Recent experiments have observed that the chemical and photophysical properties of molecules can be modified inside an optical Fabry-Perot microcavity under collective vibrational strong coupling (VSC) conditions, and such modification is currently not well understood by theory. In an effort to understand the origin of such cavity induced phenomena, some recent studies have focused on the effect of the cavity environment on the nonlinear optical response of the molecular subsystem. Here, we use a recently proposed protocol for classical cavity molecular dynamics (CavMD) simulations to numerically investigate the linear and nonlinear response of liquid carbon dioxide under such VSC conditions following an optical pulse excitation. We find that applying a strong pulse of excitation to the lower hybrid light-matter state, i.e., the lower polariton (LP), can lead to an overall molecular nonlinear absorption which is enhanced by up to two orders of magnitude relative to the excitation outside the cavity. This polariton-enhanced multiphoton absorption also causes an ultrashort LP lifetime (0.2 ps) under strong illumination. Unlike usual polariton relaxation processes -- whereby polaritonic energy transfers directly to the manifold of singly excited vibrational dark states -- under the present mechanism, the LP transfers energy directly to the manifold of higher vibrationally excited dark states; these highly excited dark states subsequently relax to the manifold of singly excited states with a lifetime of tens of ps. Because the present mechanism is generic in nature, we expect these numerical predictions to be experimentally observed in different molecular systems and in cavities with different volumes.
Selectively exciting target molecules to high vibrational states is inefficient in the liquid phase, which restricts the use of IR pumping to catalyze ground-state chemical reactions. Here, we demonstrate that this inefficiency can sometimes be solved by confining the liquid to an optical cavity under vibrational strong coupling conditions. For a liquid solution of 13CO2 solute in a 12CO2 solvent, cavity molecular dynamics simulations show that exciting a polariton (hybrid light-matter state) of the solvent with an intense laser pulse, under suitable resonant conditions, may lead to a very str…
We report the first experimental two-dimensional infrared (2D IR) spectra of novel molecular photonic excitations - vibrational-polaritons. The application of advanced 2D IR spectroscopy onto novel vibrational-polariton challenges and advances our understanding in both fields. From spectroscopy aspect, 2D IR spectra of polaritons differ drastically from free uncoupled molecules; from vibrational-polariton aspects, 2D IR uniquely resolves hybrid light-matter polariton excitations and unexpected dark states in a state-selective manner and revealed hidden interactions between them. Moreover, 2D I…
Under vibrational strong coupling (VSC), the formation of molecular polaritons may significantly modify the photo-induced or thermal properties of molecules. In an effort to understand these intriguing modifications, both experimental and theoretical studies have focused on the ultrafast dynamics of vibrational polaritons. Here, following our recent work [J. Chem. Phys., 154, 094124, (2021)], we systematically study the mechanism of polariton relaxation for liquid CO2 under a weak external pumping. Classical cavity molecular dynamics (CavMD) simulations show that polariton relaxation results f…
Strong coupling of molecular vibrations to an infrared cavity mode affects their nature by creating dressed polariton states. We show how the single and double vibrational polariton manifolds may be controlled by varying the cavity coupling strength, and probed by a time domain 2DIR technique, Double Quantum Coherence (DQC). Applications are made to the amide-I ($CO$) and amide-II ($CN$) bond vibrations of $N-methylacetamide$ (NMA).
We propose a cavity QED approach to describe light-matter interaction between an individual anharmonic molecular vibration and an infrared cavity field. Starting from a generic Morse oscillator with quantized nuclear motion, we derive a multi-level quantum Rabi model to study vibrational polaritons beyond the rotating-wave approximation. We analyze the spectrum of vibrational polaritons in detail and compare with available experiments. For high excitation energies, the spectrum exhibits a dense manifold of true and avoided level crossings as the light-matter coupling strength and cavity freque…
We have developed a non-Markovian theory of the polariton luminescence taking the molecular vibrations into account. The calculations were made in the polariton basis. We have shown that the frequency shift and the polariton spectral lines broadening strongly depend on the frequency-dependent exciton contribution to the polariton. In the single-mode microcavity our non-Markovian theory predicts the Fano resonances in the polariton luminescence, and also narrowing of the spectral lines with the increase of the total number of molecules in the case of the intramolecular nature of the low frequen…
We have developed a model in order to account for electron-vibrational effects on absorption, luminescence of molecular aggregates and exciton-polaritons in nanofibers. The model generalizes the mean-field electron-vibrational theory developed by us earlier to the systems with spatial symmetry, exciton luminescence and the exciton-polaritons with spatial dispersion. The correspondence between manifestation of electron-vibrational interaction in monomers, molecular aggregates and exciton-polariton dispersion in nanofibers is obtained by introducing the aggregate line-shape functions in terms of…
Cavity-polaritons in semiconductor photonic structures have emerged as a test bed for exploring non-equilibrium dynamics of quantum fluids in an integrated solid-state device setting. Several recent experiments demonstrated the potential of these systems for revealing quantum many-body physics in driven-dissipative systems. So far, all experiments have relied on fully integrated devices with little to no flexibility for modification of device properties. Here, we present a novel approach for realizing confined cavity-polaritons that enables in-situ tuning of the cavity length and thereby of th…
Until now, the generation of an excitonic reservoir in a cavity polariton system under quasi-resonant pumping has always been neglected. We show that in microcavities having a small Rabi splitting (typically GaAs cavities with a single quantum well), this reservoir can be efficiently populated by polariton-phonon scattering. We consider the influence of the exciton reservoir on the energy shifts of the resonantly pumped polariton modes. We show that the presence of this reservoir effectively reduces the spin anisotropy of the polariton-polariton interaction, in agreement with recent experiment…
Resonant photoelastic coupling in semiconductor nanostructures opens new perspectives for strongly enhanced light-sound interaction in optomechanical resonators. One potential problem, however, is the reduction of the cavity Q-factor induced by dissipation when the resonance is approached. We show in this letter that cavity-polariton mediation in the light-matter process overcomes this limitation allowing for a strongly enhanced photon-phonon coupling without significant lifetime reduction in the strongly-coupled regime. Huge optomechanical coupling factors in the PetaHz/nm range are envisaged…
Strong coupling between light and matter is possible with a variety of organic materials. In contrast to the simpler inorganic case, organic materials often have a complicated spectrum, with vibrationally dressed electronic transitions. Strong coupling to light competes with this vibrational dressing, and if strong enough, can suppress the entanglement between electronic and vibrational degrees of freedom. By exploiting symmetries, we can perform exact numerical diagonalization to find the polaritonic states for intermediate numbers of molecules, and use these to define and validate accurate e…
The way molecules absorb, transfer, and emit light can be modified by coupling them to optical cavities. The extent of the modification is often defined by the cavity-molecule coupling strength, which depends on the number of coupled molecules. We experimentally and numerically study the evolution of photoemission from a thin layered J-aggregated molecular material strongly coupled to a Fabry-Perot microcavity as a function of the number of coupled layers. We unveil an important difference between the strong coupling signatures obtained from reflection spectroscopy and from polariton assisted …
We study a hybrid system formed from an optomechanical resonator and a cavity mode strongly coupled to an excitonic transition inside a quantum well. We show that due to the mixing of cavity photon and exciton states, the emergent quasiparticles - polaritons - possess coupling to the mechanical mode of both dispersive and dissipative nature. We calculate the occupancies of polariton modes and reveal bistable behavior, which deviates from conventional Kerr nonlinearity or dispersive coupling cases due to the dissipative coupling. The described system serves as a good candidate for future polari…
Polaritons, mixed light-matter quasiparticles, undergo a transition to a condensed, macroscopically coherent state at low temperatures or high densities. Recent experiments show that coupling light to organic molecules inside a microcavity allows condensation at room temperature. The molecules act as saturable absorbers with transitions dressed by molecular vibrational modes. Motivated by this we calculate the phase diagram and spectrum of a modified Tavis-Cummings model, describing vibrationally dressed two-level systems, coupled to a cavity mode. Coupling to vibrational modes can induce re-e…
The nonlinear optical response of organic polaritonic matter has received increasing attention due to their enhanced and controllable nonlinear response and their potential for novel optical devices such as compact photon sources and optical and quantum information devices. Using z-scans at different wavelengths and incident powers we have studied the nonlinear optical dispersion of ultrastrongly coupled organic cavity polaritons near the lower polariton band. We show that the up to 150-fold enhancement of the nonlinear response compared to a cavity-less organic film arises from an intensity-d…
Electronic resonances can significantly enhance the photon-phonon coupling in cavity optomechanics, but are normally avoided due to absorption losses and dephasing by inhomogeneous broadening. We experimentally demonstrate that exciton-polaritons in semiconductor microcavities enable GHz optomechanics with single-particle resonant couplings reaching record values in the 10s of MHz range. Moreover, this resonant enhancement is protected from inhomogeneous broadening by the Rabi gap. Single-polariton non-linearities and the optomechanical strong-coupling regime become accessible in this platform…
In the regime of ensemble vibrational strong coupling (VSC), a macroscopic number $N$ of molecular transitions couple to each resonant cavity mode, yielding two hybrid light-matter (polariton) modes, and a reservoir of $N-1$ dark states whose chemical dynamics are essentially those of the bare molecules. This fact is seemingly in opposition to the recently reported modification of thermally activated ground electronic state reactions under VSC. Here, we provide a VSC Marcus-Levich-Jortner electron transfer model that potentially addresses this paradox: while entropy favors the transit through …
Spin transitions are studied theoretically and experimentally in a resonantly excited system of cavity polaritons in a magnetic field. Weak pair interactions in this boson system make possible fast and massive spin flips occurring at critical amplitudes due to the interplay between amplitude dependent shifts of eigenstates and the Zeeman splitting. Dominant spin of a condensate can be toggled forth and back by tuning of the pump intensity only, which opens the way for ultra-fast spin switchings of polariton condensates on a picosecond timescale.
Magnon-polaritons are hybrid light-matter quasiparticles originating from the strong coupling between magnons and photons. They have emerged as a potential candidate for implementing quantum transducers and memories. Owing to the dampings of both photons and magnons, the polaritons have limited lifetimes. However, stationary magnon-polariton states can be reached by a dynamical balance between pumping and losses, so the intrinsical nonequilibrium system may be described by a non-Hermitian Hamiltonian. Here we design a tunable cavity quantum electrodynamics system with a small ferromagnetic sph…
Hybrid halide perovskites are now considered as low-cost materials for contemporary research in photovoltaics and nanophotonics. In particular, because these materials can be solution processed, they represent a great hope for obtaining low-cost devices. While the potential of 2D layered hybrid perovskites for polaritonic devices operating at room temperature has been demonstrated in the past, the potential of the 3D perovskites has been much less explored for this particular application. Here, we report the strong exciton-photon coupling with 3D bromide hybrid perovskite. Cavity polaritons ar…
We theoretically study the transport of exciton polaritons under different applied photon potentials. The relation between the photon potentials and the thickness of the cavity layer is calculated by the finite element simulation. The theoretical analysis and numerical calculation indicate that the cavity photon potential is proportional to the thickness of the cavity layer with the coefficient being about $1.8$ meV/nm. Further, the periodic and linear photon potentials are considered to control the transport of the exciton polaritons in weak- and strong-field pump situations. In both situatio…
Quantum correlations and dissipative blockade of polaritons in a tunable fiber cavity
Institut für Quantenelektronik, ETH Zürich（苏黎世联邦理工学院量子电子学研究所）；Physikalisches Institut, Universität Bonn（波恩大学物理研究所）；Department of Physics, Universität Basel（巴塞尔大学物理系）；Univerité Paris-Saclay, UVSQ, CNRS, GEMaC（巴黎萨克雷大学、凡尔赛大学、法国国家科学研究中心、GEMaC）；Laboratorium für Festkörperphysik, ETH Zürich（苏黎世联邦理工学院固体物理实验室）
We demonstrate a new type of transition within the strong coupling regime, which alters the coupling mechanism in multimode cavities. We show that this transition drastically modifies the Hamiltonian describing the polaritons, such that different cavity modes are either entangled via the material or completely decoupled. This decoupling transition occurs due to the competition between the dissipation in the material and the finite group velocity, which governs the propagation of information across the cavity and among the molecules. The results indicate that the velocity of light, which is oft…
We report on the realization of a double barrier resonant tunneling diode for cavity polaritons, by lateral patterning of a one-dimensional cavity. Sharp transmission resonances are demonstrated when sending a polariton flow onto the device. We use a non-resonant beam can be used as an optical gate and control the device transmission. Finally we evidence distortion of the transmission profile when going to the high density regime, signature of polariton-polariton interactions.
Spontaneous Raman Scattering under Vibrational Strong Coupling: The Critical Role of Polariton Spatial Mode Coherence
Université de Strasbourg, CNRS, Institut de Physique et Chimie des Matériaux de Strasbourg（斯特拉斯堡大学）；Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière（里昂第一大学）
We address theoretically the optical parametric oscillator based on semiconductor cavity exciton-polaritons under a pulsed excitation. A "hyperspin" formalism is developed which allows, in the case of large number of polaritons, to reduce quantum dynamics of the parametric oscillator wavefunction to the Liouville equation for the classical probability distribution. Implications for the statistics of polariton ensembles are analyzed.
Motivated by the dramatic success of realizing cavity exciton-polariton condensation in experiment we consider the formation of polaritons from cavity photons and the amplitude or Higgs mode of a superconductor. Enabled by the recently predicted and observed supercurrent-induced linear coupling between these excitations and light, we find that hybridization between Higgs excitations in a disordered quasi-2D superconductor and resonant cavity photons can occur, forming Higgs-polariton states. This provides the potential for a new means to manipulate the superconducting state as well as potentia…
Polariton-mediated light-sound interaction is investigated through resonant Brillouin experiments in GaAs/AlAs multiple-quantum wells. Photoelastic coupling enhancement at exciton-polariton resonance reaches 105 at 30 K as compared to a typical bulk solid room temperature transparency value. When applied to GaAs based cavity optomechanical nanodevices, this result opens the path to huge displacement sensitivities and to novel ultrastrong-coupling cavity phenomena with optomechanical couplings g0 in the range of 100 THz.
We analyse the effect of a strong perpendicular magnetic field on an intersubband transition in a disordered doped quantum well strongly coupled to an optical cavity. The magnetic field changes the lineshape of the intersubband optical transition due to the interface roughness of the quantum well from a Lorentzian to a Gaussian one. In this regime, a novel form of magnetic-field-induced cavity protection sets in, which strongly reduces the polariton linewidth to the cavity contribution only. Implications of our results for fundamental studies of nonlinear polariton dynamics and for technologic…
Strong coupling between cavity photons and various excitations in condensed matters boosts the field of light-matter interaction and generates several exciting sub-fields, such as cavity optomechanics and cavity magnon polariton. Axion quasiparticles, emerging in topological insulators, were predicted to strongly couple with the light and generate the so-called axion polariton. Here, we demonstrate that there arises a gapless level attraction in cavity axion polariton of antiferromagnetic topological insulators, which originates from a nonlinear interaction between axion and the odd-order reso…
Strong coupling in cavity-magnon systems has shown great potential for use in spintronics and information processing technologies due to the low damping rates and long coherence times. Although such systems are conceptually similar to those coupled by magnon-polaritons (MPs), the link between magnon-cavity coupling and MPs has not been explicitly defined. In this work we establish such a connection by studying the frequency-wavevector dispersion of a strongly coupled magnon-cavity system, using a height-adjustable microwave cavity, and by modelling the observed behaviour through the system's e…
The exciton-polariton modes of a quantum dot lattice embedded in a planar optical cavity are theoretically investigated. Umklapp terms, in which an exciton interacts with many cavity modes differing by reciprocal lattice vectors, appear in the Hamiltonian due to the periodicity of the dot lattice. We focus on Bragg polariton modes obtained by tuning the exciton and the cavity modes into resonance at high symmetry points of the Brillouin Zone. Depending on the microcavity design these polaritons modes at finite in-plane momentum can be guided and can have long lifetimes. Moreover, their effecti…
The observation of spin-related phenomena of microcavity polaritons has been limited due to weak Zeeman effect of non-magnetic semiconductors. We demonstrate that the incorporation of magnetic ions into quantum wells placed in a non-magnetic microcavity results in enhanced effects of magnetic field on exciton-polaritons. We show that in such a structure the Zeeman splitting of exciton-polaritons strongly depends on the photon - exciton detuning and polariton wavevector. Our experimental data are explained by a model where the impact of magnetic field on the lower polariton state is directly in…
In the regime of strong coupling between molecular excitons and confined optical modes, the intra-molecular degrees of freedom are profoundly affected, leading to a reduced vibrational dressing of polaritons compared to bare electronically excited states. However, existing models only describe a single vibrational mode in each molecule, while actual molecules possess a large number of vibrational degrees of freedom and additionally interact with a continuous bath of phononic modes in the host medium in typical experiments. In this work, we investigate a small ensemble of molecules with an arbi…
We predict magnon polariton states circulating unidirectionally in a microwave cavity when loaded by a number of magnets on special lines. Realistic finite-element numerical simulations, including dielectric, time-dependent and non-linear effects, confirm the validity of the approximations of a fully analytical input-output model. We find that a phased antenna array can focus all power into a coherent microwave beam with controlled direction and an intensity that scales with the number of magnets.
When molecular transitions strongly couple to photon modes, they form hybrid light-matter modes called polaritons. Collective vibrational strong coupling is a promising avenue for control of chemistry, but this can be deterred by the large number of quasi-degenerate dark modes. The macroscopic occupation of a single polariton mode by excitations, as observed in Bose-Einstein condensation, offers promise for overcoming this issue. Here we theoretically investigate the effect of vibrational polariton condensation on the kinetics of electron transfer processes. Compared with excitation with infra…
We calculate the dispersion of spinor exciton-polaritons in a planar microcavity with its active region containing a single Transitional Metal Dichalcogenide (TMD) monolayer, taking into account excitonic and photonic spin-orbit coupling. We consider the radial propagation of polaritons in presence of disorder. We show that the reduction of the disorder scattering induced by the formation of polariton states allows to observe an optical Valley Hall effect, namely the coherent precession of the locked valley and polarization pseudospins leading to the formation of spatial valley-polarized domai…
Pseudorelativistic Dirac quasiparticles have emerged in a plethora of artificial graphene systems that mimic the underlying honeycomb symmetry of graphene. However, it is notoriously difficult to manipulate their properties without modifying the lattice structure. Here we theoretically investigate polaritons supported by honeycomb metasurfaces and, despite the trivial nature of the resonant elements, we unveil rich Dirac physics stemming from a non-trivial winding in the light-matter interaction. The metasurfaces simultaneously exhibit two distinct species of massless Dirac polaritons, namely …
Multidimensional coherent spectroscopy directly unravels multiply excited states that overlap in a linear spectrum. We report multidimensional coherent optical photocurrent spectroscopy in a semiconductor polariton diode and explore the excitation ladder of cavity polaritons. We measure doubly and triply avoided crossings for pairs and triplets of exciton-polaritons, demonstrating the strong coupling between light and dressed doublet and triplet semiconductor excitations. These results demonstrate that multiply excited excitonic states strongly coupled to a microcavity can be described as two …
The Rabi oscillations of a coupled spin-photon system are experimentally studied using time domain microwave transmission measurements. An external magnetic bias field is applied to control the amplitude and frequency of Rabi oscillations, which are a measure of the coherent spin-photon energy exchange and coupling strength respectively. The amplitude and frequency control is described in the time domain as the transient response of a two-level spin-photon system. This approach reveals the link between steady state and transient behaviour of the cavity-magnon-polariton, which is necessary to i…
A signature of the scattering between microcavity polaritons and longitudinal optical phonons has been observed in the electroluminescence spectrum of an intersubband device operating in the light-matter strong coupling regime. By electrical pumping we resonantly populate the upper polariton branch at different energies as a function of the applied bias. The electroluminescent signal arising from these states is seconded by a phonon replica from the lower branch.
We study the topological structure of matter-light excitations, so called polaritons, in a quantum spin Hall insulator coupled to photonic cavity modes. We identify a topological invariant in the presence of time reversal (TR) symmetry, and demonstrate the existence of a TR-invariant topological phase. We find protected helical edge states with energies below the lower polariton branch and characteristic uncoupled excitonic states, both detectable by optical techniques. Applying a Zeeman field allows us to relate the topological index to the double coverage of the Bloch sphere by the polariton…
We are interested in the emission characteristics of an atom interacting with the polaritonic excitations of a semiconductor or insulator embedded in a one-mode cavity. Since polaritons inside of the cavity exhibit intrinsic squeezing, we discuss how the squeezed polariton ground state modifies the atomic emission and how an indirect evidence of polariton squeezing outside of he cavity may be obtained.
The elementary optical excitations of a two-dimensional electron system strongly coupled to a microcavity are trion-polaritons. Using a variational approach, we demonstrate that the competition between Coulomb interaction and light-matter coupling plays a crucial role in determining the lowest-energy orbital and spin properties of trion-polaritons. When the light-matter interaction exceeds the bare trion binding, singlet and triplet trion states are mixed due to a cavity-mediated spin-orbit effect, which in turn results in a strong increase of the outer electron Bohr radius. In this strong cav…
We consider a semiconductor polymer chain coupled to a single electromagnetic mode in a cavity. The excitations of the chain have a mixed exciton-photon character and are described as polaritons. Polaritons are coupled to the lattice by the deformation potential interaction and can propagate in the chain. We find that the presence of optical excitation in the polymer induces strain on the lattice. We use a BCS variational wavefunction to calculate the chemical potential of the polaritons as a function of their density. We analyze first the case of a short chain with only two unit cells in orde…
Through a non-perturbative quantum theory, we investigate how the quasi-electron excitations of a two-dimensional electron gas are modified by strong coupling to the vacuum field of a microcavity. We show that the electronic dressed states originate from a Fano-like coupling between the bare electron states and the continuum of intersubband cavity polariton excitations. In particular, we calculate the electron spectral function modified by light-matter interactions and its impact on the electronic injection of intersubband cavity polaritons. The domain of validity of the present theoretical re…
We have theoretically and experimentally investigated the dispersion of the cavity-magnon-polariton (CMP) in a 1D configuration, created by inserting a low damping magnetic insulator into a high-quality 1D microwave cavity. By simplifying the full-wave simulation based on the transfer matrix approach in the long wavelength limit, an analytic approximation of the CMP dispersion has been obtained. The resultant coupling strength of the CMP shows different dependence on the sample thickness as well as the permittivity of the sample, determined by the parity of the cavity modes. These scaling effe…
In this work we present a tight-binding model that allows to describe with a minimal amount of parameters the band structure of exciton-polariton lattices. This model based on $s$ and $p$ non-orthogonal photonic orbitals faithfully reproduces experimental results reported for polariton graphene ribbons. We analyze in particular the influence of the non-orthogonality, the inter-orbitals interaction and the photonic spin-orbit coupling on the polarization and dispersion of bulk bands and edge states.
We study the spectrum of a one-dimensional Kitaev chain placed in a microwave cavity. In the off-resonant regime, the frequency shift of the cavity can be used to identify the topological phase transition of the coupled system. In the resonant regime, the topology of the system can be controlled via the microwave cavity occupation and, moreover, for a large number of photons (classical limit), the physics becomes similar to that of periodically-driven systems (Floquet insulators). We also analyze numerically a finite chain and show the existence of a degenerate subspace in the presence of the …
The dynamics of arbitrary-order quantum correlations in a cavity magnon-polariton system are investigated based on the quantum master equation in the coherent state representation. The phenomena of Rabi-like oscillation and level repulsion of the average cavity-photon number agree remarkably well with existing experimental observations. The competing nature of coherent and incoherent components in these two cases is further revealed by the second-order quantum coherence of the cavity photons and magnons, which can be systematically tuned by the driving microwave and thermal bath. Our results d…
We present the general kinetic formalism for the description of spin and energy relaxation of the cavity polaritons in the framework of the Born-Markov approximation. All essential mechanisms of polaritons redistribution in reciprocal space together with final state bosonic stimulation are taken into account, from our point of view. The developed theory is applied to describe our experimental results on the polarization dynamics obtained in the polariton parametric amplifier geometry (pumping at so-called magic angle). We have experimentally confirmed that the anisotropy of the polariton-polar…
We present a full analysis of the mode spectrum in a cavity formed by two parallel plates, one of which is a magneto-dielectric, e.g. a metamaterial, while the other one is metallic, and obtain dispersion relations in closed form. The optical properties of the cavity walls are described in terms of realistic models for the effective permittivity and the permeability. Surface polaritons, i.e. electromagnetic modes that have at least partly an evanescent character, are shown to dominate the Casimir interaction at small separations. We analyze in detail the s-polarized polaritons, which are a cha…
