this approach, we provide a number of examples, and we also discuss some of the limitations of our approach.

Strong coupling between WS2 monolayer excitons and a hybrid plasmon polariton at room temperature

Abstract Light–matter interactions between plasmonic and excitonic modes have attracted considerable interest in recent years. A major challenge in achieving strong coupling is the identification of suitable metallic nanostructures that combine tight field confinement with sufficiently low losses. Here, we report on a room-temperature study on the interaction of tungsten disulfide (WS2) monolayer excitons with a hybrid plasmon polariton (HPP) mode supported by nanogroove grating structures milled into single-crystalline silver flakes. By engineering the depth of the nanogroove grating, we can change the character of the HPP mode from propagating surface plasmon polariton-like (SPP-like) to localized surface plasmon resonance-like (LSPR-like). Using reflection spectroscopy, we demonstrate strong coupling with a Rabi splitting of 68 meV between the WS2 monolayer excitons and the lower HPP branch for an optimized nanograting configuration with 60 nm deep nanogrooves. In contrast, only weak coupling between the constituents is observed for shallower and deeper nanogratings since either the field confinement provided by the HPP is not sufficient or the damping is too large. The possibility to balance the field confinement and losses render nanogroove grating structures an attractive platform for future applications.

Extracting accurate light–matter couplings from disordered polaritons

Abstract The vacuum Rabi splitting (VRS) in molecular polaritons stands as a fundamental measure of collective light–matter coupling. Despite its significance, the impact of molecular disorder on VRS is not fully understood yet. This study delves into the complexities of VRS amidst various distributions and degrees of disorder. Our analysis provides precise analytical expressions for linear absorption, transmission, and reflection spectra, along with a “sum” rule, offering a straightforward protocol for extracting accurate collective light–matter coupling values from experimental data. Importantly, our study cautions against directly translating large VRS to the onset of ultrastrong coupling regime. Furthermore, for rectangular disorder, we witness the emergence of narrow side bands alongside a broad central peak, indicating an extended coherence lifetime even in the presence of substantial disorder. These findings not only enhance our understanding of VRS in disordered molecular systems but also open avenues for achieving prolonged coherence lifetimes between the cavity and molecules via the interplay of collective coupling and disorder.

Harnessing quantum plexcitons for enhanced sensitivity and selectivity of creatinine sensor

Despite their widespread usage, surface plasmon resonance (SPR) sensors have several drawbacks, including limited sensitivity and the requirement for sophisticated functionalization chemistry to enhance their performance. In contrast, using quantum states for sensing may result in an enormous increase in sensor performance. These states, however, often need a rigorously controlled environment, which limits their adoption. Recently, there has been a surge of interest in employing quantum plexcitons to solve this conundrum, which has recently been proven to be resilient and robust even in ambient conditions. Here, we report the utilization of plexcitons induced through hybridization of surface plasmon and excitons in a SPR-Otto configuration for sensing creatinine molecules. Using an organic pentamer, BOBzBT2, the ultra-strong coupling regime with a Rabi splitting of 22 % of the uncoupled energy was observed and exploited to monitor the creatinine concentrations. This demonstration proposes a way to combine the benefits of an SPR-based design with the sensitivity offered by quantum plexcitons, which is beneficial for future practical quantum sensing.

Microscopic theory of nonlinear phase space filling in polaritonic lattices

We develop a full microscopic theory for a nonlinear phase space filling (NPSF) in strongly coupled two-dimensional polaritonic lattices. Ubiquitous in polaritonic experiments, the theoretical description of NPSF, also known as nonlinear optical saturation, remains limited to perturbative treatment and homogeneous samples. In this study, we go beyond the existing theoretical description and discover the broad scope of regimes where NPSF crucially modifies the optical response. Studying the quantum effects of non-bosonicity, cooperative light-matter coupling, and Coulomb blockade, we reveal several regimes for observing the nonlinear Rabi splitting quench due to the phase space filling. Unlike prior studies, we derive nonlinear Rabi frequency scaling all the way to the saturation limit and show that the presence of a lattice potential leads to qualitatively distinct nonlinearity. We concentrate on the three regimes of NPSF: (1) planar; (2) fractured; and (3) ultralocalized. For the planar saturation, the Rabi frequency decreases exponentially as a function of exciton density. For the fractured case, where excitons form a lattice with sites exceeding the exciton size, we discover fast NPSF at low occupations. This is followed by slower NPSF as the medium becomes fully saturated. This behavior is particularly pronounced in the presence of Coulomb (or Rydberg) blockade, where regions of fast and slow NPSF depend on the strength of repulsion. For the ultralocalized NPSF, we observe the square-root saturation typical to the collection of two-level systems. Our findings shed light on recent observations of strong nonlinearity in heterobilayers of transition metal dichalcogenides where moiré lattices emerge naturally []. Finally, the developed theory opens the prospects for engineering strongly nonlinear responses of polaritonic lattices with patterned samples, driving polaritonics into the quantum regime. Published by the American Physical Society 2024

Spectroscopy of flux-driven Kerr parametric oscillators by reflection coefficient measurement

We report the spectroscopic characterization of a Kerr parametric oscillator (KPO) based on the measurement of its reflection coefficient under a two-photon drive induced by flux modulation. The measured reflection spectra show good agreement with numerical simulations in terms of their dependence on the two-photon drive amplitude. The spectra can be interpreted as changes in system’s eigenenergies, transition matrix elements, and the population of the eigenstates, although the linewidth of the resonance structure is not fully explained. We also show that the drive-amplitude dependence of the spectra can be explained analytically by using the concepts of Rabi splitting and the Stark shift. By comparing the experimentally obtained spectra with theory, we show that the two-photon drive amplitude at the device can be precisely determined, which is important for the application of KPOs in quantum information processing.

Topologically Protected Synthesizing of Fock States in a Circuit Quantum Electrodynamics Architecture

The preparation of Fock states is important for quantum information storage and processing. Herein, a two‐step protocol with topological protection for multi‐photon Fock states synthesizing in a circuit quantum electrodynamics (QED) architecture is presented. Due to photon number‐dependent vacuum Rabi splitting, the dynamics of the Jaynes–Cummings ladder in the resonant regime can be equivalent to a spin‐1/2 chain while a multi‐frequency microwave pulse is applied. Based on the topologically assisted quantum state transfer (QST)technique, multi‐photon Fock states can be conditionally generated. This method significantly reduces the complexity of experimental manipulation compared with previous multi‐step methods and is more robust as a result of topological protection. Furthermore, the protocol indicates that the circuit QED architecture could potentially provide a platform to explore the exotic phase in condensed matter.

Magnetic field-induced phase transition in spinor exciton-polaritons condensate

We theoretically study the magnetic phase transition of condensed exciton-polariton microcavities in an applied magnetic field. When the magnetic field is strong, all polariton spins are polarized parallel to the magnetic field as usual. On the contrary, in the weak magnetic-field region, the polariton polarization degree is negative, namely, anti-parallel to the magnetic field. For a strong magnetic field, the magnetic phase of the polaritons arises and leads to a paramagnetic, while around a weak magnetic field, with zero exciton–photon detunings, and weak Rabi splitting the spin polarization of the polaritons leads to a diamagnetic. Thus, magneto-polariton phase transition polarization originates from the competition between the polariton Zeeman effect and polariton–polariton interactions. Moreover, the polariton polarization strongly depends on the exciton–photon detuning and Rabi splitting and has a large negative value as they are both small. At last, we compare our theoretical results with the experiments and find they match each other very well.

Frequency-tunable single-photon router based on a microresonator containing a driven three-level emitter

We propose a frequency-tunable router of single photons with high routing efficiency, which is constructed by two waveguides mediately linked by a single-mode whispering gallery resonator with a driven three-level emitter. Quantum routing probability in the output port is obtained via the real-space Hamiltonian. By adjusting the resonator–emitter coupling and the drive, the desired continuous central frequencies for the resonance peaks of routing photons can be manipulated nearly linearly, with the assistance of Rabi splitting effect and optical Stark shift. The proposed routing system may provide potential applications in designing other frequency-modulation quantum optical devices, such as multiplexers, filters, and so on.

Whispering-Gallery Quantum-Well Exciton Polaritons in an Indium Gallium Arsenide Microdisk Cavity.

Despite appealing high-symmetry properties that enable strong spatial confinement and ultrahigh-Q, optical whispering-gallery modes of spherical and circular resonators have been absent from the field of quantum-well exciton polaritons. Here we observe whispering-gallery exciton polaritons in a gallium arsenide microdisk cavity filled with indium gallium arsenide quantum wells, the test bed materials of polaritonics. Strong coupling is evidenced in photoluminescence and resonant spectroscopy accessed through concomitant confocal microscopy and near-field optical techniques. Excitonic and optical resonances are tuned by varying temperature and disk radius, revealing Rabi splittings between 5 and 10meV. A dedicated analytical quantum model for such circular whispering-gallery polaritons is developed, which reproduces the measured values. At high power, lasing is observed and accompanied by a blueshift of the emission consistent with the regime of polariton lasing. With experimental methods and theory now established, whispering-gallery-mode polaritons in round dielectric resonators appear as a new viable platform toward low loss polaritonics.