We develop an analytical microscopic theory to describe the polaron-polariton dispersion, formed by hybridizing excitons, photons, and phonons, and their coherent dynamics inside optical cavities. Starting from a microscopic light-matter Hamiltonian, we derive a simple analytical model by pursuing a non-perturbative treatment of the phonon and photon couplings to excitons. Within our theoretical framework, the phonons are treated as classical fields that are then quantized via the Floquet formalism. We show that, to a good approximation, the entire polaron-polariton system can be described using a band picture despite the phonons breaking translational symmetry. Our theory also sheds light on the long-lived coherent ballistic motion of exciton-polaritons with high excitonic character that propagate with group velocities lower than is expected from pure exciton-polariton bands, offering a microscopic explanation for these puzzling experimental observations.
Exciton polaritons in two-dimensional semiconductors inside microcavities are powerful platforms to explore hybrid light-matter quantum systems. Here, we study a macroscopic coherent population of the lowest energy state of polaron-polaritons, which are quasiparticles formed by the dressing of exciton polaritons by particle-hole excitations in a surrounding electron gas. Using a non-perturbative many-body theory to describe exciton-electron correlations combined with a non-equilibrium theory for the macroscopically populated state, we show that the electrons strongly affect the collective prop…
Systems supporting exciton-polaritons represent solid-state optical platforms with a strong built-in optical nonlinearity provided by exciton-exciton interactions. In conventional semiconductors with hydrogen-like excitons the nonlinearity rate demonstrates the inverse scaling with the binding energy. This makes excitons stable at room temperatures weakly interacting, which obviously limits the possibilities of practical applications of the corresponding materials for nonlinear photonics. We demonstrate experimentally and theoretically, that these limitations can be substantially softened in h…
Exciton-polaritons offer a versatile platform for realization of all-optical integrated logic gates due to the strong effective optical nonlinearity resulting from the exciton-exciton interactions. In most of the current excitonic materials there exists a direct connection between the exciton robustness to thermal fluctuations and the strength of exciton-exciton interaction, making materials with highest levels of exciton nonlinearity applicable at cryogenic temperatures only. Here, we show that strong polaronic effects, characteristic for perovskite materials, allow to overcome this limitatio…
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…
Two dimensional semiconductors provide an ideal platform for exploration of linear exciton and polariton physics, primarily due to large exciton binding energy and strong light-matter coupling. These features, however, generically imply reduced exciton-exciton interactions, hindering the realisation of active optical devices such as lasers or parametric oscillators. Here, we show that electrical injection of itinerant electrons into monolayer molybdenum diselenide allows us to overcome this limitation: dynamical screening of exciton-polaritons by electrons leads to the formation of new quasi-p…
Elementary quasi-particles in a two dimensional electron system can be described as exciton-polarons since electron-exciton interactions ensures dressing of excitons by Fermi-sea electron-hole pair excitations. A relevant open question is the modification of this description when the electrons occupy flat-bands and electron-electron interactions become prominent. Here, we perform cavity spectroscopy of a two dimensional electron system in the strong-coupling regime where polariton resonances carry signatures of strongly correlated quantum Hall phases. By measuring the evolution of the polarito…
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…
The interaction between a mobile quantum impurity and a bosonic bath leads to the formation of quasiparticles, termed Bose polarons. The elementary properties of Bose polarons, such as their mutual interactions, can differ drastically from those of the bare impurities. Here, we explore Bose polaron physics in a two-dimensional nonequilibrium setting by injecting $σ^-$ polarised exciton-polariton impurities into a bath of coherent $σ^+$ polarised polaritons generated by resonant laser excitation of monolayer MoSe$_2$ embedded in an optical cavity. By exploiting a biexciton Feshbach resonance be…
We develop a theory for light propagating in an atomic Bose-Einstein condensate in the presence of strong interactions. The resulting many-body correlations are shown to have profound effects on the optical properties of this interacting medium. For weak atom-light coupling, there is a well-defined quasiparticle, the polaron-polariton, supporting light propagation with spectral features differing significantly from the noninteracting case. The damping of the polaron-polariton depends nonmonotonically on the light-matter coupling strength, initially increasing and then decreasing. This gives ri…
Two-dimensional semiconductors inside optical microcavities have emerged as a versatile platform to explore new hybrid light-matter quantum states. The strong light-matter coupling leads to the formation of exciton-polaritons, which in turn interact with the surrounding electron gas to form quasiparticles called polaron-polaritons. Here, we develop a general microscopic framework to calculate the properties of these quasiparticles such as their energy and the interactions between them. From this, we give microscopic expressions for the parameters entering a Landau theory for the polaron-polari…
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 apply the fermion commutation technique for composite bosons to polariton-polariton scattering in semiconductor planar microcavities. Derivations are presented in a simple and physically transparent fashion. A procedure of orthogonolization of the initial and final two-exciton state wavefunctions is used to calculate the effective scattering matrix elements and the scattering rates. We show how the bosonic stimulation of the scattering appears in this full fermionic approach whose equivalence to the bosonization method is thus demonstrated in the regime of low exciton density. We find an ad…
We explore the electroluminescence efficiency for a quantum mechanical model of a large number of molecular emitters embedded in an optical microcavity. We characterize the circumstances under which a microcavity enhances harvesting of triplet excitons via reverse intersystem-crossing (R-ISC) into singlet populations that can emit light. For that end, we develop a time-local master equation in a variationally optimized frame which allows for the exploration of the population dynamics of chemically relevant species in different regimes of emitter coupling to the condensed phase vibrational bath…
Polariton lasing has recently been observed in strongly coupled crystalline anthracene microcavities. A simple model is developed describing the onset of the non-linear threshold based on a master equation including the relevant relaxation processes and employing realistic material parameters. The mechanism governing the build-up of the polariton population - namely bosonic stimulated scattering from the exciton reservoir via a vibronically assisted process - is characterized and its efficiency calculated on the basis of a microscopic theory. The role of polariton-polariton bimolecular quenchi…
We present a microscopic theory of the equilibrium polariton condensate state of a semiconductor quantum well in a planar optical cavity. The theory accounts for the adjustment of matter excitations to the presence of a coherent photon field, predicts effective polariton-polariton interaction strengths that are weaker and condensate exciton fractions that are smaller than in the commonly employed exciton-photon model, and yields effective Rabi coupling strengths that depend on the detuning of the cavity photon energy relative to the bare exciton energy. The dressed quasiparticle bands that app…
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…
Microscopic Model of Exciton Polarons in 2D Wigner Crystals
Institute for Quantum Electronics, ETH Zürich（苏黎世联邦理工学院量子电子研究所）；Institute for Theoretical Physics, ETH Zürich（苏黎世联邦理工学院理论物理研究所）；Institut für Theoretische Physik, Universität Heidelberg（海德堡大学理论物理研究所）
We investigate the microscopic description of exciton-polaritons that involves electrons, holes and photons within a two-dimensional microcavity. We show that in order to recover the simplified exciton-photon model that is typically used to describe polaritons, one must correctly define the exciton-photon detuning and exciton-photon (Rabi) coupling in terms of the bare microscopic parameters. For the case of unscreened Coulomb interactions, we find that the exciton-photon detuning is strongly shifted from its bare value in a manner akin to renormalization in quantum electrodynamics. Within the…
Recent experiments in exciton-polariton systems have provided high-precision measurements of the value of the polariton-polariton interaction constant, which is a key parameter that governs the nonlinear dynamics of polariton condensates and potentially enables quantum correlated polaritons. Yet, until now, this parameter has only been addressed theoretically using perturbative treatments or approximations that do not include the composite nature of the excitons. Here, we use a recently developed microscopic description of polaritons involving electrons, holes, and photons, where the interacti…
Several microscopic pathways have been proposed to explain the large magnetic effects observed in organic semiconductors, but identifying and characterising which microscopic process actually influences the overall magnetic field response is challenging. Pulsed electrically-detected magnetic resonance provides an ideal platform for this task as it intrinsically monitors the charge carriers of interest and provides dynamical information which is inaccessible through conventional magnetoconductance measurements. Here we develop a general time domain theory to describe the spin-dependent reaction…
It is widely assumed that photons cannot be manipulated using electric or magnetic fields. Even though hybridization of photons with electronic polarization to form exciton-polaritons has paved the way to a number of ground-breaking experiments in semiconductor microcavities, the neutral bosonic nature of these quasiparticles has severely limited their response to external gauge fields. Here, we demonstrate polariton acceleration by external electric and magnetic fields in the presence of nonperturbative coupling between polaritons and itinerant electrons, leading to formation of new quasipart…
We investigate the many-body states of exciton-polaritons that can be observed by pump-probe spectroscopy. Here, a weak-probe `spin-down' polariton is introduced into a coherent state of `spin-up' polaritons created by a strong pump. We show that the $\downarrow$ impurities become dressed by excitations of the $\uparrow$ medium, and form new polaronic quasiparticles that feature two-point and three-point many-body quantum correlations, which, in the low density regime, arise from coupling to the vacuum biexciton and triexciton states respectively. In particular, we find that these correlations…
We present a quantitative microscopic analysis of the formation of exciton-polaritons, the composite particles possessing light and material components, polariton-polariton interactions, and resonant pumping dynamics in cylindrical semiconductor micropillars. We discuss how the redistribution effect can be used in devices generating photons with non zero orbital angular momenta.
Crystals of plasmonic metal nanoparticles have intriguing optical properties. They reach the regimes of ultrastrong and deep strong light-matter coupling, where the photonic states need to be included in the simulation of material properties. We propose a quantum description of the plasmon polaritons in supercrystals that starts from the dipole and quadrupole excitations of the nanoparticle building blocks and their coupling to photons. Our model excellently reproduces results of finite difference time domain simulations. It provides detailed insight into the emergence of the polariton states.…
We develop a microscopic description of an electron-doped two-dimensional semiconductor embedded in a microcavity. Specifically, we investigate the interactions between exciton-polaritons and electrons for the case where the interactions between charges are strongly screened and the system is spin polarized. As a starting point, we obtain an analytic expression for the exciton-polariton wave function, and we relate the microscopic parameters of the light-matter system to experimentally measurable quantities, such as the Rabi coupling and the cavity photon frequency. We then derive the polarito…
We present a semi-analytic and asymptotically exact solution to the problem of phonon-induced decoherence in a quantum dot-microcavity system. Particular emphasis is placed on the linear polarization and optical absorption, but the approach presented herein may be straightforwardly adapted to address any elements of the exciton-cavity density matrix. At its core, the approach combines Trotter's decomposition theorem with the linked cluster expansion. The effects of the exciton-cavity and exciton-phonon couplings are taken into account on equal footing, thereby providing access to regimes of co…
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 in 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 ang…
Bosonic condensation of microcavity polaritons is accompanied by their relaxation from the ensemble of excited states into a single quantum state. The excess of energy is transferred to the crystal lattice that eventually involves heating of the structure. Creation of the condensate results in the local increase of the temperature which leads to the red shift of the exciton energy providing the mechanism for polariton self-trapping. By employing the driven-dissipative Gross-Pitaevskii model we predict a new type of a stable localized solution supported by the thermally-induced self-trapping in…
Université de Strasbourg, CNRS, Institut de Physique et Chimie des Matériaux de Strasbourg（斯特拉斯堡大学）；Universidad Autónoma de Madrid（马德里自治大学）；ESPCI Paris, Université PSL, CNRS, Sorbonne Université（巴黎高等物理化工大学）；Laboratoire de Physique et d’Étude des Matériaux, LPEM, UMR 8213（物质物理与研究所）
Trion polaron problem in bulk and two-dimensional materials
MIPT（莫斯科物理技术学院）；University of Iceland（冰岛大学）；Vanderbilt University（范德堡大学）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）；Universidad del País Vasco（巴斯克大学）；IKERBASQUE, Basque Foundation for Science（伊克尔巴斯基克科学基金会）
We analyzed multimode Josephson junctions with exciton-polaritons (polaritonic Josephson junctions) when several coupling mechanisms of fundamental and excited states are present. The applied method is based on Keldysh-Green function formalism and takes into account polariton pseudospin. We found that mean value of circular polarization degree in intrinsic Josephson oscillations and microscopic quantum self-trapping follow an oscillator behavior whose renormalizes due to intermode interactions. The effect of an additional transfer of particles over junction barrier occurring in multimode appro…
We present a fully microscopic approach to the transition rate of two exciton-photon polaritons. The non-trivial consequences of the polariton composite nature -- here treated exactly through a development of our composite-exciton many-body theory -- lead to results noticeably different from the ones of the conventional approaches in which polaritons are mapped into elementary bosons. Our work reveals an appealing fundamental scattering which corresponds to a photon-assisted exchange -- in the absence of Coulomb process. This scattering being dominant when one of the scattered polaritons has a…
We theoretically investigate the scenario of a semiconductor quantum well in a microcavity, where the band structure is arranged such that optically excited electron-hole pairs cannot form Coulomb-bound excitonic states. However, it is still possible to form exciton polaritons (part-light, part-matter quasiparticles), where the excitons are bound via the exchange of microcavity photons rather than via Coulomb interactions. Using a diagrammatic theory, we determine the spectral response of the semiconductor microcavity, which includes exciton-polariton resonances as well as a continuum of unbou…
Transport properties of exciton-polaritons in anisotropic quantum microcavities are considered theoretically. Microscopic symmetry of the structure is taken into account by allowing for both the longitudinal-transverse (TE-TM) and anisotropic splitting of polariton states. The splitting is equivalent to an effective magnetic field acting on polariton pseudospin, and polarization conversion in microcavities is shown to be caused by an interplay of exciton-polariton spin precession and elastic scattering. In addition, we considered the spin-dependent interference of polaritons leading to weak lo…
Organic semiconductors have the remarkable property that their optical excitation not only generates charge-neutral electron-hole pairs (excitons) but also charge-separated polaron pairs with high yield. The microscopic mechanisms underlying this charge separation have been debated for many years. Here we use ultrafast two-dimensional electronic spectroscopy to study the dynamics of polaron pair formation in a prototypical polymer thin film on a sub-20-fs time scale. We observe multi-period peak oscillations persisting for up to about 1 ps as distinct signatures of vibronic quantum coherence a…
Recently, it has been demonstrated that the absorption of moderately doped two-dimensional semiconductors can be described in terms of exciton-polarons. In this scenario, attractive and repulsive polaron branches are formed due to interactions between a photo-excited exciton and a Fermi sea of excess charge carriers. These interactions have previously been treated in a phenomenological manner. Here, we present a microscopic derivation of the electron-exciton interactions which utilizes a mixture of variational and perturbative approaches. We find that the interactions feature classical charge-…
