Ultrastrong Light-matter Coupling Research Articles

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.

Quasi-static and propagating modes in three-dimensional THz circuits.

We provide an analysis of the electromagnetic modes of three-dimensional metamaterial resonators in the THz frequency range. The fundamental resonance of the structures is fully described by an analytical circuit model, which not only reproduces the resonant frequencies but also the coupling of the metamaterial with an incident THz radiation. We also demonstrate the contribution of the propagation effects, and show how they can be reduced by design. In the optimized design, the electric field energy is lumped into ultra-subwavelength (λ/100) capacitors, where we insert a semiconductor absorber based on the collective electronic excitation in a two dimensional electron gas. The optimized electric field confinement is exhibited by the observation of the ultra-strong light-matter coupling regime, and opens many possible applications for these structures in detectors, modulators and sources of THz radiation.

Landau polaritons in highly nonparabolic two-dimensional gases in the ultrastrong coupling regime

We probe ultra-strong light matter coupling between metallic terahertz metasurfaces and Landau-level transitions in high mobility 2D electron and hole gases. We utilize heavy-hole cyclotron resonances in strained Ge and electron cyclotron resonances in InSb quantum wells, both within highly non-parabolic bands, and compare our results to well known parabolic AlGaAs/GaAs quantum well (QW) systems. Tuning the coupling strength of the system by two methods, lithographically and by optical pumping, we observe a novel behavior clearly deviating from the standard Hopfield model previously verified in cavity quantum electrodynamics: an opening of a lower polaritonic gap.

Quantum fluctuations in a strongly interacting Bardeen-Cooper-Schrieffer polariton condensate at thermal equilibrium

Microcavity electron-hole-photon systems in two-dimensions are long anticipated to exhibit a crossover from Bose-Einstein condensate (BEC) to Bardeen-Cooper-Schrieffer (BCS) superfluid, when carrier density is tuned to reach the Mott transition density. Yet, theoretical understanding of such a BEC-BCS crossover largely relies on the mean-field framework and the nature of the carriers at the crossover remains unclear to some extent. Here, motivated by the recent demonstration of a BCS polariton laser {[}Hu \textit{et al.}, arXiv:1902.00142{]} and based on a simplified short-range description of the electron-hole attraction, we examine the role of quantum fluctuations in an exciton-polariton condensate at thermal equilibrium and determine the number of different type carriers at the crossover beyond mean-field. Near Mott density and with ultra-strong light-matter coupling, we find an unexpectedly large phase window for a strongly correlated BCS polariton condensate, where both fermionic Bogoliubov quasi-particles and bosonic excitons are significantly populated and strongly couple to photons. We predict its photoluminescence spectra and show that the upper polariton energy gets notably renormalized, giving rise to a high-energy side-peak at large carrier density, as observed in recent experiments.

Modulated phases of graphene quantum Hall polariton fluids

This work is placed in the context of solid-state systems in the regime of ultra-strong light-matter coupling. To date, the highest light-matter coupling strengths have been measured in experiments with polaritons in semiconductor systems under the conditions of the Integer Quantum Hall effect. Polaritons are excitations resulting from strong coupling of light with a dipole-carrying matter excitation. In Pellegrino et al. (2016), we studied the impact of electron-electron interaction on polaritons in cavities in the case of graphene under the conditions of the Integer Quantum Hall effect. By using a mean-field (Hartree-Fock) approach we have shown the possibility of formation of spatially modulated light-matter phases characterized by a wavelength that is dependent on the value of the applied static magnetic field and the concentration of carriers, which is tunable by varying the gate voltage.

Electro-optical sampling of quantum vacuum fluctuations in dispersive dielectrics

Electro-optical sampling has been recently used to perform spectrally-resolved measurements of electromagnetic vacuum fluctuations. In order to understand which information on the ground state of an interacting system can be acquired thanks to this technique, in this paper we will develop the quantum theory of electro-optical sampling in arbitrary dispersive dielectrics. Our theory shows that a measure of the time correlations of the vacuum fluctuations effectively implements an ellipsometry measurement on the quantum vacuum, allowing to access the frequency-dependent dielectric function. We discuss consequences of these results on the possibility to use electro-optical sampling to probe the population of ground-state virtual photons in the ultrastrong light-matter coupling regime.

Ultrastrong Light–Matter Coupling in Deeply Subwavelength THz LC Resonators

The ultra-strong light-matter coupling regime has been demonstrated in a novel three-dimensional inductor-capacitor (LC) circuit resonator, embedding a semiconductor two-dimensional electron gas in the capacitive part. The fundamental resonance of the LC circuit interacts with the intersubband plasmon excitation of the electron gas at $\omega_c = 3.3$~THz with a normalized coupling strength $2\Omega_R/\omega_c = 0.27$. Light matter interaction is driven by the quasi-static electric field in the capacitors, and takes place in a highly subwavelength effective volume $V_{\mathrm{eff}} = 10^{-6}\lambda_0^3$ . This enables the observation of the ultra-strong light-matter coupling with $2.4\times10^3$ electrons only. Notably, our fabrication protocol can be applied to the integration of a semiconductor region into arbitrary nano-engineered three dimensional meta-atoms. This circuit architecture can be considered the building block of metamaterials for ultra-low dark current detectors.

Vacuum-dressed cavity magnetotransport of a two-dimensional electron gas

We present a theory predicting how the linear magnetotransport of a two-dimensional electron gas is modified by a passive electromagnetic cavity resonator where no real photons are injected nor created. For a cavity photon mode with in-plane linear polarization, the dc bulk magnetoresistivity of the 2D electron gas is anisotropic. In the regime of high filling factors of the Landau levels, the envelope of the Shubnikov-de Haas oscillations is profoundly modified and the resistivity can be increased or reduced depending on the system parameters. In the limit of low magnetic fields, the resistivity along the cavity-mode polarization direction is enhanced in the ultrastrong light-matter coupling regime. Our work shows the crucial role of virtual polariton excitations in controlling the dc charge transport properties of cavity-embedded systems.

Organic Photodiodes with an Extended Responsivity Using Ultrastrong Light–Matter Coupling

In organic photodiodes (OPDs) light is absorbed by excitons, which dissociate to generate photocurrent. Here, we demonstrate a novel type of OPD in which light is absorbed by polaritons, hybrid light-matter states. We demonstrate polariton OPDs operating in the ultra-strong coupling regime at visible and infrared wavelengths. These devices can be engineered to show narrow responsivity with a very weak angle-dependence. More importantly, they can be tuned to operate in a spectral range outside that of the bare exciton absorption. Remarkably, we show that the responsivity of a polariton OPD can be pushed to near infrared wavelengths, where few organic absorbers are available, with external quantum efficiencies exceeding those of a control OPD.

Few-Electron Ultrastrong Light-Matter Coupling at 300 GHz with Nanogap Hybrid LC Microcavities.

Ultrastrong light-matter coupling allows the exploration of new states of matter through the interaction of strong vacuum fields with huge electronic dipoles. By using hybrid dipole antenna-split ring resonator-based cavities with extremely small effective mode volumes Veff/λ03 ≃ 6 × 10-10 and surfaces Seff/λ02 ≃ 3.5 × 10-7, we probe the ultrastrong light-matter coupling at 300 GHz to less than 100 electrons located in the last occupied Landau level of a high mobility two-dimensional electron gas, measuring a normalized coupling ratio of ΩR/ωc = 0.36. Effects of the extremely reduced cavity dimensions are observed as the light-matter coupled system is better described by an effective mass heavier than the uncoupled one. These results open the way to ultrastrong coupling at the single-electron level in two-dimensional electron systems.

Virtual photons in the ground state of a dissipative system

Much of the novel physics predicted to be observable in the ultrastrong light–matter coupling regime rests on the hybridisation between states with different numbers of excitations, leading to a population of virtual photons in the system’s ground state. In this article, exploiting an exact diagonalisation approach, we derive both analytical and numerical results for the population of virtual photons in presence of arbitrary losses. Specialising our results to the case of Lorentzian resonances we then show that the virtual photon population is only quantitatively affected by losses, even when those become the dominant energy scale. Our results demonstrate most of the ultrastrong-coupling phenomenology can be observed in loss-dominated systems which are not even in the standard strong coupling regime. We thus open the possibility to investigate ultrastrong-coupling physics to platforms that were previously considered unsuitable due to their large losses.

Cavity QED in the Ultrastrong Coupling Regime: Photon Bunching from the Emission of Individual Dressed Qubits

Photon antibunching in the light scattered by single quantum emitters is one of the hallmarks of quantum optics, providing an unequivocal demonstration of the quantized nature of the electromagnetic field. Antibunching can be intuitively understood by the need for a two-level system lying in its lower state after emitting a photon to be re-excited into the upper one before a second emission can take place. Here we show that such a picture breaks down in the ultrastrong light–matter coupling regime, when the coupling strength becomes comparable to the bare emitter frequency. Specializing to the cases of both a natural and an artificial atom, we thus show that a single emitter coupled to a photonic resonator can emit bunched light. The result presented herein is clear evidence of how the ultrastrong coupling regime is able to change the nature of individual atoms.

Monolithic OLED-Microwire Devices for Ultrastrong Magnetic Resonant Excitation.

Organic light-emitting diodes (OLEDs) make highly sensitive probes to test magnetic resonance phenomena under unconventional conditions since spin precession controls singlet-triplet transitions of electron-hole pairs, which in turn give rise to distinct recombination currents in conductivity. Electron paramagnetic resonance can therefore be detected in the absence of spin polarization. We exploit this characteristic to explore the exotic regime of ultrastrong light-matter coupling, where the Rabi frequency of a charge carrier spin is of the order of the transition frequency of the two-level system. To reach this domain, we have to lower the Zeeman splitting of the spin states, defined by the static magnetic field B0, and raise the strength of the oscillatory driving field of the resonance, B1. This is achieved by shrinking the OLED and bringing the source of resonant radio frequency (RF) radiation as close as possible to the organic semiconductor in a monolithic device structure, which incorporates an OLED fabricated directly on top of an RF microwire within one monolithic thin-film device structure. With an RF driving power in the milliwatt range applied to the microwire, the regime of bleaching and inversion of the magnetic resonance signal is reached due to the onset of the spin-Dicke effect. In this example of ultrastrong light-matter coupling, the individual resonant spin transitions of electron-hole pairs become indistinguishable with respect to the driving field, and superradiance of the magnetic dipole transitions sets in.

Deterministic quantum nonlinear optics with single atoms and virtual photons

We show how analogues of a large number of well-known nonlinear-optics phenomena can be realized with one or more two-level atoms coupled to one or more resonator modes. Through higher-order processes, where virtual photons are created and annihilated, an effective deterministic coupling between two states of such a system can be created. In this way, analogues of three-wave mixing, four-wave mixing, higher-harmonic and -subharmonic generation (i.e., up- and downconversion), multiphoton absorption, parametric amplification, Raman and hyper-Raman scattering, the Kerr effect, and other nonlinear processes can be realized. The effective coupling becomes weaker the more intermediate transition steps are needed. However, given the recent experimental progress in ultrastrong light-matter coupling, especially in the field of circuit quantum electrodynamics, we estimate that many of these nonlinear-optics analogues can be realized with currently available technology.

Absorption and photoluminescence in organic cavity QED

Organic microcavities can be engineered to reach exotic quantum regimes of strong and ultrastrong light-matter coupling. However, the microscopic interpretation of their spectroscopic signals can be challenging due to the competition between coherent and dissipative processes involving electrons, vibrations and cavity photons. We develop here a theoretical framework based on the Holstein-Tavis-Cummings model and a Markovian treatment of dissipation to account for previously unexplained spectroscopic features of organic microcavities consistently. We identify conditions for the formation of dark vibronic polaritons, a new class of light-matter excitations that are not visible in absorption but lead to strong photoluminescence lines. We show that photon leakage from dark vibronic polaritons can be responsible for enhancing photoluminescence at the lower polariton frequency, and also explain the apparent breakdown of reciprocity between absorption and emission in the vicinity of the bare molecular transition frequency. Successful comparison with experimental data demonstrates the applicability of our theory.

Asymmetry in polariton dispersion as function of light and matter frequencies in the ultrastrong coupling regime

In the ultrastrong light–matter coupling regime, non-perturbative effects are observed even for large detuning of the light and matter frequencies. In this regime, the rotating wave approximation breaks down and the contributions of counter-rotating and diamagnetic terms lead to significant spectral modifications. Using split ring resonators coupled to the cyclotron transition in a two dimensional electron gas, we show that the diamagnetic terms lead to an asymmetry between the light and matter branches. Our system allows tuning both, the cavity and the matter frequency over more than two octaves. We find, that the assumption of constant coupling rate Ω as function of detuning is not generally valid for the large frequency range relevant to ultrastrong coupling phenomena.

Strong and ultrastrong coupling with free-space radiation

Strong and ultra-strong light-matter coupling are remarkable phenomena of quantum electrodynamics occurring when the interaction between a matter excitation and the electromagnetic field cannot be described by usual perturbation theory. This is generally achieved by coupling an excitation with large oscillator strength to the confined electromagnetic mode of an optical microcavity. In this work we demonstrate that strong/ultra-strong coupling can also take place in the absence of optical confinement. We have studied the non-perturbative spontaneous emission of collective excitations in a dense two-dimensional electron gas that superradiantly decays into free space. By using a quantum model based on the input-output formalism, we have derived the linear optical properties of the coupled system and demonstrated that its eigenstates are mixed light-matter particles, like in any system displaying strong or ultra-strong light-matter interaction. Moreover, we have shown that in the ultra-strong coupling regime, i.e. when the radiative broadening is comparable to the matter excitation energy, the commonly used rotating-wave and Markov approximations yield unphysical results. Finally, the input-output formalism has allowed us to prove that Kirchhoff's law, describing thermal emission properties, applies to our system in all the light-matter coupling regimes considered in this work.

Collective non-perturbative coupling of 2D electrons with high-quality-factor terahertz cavity photons

Nonperturbative coupling of light with condensed matter in an optical cavity is expected to reveal a host of coherent many-body phenomena and states. In addition, strong coherent light-matter interaction in a solid-state environment is of great interest to emerging quantum-based technologies. However, creating a system that combines a long electronic coherence time, a large dipole moment, and a high cavity quality ($Q$) factor has been a challenging goal. Here, we report collective ultrastrong light-matter coupling in an ultrahigh-mobility two-dimensional electron gas in a high-$Q$ terahertz photonic-crystal cavity in a quantizing magnetic field, demonstrating a cooperativity of $\sim$360. The splitting of cyclotron resonance (CR) into the lower and upper polariton branches exhibited a $\sqrt{n_\mathrm{e}}$-dependence on the electron density ($n_\mathrm{e}$), a hallmark of collective vacuum Rabi splitting. Furthermore, a small but definite blue shift was observed for the polariton frequencies due to the normally negligible $A^2$ term in the light-matter interaction Hamiltonian. Finally, the high-$Q$ cavity suppressed the superradiant decay of coherent CR, which resulted in an unprecedentedly narrow intrinsic CR linewidth of 5.6 GHz at 2 K. These results open up a variety of new possibilities to combine the traditional disciplines of many-body condensed matter physics and cavity-based quantum optics.

Output squeezed radiation from dispersive ultrastrong light-matter coupling

We investigate the output generation of squeezed radiation of a cavity photon mode coupled to another off-resonant bosonic excitation. By modulating in time their linear interaction, we predict high degree of output squeezing when the dispersive ultrastrong coupling regime is achieved, i.e., when the interaction rate becomes comparable to the frequency of the lowest energy mode. Our work paves the way to squeezed light generation in frequency domains where the ultrastrong coupling is obtained, e.g., solid-state resonators in the GHz, THz and mid-IR spectral range.