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arXiv:1308.3588 · Physical Review A

Interactions in dye-microcavity photon condensates and the prospects for their observation

Robert A. Nyman, Marzena Hanna Szymańska

Published Mar 24, 2014• 44 citations
arXivHTMLPDF

Abstract

We derive the equation of motion for a Bose-Einstein condensate of photons in a dye-microcavity system, starting from Maxwell's equations. Our theory takes into account mirror shape, Kerr-type intensity-dependent refractive index and incoherent pumping and loss. The resulting equation is remarkably similar to the Gross-Pitaevskii equation for exciton-polariton condensates, despite the different microscopic origins. We calculate the incoherent photoluminescence spectrum of the photon condensate, which shows the Bogoliubov-type excitations around the mean field at thermal equilibrium. Both open- and closed-system models are presented to account for, respectively dissipation and inhomogeneities. Considering realistic parameters and experimental resolution, we estimate that by observing the angle-resolved spectrum of incoherent photoluminescence it is possible to resolve dimensionless interaction parameters of order ${10}^{\ensuremath{-}5}$, two orders of magnitude below current estimates. Thus we expect that this technique will lead to accurate measurements of the interactions in photon condensates.

DOI
10.1103/physreva.89.033844

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We derive the equation of motion for a Bose-Einstein condensate of photons in a dye-microcavity system, starting from Maxwell's equations. Our theory takes into account mirror shape, Kerr-type intensity-dependent refractive index and incoherent pumping and loss. The resulting equation is remarkably similar to the Gross-Pitaevskii equation for exciton-polariton condensates, despite the different microscopic origins. We calculate the incoherent photoluminescence spectrum of the photon condensate, which shows the Bogoliubov-type excitations around the mean field at thermal equilibrium. Both open- and closed-system models are presented to account for, respectively dissipation and inhomogeneities. Considering realistic parameters and experimental resolution, we estimate that by observing the angle-resolved spectrum of incoherent photoluminescence it is possible to resolve dimensionless interaction parameters of order 10\ensuremath−5{10}^{\ensuremath{-}5}10\ensuremath−5, two orders of magnitude below current estimates. Thus we expect that this technique will lead to accurate measurements of the interactions in photon condensates.
Superfluidity and Bose–Einstein condensation are usually considered as two closely related phenomena. Indeed, in most macroscopic quantum systems, like liquid helium, ultracold atomic Bose gases, and exciton-polaritons, condensation and superfluidity occur in parallel. In photon Bose–Einstein condensates realized in the dye microcavity system, thermalization does not occur by direct interaction of the condensate particles as in the above described systems, i.e. photon–photon interactions, but by absorption and re-emission processes on the dye molecules, which act as a heat reservoir. Currently, there is no experimental evidence for superfluidity in the dye microcavity system, though effective photon interactions have been observed from thermo-optic effects in the dye medium. In this work, we theoretically investigate the implications of effective thermo-optic photon interactions, a temporally delayed and spatially non-local effect, on the photon condensate, and derive the resulting Bogoliubov excitation spectrum. The calculations suggest a linear photon dispersion at low momenta, fulfilling the Landau's criterion of superfluidity. We envision that the temporally delayed and long-range nature of the thermo-optic photon interaction offer perspectives for novel quantum fluid phenomena.
We have observed momentum- and position-resolved spectra and images of the photoluminescence from thermalized and condensed dye-microcavity photons. The spectra yield the dispersion relation and the potential energy landscape for the photons. From this dispersion relation, below condensation threshold, we find that the effective mass is that of a bare cavity photon, not a polariton. Above threshold, we place an upper bound on the dimensionless two-dimensional interaction strength of $\stackrel{\ifmmode \tilde{}\else \~{}\fi{}}{g}\ensuremath{\lesssim}{10}^{\ensuremath{-}3}$, which is compatible with existing estimates. Both photon-photon and photon-molecule interactions are weak. The temperature is found to be independent of momentum, but dependent on pump spot size, indicating that the system is ergodic but not perfectly at thermal equilibrium. Condensation always happens first in the mode with lowest potential and lowest kinetic energy, although at very high pump powers multimode condensation occurs into other modes.
A theory of Bose-Einstein condensation of light in a dye-filled optical microcavity is presented. The theory is based on the hierarchical maximum entropy principle and allows one to investigate the fluctuating behavior of the photon gas in the microcavity for all numbers of photons, dye molecules, and excitations at all temperatures, including the whole critical region. The master equation describing the interaction between photons and dye molecules in the microcavity is derived and the equivalence between the hierarchical maximum entropy principle and the master equation approach is shown. The cases of a fixed mean total photon number and a fixed total excitation number are considered, and a much sharper, nonparabolic onset of a macroscopic Bose-Einstein condensation of light in the latter case is demonstrated. The theory does not use the grand canonical approximation, takes into account the photon polarization degeneracy, and exactly describes the microscopic, mesoscopic, and macroscopic Bose-Einstein condensation of light. Under certain conditions, it predicts sub-Poissonian statistics of the photon condensate and the polarized photon condensate, and a universal relation takes place between the degrees of second-order coherence for these condensates. In the macroscopic case, there appear a sharp jump in the degrees of second-order coherence, a sharp jump and kink in the reduced standard deviations of the fluctuating numbers of photons in the polarized and whole condensates, and a sharp peak, a cusp, of the Mandel parameter for the whole condensate in the critical region. The possibility of nonclassical light generation in the microcavity with the photon Bose-Einstein condensate is predicted.
Based on the Lindblad master equation approach we obtain a detailed microscopic model of photons in a dye-filled cavity, which features condensation of light. To this end we generalise a recent non-equilibrium approach of Kirton and Keeling such that the dye-mediated contribution to the photon–photon interaction in the light condensate is accessible due to an interplay of coherent and dissipative dynamics. We describe the steady-state properties of the system by analysing the resulting equations of motion of both photonic and matter degrees of freedom. In particular, we discuss the existence of two limiting cases for steady states: photon Bose–Einstein condensate and laser-like. In the former case, we determine the corresponding dimensionless photon–photon interaction strength by relying on realistic experimental data and find a good agreement with previous theoretical estimates. Furthermore, we investigate how the dimensionless interaction strength depends on the respective system parameters.
In this thesis we study Bose-Einstein condensation of photons. In Chapter 1 we describe the current experimental set-up and we explain the two important features of the Bose-Einstein condensate of light: dissipation through the interaction with the external reservoir of dye molecules and driving by the external pumping. In Chapter 2 we use the Schwinger-Keldysh formalism to describe the complete time evolution of the light. We show that the finite-lifetime effects of the photons due to the interaction with the dye can be characterized by a single dimensionless parameter, that depends on the power of the external laser pumping the dye. We also determine spectral functions and collective modes of the photon gas in both the normal and the Bose-Einstein condensed phases. In Chapter 3 we demonstrate that the finite-lifetime effects on the spatial first-order correlation functions of the condensed light are negligible, but are important for the temporal first-order correlations. Furthermore, we show that in the normal state the first-order correlations of the photons are suppressed by the interaction with the dye. In Chapter 4 we develop a model to describe the effect of interactions on the number fluctuations in Bose-Einstein condensates. We find good agreement between the observed number fluctuations in the light Bose-Einstein condensate and the results of our model for different interaction strenghts. In Chapter 5 we propose an experiment to observe phase diffusion in the Bose-Einstein condensate of photons and we predict the outcome of individual measurements. In our model we incorporate quantum and thermal fluctuations as well as the finite-lifetime effects. In Chapter 6 we investigate the light in the presence of a periodic potential and we study the transition from a superfluid to a Mott-insulator. We demonstrate that in this system the true Mott-insulating state is longer present due the interactions with the dye molecules. Finally, in Chapter 7 we consider Bose-Einstein condensation of light in nano-fabricated semiconductor microcavities. We demonstrate that in this system there is also a single dimensionless damping parameter that depends on the external pumping. We propose to use the experimental freedom to investigate the superfluidity of the photons via the excitation of scissors modes. We determine the frequency and damping of these scissors modes. We also calculate the density-density correlations of the excited light fluid and we show that this contains a signature of the dynamical Casimir effect.
In this paper, a mathematical model for photon condensation in an optical microcavity is considered based on Gross-Pitaevskii equation. The interaction of photons with fluorescent dye molecules in an optical microcavity resembles electron-ion interaction in a periodic lattice. The system is modelled analogous to Kronig-Penney model for electrons in a one-dimensional periodic lattice. The laser used as the light source gives rise to nonlinearity due to the deformation of electron orbits in the fluorescent dye. To accommodate the optical Kerr effect which arises due to this nonlinear interaction, the resultant Schrödinger equation is modified, which assumes the form of Gross-Pitaevskii equation. The model is validated using equation of state, whose virial coefficients can be evaluated from grand canonical ensemble scheme taking into account the interaction between photons and fluorescent dye molecules.