Observation of nonlinear response and Onsager regression in a photon Bose-Einstein condensate.

The quantum regression theorem states that the correlations of a system at two different times are governed by the same equations of motion as the single-time averages. This provides a powerful framework for the investigation of the intrinsic microscopic behaviour of physical systems by studying their macroscopic response to a controlled external perturbation. Here we experimentally demonstrate that the two-time particle number correlations in a photon Bose-Einstein condensate inside a dye-filled microcavity exhibit the same dynamics as the response of the condensate to a sudden perturbation of the dye molecule bath. This confirms the regression theorem for a quantum gas, and, moreover, demonstrates it in an unconventional form where the perturbation acts on the bath and only the condensate response is monitored. For strong perturbations, we observe nonlinear relaxation dynamics which our microscopic theory relates to the equilibrium fluctuations, thereby extending the regression theorem beyond the regime of linear response.

Frequency conversion to the telecom O-band using pressurized hydrogen.

Large-scale quantum networks rely on optical fiber networks and photons as so-called flying qubits for information transport. While dispersion and absorption of optical fibers are minimum at the infrared telecom wavelengths, most atomic and solid state platforms operate at visible or near-infrared wavelengths. Quantum frequency conversion is required to bridge these two wavelength regimes, and nonlinear crystals are currently employed for this process. Here, we report a novel approach of frequency conversion to the telecom band. This interaction is based on coherent Stokes Raman scattering (CSRS), a four-wave mixing process resonantly enhanced in a dense molecular hydrogen gas. We show the conversion of photons from 863 nm to the telecom O-band and demonstrate that the input polarization state is preserved. This process is intrinsically broadband and can be adapted to any other wavelength.

Fluctuation-Dissipation Relation for a Bose-Einstein Condensate of Photons.

For equilibrium systems, the magnitude of thermal fluctuations is closely linked to the dissipative response to external perturbations. This fluctuation-dissipation relation has been described for material particles in a wide range of fields. Here, we experimentally probe the relation between the number fluctuations and the response function for a Bose-Einstein condensate of photons coupled to a dye reservoir, demonstrating the fluctuation-dissipation relation for a quantum gas of light. The observed agreement of the scale factor with the environment temperature both directly confirms the thermal nature of the optical condensate and demonstrates the validity of the fluctuation-dissipation theorem for a Bose-Einstein condensate.

Frequency conversion in pressurized hydrogen.

State-preserving frequency conversion in the optical domain is a necessary component in many configurations of quantum information processing and communication. Thus far, nonlinear crystals are used for this purpose. Here, we report on an approach based on coherent anti-Stokes Raman scattering (CARS) in a dense molecular hydrogen gas. This four-wave mixing process sidesteps the limitations imposed by crystal properties, it is intrinsically broadband and does not generate an undesired background. We demonstrate this method by converting photons from 434 nm to 370 nm and show that their polarization is preserved.

Converting single photons from an InAs/GaAs quantum dot into the ultraviolet: preservation of second-order correlations.

Wavelength conversion at the single-photon level is required to forge a quantum network from distinct quantum devices. Such devices include solid-state emitters of single or entangled photons, as well as network nodes based on atoms or ions. Here we demonstrate the conversion of single photons emitted from a III-V semiconductor quantum dot at 853 nm via sum frequency conversion to the wavelength of the strong transition of Yb+ ions at 370 nm. We measure the second-order correlation function of both the unconverted and the converted photon and show that the single-photon character of the quantum dot emission is preserved during the conversion process.

Compressibility and the equation of state of an optical quantum gas in a box.

The compressibility of a medium, quantifying its response to mechanical perturbations, is a fundamental property determined by the equation of state. For gases of material particles, studies of the mechanical response are well established, in fields from classical thermodynamics to cold atomic quantum gases. We demonstrate a measurement of the compressibility of a two-dimensional quantum gas of light in a box potential and obtain the equation of state for the optical medium. The experiment was carried out in a nanostructured dye-filled optical microcavity. We observed signatures of Bose-Einstein condensation at high phase-space densities in the finite-size system. Upon entering the quantum degenerate regime, the measured density response to an external force sharply increases, hinting at the peculiar prediction of an infinite compressibility of the deeply degenerate Bose gas.

Sapphire optical viewport for high pressure and temperature applications.

We describe the design of a soldered sapphire optical viewport, which is useful for spectroscopic applications of samples at high temperatures and high pressures. The sapphire window is bonded via active soldering to a metal flange with a structure of two c-shaped rings made of different metallic materials in between, so as to mitigate thermally induced stress. A spectroscopic cell equipped with two of the optical viewports has been successfully operated with alkali metals in a noble gas environment at temperatures in the range of 20-450 °C at noble gas pressures from 10-6 mbar to 330 bars. In the upper pressure range, we observe a leakage rate smaller than our readout accuracy of 30 mbar per day.

Observation of a non-Hermitian phase transition in an optical quantum gas.

Quantum gases of light, such as photon or polariton condensates in optical microcavities, are collective quantum systems enabling a tailoring of dissipation from, for example, cavity loss. This characteristic makes them a tool to study dissipative phases, an emerging subject in quantum many-body physics. We experimentally demonstrate a non-Hermitian phase transition of a photon Bose-Einstein condensate to a dissipative phase characterized by a biexponential decay of the condensate's second-order coherence. The phase transition occurs because of the emergence of an exceptional point in the quantum gas. Although Bose-Einstein condensation is usually connected to lasing by a smooth crossover, the observed phase transition separates the biexponential phase from both lasing and an intermediate, oscillatory condensate regime. Our approach can be used to study a wide class of dissipative quantum phases in topological or lattice systems.

Thermally condensing photons into a coherently split state of light.

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.

First-order spatial coherence measurements in a thermalized two-dimensional photonic quantum gas.

Phase transitions between different states of matter can profoundly modify the order in physical systems, with the emergence of ferromagnetic or topological order constituting important examples. Correlations allow the quantification of the degree of order and the classification of different phases. Here we report measurements of first-order spatial correlations in a harmonically trapped two-dimensional photon gas below, at and above the critical particle number for Bose-Einstein condensation, using interferometric measurements of the emission of a dye-filled optical microcavity. For the uncondensed gas, the transverse coherence decays on a length scale determined by the thermal de Broglie wavelength of the photons, which shows the expected scaling with temperature. At the onset of Bose-Einstein condensation, true long-range order emerges, and we observe quantum statistical effects as the thermal wave packets overlap. The excellent agreement with equilibrium Bose gas theory prompts microcavity photons as promising candidates for studies of critical scaling and universality in optical quantum gases.Phase transitions in quantum matter are related to correlation effects and they can change the ordering of material. Here the authors measure the first-order spatial correlation and the de Broglie wavelength for both thermal and condensed form of a photonic Bose gas in a dye-filled optical microcavity.

Calorimetry of a Bose-Einstein-condensed photon gas.

Phase transitions, as the condensation of a gas to a liquid, are often revealed by a discontinuous behaviour of thermodynamic quantities. For liquid helium, for example, a divergence of the specific heat signals the transition from the normal fluid to the superfluid state. Apart from liquid helium, determining the specific heat of a Bose gas has proven to be a challenging task, for example, for ultracold atomic Bose gases. Here we examine the thermodynamic behaviour of a trapped two-dimensional photon gas, a system that allows us to spectroscopically determine the specific heat and the entropy of a nearly ideal Bose gas from the classical high temperature to the Bose-condensed quantum regime. The critical behaviour at the phase transition is clearly revealed by a cusp singularity of the specific heat. Regarded as a test of quantum statistical mechanics, our results demonstrate a quantitative agreement with its predictions at the microscopic level.

Spontaneous Symmetry Breaking and Phase Coherence of a Photon Bose-Einstein Condensate Coupled to a Reservoir.

We examine the phase evolution of a Bose-Einstein condensate of photons generated in a dye microcavity by temporal interference with a phase reference. The photoexcitable dye molecules constitute a reservoir of variable size for the condensate particles, allowing for grand canonical statistics with photon bunching, as in a lamp-type source. We directly observe phase jumps of the condensate associated with the large statistical number fluctuations and find a separation of correlation time scales. For large systems, our data reveal phase coherence and a spontaneously broken symmetry, despite the statistical fluctuations.

Observation of grand-canonical number statistics in a photon Bose-Einstein condensate.

We report measurements of particle number correlations and fluctuations of a photon Bose-Einstein condensate in a dye microcavity using a Hanbury Brown-Twiss experiment. The photon gas is coupled to a reservoir of molecular excitations, which serve as both heat bath and particle reservoir to realize grand-canonical conditions. For large reservoirs, we observe strong number fluctuations of the order of the total particle number extending deep into the condensed phase. Our results demonstrate that Bose-Einstein condensation under grand-canonical ensemble conditions does not imply second-order coherence.

Statistical physics of Bose-Einstein-condensed light in a dye microcavity.

We theoretically analyze the temperature behavior of paraxial light in thermal equilibrium with a dye-filled optical microcavity. At low temperatures the photon gas undergoes Bose-Einstein condensation, and the photon number in the cavity ground state becomes macroscopic with respect to the total photon number. Owing to a grand-canonical excitation exchange between the photon gas and the dye molecule reservoir, a regime with unusually large fluctuations of the condensate number is predicted for this system that is not observed in present atomic physics Bose-Einstein condensation experiments.

Bose-Einstein condensation of photons in an optical microcavity.

Bose-Einstein condensation (BEC)-the macroscopic ground-state accumulation of particles with integer spin (bosons) at low temperature and high density-has been observed in several physical systems, including cold atomic gases and solid-state quasiparticles. However, the most omnipresent Bose gas, blackbody radiation (radiation in thermal equilibrium with the cavity walls) does not show this phase transition. In such systems photons have a vanishing chemical potential, meaning that their number is not conserved when the temperature of the photon gas is varied; at low temperatures, photons disappear in the cavity walls instead of occupying the cavity ground state. Theoretical works have considered thermalization processes that conserve photon number (a prerequisite for BEC), involving Compton scattering with a gas of thermal electrons or photon-photon scattering in a nonlinear resonator configuration. Number-conserving thermalization was experimentally observed for a two-dimensional photon gas in a dye-filled optical microcavity, which acts as a 'white-wall' box. Here we report the observation of a Bose-Einstein condensate of photons in this system. The cavity mirrors provide both a confining potential and a non-vanishing effective photon mass, making the system formally equivalent to a two-dimensional gas of trapped, massive bosons. The photons thermalize to the temperature of the dye solution (room temperature) by multiple scattering with the dye molecules. Upon increasing the photon density, we observe the following BEC signatures: the photon energies have a Bose-Einstein distribution with a massively populated ground-state mode on top of a broad thermal wing; the phase transition occurs at the expected photon density and exhibits the predicted dependence on cavity geometry; and the ground-state mode emerges even for a spatially displaced pump spot. The prospects of the observed effects include studies of extremely weakly interacting low-dimensional Bose gases and new coherent ultraviolet sources.

Frequency matching in light-storage spectroscopy of atomic Raman transitions.

We investigate the storage of light in an atomic sample with a Lambda-type coupling scheme driven by optical fields at variable two-photon detuning. In the presence of electromagnetically induced transparency (EIT), light is stored and retrieved from the sample by dynamically varying the group velocity. It is found that for any two-photon detuning of the input light pulse within the EIT transparency window, the carrier frequency of the retrieved light pulse matches the two-photon resonance frequency with the atomic ground state transition and the control field. This effect which is not based on spectral filtering is investigated both theoretically and experimentally. It can be used for high-speed precision measurements of the two-photon resonance as employed, e.g., in optical magnetometry.

Instant single-photon Fock state tomography.

Heralded single photons are prepared at a rate of approximately 100 kHz via conditional measurements on polarization-nondegenerate biphotons produced in a periodically poled potassium-titanyl phosphate crystal. The single-photon Fock state is characterized using high-frequency pulsed optical homodyne tomography with a fidelity of (57.6+/-0.1)%. The state preparation and detection rates allowed us to perform on-the-fly alignment of the apparatus based on real-time analysis of the quadrature measurement statistics.

Resonance beating of light stored using atomic spinor polaritons.

We investigate the storage of light in atomic rubidium vapor using a multilevel-tripod scheme. In the system, two collective dark polariton modes exist, forming an effective spinor quasiparticle. Storage of light is performed by dynamically reducing the optical group velocity to zero. After releasing the stored pulse, a beating of the two reaccelerated optical modes is monitored. The observed beating signal oscillates at an atomic transition frequency, opening the way to novel quantum limited measurements of atomic resonance frequencies and quantum switches.

Adiabatic frequency conversion of optical information in atomic vapor.

We experimentally demonstrate a communication protocol that enables frequency conversion and routing of quantum information in an adiabatic and thus robust way. The protocol is based on electromagnetically induced transparency (EIT) in systems with multiple excited levels: transfer and/or distribution of optical states between different signal modes is implemented by adiabatically changing the control fields. The proof-of-principle experiment is performed using the hyperfine levels of the rubidium D1 line.

Time-resolved probing of the ground state coherence in rubidium.

We demonstrate the preparation and probing of the coherence between the hyperfine ground states |S(1/2),F=1> and |5S(1/2),F=2> of the Rb87 isotope. The effects of various coherence control techniques, i.e., fractional stimulated Raman adiabatic passage and coherent population return, on the coherence are investigated. These techniques are implemented using nearly degenerate pump and Stokes lasers at 795 nm (Rb D1 transition), which couple the two hyperfine ground states via the excited state |5P(1/2),F=1> through a resonant two-photon process in which a coherent superposition of the two hyperfine ground states is established. The medium is probed by an additional weak laser, which generates a four-wave mixing signal proportional to the ground state coherence and allows us to monitor its evolution in time. The experimental data are compared with numerical simulations.