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arXiv:1410.5713 · Physical Review A

Thermalization kinetics of light: From laser dynamics to equilibrium condensation of photons

Julian Schmitt, Tobias Damm, David Dung, Frank Vewinger, Jan Klaers, Martin Weitz

Published Jul 27, 2015• 89 citations
arXivHTMLPDF

Abstract

We report a time-resolved study of the thermalization dynamics and the lasing to photon Bose-Einstein condensation crossover by in situ monitoring the photon kinetics in a dye microcavity. When the equilibration of the light to the dye temperature by absorption and reemission is faster than photon loss in the cavity, the optical spectrum becomes Bose-Einstein distributed and photons accumulate at low-energy states, forming a Bose-Einstein condensate. The thermalization of the photon gas and its evolution from nonequilibrium initial distributions to condensation is monitored in real time. In contrast, if photons leave the cavity before they thermalize, the system operates as a laser.

DOI
10.1103/physreva.92.011602

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We examine in detail the mechanisms behind thermalization and Bose-Einstein condensation (BEC) of a gas of photons in a dye-filled microcavity. We derive a microscopic quantum model, based on that of a standard laser, and show how this model can reproduce the behavior of recent experiments. Using the rate-equation approximation of this model, we show how a thermal distribution of photons arises. We go on to describe how the nonequilibrium effects in our model can cause thermalization to break down as one moves away from the experimental parameter values. In particular, we examine the effects of changing cavity length, and of altering the vibrational spectrum of the dye molecules. We are able to identify two measures which quantify whether the system is in thermal equilibrium. Using these, we plot ``phase diagrams'' distinguishing BEC and standard lasing regimes. Going beyond the rate-equation approximation, our quantum model allows us to investigate both the second-order coherence g(2){g}^{(2)}g(2) and the linewidth of the emission from the cavity. We show how the linewidth collapses as the system transitions to a Bose condensed state, and compare the results to the Schawlow-Townes linewidth.
Photon condensation in semiconductor microcavities is a transformative technique for engineering quantum states of light at room temperature by tailoring strong but incoherent light-matter interactions. While continuous-wave and electrical pumping offer exceptional prospects for miniaturized quantum photonic technologies, harnessing these requires conceptual advances in understanding nonequilibrium light-matter dynamics in semiconductors. We resolve this challenge through an \textit{ab initio} quantum kinetic theory capturing how Coulomb interactions of optically excited carriers and phonon scattering mediate photon thermalization and condensation in semiconductors. Our microscopic model shows that at high carrier densities, thermalization is dominated by carrier-carrier Coulomb scattering, in clear contrast to the rovibrational relaxation that governs dye-based photon condensates. The theory predicts a rich nonequilibrium phase diagram with thermal, Bose-condensed, multimode, and lasing phases, quantitatively in agreement with recent experiments. Crucially, we identify how cavity detuning controls transitions between equilibrium and gain-dominated regimes, enabling tailored design of coherent light sources. This work thus provides the foundation for semiconductor-based quantum photonic devices operating beyond conventional laser paradigms.
The experimental realization of a Bose-Einstein condensate of photons, first achieved in 2010 at Bonn University, allowed for new ways to probe the properties of condensates. For thermal light in free space the chemical potential is zero and condensation is not possible. By confining light to a microcavity, the transverse degrees of freedom behave as massive bosons which can have nonzero chemical potential. The gas of thermal photons can be brought to thermalize with a fluorescent dye though absorption and emission cycles. By pumping the dye molecules with a laser, the chemical potential can be increased and the photons will condense. \nWe have built a setup with which we can spatially and spectrally resolve the photon distribution in such a dye-filled microcavity. This allows us to study the shape and occupation of the low energy transverse modes of the cavity. We use this to investigate the thermalization process of the photon gas. A rate equation model is presented and qualitatively compared to experimental data. We find that the photon gas is not in thermal equilibrium.\nWe also investigate effective photon-photon interactions by measuring the spatial extent of the condensate. We find an effective interaction in the form of thermal lensing. As the thermal lensing depends on the interaction between the photon gas and the dye, we find that the model used for thermalization can also make good predictions about effective photon-photon interactions.
Abstract Photon condensation in semiconductor microcavities is a transformative technique for engineering quantum states of light at room temperature by tailoring strong but incoherent light-matter interactions. While continuous-wave and electrical pumping offer exceptional prospects for miniaturized quantum photonic technologies, harnessing these requires conceptual advances in understanding non-equilibrium light-matter dynamics in semiconductors. We resolve this challenge through an ab initio quantum kinetic theory capturing how Coulomb interactions of optically excited carriers and phonon scattering mediate photon thermalization and condensation in semiconductors. Our microscopic model shows that at high carrier densities, thermalization is dominated by carrier–carrier Coulomb scattering, in clear contrast to the rovibrational relaxation that governs dye-based photon condensates. The theory predicts a rich nonequilibrium phase diagram with thermal, Bose-condensed, multimode, and lasing phases, quantitatively in agreement with recent experiments. Crucially, we identify how cavity detuning controls transitions between equilibrium and gain-dominated regimes, enabling tailored design of coherent light sources. This work thus provides the foundation for semiconductor-based quantum photonic devices operating beyond conventional laser paradigms.