The quest to realize strongly interacting photons remains an outstanding challenge both for fundamental science and for applications. Here, we explore mediated photon-photon interactions in a highly imbalanced two-component mixture of exciton polaritons in a semiconductor microcavity. Using a theory that takes into account nonperturbative correlations between the excitons as well as strong light-matter coupling, we demonstrate the high tunability of an effective interaction between quasiparticles formed by minority component polaritons interacting with a Bose-Einstein condensate (BEC) of a majority component polaritons. In particular, the interaction, which is mediated by sound modes in the BEC can be made strong enough to support a bound state of two quasiparticles. Since these quasiparticles consist partly of photons, this in turn corresponds to a dimer state of photons propagating through the BEC. This gives rise to a new light transmission line where the dimer wave function is directly mapped onto correlations between the photons. Our findings open new routes for highly nonlinear optical materials and novel hybrid light-matter quantum systems.
The quest to realize strongly interacting photons remains an outstanding challenge both for fundamental science and for applications. Here, we explore mediated photon-photon interactions in a highly imbalanced two-component mixture of exciton polaritons in a semiconductor microcavity. Using a theory that takes into account nonperturbative correlations between the excitons as well as strong light-matter coupling, we demonstrate the high tunability of an effective interaction between quasiparticles formed by minority component polaritons interacting with a Bose-Einstein condensate (BEC) of a majority component polaritons. In particular, the interaction, which is mediated by sound modes in the BEC can be made strong enough to support a bound state of two quasiparticles. Since these quasiparticles consist partly of photons, this in turn corresponds to a dimer state of photons propagating through the BEC. This gives rise to a new light transmission line where the dimer wave function is directly mapped onto correlations between the photons. Our findings open new routes for highly nonlinear optical materials and novel hybrid light-matter quantum systems.
Bose-Einstein condensation (BEC) is a thermodynamic phase transition of an interacting Bose gas. Its key signatures are remarkable quantum effects like superfluidity and a phonon-like Bogoliubov excitation spectrum, which have been verified for atomic BECs. In the solid state, BEC of exciton-polaritons has been reported. Polaritons are strongly coupled light-matter quasiparticles in semiconductor microcavities and composite bosons. However, they are subject to dephasing and decay and need external pumping to reach a steady state. Accordingly the polariton BEC is a nonequilibrium process of a degenerate polariton gas in self-equilibrium, but out of equilibrium with the baths it is coupled to and therefore deviates from the thermodynamic phase transition seen in atomic BECs. Here we show that key signatures of BEC can even be observed without fulfilling the self-equilibrium condition in a highly photonic quantum degenerate nonequilibrium system.
The hybridization of light and matter excitations in the form of polaritons has enabled major advances in understanding and controlling optical nonlinearities. Entering the quantum regime of strong interactions between individual photons has, however, remained challenging since the strength of achievable polariton interactions is typically limited by the available interactions in the material. Here, we investigate collisions between dark-state polaritons in three-level systems and discover a resonant process that yields effective interactions, which are much larger than the underlying interaction between their matter constituents. We systematically investigate the underlying mechanism and demonstrate a substantial enhancement of polariton interactions by several orders of magnitude. This suggests a promising approach to quantum nonlinear optics in a range of physical settings, from atomic gases to excitons in semiconductors and two-dimensional bilayer materials.
Strong light-matter coupling gives rise to polaritons - hybrid excitations whose mixed photonic and matter character enables control over optical, electronic and chemical properties. This Feature Article surveys the main architectures supporting polariton formation, including photonic microcavities, plasmonic nanostructures, open cavities and metasurfaces, and outlines how inorganic semiconductors, organic aggregates and hybrid systems access strong and ultrastrong coupling. Key phenomena such as coherent dynamics, vibronic interactions, dark-state reservoirs and polariton-mediated energy and electron transport are discussed, together with the experimental and theoretical tools used to study them. We highlight examples where strong coupling modifies charge transport, energy flow and chemical reactivity, and we summarize emerging regimes, including intermediate and dark-strong coupling, that broaden the landscape of hybrid light-matter physics.
BEC of exciton-polaritons and related effects such as superfluidity1,2, spontaneous symmetry breaking3,4 and quantised vortices5,6 open way to creation of novel light sources7 and optical logic elements8. Remarkable observations of exciton-polariton BEC in microcavities9-12 have been reported in the recent ten years. Very recently, thermalisation and subsequent condensation of cavity photons in a dye-filled microcavity have been observed13. Here we show that BEC of both exciton-polaritons and photons can be created in the same system under different optical excitation conditions. A dynamic phase transition between a photon and a polariton BEC takes place after a single high-power excitation pulse and we find both condensed states in thermal equilibrium with the excited states. At the crossover, photons and polaritons coexist, which results in a decrease in the long-range spatial coherence. Build-up and successive depinning of polarisation is observed at the threshold of both polariton and photon condensation.
We develop a many-body theory for the properties of exciton-polaritons interacting strongly with a Bose-Einstein condensate (BEC) of exciton-polaritons in another spin state. Interactions lead to the presence of a two-body bound state, the biexciton, giving rise to a Feshbach resonance in the polariton spectrum when its energy is equal to that of two free polaritons. Using the minimal set of terms to describe this resonance, our theory recovers the main findings of two experiments probing interaction effects for upper and lower polaritons in a BEC. This strongly supports that Feshbach physics has, indeed, been realized, and we furthermore extract the energy and decay of the biexciton from the experimental data. The decay rate is predicted to be much larger than that coming from its dissociation into two free polaritons, indicating that other decay channels are important.
Bose-Einstein condensates of exciton-polaritons in inorganic semiconductor microcavities are known to possess strong interparticle interactions attributed to their excitonic component. The interactions play a crucial role in the nonlinear dynamics of such systems and can be witnessed as the high energy shift of polariton states. However, the localised nature of Frenkel excitons in strongly coupled organic microcavities precludes interparticle Coulomb exchange-interactions that affect nonlinear dynamics and change mechanisms of polariton energy shifts accordingly. We have scrutinized the origins of energy shifts in connection with nonlinear dynamics in Frenkel exciton-polariton condensates and examined the possible contributions: intracavity optical Kerr-effect, gain-induced frequency pulling, polariton interactions and effects related to saturation of optical transitions for "dark"- and "bright" molecules [1]. Unlike the conventional strongly coupled semiconductor microcavities, we have shown that nonlinear interactions within the condensate do not rely on polariton interactions but instead originated from Pauli-blocking principle forbidding double excitation of the same molecular states. We have developed a theoretical model explaining the omnipresent energy shift of the condensate wavefunction together with its spectral and polarization features at the BEC transition in a consistent way. The crucial role of intermolecular energy transfer and “dark” exciton reservoir has been demonstrated for the first time. We believe the principles explored in this work are relevant to other systems exhibiting strong coupling of Frenkel excitons with a cavity mode, regardless of a cavity type, whether one dealing with Fabry-Perot cavities or plasmonic nanocavities etc and; therefore, provide general insight on nonlinear phenomena in composite light-matter condensates. [1] T. Yagafarov, D. Sannikov, A. Zasedatelev, K. Georgiou, A. Baranikov, O. Kyriienko, I. Shelykh, L. Gai, Z. Shen, D. G. Lidzey, P. Lagoudakis, Mechanisms of blueshifts in organic polariton condensates, Commun Phys 3, 18 (2020). https://doi.org/10.1038/s42005-019-0278-6