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Funding: The authors acknowledge funding support from the Army Research Office, NTT Research, and the QNEXT DOE National Quantum Information Science Research Center. B.M. acknowledges funding from the Q-NEXT DOE National Quantum Information Science Research Center and the NSF Graduate Research Fellowship. Cavity quantum electrodynamics (QED) with cooperativity far greater than unity enables high-fidelity quantum sensing and information processing. The high-cooperativity regime is often reached through the use of short single-mode resonators. More complicated multimode resonators, such as the near-confocal optical Fabry-Prot cavity, can provide intracavity atomic imaging in addition to high cooperativity. This capability has recently proved important for exploring quantum many-body physics in the driven-dissipative setting. In this work, we show that a confocal-cavity–QED microscope can realize cooperativity in excess of 110. This cooperativity is on par with the very best single-mode cavities (which are far shorter) and 21 times greater than single-mode resonators of similar length and mirror radii. The 1.7-μm imaging resolution is naturally identical to the photon-mediated interaction range. We measure these quantities by determining the threshold of cavity superradiance when small optically tweezed Bose-Einstein condensates are pumped at various intracavity locations. Transmission measurements of an ex situ cavity corroborate these results. We provide a theoretical description that shows how cooperativity enhancement arises from the dispersive coupling to the atoms of many near-degenerate modes. Publisher PDF

We study how polariton condensation modifies charge transport in organic materials. In typical organic materials, charge transport proceeds via incoherent hopping. We therefore provide an approach to determine how the rate and final state of this hopping process is affected by strong matter-light coupling and polariton condensation. We show how the hopping process may create excitations when starting from a state with a finite excitation density. That is, how hopping can change the state of a lower polariton condensate by creating upper polaritons, optically inactive excitonic dark states, or by exciting vibrational sidebands. While the matrix elements for these processes can be large, for typical materials at room temperature, such excitations are suppressed by thermal factors, and ground state processes dominate. We thus study how the ground state hopping rate depends on condensate density, matter-light coupling, and cavity photon detuning. All these factors change the vibrational configuration associated with the optically active molecules, which can enhance or suppress hopping by increasing or decreasing the vibrational overlap with the state of a charged molecule. We show that hopping rates can be exponentially sensitive to detuning and condensate density, allowing an increase or decrease of hopping rate by two orders of magnitude., Comment: 21 pages, 8 figures

We study the dynamics of multimode polariton lasing in organic microcavities by using a second-order cumulant equation approach. By inspecting the time evolution of the photon mode occupations, we show that if multiple lasing peaks are observed in time-integrated mode occupations, the reason can be either bi-modal lasing or temporal switching between several modes. The former takes place within a narrow range of parameters while the latter occurs more widely. We find that the origin of the temporal switching is different in the weak- and strong-coupling regimes. At weak coupling slope efficiency is the determining factor, while for strong coupling it is changes in the eigenmodes and gain spectrum upon pumping. This difference is revealed by investigating the photoluminescence and momentum-resolved gain spectra. Our results underscore the importance of understanding the time evolution of the populations when characterizing the lasing behaviour of a multimode polariton system, and show how these features differ between weak and strong coupling., Comment: 15 pages, 13 figures

We introduce a numerical method to determine the Hamiltonian of Mean Force (HMF) Gibbs state for a quantum system strongly coupled to a reservoir. The method adapts the Time Evolving Matrix Product Operator (TEMPO) algorithm to imaginary time propagation. By comparing the real-time and imaginary-time propagation for a generalized spin-boson model, we confirm that the HMF Gibbs state correctly predicts the steady state. We show that the numerical dynamics match the polaron master equation at strong coupling. We illustrate the potential of the imaginary-time TEMPO approach by exploring reservoir-induced entanglement between qubits., Comment: 8 pages, 7 figures

Description, In a major step toward the development of a quantum battery, superabsorption has been achieved in an organic microcavity., The rate at which matter emits or absorbs light can be modified by its environment, as markedly exemplified by the widely studied phenomenon of superradiance. The reverse process, superabsorption, is harder to demonstrate because of the challenges of probing ultrafast processes and has only been seen for small numbers of atoms. Its central idea—superextensive scaling of absorption, meaning larger systems absorb faster—is also the key idea underpinning quantum batteries. Here, we implement experimentally a paradigmatic model of a quantum battery, constructed of a microcavity enclosing a molecular dye. Ultrafast optical spectroscopy allows us to observe charging dynamics at femtosecond resolution to demonstrate superextensive charging rates and storage capacity, in agreement with our theoretical modeling. We find that decoherence plays an important role in stabilizing energy storage. Our work opens future opportunities for harnessing collective effects in light-matter coupling for nanoscale energy capture, storage, and transport technologies.

We show how to simulate a model of many molecules with both strong coupling to many vibrational modes and collective coupling to a single photon mode. We do this by combining process tensor matrix product operator methods with a mean-field approximation which reduces the dimension of the problem. We analyze the steady-state of the model under incoherent pumping to determine the dependence of the polariton lasing threshold on cavity detuning, light-matter coupling strength, and environmental temperature. Moreover, by measuring two-time correlations, we study quadratic fluctuations about the mean-field to calculate the photoluminescence spectrum. Our method enables one to simulate many-body systems with strong coupling to multiple environments, and to extract both static and dynamical properties., 7 pages, 3 figures plus supplementary material

R.P. was supported by the EPSRC Scottish Doctoral Training Centre in Condensed Matter Physics (CM-CDT), Grant No. EP/L015110/1. We consider a generalized Dicke model with U(1) symmetry, which can undergo a transition to a superradiant state that spontaneously breaks this symmetry. By exploiting the difference in timescale between atomic and cavity dynamics, one may eliminate the cavity dynamics, providing an atom-only theory. We show that the standard Redfield theory cannot describe the transition to the superradiant state, but including higher-order corrections does recover the transition. Our work reveals how the forms of effective theories must vary for models with continuous symmetry, and provides a template to develop effective theories of more complex models. Publisher PDF

We introduce a near-term experimental platform for realizing an associative memory. It can simultaneously store many memories by using spinful bosons coupled to a degenerate multimode optical cavity. The associative memory is realized by a confocal cavity QED neural network, with the cavity modes serving as the synapses, connecting a network of superradiant atomic spin ensembles, which serve as the neurons. Memories are encoded in the connectivity matrix between the spins, and can be accessed through the input and output of patterns of light. Each aspect of the scheme is based on recently demonstrated technology using a confocal cavity and Bose-condensed atoms. Our scheme has two conceptually novel elements. First, it introduces a new form of random spin system that interpolates between a ferromagnetic and a spin-glass regime as a physical parameter is tuned---the positions of ensembles within the cavity. Second, and more importantly, the spins relax via deterministic steepest-descent dynamics, rather than Glauber dynamics. We show that this nonequilibrium quantum-optical scheme has significant advantages for associative memory over Glauber dynamics: These dynamics can enhance the network's ability to store and recall memories beyond that of the standard Hopfield model. Surprisingly, the cavity QED dynamics can retrieve memories even when the system is in the spin glass phase. Thus, the experimental platform provides a novel physical instantiation of associative memories and spin glasses as well as provides an unusual form of relaxational dynamics that is conducive to memory recall even in regimes where it was thought to be impossible., Comment: 35 pages, 16 figures, 6 appendices

Quantised sound waves -- phonons -- govern the elastic response of crystalline materials, and also play an integral part in determining their thermodynamic properties and electrical response (e.g., by binding electrons into superconducting Cooper pairs). The physics of lattice phonons and elasticity is absent in simulators of quantum solids constructed of neutral atoms in periodic light potentials: unlike real solids, traditional optical lattices are silent because they are infinitely stiff. Optical-lattice realisations of crystals therefore lack some of the central dynamical degrees of freedom that determine the low-temperature properties of real materials. Here, we create an optical lattice with phonon modes using a Bose-Einstein condensate (BEC) coupled to a confocal optical resonator. Playing the role of an active quantum gas microscope, the multimode cavity QED system both images the phonons and induces the crystallisation that supports phonons via short-range, photon-mediated atom-atom interactions. Dynamical susceptibility measurements reveal the phonon dispersion relation, showing that these collective excitations exhibit a sound speed dependent on the BEC-photon coupling strength. Our results pave the way for exploring the rich physics of elasticity in quantum solids, ranging from quantum melting transitions to exotic ``fractonic'' topological defects in the quantum regime., Comment: 7 pages, 4 figures; supplement with 22 pages, 6 figures

We present a general method to efficiently design optimal control sequences for non-Markovian open quantum systems, and illustrate it by optimizing the shape of a laser pulse to prepare a quantum dot in a specific state. The optimization of control procedures for quantum systems with strong coupling to structured environments -- where time-local descriptions fail -- is a computationally challenging task. We modify the numerically exact time evolving matrix product operator (TEMPO) method, such that it allows the repeated computation of the time evolution of the reduced system density matrix for various sets of control parameters at very low computational cost. This method is potentially useful for studying numerous optimal control problems, in particular in solid state quantum devices where the coupling to vibrational modes is typically strong., Comment: 6 pages, 3 figures

We present calculations of the time-evolution of the driven-dissipative XYZ model using the infinite Projected Entangled Pair Operator (iPEPO) method, introduced by [A. Kshetrimayum, H. Weimer and R. Or\'us, Nat. Commun. 8, 1291 (2017)]. We explore the conditions under which this approach reaches a steady state. In particular, we study the conditions where apparently converged calculations may become unstable with increasing bond dimension of the tensor-network ansatz. We discuss how more reliable results could be obtained., Comment: Submission to SciPost

The Peierls instability toward a charge density wave is a canonical example of phonon-driven strongly correlated physics and is intimately related to topological quantum matter and exotic superconductivity. We propose a method to realize an analogous photon-mediated Peierls transition, using a system of one-dimensional tubes of interacting Bose or Fermi atoms trapped inside a multimode confocal cavity. Pumping the cavity transversely engineers a cavity-mediated metal--to--insulator transition in the atomic system. For strongly interacting bosons in the Tonks-Girardeau limit, this transition can be understood (through fermionization) as being the Peierls instability. We extend the calculation to finite values of the interaction strength and derive analytic expressions for both the cavity field and mass gap. They display nontrivial power law dependence on the dimensionless matter-light coupling., Comment: 6 pages, 2 figures; supplement of 4 pages; published version

We present a beyond-mean-field approach to predict the nature of organic polariton lasing, accounting for all relevant photon modes in a planar microcavity. Starting from a microscopic picture, we show how lasing can switch between polaritonic states resonant with the maximal gain, and those at the bottom of the polariton dispersion. We show how the population of non-lasing modes can be found, and by using two-time correlations, we show how the photoluminescence spectrum (of both lasing and non-lasing modes) evolves with pumping and coupling strength, confirming recent experimental work on the origin of blueshift for polariton lasing., 6 pages, 4 figures, plus supplemental material

We investigate the phases of two-dimensional electron-hole systems strongly coupled to a microcavity photon field in the limit of extreme charge imbalance. Using variational wave functions, we examine the competition between different electron-hole paired states for the specific cases of semiconducting III-V single quantum wells, electron-hole bilayers, and transition metal dichalcogenide monolayers embedded in a planar microcavity. We show how the Fermi sea of excess charges modifies both the electron-hole bound state (exciton) properties and the dielectric constant of the cavity active medium, which in turn affects the photon component of the many-body polariton ground state. On the one hand, long-range Coulomb interactions and Pauli blocking of the Fermi sea promote electron-hole pairing with finite center-of-mass momentum, corresponding to an excitonic roton minimum. On the other hand, the strong coupling to the ultra-low-mass cavity photon mode favors zero-momentum pairs. We discuss the prospect of observing different types of electron-hole pairing in the photon spectrum., 18 pages, 14 figures

Strong coupling between light and matter is possible with a variety of organic materials. In contrast to the simpler inorganic case, organic materials often have a complicated spectrum, with vibrationally dressed electronic transitions. Strong coupling to light competes with this vibrational dressing, and if strong enough, can suppress the entanglement between electronic and vibrational degrees of freedom. By exploiting symmetries, we can perform exact numerical diagonalization to find the polaritonic states for intermediate numbers of molecules, and use these to define and validate accurate expressions for the lower polariton states and strong-coupling spectrum in the thermodynamic limit. Using this approach, we find that vibrational decoupling occurs as a sharp transition above a critical matter-light coupling strength. We also demonstrate how the polariton spectrum evolves with the number of molecules, recovering classical linear optics results only at large $N$., 14+3 pages, 8 figures. v3 updated to published version

We study two-dimensional charge-imbalanced electron-hole systems embedded in an optical microcavity. We find that strong coupling to photons favors states with pairing at zero or small center of mass momentum, leading to a condensed state with spontaneously broken time-reversal and rotational symmetry, and unpaired carriers that occupy an anisotropic crescent-shaped sliver of momentum space. The crescent state is favoured at moderate charge imbalance, while a Fulde--Ferrel--Larkin--Ovchinnikov-like state --- with pairing at large center of mass momentum --- occurs instead at strong imbalance. The crescent state stability results from long-range Coulomb interactions in combination with extremely long-range photon-mediated interactions., Comment: 6 pages, 4 figures, plus supplemental material

Funding: J. K. acknowledges support from SU2P. Sign-changing interactions constitute a crucial ingredient in the creation of frustrated many-body systems such as spin glasses. We present here the demonstration of a photon-mediated sign-changing interaction between Bose-Einstein-condensed atoms in a confocal cavity. The interaction between two atoms is of an unusual, nonlocal form proportional to the cosine of the inner product of the atoms’ position vectors. This interaction arises from the differing Gouy phase shifts of the cavity’s degenerate modes. The interaction drives a nonequilibrium Dicke-type phase transition in the system leading to atomic checkerboard density-wave order. Because of the Gouy phase anomalies, the checkerboard pattern can assume either a sinelike or cosinelike character. This state is detected via the holographic imaging of the cavity’s superradiant emission. Together with a companion paper [Y. Guo, V. D. Vaidya, R. M. Kroeze, R. A. Lunney, B. L. Lev, and J. Keeling, Emergent and broken symmetries of atomic self-organization arising from Gouy phases in multimode cavity QED, Phys. Rev. A 99, 053818 (2019)], we explore this interaction’s influence on superradiant phase transitions in multimode cavities. Employing this interaction in cavity QED spin systems may enable the creation of artificial spin glasses and quantum neural networks. Postprint Postprint

Optical cavities can induce photon-mediated interactions among intracavity-trapped atoms. Multimode cavities provide the ability to tune the form of these interactions, e.g., by inducing a nonlocal, sign-changing term to the interaction. By accounting for the Gouy phase shifts of the modes in a nearly degenerate, confocal, Fabry-Perot cavity, we provide a theoretical description of this interaction, along with additional experimental confirmation to complement that presented in the companion paper, Ref. [1]. Furthermore, we show that this interaction should be written in terms of a complex order parameter, allowing for a U(1)-symmetry to emerge. This symmetry corresponds to the phase of the atomic density wave arising from self-organization when the cavity is transversely pumped above a critical threshold power. We theoretically and experimentally show how this phase depends on the position of the Bose-Einstein condensate (BEC) within the cavity and discuss mechanisms that break the U(1)-symmetry and lock this phase. We then consider alternative Fabry-Perot multimode cavity geometries (i.e., beyond the confocal) and schemes with more than one pump laser and show that these provide additional capabilities for tuning the cavity-meditated interaction among atoms, including the ability to restore the U(1)-symmetry despite the presence of symmetry-breaking effects. These photon-mediated interactions may be exploited for realizing quantum liquid crystalline states and spin glasses using multimode optical cavities., Comment: 15 pages, 5 figures

We investigate how to describe the dissipative spin dynamics of the driven-dissipative Dicke model, describing $N$ two-level atoms coupled to a cavity mode, after adiabatic elimination of the cavity mode. To this end, we derive a Redfield master equation which goes beyond the standard secular approximation and large detuning limits. We show that the secular (or rotating wave) approximation and the large detuning approximation both lead to inadequate master equations, that fail to predict the Dicke transition or the damping rates of the atomic dynamics. In contrast, the full Redfield theory correctly predicts the phase transition and the effective atomic damping rates. Our work provides a reliable framework to study the full quantum dynamics of atoms in a multimode cavity, where a quantum description of the full model becomes intractable., 11 pages, 2 figures

We calculate the fluorescence spectra of a driven lattice of coupled cavities. To do this, we extend methods of evaluating two-time correlations in infinite lattices to open quantum systems; this allows access to momentum resolved fluorescence spectrum. We illustrate this for a driven-dissipative transverse field anisotropic XY model. By studying the fluctuation dissipation theorem, we find the emergence of a quasi-thermalized steady state with a temperature dependent on system parameters; for blue detuned driving, we show this effective temperature is negative. In the low excitation density limit, we compare these numerical results to analytical spin-wave theory, providing an understanding of the form of the distribution function and the origin of quasi-thermalization., Comment: 12 pages, 6 figures

Following experimental realizations of room temperature polariton lasing with organic molecules, we present a microscopic model that allows us to explore the crossover from weak to strong matter-light coupling. We consider a non-equilibrium Dicke-Holstein model, including both strong coupling to vibrational modes and strong matter-light coupling, providing the phase diagram of this model in the thermodynamic limit. We discuss the mechanism of polariton lasing, uncovering a process of self-tuning, and identify the relation and distinction between regular dye lasers and organic polariton lasers., 6 pages, 4 figures, plus supplemental material

The Dicke model describes the coupling between a quantized cavity field and a large ensemble of two-level atoms. When the number of atoms tends to infinity, this model can undergo a transition to a superradiant phase, belonging to the mean-field Ising universality class. The superradiant transition was first predicted for atoms in thermal equilibrium and was recently realized with a quantum simulator made of atoms in an optical cavity, subject to both dissipation and driving. In this Progress Report, we offer an introduction to some theoretical concepts relevant to the Dicke model, reviewing the critical properties of the superradiant phase transition, and the distinction between equilibrium and nonequilibrium conditions. In addition, we explain the fundamental difference between the superradiant phase transition and the more common lasing transition. Our report mostly focuses on the steady states of atoms in single-mode optical cavities, but we also mention some aspects of real-time dynamics, as well as other quantum simulators, including superconducting qubits, trapped ions, and using spin-orbit coupling for cold atoms. These realizations differ in regard to whether they describe equilibrium or non-equilibrium systems., Invited Progress Report; 21 pages, 6 figures

We consider the orientational alignment of dipoles due to strong matter light coupling, for a non-vanishing density of excitations. We compare various approaches to this problem in the limit of large numbers of emitters, and show that direct Monte Carlo integration, mean-field theory, and large deviation methods match exactly in this limit. All three results show that orientational alignment develops in the presence of a macroscopically occupied polariton mode, and that the dipoles asymptotically approach perfect alignment in the limit of high density or low temperature., 7 pages, 4 figures

HMC acknowledges studentship funding from EPSRC under grant no. EP/G03673X/1. PGK acknowledges support from EPSRC (EP/M010910/1). BWL acknowledges support from EPSRC (EP/K025562/1). PRE acknowledges funding from SFI (15/IACA/3402). JK acknowledges financial support from EPSRC programs “TOPNES” (EP/I031014/1) and “Hybrid-Polaritonics” (EP/M025330/1). The interaction of a quantum system with its environment causes decoherence, setting a fundamental limit on its suitability for quantum information processing. However, we show that if the system consists of coupled parts with different internal energy scales then the interaction of one part with a thermal bath need not lead to loss of coherence from the other. Remarkably, we find that the protected part can remain coherent for longer when the coupling to the bath becomes stronger or the temperature is raised. Our theory will enable the design of decoherence-resistant hybrid quantum computers. Publisher PDF

We observe the joint spin-spatial (spinor) self-organization of a two-component BEC strongly coupled to an optical cavity. This unusual nonequilibrium Hepp-Lieb-Dicke phase transition is driven by an off-resonant two-photon Raman transition formed from a classical pump field and the emergent quantum dynamical cavity field. This mediates a spinor-spinor interaction that, above a critical strength, simultaneously organizes opposite spinor states of the BEC on opposite checkerboard configurations of an emergent 2D lattice. The resulting spinor density-wave polariton condensate is observed by directly detecting the atomic spin and momentum state and by holographically reconstructing the phase of the emitted cavity field. The latter provides a direct measure of the spin state, and a spin-spatial domain wall is observed. The photon-mediated spin interactions demonstrated here may be engineered to create dynamical gauge fields and quantum spin glasses., Comment: 7 pages, 4 figures plus supplement of 5 pages and 3 figures

Optical cavity QED provides a platform with which to explore quantum many-body physics in driven-dissipative systems. Single-mode cavities provide strong, infinite-range photon-mediated interactions among intracavity atoms. However, these global all-to-all couplings are limiting from the perspective of exploring quantum many-body physics beyond the mean-field approximation. The present work demonstrates that local couplings can be created using multimode cavity QED. This is established through measurements of the threshold of a superradiant, self-organization phase transition versus atomic position. Specifically, we experimentally show that the interference of near-degenerate cavity modes leads to both a strong and tunable-range interaction between Bose-Einstein condensates (BECs) trapped within the cavity. We exploit the symmetry of a confocal cavity to measure the interaction between real BECs and their virtual images without unwanted contributions arising from the merger of real BECs. Atom-atom coupling may be tuned from short range to long range. This capability paves the way toward future explorations of exotic, strongly correlated systems such as quantum liquid crystals and driven-dissipative spin glasses., 16 pages, 8 figures

As recently realized experimentally [L\'eonard et al., Nature 543, 87 (2017)], one can engineer models with continuous symmetries by coupling two cavity modes to trapped atoms, via a Raman pumping geometry. Considering specifically cases where internal states of the atoms couple to the cavity, we show an extended range of parameters for which continuous symmetry breaking can occur, and we classify the distinct steady states and time-dependent states that arise for different points in this extended parameter regime., Comment: 10 pages, 7 figures

Funding: “Laidlaw Research Internship” scheme at the University of St Andrews (RIM), EPSRC (EP/M010910/1) (PGK), EPSRC programs “TOPNES” (EP/I031014/1) and “Hybrid polaritonics” (EP/M025330/1) (JK). It has previously been shown that a dye-filled microcavity can produce a Bose-Einstein condensate of photons. Thermalization of photons is possible via repeated absorption and re-emission by the dye molecules. In this paper, we theoretically explore the behavior of the polarization of light in this system. We find that in contrast to the near complete thermalization between different spatial modes of light, thermalization of polarization states is expected to generally be incomplete. We show that the polarization degree changes significantly from below to above threshold, and explain the dependence of polarization on all relevant material parameters. Postprint

We show that dephasing of individual atoms destroys the superradiance transition of the Dicke model, but that adding individual decay toward the spin down state can restore this transition. To demonstrate this, we present a method to give an exact solution for the $N$ atom problem with individual dephasing which scales polynomially with $N$. By comparing finite size scaling of our exact solution to a cumulant expansion, we confirm the destruction and restoration of the superradiance transition holds in the thermodynamic limit., 5 pages, 2 figures, updated to published version

Phase transitions, where observable properties of a many-body system change discontinuously, can occur in both open and closed systems. By placing cold atoms in optical cavities and inducing strong coupling between light and excitations of the atoms, one can experimentally study phase transitions of open quantum systems. Here we observe and study a non-equilibrium phase transition, the condensation of supermode-density-wave polaritons. These polaritons are formed from a superposition of cavity photon eigenmodes (a supermode), coupled to atomic density waves of a quantum gas. As the cavity supports multiple photon spatial modes and because the light–matter coupling can be comparable to the energy splitting of these modes, the composition of the supermode polariton is changed by the light–matter coupling on condensation. By demonstrating the ability to observe and understand density-wave-polariton condensation in the few-mode-degenerate cavity regime, our results show the potential to study similar questions in fully multimode cavities., When a single mode optical cavity is coupled to a Bose-Einstein condensate, one usually observes a single mode of light when strongly pumped. Here the authors observe a supermode in the output of a multimode cavity and relate this to a signature of a nonequilibrium condensation phase transition.

Finding efficient descriptions of how an environment affects a collection of discrete quantum systems would lead to new insights into many areas of modern physics. Markovian, or time-local, methods work well for individual systems, but for groups a question arises: does system-bath or inter-system coupling dominate the dissipative dynamics? The answer has profound consequences for the long-time quantum correlations within the system. We consider two bosonic modes coupled to a bath. By comparing an exact solution to different Markovian master equations, we find that a smooth crossover of the equations-of-motion between dominant inter-system and system-bath coupling exists -- but requires a non-secular master equation. We predict a singular behaviour of the dynamics, and show that the ultimate failure of non-secular equations of motion is essentially a failure of the Markov approximation. Our findings justify the use of time-local theories throughout the crossover between system-bath dominated and inter-system-coupling dominated dynamics., 10 pages, 3 figures. v2: improved introduction, added analysis of positivity, corrected typos. v3: corrected typos in eqs. 5 and 23

We show that short-range correlations have a dramatic impact on the steady-state phase diagram of quantum driven-dissipative systems. This effect, never observed in equilibrium, follows from the fact that ordering in the steady state is of dynamical origin, and is established only at very long times, whereas in thermodynamic equilibrium it arises from the properties of the (free) energy. To this end, by combining the cluster methods extensively used in equilibrium phase transitions to quantum trajectories and tensor-network techniques, we extend them to nonequilibrium phase transitions in dissipative many-body systems. We analyze in detail a model of spin-1=2 on a lattice interacting through an XYZ Hamiltonian, each of them coupled to an independent environment that induces incoherent spin flips. In the steady-state phase diagram derived from our cluster approach, the location of the phase boundaries and even its topology radically change, introducing reentrance of the paramagnetic phase as compared to the single-site mean field where correlations are neglected. Furthermore, a stability analysis of the cluster mean field indicates a susceptibility towards a possible incommensurate ordering, not present if short-range correlations are ignored., Published version. 18 pages, 15 figures

Strong coupling between cavity photons and molecular vibrations can lead to the formation of vibron-polaritons. In a recent experiment with PVAc molecules in a metal-metal microcavity [A.Shalabney et al., Ang.Chem.Int.Ed. 54 7971 (2015)], such a coupling was observed to enhance the Raman scattering probability by several orders of magnitude. Inspired by this, we theoretically analyze the effect of strong photon-vibron coupling on the Raman scattering amplitude of organic molecules. This problem has recently been addressed in [J.del Pino, J.Feist and F.J.Garcia-Vidal; J.Phys.Chem.C 119 29132 (2015)] using exact numerics for a small number of molecules. In this paper we derive compact analytic results for any number of molecules, also including the ultra-strong coupling regime. Our calculations predict a division of the Raman signal into upper and lower polariton modes,with some enhancement to the lower polariton Raman amplitude due to the mode softening under strong coupling., 11 pages, 4 figures

We study theoretically the effects of pump-spot size and location on photon condensates. By exploring the inhomogeneous molecular excitation fraction, we make clear the relation between spatial equilibration, gain clamping and thermalization in a photon condensate. This provides a simple understanding of several recent experimental results. We find that as thermalization breaks down, gain clamping is imperfect, leading to "transverse spatial hole burning" and multimode condensation. This opens the possibility of engineering the gain profile to control the condensate structure., Comment: Further extended, including new figures. Now 10 figures

Previous realizations of synthetic gauge fields for ultracold atoms do not allow the spatial profile of the field to evolve freely. We propose a scheme which overcomes this restriction by using the light in a multimode cavity, in conjunction with Raman coupling, to realize an artificial magnetic field which acts on a Bose-Einstein condensate of neutral atoms. We describe the evolution of such a system, and present the results of numerical simulations which show dynamical coupling between the effective field and the matter on which it acts. Crucially, the freedom of the spatial profile of the field is sufficient to realize a close analogue of the Meissner effect, where the magnetic field is expelled from the superfluid. This back-action of the atoms on the synthetic field distinguishes the Meissner-like effect described here from the Hess-Fairbank suppression of rotation in a neutral superfluid observed elsewhere., Comment: main text of 6 pages, 3 figures; supplemental materials of 2 pages, 1 figure

We examine in detail the mechanisms behind thermalization and Bose-Einstein condensation 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 non-equilibrium 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, $g^{(2)}$, 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., 17 pages, 12 figures

We explore the phase diagram of the dissipative Rabi-Hubbard model, as could be realized by a Raman-pumping scheme applied to a coupled cavity array. There exist various exotic attractors, including ferroelectric, antiferroelectric, and inccomensurate fixed points, as well as regions of persistent oscillations. Many of these features can be understood analytically by truncating to the two lowest lying states of the Rabi model on each site. We also show that these features survive beyond mean-field, using Matrix Product Operator simulations., 5pages, 3 figures, plus supplementary material. Final version, as published

Starting from a microscopic model, we investigate the optical spectra of molecules in strongly-coupled organic microcavities examining how they might self-consistently adapt their coupling to light. We consider both rotational and vibrational degrees of freedom, focusing on features which can be seen in the peak in the center of the spectrum at the bare excitonic frequency. In both cases we find that the matter-light coupling can lead to a self-consistent change of the molecular states, with consequent temperature-dependent signatures in the absorption spectrum. However, for typical parameters, these effects are much too weak to explain recent measurements. We show that another mechanism which naturally arises from our model of vibrationally dressed polaritons has the right magnitude and temperature dependence to be at the origin of the observed data., Comment: 14 pages, 6 figure

Following the experimental realization of Dicke superradiance in Bose gases coupled to cavity light fields, we investigate the behavior of ultracold fermions in a transversely pumped cavity. We focus on the equilibrium phase diagram of spinless fermions coupled to a single cavity mode and establish a zero temperature transition to a superradiant state. In contrast to the bosonic case, Pauli blocking leads to lattice commensuration effects that influence self-organization in the cavity light field. This includes a sequence of discontinuous transitions with increasing atomic density and tricritical superradiance. We discuss the implications for experiment. Publisher PDF

Polaritons, mixed light-matter quasiparticles, undergo a transition to a condensed, macroscopically coherent state at low temperatures or high densities. Recent experiments show that coupling light to organic molecules inside a microcavity allows condensation at room temperature. The molecules act as saturable absorbers with transitions dressed by molecular vibrational modes. Motivated by this we calculate the phase diagram and spectrum of a modified Tavis-Cummings model, describing vibrationally dressed two-level systems, coupled to a cavity mode. Coupling to vibrational modes can induce re-entrance, i.e. a normal-condensed-normal sequence with decreasing temperature and can drive the transition first order., 6 pages, 3 figures

We study the nonequilibrium steady state (NESS) of a driven dissipative one-dimensional system near a critical point, and explore how the quantum correlations compare to the known critical behavior in the ground state. The model we study corresponds to a cavity array driven parametrically at a two photon resonance, equivalent in a rotating frame to a transverse field anisotropic $XY$ model [C.-E. Bardyn and A. Imamo\ifmmode \breve{g}\else \u{g}\fi{}lu, Phys. Rev. Lett. 109, 253606 (2012)]. Depending on the sign of transverse field, the steady state of the open system can be either related to the ground state or to the maximum energy state. In both cases, many properties of the entanglement are similar to the ground state, although no critical behavior occurs. As one varies from the Ising limit to the isotropic $XY$ limit, entanglement range grows. The isotropic limit of the NESS is, however, singular, with simultaneously diverging range and vanishing magnitude of entanglement. This singular limiting behavior is quite distinct from the ground state behavior; it can, however, be understood analytically within spin-wave theory.

We consider the possible phases of microcavity polaritons tuned near a bipolariton Feshbach resonance. We show that, as well as the regular polariton superfluid phase, a "molecular" superfluid exists, with (quasi-)long-range order only for pairs of polaritons. We describe the experimental signatures of this state. Using variational approaches we find the phase diagram (critical temperature, density and exciton-photon detuning). Unlike ultracold atoms, the molecular superfluid is not inherently unstable, and our phase diagram suggests it is attainable in current experiments., paper (4 pages, 3 figures), Supplemental Material (7 pages, 8 figures)

We use the Bloch-Redfield-Wangsness theory to calculate the effects of acoustic phonons in coherent control experiments, where quantum-dot excitons are driven by shaped laser pulses. This theory yields a generalized Lindblad equation for the density operator of the dot, with time-dependent damping and decoherence due to phonon transitions between the instantaneous dressed states. It captures similar physics to the form recently applied to Rabi oscillation experiments [A. J. Ramsay et al., Phys. Rev. Lett. 104, 017402 (2010)], but guarantees positivity of the density operator. At sufficiently low temperatures, it gives results equivalent to those of fully non-Markovian approaches [S. Luker et al., Phys. Rev. B 85, 121302 (2012)], but is significantly simpler to simulate. Several applications of this theory are discussed. We apply it to adiabatic rapid passage experiments, and show how the pulses can be shaped to maximize the probability of creating a single exciton using a frequency-swept laser pulse. We also use this theory to propose and analyze methods to determine the phonon density of states experimentally, i.e. phonon spectroscopy, by exploring the dependence of the effective damping rates on the driving field., 12 pages, 10 figures. v2: Typos corrected, additional discussion and figure

We develop a nonequilibrium model of condensation and lasing of photons in a dye filled microcavity. We examine in detail the nature of the thermalization process induced by absorption and emission of photons by the dye molecules, and investigate when the photons are able to reach a thermal equilibrium Bose-Einstein distribution. At low temperatures, or large cavity losses, the absorption and emission rates are too small to allow the photons to reach thermal equilibrium and the behavior becomes more like that of a conventional laser., 5 pages, 3 figures

We report the experimental observation and a theoretical explanation of collective suppression of linewidths for multiple superconducting qubits coupled to a good cavity. This demonstrates how strong qubit-cavity coupling can significantly modify the dephasing and dissipation processes that might be expected for individual qubits, and can potentially improve coherence times in many-body circuit QED. Publisher PDF

Exciton-polariton condensates display a variety of intriguing pattern-forming behaviors, particularly when confined in potential traps. It has previously been predicted that triangular lattices of vortices of the same sign will form spontaneously as the result of surface instabilities in a harmonic trap. However, natural disorder, deviation of the external potential from circular symmetry, or higher-order terms modifying the dynamical equations may all have detrimental effects and destabilize the circular trajectories of vortices. Here we address these issues, by characterizing the robustness of the vortex lattice against disorder and deformations of the trapping potential. Since most experiments use time integrated measurements it would be hard to observe directly the rotating vortex lattices or distinguish them from vortex-free states. We suggest how these difficulties can be overcome and present an experimentally viable interference-imaging scheme that would allow the detection of rotating vortex lattices., Comment: 12 pages, 12 figures

We study the coherence and fluorescence properties of the coherently pumped and dissipative Jaynes-Cummings-Hubbard model describing polaritons in a coupled-cavity array. At weak hopping we find strong signatures of photon blockade similar to single-cavity systems. At strong hopping the state of the photons in the array depends on its size. While the photon blockade persists in a dimer consisting of two coupled cavities, a coherent state forms on an extended lattice, which can be described in terms of a semi-classical model.

We study the interplay of disorder with pumping and decay in coupled qubit-cavity arrays, the Jaynes-Cummings-Hubbard model. We find that relatively weak disorder can wash out the bistability present in the clean pumped system, and that moreover, the combination of disorder in on-site energies and decay can lead to effective phase disorder. To explore these questions, we present a non- equilibrium generalisation of Stochastic-Mean-Field theory, providing a simple tool to address such questions. This technique is developed for rather general forms of light-matter coupling, driving, dissipation, and on-site disorder, making it applicable to a wide range of systems., Comment: 7 pages, 4 figures

Motivated by experiments observing self-organization of cold atoms in optical cavities we investigate the collective dynamics of the associated nonequilibrium Dicke model. The model displays a rich semiclassical phase diagram of long time attractors including distinct superradiant fixed points, bistable and multistable coexistence phases and regimes of persistent oscillations. We explore the intrinsic timescales for reaching these asymptotic states and discuss the implications for finite duration experiments. On the basis of a semiclassical analysis of the effective Dicke model we find that sweep measurements over 200ms may be required in order to access the asymptotic regime. We briefly comment on the corrections that may arise due to quantum fluctuations and states outside of the effective two-level Dicke model description., 27 pages, 20 figures

I calculate the superfluid density of a non-equilibrium steady state condensate of particles with finite lifetime. Despite the absence of a simple Landau critical velocity, a superfluid response survives, but dissipation reduces the superfluid fraction. I also suggest an idea for how the superfluid density of an example of such a system, i.e. microcavity polaritons, might be measured., 4 pages, 3 figures