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 cavity coupling regime, the trion-polariton consists of an exciton-polariton surrounded by a weakly bound electron and is reminiscent of a coherent Rydberg excitation.
We theoretically investigate the nonlinearity of trion-polaritons in a two-dimensional material that arises from Coulomb interaction between quasiparticles. To evaluate the interaction constant, we solve a three-body Wannier equation precisely by expanding trion wavefunctions into a Gaussian basis. Using these wavefunctions, we calculate the trion-polariton interaction energies for the exchange processes, resolving the outstanding question of trion-trion scattering. We find that the nonlinearity is the result of the competition between different scattering channels. Such a cancellation effect …
We study a 2D system of trion-polaritons at the quantum level and demonstrate that for monolayer semiconductors they can exhibit a strongly nonlinear optical response. The effect is due to the composite nature of trion-based excitations resulting in their nontrivial quantum statistical properties, and enhanced phase space filling effects. We present the full quantum theory to describe the statistics of trion-polaritons, and demonstrate that the associated nonlinearity persists at the level of few quanta, where two qualitatively different regimes of photon antibunching are present for weak and …
Highly nonlinear optical materials with strong effective photon-photon interactions (Kerr-like nonlinearity) are required in the development of novel quantum sources of light as well as for ultrafast and quantum optical signal processing circuitry. Here we report very large Kerr-like nonlinearities by employing strong optical transitions of charged excitons (trions) observed in semiconducting transition metal dichalcogenides (TMDCs). By hybridising trions in monolayer MoSe$_2$ at low electron densities with a microcavity mode, we realise trion-polaritons exhibiting significant energy shifts at…
We present a many-body theory for exciton-trion-polaritons in doped two-dimensional materials. Exciton-trion-polaritons are robust coherent hybrid excitations involving excitons, trions, and photons. Signatures of these polaritons have been recently seen in experiments. In these polaritons, the 2-body exciton states are coupled to the material ground state via exciton-photon interaction and the 4-body trion states are coupled to the exciton states via Coulomb interaction. The trion states are not directly optically coupled to the material ground state. The energy-momentum dispersion of these p…
We theoretically investigate the trion-polariton and the effects of a two-dimensional electron gas on its single particle properties. Focussing on the trion and exciton transitions, we set up an effective model and calculate the optical absorption of the quantum well containing the 2DEG. Including the light-matter coupling, we compute the Rabi splitting and polariton lineshapes as a function of 2DEG density. The role of finite temperature is investigated. The spatial extent of the trion-polariton is also calculated. We find a substantial charge build-up at short distances as long as the Rabi f…
Using the composite boson (coboson) many-body formalism, we determine under which conditions "trion-polariton" can exist. Dipolar attraction can bind an exciton and an electron into a trion having an energy well separated from the exciton energy. Yet, the existence of long-lived "trion-polariton" is a priori implausible not only because the photon-trion coupling, which scales as the inverse of the sample volume, is vanishingly small, but mostly because this coupling is intrinsically "weak". Here, we show that a moderately dense Fermi sea renders its observation possible: on the pro side, the F…
The nature of trions and their interaction with light has remained a puzzle. The composition and dispersion of polaritons involving trions provide insights into this puzzle. Trions and excitons in doped two-dimensional (2D) materials are not independent excitations but are strongly coupled as a result of Coulomb interactions. When excitons in doped 2D materials are also strongly coupled with light inside an optical waveguide, the resulting polariton states are coherent superpositions of exciton, trion, and photon states. We realize these exciton-trion-polaritons by coupling an electron-doped m…
Transition metal dichalcogenides represent an ideal testbed to study excitonic effects, spin-related phenomena and fundamental light-matter coupling in nanoscopic condensed matter systems. In particular, the valley degree of freedom, which is unique to such direct band gap monolayers with broken inversion symmetry, adds fundamental interest in these materials. Here, we implement a Tamm-plasmon structure with an embedded MoSe2 monolayer and study the formation of polaritonic quasi-particles. Strong coupling conditions between the Tamm-mode and the trion resonance of MoSe2 are established, yield…
Highly nonlinear Moiré exciton and trion polaritons
Laboratory for Physical Sciences, University of Maryland（马里兰大学物理科学实验室）；University of Rochester（罗切斯特大学）；University of Notre Dame（圣母大学）；The Institute of Optics, University of Rochester（罗切斯特大学光学研究所）
We develop a theoretical description of Coulomb interactions between trions (charged excitons) that define a nonlinear optical response in doped two-dimensional semiconductors. First, we formulate a microscopic theory of trion-trion interactions based on composite nature of these particles, and account for all possible exchange processes. Next, we calculate numerically the trion binding energies and corresponding three-body wavefunctions using a basis set with high expressivity. Then, using the obtained wavefunctions we calculate the matrix elements of two-trion scattering, and compare the con…
Monolayer transition metal dichalcogenides, known for exhibiting strong excitonic resonances, constitute a very interesting and versatile platform for investigation of light-matter interactions. In this work we report on a strong coupling regime between excitons in monolayer WSe2 and photons confined in an open, voltage-tunable dielectric microcavity. The tunability of our system allows us to extend the exciton-polariton state over a wide energy range and, in particular, to bring the excitonic component of the lower polariton mode into resonance with other excitonic transitions in monolayer WS…
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…
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 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 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…
We describe a design to implement a two-qubit geometric phase gate, by which a pair of electrons confined in adjacent quantum dots are entangled. The entanglement is a result of the Coulomb exchange interaction between the optically excited exciton-polaritons and the localized spins. This optical coupling, resembling the electron-electron Ruderman-Kittel-Kasuya-Yosida (RKKY) inter- actions, offers high speed, high fidelity two-qubit gate operation with moderate cavity quality factor Q. The errors due to the finite lifetime of the polaritons can be minimized by optimizing the optical pulse para…
Realising strong photon-photon interactions in a solid-state setting is a major goal with far reaching potential for optoelectronic applications. Using Landau's quasiparticle framework combined with a microscopic many-body theory, we explore the interactions between exciton-polaritons and trions in a two-dimensional semiconductor injected with an electron gas inside a microcavity. We show that particle-hole excitations in the electron gas mediate an attractive interaction between the polaritons, whereas a trion-polariton interaction mediated by the exchange of an electron is either repulsive o…
In a circuit quantum eletrodynamic system, a chain of N qubits inhomogeneously coupled to a cavity field forms a mesoscopic quasi-lattice, which is characterized by its degree of deformation from a normal lattice. This deformation is a function of the relative spacing, that is the ratio of the qubit spacing to the cavity wavelength. A polariton mode arise in the quasi-lattice as the dressed mode of the lattice excitation by the cavity photon. We show that the transition probability of the polariton mode is either enhanced or decreased compared to that of a single qubit by the deformation, givi…
We theoretically propose a biphoton entanglement-enhanced multidimensional spectroscopic technique as a probe for the dissipative polariton dynamics in the ultrafast regime. It is applied to the cavity-confined monomeric photosynthetic complex that represents a prototypical multi-site excitonic quantum aggregate. The proposed technique is shown to be particularly sensitive to inter-manifold polariton coherence between the two and one-excitation subspaces. It is demonstrated to be able to monitor the dynamical role of cavity-mediated excitonic correlations, and dephasing in the presence of phon…
We propose an all optical quantum computation scheme, with trapped electron spin qubits, using their Coulomb exchange interaction with optically excited microcavity exciton-polaritons. This paper describes a single qubit rotation, which together with two-qubit controlled-z gate presented in PRB 85, 241403(R) (2012), form a set of universal logic gates. The errors due to finite cavity lifetime and incorrect orientation of the rotation axis are minimized by optimizing pump pulse parameters. With projective homodyne phase measurement and initialization, our scheme is a promising candidate for the…
Considering two-level media in the array of weakly coupled nano-cavities, we reveal a variety of dynamical regimes, such as diffusion, self-trapping, soliton, and breathers for the wave-packets in the presence of photon tunneling processes between the next-nearest cavities. We focus our attention on the low branch (LB) bright polariton soliton formation, due to the two-body polariton-polariton scattering processes. When detuning frequency is manipulated adiabatically, the low-branch lattice polariton localized states, i.e., that are solitons and breathers evolving between photon-like and matte…
Electric dipole transitions between different cavity polariton branches or between dressed atomic states with the same excitation number are strictly forbidden in centro-symmetric systems. For doped quantum wells in semiconductor microcavities, the strong coupling between an intersubband transition in the conduction band and a cavity mode produces two branches of intersubband cavity polaritons, whose normal-mode energy splitting is tunable and can be in the terahertz region. Here, we show that, by using asymmetric quantum wells, it is possible to have allowed dipolar transitions between differ…
Semiconductor microresonators embedding quantum wells can host tightly confined and mutually interacting excitonic, optical and mechanical modes at once. We theoretically investigate the case where the system operates in the strong exciton-photon coupling regime, while the optical and excitonic resonances are parametrically modulated by the interaction with a mechanical mode. Owing to the large exciton-phonon coupling at play in semiconductors, we predict an enhancement of polariton-phonon interactions by two orders of magnitude with respect to mere optomechanical coupling: a near-unity single…
We present a microscopic semi-analytical theory for the description of organic molecules interacting strongly with a cavity mode. Exciton-vibration coupling within the molecule and exciton-cavity interaction are treated on an equal footing by employing a temperature-dependent variational approach. The interplay between strong exciton-vibration coupling and strong exciton-cavity coupling gives rise to a hybrid ground state, which we refer to as the lower polaron polariton. Explicit expressions for the ground-state wave function, the zero-temperature quasiparticle weight of the lower polaron pol…
We consider molecules confined to a microcavity whose dimensions are such that an excitation of the molecule is nearly resonant with a cavity mode. We investigate the situation where the excitation energies of the molecules are randomly distributed with a mean value of $ε_a$ and variance $σ$. For this case, we find a solution that approaches the exact result for large values of the number density $\mathscr{N}$ of the molecules. We find the conditions for the existence of the polaritonic states, as well as expressions for their energies. The polaritonic states are quite stable against disorder.…
The dynamics of a mobile quantum impurity in a degenerate Fermi system is a fundamental problem in many-body physics. The interest in this field has been renewed due to recent ground-breaking experiments with ultra-cold Fermi gases. Optical creation of an exciton or a polariton in a two-dimensional electron system embedded in a microcavity constitutes a new frontier for this field due to an interplay between cavity-coupling favoring ultra-low mass polariton formation and exciton-electron interactions leading to polaron or trion formation. Here, we present cavity spectroscopy of gate-tunable mo…
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 study theoretically the entanglement of two-photon states in the ground state of the intersubband cavity system, the so-called polariton vacuum. The system consists of a sequence of doped quantum wells located inside a microcavity and the photons can interact with intersubband excitations inside the quantum wells. Using an explicit solution for the ground state of the system, operated in the ultrastrong coupling regime, a post-selection is introduced, where only certain two-photon states are considered and analyzed for mode entanglement. We find that a fast quench of the coupling creates en…
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…
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 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 …
Strong coupling between light and the fundamental excitations of a two-dimensional electron gas (2DEG) are of foundational importance both to pure physics and to the understanding and development of future photonic nanotechnologies. Here we study the relationship between spin polarization of a 2DEG in a monolayer semiconductor, MoSe$_2$, and light-matter interactions modified by a zero-dimensional optical microcavity. We find robust spin-susceptibility of the 2DEG to simultaneously enhance and suppress trion-polariton formation in opposite photon helicities. This leads to observation of a gian…
We report the first observation of the magnon-polariton bistability in a cavity magnonics system consisting of cavity photons strongly interacting with the magnons in a small yttrium iron garnet (YIG) sphere. The bistable behaviors are emerged as sharp frequency switchings of the cavity magnon-polaritons (CMPs) and related to the transition between states with large and small number of polaritons. In our experiment, we align, respectively, the [100] and [110] crystallographic axes of the YIG sphere parallel to the static magnetic field and find very different bistable behaviors (e.g., clockwis…
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.
We apply a microscopic theory of exciton-polaritons in cavity-confined monolayer transition-metal dichalcogenides including both optical polarizations in the monolayer plane, allowing to describe how chiral cavity photons interact with the valley degrees of freedom of the active material. Upon polariton formation, the degenerate excitons inhabiting the two inequivalent valleys are shown to assume bonding and antibonding superpositions as a result of cavity-mediated intravalley interactions combined with intervalley Coulomb interactions. This is representative of a polariton-induced coherent mi…
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 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…
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…
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.
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…
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…
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…
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.
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…
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…
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.
