The interaction of quantum light with matter like that inside a cavity is known to give rise to mixed light-matter states called polaritons. We discuss the impact of rotation of the cavity on the polaritons. It is shown that the number of polaritons increases due to this rotation. The structure of the original polaritons is modified and new ones are induced by the rotation that strongly depend on the angular velocity and the choice of axis of rotation. In molecules the rotation can change the number of light-induced conical intersections and their dimensionality and hence strongly impact their quantum dynamics. General consequences are discussed.
Recent studies of quantum phase transitions in coupled atom-cavity arrays have focused on the similarities between such systems and the Bose-Hubbard model. However, the bipartite nature of the atom-cavity systems that make up the array introduces some differences. In order to examine the unique features of the coupled-cavity system, the behavior of a simple two-site model is studied over a wide range of parameters. Four regions are identified, in which the ground state of the system may be classified as either a polaritonic insulator, a photonic superfluid, an atomic insulator, or a polaritoni…
We demonstrate a scheme for quantum communication between the ends of an array of coupled cavities. Each cavity is doped with a single two level system (atoms or quantum dots) and the detuning of the atomic level spacing and photonic frequency is appropriately tuned to achieve photon blockade in the array. We show that in such a regime, the array can simulate a dual rail quantum state transfer protocol where the arrival of quantum information at the receiving cavity is heralded through a fluorescence measurement. Communication is also possible between any pair of cavities of a network of conne…
We consider molecules confined to a microcavity whose dimensions are such that an excitation of the molecule is nearly resonant with a cavity mode. We investigate the situation where the excitation energies of the molecules are randomly distributed with a mean value of $ε_a$ and variance $σ$. For this case, we find a solution that approaches the exact result for large values of the number density $\mathscr{N}$ of the molecules. We find the conditions for the existence of the polaritonic states, as well as expressions for their energies. The polaritonic states are quite stable against disorder.…
We present a full analysis of the mode spectrum in a cavity formed by two parallel plates, one of which is a magneto-dielectric, e.g. a metamaterial, while the other one is metallic, and obtain dispersion relations in closed form. The optical properties of the cavity walls are described in terms of realistic models for the effective permittivity and the permeability. Surface polaritons, i.e. electromagnetic modes that have at least partly an evanescent character, are shown to dominate the Casimir interaction at small separations. We analyze in detail the s-polarized polaritons, which are a cha…
Nonadiabatic phenomena are investigated in the rovibrational motion of molecules confined in an infrared cavity. Conical intersections (CIs) between vibrational polaritons, similar to CIs between electronic polaritonic surfaces, are found. The spectral, topological, and dynamic properties of the vibrational polaritons show clear fingerprints of nonadiabatic couplings between molecular vibration, rotation and the cavity photonic mode. Furthermore, it is found that for the investigated system, composed of two rovibrating HCl molecules and the cavity mode, breaking the molecular permutational sym…
In a previous work [Phys. Rev. Lett. 123, 047202 (2019)] a translationally invariant framework called quantum-electrodynamical Bloch (QED-Bloch) theory was introduced for the description of periodic materials in homogeneous magnetic fields and strongly coupled to the quantized photon field in the optical limit. For such systems, we show that QED-Bloch theory predicts the existence of fractal polaritonic spectra as a function of the cavity coupling strength. In addition, for the energy spectrum as a function of the relative magnetic flux we find that a terahertz cavity can modify the standard H…
The electromagnetic field in an optical cavity can dramatically modify and even control chemical reactivity via vibrational strong coupling (VSC). Since the typical vibration and cavity frequencies are considerably higher than thermal energy, it is essential to adopt a quantum description of cavity-catalyzed adiabatic chemical reactions. Using quantum transition state theory (TST), we examine the coherent nature of adiabatic reactions and derive the cavity-induced changes in eigen frequencies, zero-point-energy, and quantum tunneling. The resulting quantum TST calculation allows us to explain …
Bipartite entanglement entropies are calculated for the ground state of the two-excitation subspace in a two-site coupled cavity model. Each region in the phase diagram (atomic insulator, polaritonic insulator, photonic superfluid, and polaritonic superfluid) is found to be characterized by unique entanglement properties. In particular, the polaritonic superfluid region exhibits multipartite entanglement among the two atoms and two cavity fields. This system provides a toy model in which a number of intriguing aspects of entanglement can be studied, such as the relationship of entanglement to …
The exact time-dependent potential energy surface driving the nuclear dynamics was recently shown to be a useful tool to understand and interpret the coupling of nuclei, electrons, and photons, in cavity settings. Here we provide a detailed analysis of its structure for exactly-solvable systems that model two phenomena: cavity-induced suppression of proton-coupled electron transfer and its dependence on the initial state, and cavity-induced electronic excitation. We demonstrate the inadequacy of simply using a weighted average of polaritonic surfaces to determine the dynamics. Such a weighted …
I investigate the tunneling decay rate of a polaritonic system formed by a strong coupling between a vacuum cavity mode and $N$ metastable systems. Using a simple model potential, I find the instanton solutions controlling the low-temperature tunneling rate. The resulting rate modification due to the cavity is proportional to the mean of the second power of the light-matter coupling. No collective effect that would enhance the rates by a factor of $\sqrt{N}$ is present, which is in line with the results in the thermal activation regime.
We analyze the quantum phase transition-like behavior in the lowest energy state of a two-site coupled atom-cavity system, where each cavity contains one atom but the total excitation number is not limited to two. Utilizing the variance of the total excitation number to distinguish the insulator and superfluid states, and the variance of the atomic excitation number to identify the polaritonic characteristics of these states, we find that the total excitation number plays a significant role in the lowest-energy-state phase transitions. In both the small hopping regime and the small atom-field …
Laser control of solids was so far mainly discussed in the context of strong classical nonlinear light-matter coupling in a pump-probe framework. Here we propose a quantum-electrodynamical setting to address the coupling of a low-dimensional quantum material to quantized electromagnetic fields in quantum cavities. Using a protoypical model system describing FeSe/SrTiO$_3$ with electron-phonon long-range forward scattering, we study how the formation of phonon polaritons at the 2D interface of the material modifies effective couplings and superconducting properties in a Migdal-Eliashberg simula…
In this review we present the theoretical foundations and first principles frameworks to describe quantum matter within quantum electrodynamics (QED) in the low-energy regime. Having a rigorous and fully quantized description of interacting photons, electrons and nuclei/ions, from weak to strong light-matter coupling regimes, is pivotal for a detailed understanding of the emerging fields of polaritonic chemistry and cavity materials engineering. The use of rigorous first principles avoids ambiguities and problems stemming from using approximate models based on phenomenological descriptions of …
It has been experimentally demonstrated that reaction rates for molecules embedded in microfluidic optical cavities are altered when compared to rates observed under "ordinary" reaction conditions. However, precise mechanisms of how strong coupling of an optical cavity mode to molecular vibrations affect the reactivity and how resonance behavior emerges are still under dispute. In the present work, we approach these mechanistic issues from the perspective of a thermal model reaction, the inversion of ammonia along the umbrella mode, in presence of a single cavity mode of varying frequency and …
We use the scattering matrix formalism to analyze photon blockade in coherently-driven CQED systems with a weak drive. By approximating the weak coherent drive by an input single- and two-photon Fock state, we reduce the computational complexity of the transmission and the two-photon correlation function from exponential to polynomial in the number of emitters. This enables us to easily analyze cavity-based systems containing $\sim$50 quantum emitters with modest computational resources. Using this approach we study the coherence statistics of polaritonic photon blockade while increasing the n…
Competing pathways in polaritonic chemistry and general harmonic environments
University of Copenhagen（哥本哈根大学）；Niels Bohr Institute, University of Copenhagen（尼尔斯·玻尔研究所，哥本哈根大学）；Flatiron Institute（平顿研究所）；Bates College（贝茨学院）；City College of New York（纽约市立学院）；The Graduate Center, City University of New York（纽约市立大学研究生院）
We study the case of two polaritonic qubits localized in two separate cavities coupled by a fiber/additional cavity. We show that surprisingly enough, even a coherent classical pump in the intermediate cavity/fiber can lead to the creation of entanglement between the two ends in the steady state. The stationary nature of this entanglement and its survival under dissipation opens possibilities for its production under realistic laboratory conditions. To facilitate the verification of the entanglement in an experiment we also construct the relevant entanglement witness measurable by accessing on…
The photon blockade (PB) effect in emitter-cavity systems depends on the anharmonicity of the ladder of dressed energy eigenstates. The recent developments in color center photonics are leading toward experimental demonstrations of multi-emitter-cavity solid-state systems with an expanded set of energy levels compared to the traditionally studied single-emitter systems. We focus on the case of N = 2 nonidentical quasi-atoms strongly coupled to a nanocavity in the bad cavity regime (with parameters within reach of the color center systems), and discover three PB mechanisms: polaritonic, subradi…
We investigate the single-photon transport properties of a one-dimensional coupled cavity array (CCA) containing a single qubit in its central site by coupling the CCA to two transmission lines supporting propagating bosonic modes with linear dispersion. We find that even in the nominally weak light-matter coupling regime, the transmission through a long array exhibits two ultra-narrow resonances corresponding to long-lived self-protected polaritonic states localized around the site containing the qubit. The lifetime of these states is found to increase exponentially with the number of array s…
The first exact quantum simulation of a real molecular system (HD$^+$) under strong ro-vibrational coupling to a quantized optical cavity mode in thermal equilibrium is presented. Theoretical challenges in describing strongly coupled systems of mixed quantum statistics (Bosons and Fermions) are discussed and circumvented by the specific choice of our molecular system. Our exact simulations reveal the absence of a zero temperature for the strongly coupled matter and light subsystems, due to cavity induced non-equilibrium conditions. Furthermore, we explore the temperature dependency of light-ma…
We study the collective effects of an ensemble of organic molecules confined in an optical cavity based on Holstein-Tavis-Cummings model. By using the quantum Langevin approach and adiabatically eliminating the degree of freedom of the vibrational motion, we analytically obtain the expression of the cavity transmission spectrum to analyze the features of polaritonic states. As an application, we show that the dependence for the frequency shift of the lower polaritonic state on the number of molecules can be used in the detection of the ultra-cold molecules. We also numerically analyze the fluo…
We investigate theoretically the coupling of a cavity mode to a continuous distribution of emitters. We discuss the influence of the emitters inhomogeneous broadening on the existence and on the coherence properties of the polaritonic peaks. We find that their coherence depends crucially on the shape of the distribution and not only on its width. Under certain conditions the coupling to the cavity protects the polaritonic states from inhomogeneous broadening, resulting in a longer storage time for a quantum memory based on emitters ensembles. When two different ensembles of emitters are couple…
We show that polaritons in an array of interacting micro-cavities with strong atom-photon coupling can form a two-component Bose-Hubbard model. Both polariton species are thereby protected against spontaneous emission as their atomic part is stored in two ground states of the atoms. The parameters of the effective model can be tuned via the driving strength of external lasers. We also describe a method to measure the number statistics in one cavity for each polariton species independently.
Strong coupling between vibrational transitions in molecules within a resonant optical microcavity leads to the formation of collective, delocalized vibrational polaritons. There are many potential applications of "polaritonic chemistry," ranging from modified chemical reactivity to quantum in-formation processing. One challenge in obtaining the polaritonic response is to remove a background contribution due to the uncoupled molecules that generate an ordinary 2D-IR spectrum whose amplitude is filtered by the polariton transmission spectrum. We show that most features in 2D-IR spectra of vibra…
We study a system of interacting matter quasiparticles strongly coupled to photons inside an optomechanical cavity. The resulting normal modes of the system are represented by hybrid polaritonic quasiparticles, which acquire effective nonlinearity. Its strength is influenced by the presence of the mechanical mode and depends on the resonance frequency of the cavity. This leads to an interactive type of optomechanical coupling, being distinct from the previously studied dispersive and dissipative couplings in optomechanical systems. The emergent interactive coupling is shown to generate effecti…
We study the interplay between disorder and light-matter coupling by considering a disordered one-dimensional chain of lossy dipoles coupled to a multimode optical cavity, through a microscopically derived Hamiltonian. Such a system, hosting polaritonic excitations, may be realized experimentally in a wide range of platforms under strong light-matter coupling. By analyzing both the eigenspectrum and the driven-dissipative transport properties of our system, we find that in the strong-coupling regime, increasing disorder leads almost uncoupled dark states to acquire a photonic part, allowing th…
We consider a coupled-cavity array, where each cavity interacts with an atom under the rotating-wave approximation. For a staggered pattern of inter-cavity couplings, a pair of field normal modes each bi-localized at the two array ends arise. A rich structure of dynamical regimes can hence be addressed depending on which resonance condition between the atom and field modes is set. We show that this can be harnessed to carry out high-fidelity quantum-state transfer (QST) of photonic, atomic or polaritonic states. Moreover, by partitioning the array into coupled modules of smaller length, the QS…
Condensed matter physics and quantum electrodynamics (QED) have been long considered as distinct disciplines. This situation is changing by the progress in cavity QED materials. Motivated by these advances we aim to bridge these fields by merging fundamental concepts coming from both sides. In the first part of the thesis we present how non-relativistic QED can be constructed and we discuss the light-matter interaction in different gauges and that neglecting particular quadratic terms can lead to instabilities. In the second part, we revisit the Sommerfeld model of the free electron gas in cav…
Recent experiments have demonstrated an open system realization of the Dicke quantum phase transition in the motional degrees of freedom of an optically driven Bose-Einstein condensate in a cavity. Relevant collective excitations of this light-matter system are polaritonic in nature, allowing access to the quantum critical behavior of the Dicke model through light leaking out of the cavity. This opens the path to using photodetection based quantum optical techniques to study the dynamics and excitations of this elementary quantum critical system. We first discuss the photon flux observed at th…
It has previously been shown theoretically that the exchange of linear momentum between the light field in an optical cavity and a vibrating end mirror can entangle the electromagnetic field with the vibrational motion of that mirror. In this paper we consider the rotational analog of this situation and show that radiation torque can similarly entangle a Laguerre-Gaussian cavity mode with a rotating end mirror. We examine the mirror-field entanglement as a function of ambient temperature, radiation detuning and orbital angular momentum carried by the cavity mode.
This perspective provides a brief introduction into the theoretical complexity of polaritonic chemistry, which emerges from the hybrid nature of strongly coupled light-matter states. To tackle this complexity, the importance of ab initio methods is highlighted. Based on those, novel ideas and research avenues are developed with respect to quantum collectivity, as well as for resonance phenomena immanent in reaction rates under vibrational strong coupling. Indeed, fundamental theoretical questions arise about the mesoscopic scale of quantum-collectively coupled molecules, when considering the d…
We study the photon generation from arbitrary initial state in cavity QED due to the combined action of the anti-rotating term present in the Rabi Hamiltonian and Lindblad-type dephasing. We obtain a simple set of differential equations describing this process and deduce useful formulae for the moments of the photon number operator, demonstrating analytically that the average photon number increases linearly with time in the asymptotic limit.
Rayleigh scattering is usually considered to be the elastic scattering of photons from sub-wavelength physical objects, such as small particles or molecules. Here, we present the spectroscopic study of the scattering properties of molecules embedded in an optical cavity under strong coupling conditions, where the collective interaction between the molecules and the cavity gives rise to composite light-matter excitations known as cavity polaritons. We show that the polaritonic states exhibit strong resonant Rayleigh scattering, reaching 25% efficiency. Since the polaritonic wavefunctions in suc…
We study quantum optics with the atoms coupled to the quantized electromagnetic (EM) field in a non-inertial reference frame by making use of quantum field theory in curved spacetime. We rigorously establish the microscopic model for a two-level atom interacting with the quantized EM field in a rotating ring cavity by deriving a Jaynes-Cummings (JC) type Hamiltonian. Due to the two fold degeneracy of the ring cavity modes, the Rabi splitting exhibits three rather than two resonant frequency peaks. We find that the heights of the two side peaks show a sensitive linear dependence on the rotating…
We describe a new type of spatially periodic structure (lattice models): a polaritonic crystal (PolC) formed by a two-dimensional lattice of trapped two-level atoms interacting with quantised electromagnetic field in a cavity (or in a one-dimensional array of tunnelling-coupled microcavities), which allows polaritons to be fully localised. Using a one-dimensional polaritonic crystal as an example, we analyse conditions for quantum degeneracy of a low-branch polariton gas and those for quantum optical information recording and storage.
