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arXiv:2411.14838 · Physical Review Letters

Thermodynamics and State Preparation in a Two-State System of Light

Christian Kurtscheid, Andreas Redmann, Frank Vewinger, Julian Schmitt, Martin Weitz

Published Sep 30, 2025• 1 citation
arXivHTMLPDF

Abstract

The coupling of two-level quantum systems to the thermal environment is a fundamental problem with applications of such usually single-particle or fermionic systems ranging from qubit state preparation to spin models. The present Letter studies the elementary problem of the thermodynamics of an ensemble of bosons populating a two-level system. Using an optical dye microcavity platform, we thermalize photons in a two-mode system at conditions of tunable chemical potential, demonstrating the statistical mechanical problem of N bosons populating a two-level system, coupled to a heat bath. Under pulsed excitation, we observe Josephson oscillations between the two quantum states, which verifies the possibility for coherent manipulation. In contrast, under stationary conditions, the thermalization of the two-mode system is observed, arising from radiative coupling of photons to the dye. As the energetic splitting between eigenstates is 2 orders of magnitude smaller than thermal energy, at low occupations, an almost equal distribution of the occupation of the modes is observed, as expected from Boltzmann statistics. For larger occupation, we observe efficient population of the ground state and saturation of the upper level at high filling, expected from quantum statistics. Our experiment holds promise for state preparation in quantum technologies as well as for quantum thermodynamics studies.

DOI
10.1103/kynj-l87s

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The coupling of two-level quantum systems to the thermal environment is a fundamental problem with applications of such usually single-particle or fermionic systems ranging from qubit state preparation to spin models. The present Letter studies the elementary problem of the thermodynamics of an ensemble of bosons populating a two-level system. Using an optical dye microcavity platform, we thermalize photons in a two-mode system at conditions of tunable chemical potential, demonstrating the statistical mechanical problem of N bosons populating a two-level system, coupled to a heat bath. Under pulsed excitation, we observe Josephson oscillations between the two quantum states, which verifies the possibility for coherent manipulation. In contrast, under stationary conditions, the thermalization of the two-mode system is observed, arising from radiative coupling of photons to the dye. As the energetic splitting between eigenstates is 2 orders of magnitude smaller than thermal energy, at low occupations, an almost equal distribution of the occupation of the modes is observed, as expected from Boltzmann statistics. For larger occupation, we observe efficient population of the ground state and saturation of the upper level at high filling, expected from quantum statistics. Our experiment holds promise for state preparation in quantum technologies as well as for quantum thermodynamics studies.
We investigate thermodynamic properties of a two-dimensional photon gas confined by a dye-filled optical microcavity. A thermally equilibrated state of the photon gas is achieved by radiative coupling to a heat bath that is realized with dye molecules embedded in a polymer at room temperature. The chemical potential of the gas is freely adjustable. The optical microcavity consisting of two curved mirrors induces both a non-vanishing effective photon mass and a harmonic trapping potential for the photons. While previous experiments of our group have used liquid dye solutions, the measurements described here are based on dye molecules incorporated into a polymer host matrix. The solid state material allows a simplified operation of the experimental scheme. We furthermore describe studies of fluorescence properties of dye-doped polymers, and verify the applicability of Kennard–Stepanov theory in this system. In the future, dye-based solid state systems hold promise for the realization of single-mode light sources in thermal equilibrium based on Bose–Einstein condensation of photons, as well as for solar energy concentrators.
The quantum state of light plays a crucial role in a wide range of fields, from quantum information science to precision measurements. Whereas complex quantum states can be created for electrons in solid-state materials through mere cooling, optical manipulation and control builds on nonthermodynamic methods. Using an optical dye microcavity, we show that photon wave packets can be split through thermalization within a potential with two minima subject to tunnel coupling. At room temperature, photons condense into a quantum-coherent bifurcated ground state. Fringe signals upon recombination show the relative coherence between the two wells, demonstrating a working interferometer with the nonunitary thermodynamic beam splitter. Our energetically driven optical-state preparation method provides a route for exploring correlated and entangled optical many-body states.
The quantum state of light plays a crucial role in a wide range of fields, from quantum information science to precision measurements. Whereas complex quantum states can be created for electrons in solid-state materials through mere cooling, optical manipulation and control builds on nonthermodynamic methods. Using an optical dye microcavity, we show that photon wave packets can be split through thermalization within a potential with two minima subject to tunnel coupling. At room temperature, photons condense into a quantum-coherent bifurcated ground state. Fringe signals upon recombination show the relative coherence between the two wells, demonstrating a working interferometer with the nonunitary thermodynamic beam splitter. Our energetically driven optical-state preparation method provides a route for exploring correlated and entangled optical many-body states.
The trapping and cooling of photon gases in microcavities has been used to create Bose-Einstein condensates. We investigate the conditions required for condensation in dye-filled microcavities, with photon populations created either by driving a transition of the dye, or by coupling the cavity modes to a thermal photon reservoir such as sunlight. We find that the threshold pump temperature, above which condensation appears, is determined by the second law of thermodynamics. The minimum achievable threshold is that of a reversible three-level heat engine, which we show arises in the dye-pumped case, and for pumping of the modes of a two-level cavity. For a many-level cavity condensation occurs at a similar but higher temperature. Our results show that photon condensates can be produced by pumping with incoherent thermal sources, opening possibilities for coherent light generation, energy harvesting, and experimental studies of quantum heat engines.
Through trapping light in a dye-filled optical microcavity, one can engineer a gapped band structure for photons, causing them to behave as massive bosons moving in two dimensions. Repeated absorption and emission by the dye can lead to a thermal distribution and Bose- Einstein condensation. In this thesis, I study photonic condensates beyond the equilibrium thermodynamic Bose-Einstein condensation limit in three ways. First, I describe a method for fine control of the trapping potential for light allowing for future study of thermalised light in box potentials and 1D potentials as well as others, expected to show quasi-condensation and possibly superfluid behaviour, rather than ideal Bose-Einstein condensation. Second, I show how this fabrication technique has been used to define tight trapping potentials with only a few thermally accessible energy levels. In these systems, dominance of the ground- state population and build-up of coherence occur at photon numbers less than ten, raising interesting questions about how to define condensation. I discuss these questions through the relevant chapter. Third, pulsed-pump experiments show interesting temporal dynamics including jitter in the formation time of a condensate after a pump pulse due to the stochastic nature of the emission processes involved. I show how the non-stationary two-time correlation function g(2)(t1, t2) is a powerful tool for characterising these temporal dynamics and I interpret the results in a more general framework of the evolution of a probability density function through an effective free energy landscape, driven by drift terms and stochastic forces.
We review recent experiments on the Bose-Einstein condensation of photons in a dye-filled optical microresonator. The most well-known example of a photon gas, photons in blackbody radiation, does not show Bose-Einstein condensation. Instead of massively populating the cavity ground mode, photons vanish in the cavity walls when they are cooled down. The situation is different in an ultrashort optical cavity imprinting a low-frequency cutoff on the photon energy spectrum that is well above the thermal energy. The latter allows for a thermalization process in which both temperature and photon number can be tuned independently of each other or, correspondingly, for a nonvanishing photon chemical potential. We here describe experiments demonstrating the fluorescence-induced thermalization and Bose-Einstein condensation of a two-dimensional photon gas in the dye microcavity. Moreover, recent measurements on the photon statistics of the condensate, showing Bose-Einstein condensation in the grand-canonical ensemble limit, will be reviewed. Introduction Quantum statistical effects become relevant when a gas of particles is cooled, or its density is increased, to the point where the associated de Broglie wavepackets spatially overlap. For particles with integer spin (bosons), the phenomenon of Bose-Einstein condensation (BEC) then leads to macroscopic occupation of a single quantum state at finite temperatures [1]. Bose-Einstein condensation in the gaseous case was first achieved in 1995 by laser and subsequent evaporative cooling of a dilute cloud of alkali atoms [2, 3, 4], as detailed in Chapter 3 of this volume. The condensate atoms can be described by a macroscopic singleparticle wavefunction, similar to the case of liquid helium [1]. Bose-Einstein condensation has also been observed for exciton-polaritons, which are hybrid states of matter and light [5, 6, 7] (see Chapter 4), magnons [8] (see Chapter 25), and other physical systems. Other than material particles, photons usually do not show Bose-Einstein condensation [9]. In blackbody radiation, the most common Bose gas, photons at low temperature disappear, instead of condensing to a macroscopically occupied ground-state mode. In this system, photons have a vanishing chemical potential, meaning that the number of photons is determined by the available thermal energy and cannot be tuned independently from temperature.