Ultrastrong Light-matter Coupling Research Articles

Self-Hybridized Vibrational-Mie Polaritons in Water Droplets

We study the self-hybridization between Mie modes supported by water droplets with stretching and bending vibrations in water molecules. Droplets with radii >2.7 μm are found to be polaritonic on the onset of the ultrastrong light-matter coupling regime. Similarly, the effect is observed in larger deuterated water droplets at lower frequencies. Our results indicate that polaritonic states are ubiquitous and occur in water droplets in mists, fogs, and clouds. This finding may have implications not only for polaritonic physics but also for aerosol and atmospheric sciences. Published by the American Physical Society 2024

Lindblad Master Equation Capable of Describing Hybrid Quantum Systems in the Ultrastrong Coupling Regime.

Despite significant theoretical efforts devoted to studying the interaction between quantized light modes and matter, the so-called ultrastrong coupling regime still presents significant challenges for theoretical treatments and prevents the use of many common approximations. Here we demonstrate an approach that can describe the dynamics of hybrid quantum systems in any regime of interaction for an arbitrary electromagnetic (EM) environment. We extend a previous method developed for few-mode quantization of arbitrary systems to the case of ultrastrong light-matter coupling, and show that even such systems can be treated using a Lindblad master equation where decay operators act only on the photonic modes by ensuring that the effective spectral density of the EM environment is sufficiently suppressed at negative frequencies. We demonstrate the validity of our framework and show that it outperforms current state-of-the-art master equations for a simple model system, and then study a realistic nanoplasmonic setup where existing approaches cannot be applied.

Sculpting ultrastrong light-matter coupling through spatial matter structuring.

The central theme of cavity quantum electrodynamics is the coupling of a single optical mode with a single matter excitation, leading to a doublet of cavity polaritons which govern the optical properties of the coupled structure. Especially in the ultrastrong coupling regime, where the ratio of the vacuum Rabi frequency and the quasi-resonant carrier frequency of light, ΩR/ω c, approaches unity, the polariton doublet bridges a large spectral bandwidth 2ΩR, and further interactions with off-resonant light and matter modes may occur. The resulting multi-mode coupling has recently attracted attention owing to the additional degrees of freedom for designing light-matter coupled resonances, despite added complexity. Here, we experimentally implement a novel strategy to sculpt ultrastrong multi-mode coupling by tailoring the spatial overlap of multiple modes of planar metallic THz resonators and the cyclotron resonances of Landau-quantized two-dimensional electrons, on subwavelength scales. We show that similarly to the selection rules of classical optics, this allows us to suppress or enhance certain coupling pathways and to control the number of light-matter coupled modes, their octave-spanning frequency spectra, and their response to magnetic tuning. This offers novel pathways for controlling dissipation, tailoring quantum light sources, nonlinearities, correlations as well as entanglement in quantum information processing.

Ultrasmall and tunable TeraHertz surface plasmon cavities at the ultimate plasmonic limit

The ability to confine THz photons inside deep-subwavelength cavities promises a transformative impact for THz light engineering with metamaterials and for realizing ultrastrong light-matter coupling at the single emitter level. To that end, the most successful approach taken so far has relied on cavity architectures based on metals, for their ability to constrain the spread of electromagnetic fields and tailor geometrically their resonant behavior. Here, we experimentally demonstrate a comparatively high level of confinement by exploiting a plasmonic mechanism based on localized THz surface plasmon modes in bulk semiconductors. We achieve plasmonic confinement at around 1 THz into record breaking small footprint THz cavities exhibiting mode volumes as low as {V}_{cav}/{lambda }_{0}^{3} sim 1{0}^{-7}-1{0}^{-8}, excellent coupling efficiencies and a large frequency tunability with temperature. Notably, we find that plasmonic-based THz cavities can operate until the emergence of electromagnetic nonlocality and Landau damping, which together constitute a fundamental limit to plasmonic confinement. This work discloses nonlocal plasmonic phenomena at unprecedentedly low frequencies and large spatial scales and opens the door to novel types of ultrastrong light-matter interaction experiments thanks to the plasmonic tunability.

Polaritonic linewidth asymmetry in the strong and ultrastrong coupling regime

Abstract The intriguing properties of polaritons resulting from strong and ultrastrong light–matter coupling have been extensively investigated. However, most research has focused on spectroscopic characteristics of polaritons, such as their eigenfrequencies and Rabi splitting. Here, we study the decay rates of a plasmon–microcavity system in the strong and ultrastrong coupling regimes experimentally and numerically. We use a classical scattering matrix approach, approximating our plasmonic system with an effective Lorentz model, to obtain the decay rates through the imaginary part of the complex quasinormal mode eigenfrequencies. Our classical model automatically includes all the interaction terms necessary to account for ultrastrong coupling without dealing with the rotating-wave approximation and the diamagnetic term. We find an asymmetry in polaritonic decay rates, which deviate from the expected average of the uncoupled system’s decay rates at zero detuning. Although this phenomenon has been previously observed in exciton–polaritons and attributed to their disorder, we observe it even in our homogeneous system. As the coupling strength of the plasmon–microcavity system increases, the asymmetry also increases and can become so significant that the lower (upper) polariton decay rate reduction (increase) goes beyond the uncoupled decay rates, γ − < γ 0,c < γ +. Furthermore, our findings demonstrate that polaritonic linewidth asymmetry is a generic phenomenon that persists even in the case of bulk polaritons.

Electronic transport driven by collective light-matter coupled states in a quantum device

In the majority of optoelectronic devices, emission and absorption of light are considered as perturbative phenomena. Recently, a regime of highly non-perturbative interaction, ultra-strong light-matter coupling, has attracted considerable attention, as it has led to changes in the fundamental properties of materials such as electrical conductivity, rate of chemical reactions, topological order, and non-linear susceptibility. Here, we explore a quantum infrared detector operating in the ultra-strong light-matter coupling regime driven by collective electronic excitations, where the renormalized polariton states are strongly detuned from the bare electronic transitions. Our experiments are corroborated by microscopic quantum theory that solves the problem of calculating the fermionic transport in the presence of strong collective electronic effects. These findings open a new way of conceiving optoelectronic devices based on the coherent interaction between electrons and photons allowing, for example, the optimization of quantum cascade detectors operating in the regime of strongly non-perturbative coupling with light.

Ultrastrong magnon-photon coupling, squeezed vacuum, and entanglement in superconductor/ferromagnet nanostructures

Ultrastrong light-matter coupling opens exciting possibilities to generate squeezed quantum states and entanglement. We propose achieving this regime in superconducting hybrid nanostructures with ferromagnetic interlayers. Strong confinement of the electromagnetic field between superconducting plates results in the existence of magnon-polariton (MP) modes with ultrastrong magnon-photon coupling, ultrahigh cooperativity, and colossal group velocities. These modes provide a numerically accurate explanation of recent experiments and have intriguing quantum properties. The MP quantum vacuum consists of the squeezed magnon and photon states with the degree of squeezing controlled in wide limits by the external magnetic field. The ground-state population of virtual photons and magnons is vast and can be used for generating correlated magnon and photon pairs. MP excitations contain bipartite entanglement between magnons and photons. Our results indicate that superconducting/ferromagnet nanostructures are very promising for quantum magnonics.

Positronium density measurements using polaritonic effects

Recent experimental advances in Positronium (Ps) physics have made it possible to produce dense Ps ensembles in which Ps-Ps interactions may occur, leading to the production of Ps$_2$ molecules and paving the way to the realization of a Ps Bose-Einstein Condensate (BEC). In order to achieve this latter goal it would be advantageous to develop new methods to measure Ps densities in real-time. Here we describe a possible approach to do this using polaritonic methods: using realistic experimental parameters we demonstrate that a dense Ps gas can be strongly coupled to the photonic field of a distributed Bragg reflector microcavity. In this strongly coupled regime, the optical spectrum of the system is composed of two hybrid positronium-polariton resonances separated by the vacuum Rabi splitting, which is proportional to the square root of the Ps density. Given that polaritons can be created on a sub-cycle timescale, a spectroscopic measurement of the vacuum Rabi splitting could be used as an ultra-fast Ps density measurement in regimes relevant to Ps BEC formation. Moreover, we show how positronium-polaritons could potentially enter the ultrastrong light-matter coupling regime, introducing a radically novel platform to explore its non-perturbative phenomenology.

Controlling the strong light-matter coupling in metal-dielectric optical resonators using spin-crossover molecules

We report the observation of (ultra)strong light-matter coupling, in the UV spectral region, between optical modes of a metal/dielectric bilayer nanocavity and the electronic excitations of spin-crossover (SCO) molecules. By thermally switching the SCO molecules between their low-spin and high-spin states, we demonstrate the possibility of fine-tuning the light-molecule hybridization strength, allowing a reversible switching between strong- (with Rabi splitting values of up to 550 meV) and weak-coupling regimes within a single photonic resonator. As a result, we show that spin-crossover molecular compounds constitute a novel, promising class of active nanomaterials in the context of tuneable and reconfigurable polaritonic devices.

Spontaneous Scattering of Raman Photons from Cavity-QED Systems in the Ultrastrong Coupling Regime.

We show that spontaneous Raman scattering of incident radiation can be observed in cavity-QED systems without external enhancement or coupling to any vibrational degree of freedom. Raman scattering processes can be evidenced as resonances in the emission spectrum, which become clearly visible as the cavity-QED system approaches the ultrastrong coupling regime. We provide a quantum mechanical description of the effect, and show that ultrastrong light-matter coupling is a necessary condition for the observation of Raman scattering. This effect, and its strong sensitivity to the system parameters, opens new avenues for the characterization of cavity QED setups and the generation of quantum states of light.

Fast Generation of 2N‐Photon Fock States using Shortcuts to Adiabaticity and Ultrastrong Light–Matter Coupling

AbstractBy using shortcuts to adiabatic (STA) method, the proposal is to implement a fast multi‐photon down‐conversion, which can rapidly create 2N photons from the quantum vacuum based on the counter‐rotating effect of an ultrastrong light–matter coupling. The energy for the produced photons is given by a high‐frequency pump field. The STA method is used to design the driving fields to induce a rapid population transfer. Such an accelerated evolution can restrain the influence of decoherence during the evolution, so as to generate Fock states from vacuum with high fidelities.

Reduced-density-matrix-based ab initio cavity quantum electrodynamics

A reduced-density-matrix (RDM)-based approach to {\em ab initio} cavity quantum electrodynamics (QED) is developed. The expectation value of the Pauli-Fierz Hamiltonian is expressed in terms of one- and two-body electronic and photonic RDMs, and the elements of these RDMs are optimized directly in polynomial time by semidefinite programming techniques, without knowledge of the full wave function. QED generalizations of important ensemble $N$-representability conditions are derived and enforced in this procedure. The resulting approach is applied to the description of classic ground-state strong electron correlation problems, augmented by the presence of ultrastrong light-matter coupling. First, we assess cavity-induced changes to the singlet-triplet energy gap of the linear oligoacene series; for a heptacene molecule, this gap can change by as much as 1.9 kcal mol$^{-1}$ (or 15\%) when the molecule is aligned along the cavity mode polarization axis. We also explore the metal-insulator transition in linear hydrogen chains and demonstrate that strong electron-photon interactions increase the insulating character of these systems under all coupling strengths considered.

Dynamical stabilization by vacuum fluctuations in a cavity: Resonant electron scattering in the ultrastrong light-matter coupling regime

We developed a theory of electron scattering by a short-range repulsive potential in a cavity. In the regime of ultrastrong electron coupling to the cavity electromagnetic field, the vacuum fluctuations of the field result in the dynamical stabilization of a quasistationary polariton state confined in the core of the repulsive potential. When the energy of a free electron coincides with the energy of the confined state, the extremely efficient resonant nonelastic scattering of the electron accompanied by emission of a cavity photon appears. This effect is discussed as a basis for possible free-electron sources of nonclassical light.

Population of Subradiant States in Carbon Nanotube Microcavities in the Ultrastrong Light–Matter Coupling Regime

Population of Subradiant States in Carbon Nanotube Microcavities in the Ultrastrong Light–Matter Coupling Regime

Effective theory of lattice electrons strongly coupled to quantum electromagnetic fields

Recent experiments have revealed the tantalizing possibility of fabricating lattice electronic systems strongly coupled to quantum fluctuations of electromagnetic fields, e.g., by means of geometry confinement from a cavity or artificial gauge fields in quantum simulators. In this work, we develop a high-frequency expansion to construct the effective models for lattice electrons strongly coupled to a continuum of off-resonant photon modes with arbitrary dispersion. The theory is nonperturbative in the light-matter coupling strength, and is therefore particularly suitable for the ultrastrong light-matter coupling regime. Using the effective models, we demonstrate how the dispersion and topology of the electronic energy bands can be tuned by the cavity. In particular, quasi-one-dimensional physics can emerge in a two-dimensional square lattice due to a spatially anisotropic band renormalization, and a topologically nontrivial anomalous quantum Hall state can be induced in a honeycomb lattice when the cavity setup breaks time-reversal symmetry. We also demonstrate that the photon-mediated interaction induces an unconventional superconducting paired phase distinct from the pair-density-wave state discussed in models with truncated light-matter coupling. Finally, we study a realistic setup of a Fabry-P\'{e}rot cavity. Our work provides a systematic framework to explore the emergent phenomena due to strong light-matter coupling and points out new directions of engineering orders and topological states in solids.

Polaritonic nonlocality in light–matter interaction

Sub-wavelength electromagnetic field localization has been central in photonic research in the last decade, allowing to enhance sensing capabilities as well as increasing the coupling between photons and material excitations. The ultrastrong light-matter coupling regime in the THz range with split-ring resonators coupled to magnetoplasmons has been widely investigated, achieving successive world-records for the largest light-matter coupling ever achieved. Ever shrinking resonators have allowed to approach the regime of few electrons strong coupling, in which single-dipole properties can be modified by the vacuum field. Here we demonstrate, theoretically and experimentally, the existence of a limit to the possibility of arbitrarily increasing electromagnetic confinement in polaritonic systems. Strongly sub-wavelength fields can excite a continuum of high-momenta propagative magnetoplasmons. This leads to peculiar nonlocal polaritonic effects, as certain polaritonic features disappear and the system enters in the regime of bound-to-continuum strong coupling. Emerging nonlinearities due to the local breaking of Kohn's theorem are also reported.

Cavity-Free Ultrastrong Light-Matter Coupling.

Strong coupling between light and matter can occur when the interaction strength between a confined electromagnetic field and a molecular resonance exceeds the losses to the environment, leading to the formation of hybrid light–matter states known as polaritons. Ultrastrong coupling occurs when the coupling strength becomes comparable to the transition energy of the system. It is widely assumed that the confined electromagnetic fields necessary for strong coupling to organic molecules can only be achieved with external structures such as Fabry–Pérot resonators, plasmonic nanostructures, or dielectric resonators. Here we show experimentally that such structures are unnecessary and that a simple dielectric film of dye molecules supports sufficiently modified vacuum electromagnetic fields to enable room-temperature ultrastrong light-matter coupling. Our results may be of use in the design of experiments to probe polaritonic chemistry and suggest that polaritonic states are perhaps easier to realize than previously thought.

Plasmon polaritons in nanoparticle supercrystals: Microscopic quantum theory beyond the dipole approximation

Crystals of plasmonic metal nanoparticles have intriguing optical properties. They reach the regimes of ultrastrong and deep strong light-matter coupling, where the photonic states need to be included in the simulation of material properties. We propose a quantum description of the plasmon polaritons in supercrystals that starts from the dipole and quadrupole excitations of the nanoparticle building blocks and their coupling to photons. Our model excellently reproduces results of finite difference time domain simulations. It provides detailed insight into the emergence of the polariton states. Using the example of a face centered cubic crystals we show that the dipole and quadrupole states mix in many high symmetry directions of the Brilouin zone. A proper description of the plasmon and plasmon-polariton band structure is only possible when including the quadrupole-derived states. Our model leads to an expression of the reduced coupling strength in nanoparticle supercrystals that we show to enter the deep strong coupling regime for metal fill fractions above $0.8$. In addition to the plasmon-polariton energies we analyse the relative contributions of the dipole, quadrupole, and photonic states to their eigenfunctions and are able to demonstrate the decoupling of light in the deep strong coupling regime. Our results pave the way for a better understanding of the quantum properties of metallic nanoparticle supercrystals in the ultrastrong and deep-strong coupling regime.

Understanding radiative transitions and relaxation pathways in plexcitons

Summary Molecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of polaritonic light-matter states, called plexcitons. Such systems are tunable, scalable, easy to synthesize, and offer sub-wavelength confinement, all while giving access to the ultrastrong light-matter coupling regime, promising a plethora of applications. However, the complexity of these materials prevented the understanding of their excitation and relaxation phenomena. Here, we follow the relaxation pathways in plexcitons and conclude that while the metal destroys the optical coherence, the molecular aggregate coupled to surface processes significantly contributes to the energy dissipation. We use two-dimensional electronic spectroscopy with theoretical modeling to assign the different relaxation processes to either molecules or metal nanoparticle. We show that the dynamics beyond a few femtoseconds has to be considered in the language of hot electron distributions instead of the accepted lower and upper polariton branches and establish the framework for further understanding.

Gauge invariance of the Dicke and Hopfield models

The Dicke model, which describes the dipolar coupling between N two-level atoms and a quantized electromagnetic field, seemingly violates gauge invariance in the presence of ultrastrong light-matter coupling, a regime that is now experimentally accessible in many physical systems. Specifically, it has been shown that, while the two-level approximation can work well in the dipole gauge, the Coulomb gauge fails to provide the correct spectra in the ultrastrong coupling regime. Here we show that, taking into account the nonlocality of the atomic potential induced by the two-level approximation, gauge invariance is fully restored for arbitrary interaction strengths, even in the limit of N going to infinity. Finally, we express the Hopfield model, a general description based on the quantization of a linear dielectric medium, in a manifestly gauge invariant form, and show that the Dicke model in the dilute regime can be regarded as a particular case of the more general Hopfield model.