Strong Coupling Regime Research Articles

Homonuclear J-coupling spectroscopy using J-synchronized echo detection

In the strong coupling regime with J-coupling much larger than chemical shift differences, J-coupling spectroscopy enables spectral identification of molecules even when conventional NMR fails. While this classically required the presence of a heteronucleus, we recently showed that J-coupling spectra can be acquired in many homonuclear systems using spin-lock induced crossing (SLIC). Here, we present an alternative method using a spin echo train in lieu of a spin-locking SLIC pulse, which has a number of advantages. In particular, spin echo acquisition within the pulse train enables simultaneous collection of time and frequency data. The resulting 2D spectrum can be used to study dynamic spin evolution, and the time domain data can be averaged to create a 1D J-coupling spectrum with increased signal-to-noise ratio.

Fermi Surface Expansion above Critical Temperature in a Hund Ferromagnet.

Using a cluster extension of the dynamical mean-field theory, we show that strongly correlated metals subject to Hund's physics exhibit significant electronic structure modulations above magnetic transition temperatures. In particular, in a ferromagnet having a large local moment due to Hund's coupling (Hund's ferromagnet), the Fermi surface expands even above the Curie temperature (T_{C}) as if a spin polarization occurred. Behind this phenomenon, effective "Hund's physics" works in momentum space, originating from ferromagnetic fluctuations in the strong-coupling regime. The resulting significantly momentum-dependent (spatially nonlocal) electron correlations induce an electronic structure reconstruction involving a Fermi surface volume change and a redistribution of the momentum-space occupation. Our finding will give a deeper insight into the physics of Hund's ferromagnets above T_{C}.

Twist Angle Tuning of Moiré Exciton Polaritons in van der Waals Heterostructures.

Twisted atomically thin semiconductors are characterized by moiré excitons. Their optical signatures and selection rules are well understood. However, their hybridization with photons in the strong coupling regime for heterostructures integrated in an optical cavity has not been the focus of research yet. Here, we combine an excitonic density matrix formalism with a Hopfield approach to provide microscopic insights into moiré exciton polaritons. In particular, we show that exciton-light coupling, polariton energy, and even the number of polariton branches can be controlled via the twist angle. We find that these new hybrid light-exciton states become delocalized relative to the constituent excitons due to the mixing with light and higher-energy excitons. The system can be interpreted as a natural quantum metamaterial with a periodicity that can be engineered via the twist angle. Our study presents a significant advance in microscopic understanding and control of moiré exciton polaritons in twisted atomically thin semiconductors.

Floquet analysis of extended Rabi models based on high-frequency expansion

The extended quantum Rabi models make a significant contribution to understanding of the quantum nature of the atom-light interaction. We transform two kinds of extended quantum Rabi model, the anisotropic Rabi model and the asymmetric Rabi model, into the rotating frame and regard them as periodically driven quantum systems. The analytical solutions of the quasienergy spectrum as well as the Floquet modes for both models are constructed by applying the Floquet theory and the high-frequency expansion, which is applied to the nonstroboscopic dynamics of physical observables such as atomic inversion, transverse magnetization, and atom-field correlation. For the anisotropic Rabi model, the quasienergy fits well with the numerical results even when the rotating-wave coupling is in the deep strong-coupling regime $g\ensuremath{\simeq}\ensuremath{\hbar}\ensuremath{\omega}$ if the counter-rotating term is small enough compared to the driving frequency. Avoided level crossing may occur for quasienergy with the same parity when the positive branch spectrum lines for the total excitation number $N$ cross the negative branch lines for $N+2$, while the high-frequency expansion fails to predict this due to the conservation of the total excitation number. Furthermore, we present analytical and numerical studies of the long-time evolution of population and conclude that the analytical method is credible for the population dynamics. For the asymmetric Rabi model, we find that the external bias field which breaks the parity symmetry of the total excitation number tends to cluster the upper and lower branches into two bundles, and the detuning induced gap in the first temporal Brillouin zone shows a quadratic dependence on the bias. Fourier analysis is applied to extract the frequency composition and two-frequency driving behavior is revealed. Varying the bias strength will change the time-averaged value of the oscillation, which shows how the bias competes with the detuning and atom-field coupling in the driving dynamics. Both models prove that treating the Hamiltonian in the rotating frame by Floquet theory gives an alternative tool in the study of interaction between atom and light.

Plasmon-induced coherence, exciton-induced transparency, and Fano interference for hybrid plasmonic systems in strong coupling regime.

We present an analytical model describing the transition to a strong coupling regime for an ensemble of emitters resonantly coupled to a localized surface plasmon in a metal-dielectric structure. The response of a hybrid system to an external field is determined by two distinct mechanisms involving collective states of emitters interacting with the plasmon mode. The first mechanism is the near-field coupling between the bright collective state and the plasmon mode, which underpins the energy exchange between the system components and gives rise to exciton-induced transparency minimum in scattering spectra in the weak coupling regime and to emergence of polaritonic bands as the system transitions to the strong coupling regime. The second mechanism is the Fano interference between the plasmon dipole moment and the plasmon-induced dipole moment of the bright collective state as the hybrid system interacts with the radiation field. The latter mechanism is greatly facilitated by plasmon-induced coherence in a system with the characteristic size below the diffraction limit as the individual emitters comprising the collective state are driven by the same alternating plasmon near field and, therefore, all oscillate in phase. This cooperative effect leads to scaling of the Fano asymmetry parameter and of the Fano function amplitude with the ensemble size, and therefore, it strongly affects the shape of scattering spectra for large ensembles. Specifically, with increasing emitter numbers, the Fano interference leads to a spectral weight shift toward the lower energy polaritonic band.

Generalization of the Tavis-Cummings model for multi-level anharmonic systems: Insights on the second excitation manifold.

Confined electromagnetic modes strongly couple to collective excitations in ensembles of quantum emitters, producing light-matter hybrid states known as polaritons. Under such conditions, the discrete multilevel spectrum of molecular systems offers an appealing playground for exploring multiphoton processes. This work contrasts predictions from the Tavis-Cummings model in which the material is a collection of two-level systems, with the implications of considering additional energy levels with harmonic and anharmonic structures. We discuss the exact eigenspectrum, up to the second excitation manifold, of an arbitrary number N of oscillators collectively coupled to a single cavity mode in the rotating-wave approximation. Elaborating on our group-theoretic approach [New J. Phys. 23, 063081 (2021)], we simplify the brute-force diagonalization of N2 × N2 Hamiltonians to the eigendecomposition of, at most, 4 × 4 matrices for arbitrary N. We thoroughly discuss the eigenstates and the consequences of weak and strong anharmonicities. Furthermore, we find resonant conditions between bipolaritons and anharmonic transitions where two-photon absorption can be enhanced. Finally, we conclude that energy shifts in the polaritonic states induced by anharmonicities become negligible for large N. Thus, calculations with a single or few quantum emitters qualitatively fail to represent the nonlinear optical response of the collective strong coupling regime. Our work highlights the rich physics of multilevel anharmonic systems coupled to cavities absent in standard models of quantum optics. We also provide concise tabulated expressions for eigenfrequencies and transition amplitudes, which should serve as a reference for future spectroscopic studies of molecular polaritons.

Flexural deformations and collapse of bilayer two-dimensional crystals by interlayer excitons

We develop a consistent theory of the interlayer exciton-polaron formed in atomically-thin bilayers. Coulomb attraction between an electron and a hole situated in the different layers results in their flexural deformation and provides an efficient mechanism of the exciton coupling with flexural phonons. We study the effect of layers tension on the polaron binding energy and effective mass leading to suppression of polaron formation by the tension both in the weak and strong coupling regimes. We also consider the role of the nonlinearity related to the interaction between the out- and in-plane lattice displacements and obtain the criterion of the layer sticking, where the exciton collapses, due to the Coulomb attraction between the charge carriers.

The Ergodic GN Model for Space-Division Multiplexing With Strong Mode Coupling

The Gaussian noise (GN) model, thanks to its simplicity, is the most widely used model to describe the nonlinear interference (NLI) in fiber-optic systems. This paper gives an extension of the GN model to space-division multiplexed (SDM) systems operating in the regime of strong coupling between modes, where the understanding of the effect of spatial mode dispersion (SMD) on the accumulation of the NLI noise stands as an open problem of utmost importance. We show that SMD may significantly reduce the NLI power and that a reliable estimation can be done with the extended GN model in very fast times, of the order of seconds per channel. We derive a closed-form expression for the NLI power averaged with respect to the frequency-dependence random-mode coupling introduced by mode dispersion, and show that its random fluctuations around the average value are negligible for all practical purposes. The derived expression is proved to be very accurate in the relevant range of SMD values. Scaling properties of the NLI variance with respect to the main system parameters are also discussed to gain some physical insight.

Universal model of strong coupling at the nonlinear resonance in open cavity-QED systems

Many molecular, quantum-dot, and optomechanical nanocavity-QED systems demonstrate strong nonlinear interactions between electrons, photons, and phonon (vibrational) modes. We show that such systems can be described by a universal model in the vicinity of the nonlinear resonance involving all three degrees of freedom. We solve the nonperturbative quantum dynamics in the strong-coupling regime of the nonlinear resonance, taking into account quantization, dissipation, and fluctuations of all fields. We find analytic solutions for quantum states in the rotating-wave approximation which demonstrate tripartite quantum entanglement once the strong-coupling regime is reached. We show how the strong coupling at the nonlinear resonance modifies photon emission and vibrational spectra, and how the observed spectra can be used to extract information about relaxation rates and the nonlinear coupling strength in specific systems.

Topologically driven Rabi-oscillating interference dislocation

Abstract Quantum vortices are the quantized version of classical vortices. Their center is a phase singularity or vortex core around which the flow of particles as a whole circulates and is typical in superfluids, condensates and optical fields. However, the exploration of the motion of the phase singularities in coherently-coupled systems is still underway. We theoretically analyze the propagation of an interference dislocation in the regime of strong coupling between light and matter, with strong mass imbalance, corresponding to the case of microcavity exciton–polaritons. To this end, we utilize combinations of vortex and tightly focused Gaussian beams, which are introduced through resonant pulsed pumping. We show that a dislocation originates from self-interference fringes, due to the non-parabolic dispersion of polaritons combined with moving Rabi-oscillating vortices. The morphology of singularities is analyzed in the Poincaré space for the pseudospin associated to the polariton states. The resulting beam carries orbital angular momentum with decaying oscillations due to the loss of spatial overlap between the normal modes of the polariton system.

A Note on Gauged Baby Skyrmions

In this paper we study a gauged version of the two dimensional Skyrme model of nuclear physics; the field configurations are couples (u, A), where u:{mathbb {R}}^2rightarrow S^2 is a map constant at infinity, which can be classified by its topological degree, and A:{mathbb {R}}^2rightarrow {mathbb {R}}^2 is the gauge field. We prove the existence of rotationally symmetric field configurations which minimize the gauged Skyrme energy on every topological sector (gauged baby skyrmions). Moreover we study the behavior of these skyrmions in the case of weak or strong coupling with the gauge field. In particular, we show that, as observed by many authors by means of numerical simulations, in the strong coupling regime the magnetic flux associated with the gauge field becomes quantized.

Optomagnonics in Dispersive Media: Magnon-Photon Coupling Enhancement at the Epsilon-near-Zero Frequency.

Reaching strong light-matter coupling in solid-state systems has long been pursued for the implementation of scalable quantum devices. Here, we put forward a system based on a magnetized epsilon-near-zero (ENZ) medium, and we show that strong coupling between magnetic excitations (magnons) and light can be achieved close to the ENZ frequency due to a drastic enhancement of the magneto-optical response. We adopt a phenomenological approach to quantize the electromagnetic field inside a dispersive magnetic medium in order to obtain the frequency-dependent coupling between magnons and photons. We predict that, in the epsilon-near-zero regime, the single-magnon single-photon coupling can be comparable to the magnon frequency for a small magnetic volume and perfect mode overlap. For state-of-the-art illustrative values, this would correspond to achieving the single-magnon strong coupling regime, where the coupling rate is larger than all the decay rates. Finally, we show that the nonlinear energy spectrum intrinsic to this coupling regime can be probed via the characteristic multiple magnon sidebands in the photon power spectrum.

Microscopic theory of exciton and trion polaritons in doped monolayers of transition metal dichalcogenides

We study a doped transition metal dichalcogenide (TMDC) monolayer in an optical microcavity. Using the microscopic theory, we simulate spectra of quasiparticles emerging due to the interaction of material excitations and a high-finesse optical mode, providing a comprehensive analysis of optical spectra as a function of Fermi energy and predicting several modes in the strong light-matter coupling regime. In addition to exciton-polaritons and trion-polaritons, we report polaritonic modes that become bright due to the interaction of excitons with free carriers. At large doping, we reveal strongly coupled modes corresponding to excited trions that hybridize with a cavity mode. We also demonstrate that the increase of carrier concentration can change the nature of the system’s ground state from the dark to the bright one. Our results offer a unified description of polaritonic modes in a wide range of free electron densities.

Radiative decay of an emitter due to non-Markovian interactions with dissipating matter

It is known that the more tractable Markovian models of coupling suited for weak interactions may overestimate the Rabi frequency notably when applied to the strong-coupling regime. Here, a more significant consequence of the non-Markovian interaction between a photon emitter and dissipating matter such as resonant plasmonic nanoparticles is described. A large increase of radiative decay and a diminished non-radiative loss is shown, which unravels the origin of unexpected large enhancements of surface-enhanced-Raman-spectroscopy, as well as the anomalous enhancements of emission due to extremely small fully absorbing metal nanoparticles less than 10 nm in dimensions. We construct the mixture of pure states of the coupled emitter-nanoparticle system, unlike conventional methods that rely on the orthogonal modes of the nanoparticle alone.

Many-body approach to superfluid nuclei in axial geometry

Starting from a general many-body fermionic Hamiltonian, we derive the equations of motion (EOM) for nucleonic propagators in a superfluid system. The resulting EOM is of the Dyson type formulated in the basis of Bogoliubov's quasiparticles. As the leading contributions to the dynamical kernel of this EOM in strongly-coupled regimes contain phonon degrees of freedom in various channels, an efficient method of calculating phonon's characteristics is required to successfully model these kernels. The traditional quasiparticle random phase approximation (QRPA) solvers are typically used for this purpose in nuclear structure calculations, however, they become very prohibitive in nonspherical geometries. In this paper, by linking the notion of the quasiparticle-phonon vertex to the variation of the Bogoliubov's Hamiltonian, we show that the recently developed finite-amplitude method (FAM) can be efficiently employed to compute the vertices within the FAM-QRPA. To illustrate the validity of the method, calculations based on the relativistic density-dependent point-coupling Lagrangian are performed for the single-nucleon states in heavy and medium-mass nuclei with axial deformations. The cases of $^{38}\mathrm{Si}$ and $^{250}\mathrm{Cf}$ are presented and discussed.

Hybrid plasmonic-photonic microcavity for enhanced light-matter interaction

Cavity quantum electrodynamics focuses on enhancing the light-matter interactions for a broad spectrum of applications, including lasers, quantum information processing, spectroscopy, and imaging. As photonic cavities confine light with the constraint of diffraction limit while plasmonic cavities suffer from Ohmic loss, hybrid plasmonic-photonic microcavities have emerged as a versatile platform to overcome the limitations in pure systems and enhance lightmatter interactions reaching the strong coupling regime. The present Perspective starts from the fundamentals of light-matter interaction, followed by the review of both theoretical and experimental developments achieved recently in hybrid plasmonic-photonic systems. Together with the fascinating optical properties of hybrid systems, diverse potential applications are discussed, for example, quantum state preparation and operation, nonlinear optics, molecular spectroscopy, and sensing. The possible challenges posed to nanofabrication and characterization are also briefly covered.

Theory of Nonlinear Excitonic Response of Hybrid Organic Perovskites in the Regime of Strong Light-Matter Coupling

We present a quantitative study of the nonlinear optical response of layered perovskites placed inside planar photonic microcavities in the regime of strong light matter coupling, when excitonic and photonic modes hybridize and give rise to cavity polaritons. Two sources of nonlinearity are specified, the saturation of the excitonic transition with increase of the optical pump and Coulomb interaction between the excitons. It is demonstrated, that peculiar form of the interaction potential, specific to multilayer structure of organic perovskites, is responsible for substantial increase of the exciton binding energy and Rabi splitting with respect to conventional semiconductor systems. This results in dominant contribution of the Rabi splitting quench effect in the nonlinear optical response. Moreover, due to the tightly bound character of excitons, the density of Mott transition is essentially higher, allowing to reach extremely large polariton blueshifts of about 50 meV, which is order of magnitude higher than in conventional semiconductors.

Unified Scattering and Photoluminescence Spectra for Strong Plasmon-Exciton Coupling.

The strong coupling between excitons and single plasmonic nanocavities enables plexcitonic states in nanoscale systems at room temperature. Here we demonstrate the strong coupling of surface plasmon modes of metal nanowires and excitons in monolayer semiconductors, with Rabi splitting manifested in both scattering and photoluminescence (PL) spectra. By utilizing the propagation properties of surface plasmons on the nanowires, the PL emitted through the scattering of plasmon-exciton hybrid modes is extracted. The analytically calculated scattering and PL spectra well reproduce the experimental results. These findings unify the scattering and PL spectra in the plexcitonic system and eliminate the ambiguities of PL emission, shedding new light on understanding the rich spectral phenomena in the plasmon-exciton strong coupling regime.

Cavity-altered thermal isomerization rates and dynamical resonant localization in vibro-polaritonic chemistry

It has been experimentally demonstrated that reaction rates for molecules embedded in microfluidic optical cavities are altered when compared to rates observed under "ordinary" reaction conditions. However, precise mechanisms of how strong coupling of an optical cavity mode to molecular vibrations affects the reactivity and how resonance behavior emerges are still under dispute. In the present work, we approach these mechanistic issues from the perspective of a thermal model reaction, the inversion of ammonia along the umbrella mode, in the presence of a single-cavity mode of varying frequency and coupling strength. A topological analysis of the related cavity Born-Oppenheimer potential energy surface in combination with quantum mechanical and transition state theory rate calculations reveals two quantum effects, leading to decelerated reaction rates in qualitative agreement with experiments: the stiffening of quantized modes perpendicular to the reaction path at the transition state, which reduces the number of thermally accessible reaction channels, and the broadening of the barrier region, which attenuates tunneling. We find these two effects to be very robust in a fluctuating environment, causing statistical variations of potential parameters, such as the barrier height. Furthermore, by solving the time-dependent Schrödinger equation in the vibrational strong coupling regime, we identify a resonance behavior, in qualitative agreement with experimental and earlier theoretical work. The latter manifests as reduced reaction probability when the cavity frequency ωc is tuned resonant to a molecular reactant frequency. We find this effect to be based on the dynamical localization of the vibro-polaritonic wavepacket in the reactant well.

Fulfillment of sum rules and Ward identities in the multiloop functional renormalization group solution of the Anderson impurity model

We investigate several fundamental characteristics of the multiloop functional renormalization group (mfRG) flow by hands of its application to a prototypical many-electron system: the Anderson impurity model (AIM). We first analyze the convergence of the algorithm in the different parameter regions of the AIM. As no additional approximation is made, the multiloop series for the local self-energy and response functions converge perfectly to the corresponding results of the parquet approximation (PA) in the weak- to intermediate-coupling regime. Small oscillations of the mfRG solution as a function of the loop order gradually increase with the interaction, hindering a full convergence to the PA in the strong-coupling regime, where perturbative resummation schemes are no longer reliable. By exploiting the converged results, we inspect the fulfillment of (i) sum rules associated to the Pauli principle and (ii) Ward identities related to conservation laws. For the Pauli principle, we observe a systematic improvement by increasing the loop order and including the multiloop corrections to the self-energy. This is consistent with the preservation of crossing symmetries and two-particle self-consistency in the PA. For the Ward identities, we numerically confirm a visible improvement by means of the Katanin substitution. At weak coupling, violations of the Ward identity are further reduced by increasing the loop order in mfRG. In this regime, we also determine the precise scaling of the deviations of the Ward identity as a function of the electronic interaction. For larger interaction values, the overall behavior becomes more complex, and the benefits of the higher-loop terms are mostly present in the contributions at large frequencies.