Quantized Cavity Mode Research Articles

Cavity Born-Oppenheimer Hartree-Fock Ansatz: Light-Matter Properties of Strongly Coupled Molecular Ensembles.

Experimental studies indicate that optical cavities can affect chemical reactions through either vibrational or electronic strong coupling and the quantized cavity modes. However, the current understanding of the interplay between molecules and confined light modes is incomplete. Accurate theoretical models that take into account intermolecular interactions to describe ensembles are therefore essential to understand the mechanisms governing polaritonic chemistry. We present an ab initio Hartree-Fock ansatz in the framework of the cavity Born-Oppenheimer approximation and study molecules strongly interacting with an optical cavity. This ansatz provides a nonperturbative, self-consistent description of strongly coupled molecular ensembles, taking into account the cavity-mediated dipole self-energy contributions. To demonstrate the capability of the cavity Born-Oppenheimer Hartree-Fock ansatz, we study the collective effects in ensembles of strongly coupled diatomic hydrogen fluoride molecules. Our results highlight the importance of the cavity-mediated intermolecular dipole-dipole interactions, which lead to energetic changes of individual molecules in the coupled ensemble.

Cavity-catalyzed hydrogen transfer dynamics in an entangled molecular ensemble under vibrational strong coupling.

Microcavities have been shown to influence the reactivity of molecular ensembles by strong coupling of molecular vibrations to quantized cavity modes. In quantum mechanical treatments of such scenarios, frequently idealized models with single molecules and scaled, effective molecule-cavity interactions or alternatively ensemble models with simplified model Hamiltonians are used. In this work, we go beyond these models by applying an ensemble variant of the Pauli-Fierz Hamiltonian for vibro-polaritonic chemistry and numerically solve the underlying time-dependent Schrödinger equation to study the cavity-induced quantum dynamics in an ensemble of thioacetylacetone (TAA) molecules undergoing hydrogen transfer under vibrational strong coupling (VSC) conditions. Beginning with a single molecule coupled to a single cavity mode, we show that the cavity indeed enforces hydrogen transfer from an enol to an enethiol configuration with transfer rates significantly increasing with light-matter interaction strength. This positive effect of the cavity on reaction rates is different from several other systems studied so far, where a retarding effect of the cavity on rates was found. It is argued that the cavity "catalyzes" the reaction by transfer of virtual photons to the molecule. The same concept applies to ensembles with up to N = 20 TAA molecules coupled to a single cavity mode, where an additional, significant, ensemble-induced collective isomerization rate enhancement is found. The latter is traced back to complex entanglement dynamics of the ensemble, which we quantify by means of von Neumann-entropies. A non-trivial dependence of the dynamics on ensemble size is found, clearly beyond scaled single-molecule models, which we interpret as transition from a multi-mode Rabi to a system-bath-type regime as N increases.

Semiclassical and quantum nonlinear spectra of a strongly coupled single Λ-type three-level atom-cavity QED system

We present detailed numerical simulations of semiclassical and quantum spectra of a cavity QED system consisting of a single three-level atom in Λ-configuration interacting with a quantized cavity mode through one of its transitions while its other transition is driven by a coherent classical field. We compute the semiclassical and quantum spectra of the system under various levels of external driving field strengths. In the semiclassical approach, we neglect the correlations between the cavity and atomic operators, whereas in the quantum case no such assumption is made. Our results show that the two approaches yield identical results under sufficiently weak driving field conditions. However, the two approaches yield starkly different results at stronger driving field intensities: the fully quantum approach yields a well-defined multiphoton spectrum whereas the semiclassical approach results in a bistable spectrum. Furthermore, our calculations reveal a complex Raman structure at the position of the dark-state transition.

Nonlinear optical response properties of a quantum dot embedded in a semiconductor microcavity: possible applications in quantum communication platforms

We theoretically investigate optical bistability, mechanically induced absorption (MIA) and Fano resonance of a hybrid system comprising of a single quantum dot (QD) embedded in a solid-state microcavity interacting with the quantized cavity mode and the deformation potential associated with the lattice vibration. We find that the bistability can be tuned by the QD-cavity mode coupling. We further show that the normalized power transmission displays anomalous dispersion indicating that the system can be used to generate slow light. We also demonstrate the possibility of using the system as all optomechanical Kerr switch.

Quantum frequency locking and downconversion in a driven qubit-cavity system

We study a periodically driven qubit coupled to a quantized cavity mode. Despite its apparent simplicity, this system supports a rich variety of exotic phenomena, such as topological frequency conversion as recently discovered in [Martin et al, PRX 7, 041008 (2017)]. Here we report on a qualitatively different phenomenon that occurs in this platform, where the cavity mode's oscillations lock their frequency to a rational fraction $r/q$ of the driving frequency $\Omega$. This phenomenon, which we term quantum frequency locking, is characterized by the emergence of $q$-tuplets of stationary (Floquet) states whose quasienergies are separated by $\Omega/q$, up to exponentially small corrections. The Wigner functions of these states are nearly identical, and exhibit highly-regular and symmetric structure in phase space. Similarly to Floquet time crystals, these states underlie discrete time-translation symmetry breaking in the model. We develop a semiclassical approach for analyzing and predicting quantum frequency locking in the model, and use it to identify the conditions under which it occurs.

Fast generation of microwave photon Fock states in a superconducting nanocircuit

Abstract Optimal generation of photon Fock states is of significance for quantum information processing and state engineering. Here an efficient scheme is proposed for fast generation of photon Fock states in a superconducting nanocircuit via counterdiabatic driving. A Cooper-pair box circuit, behaving as an effective three-level artificial atom, is driven by a quantized cavity mode and two classical fields. By the technique of shortcuts to adiabaticity with counterdiabatic driving, we first generate a single-photon Fock state by performing population transfer within a composite system, consisting of the atom qutrit and microwave photons. Assisted by an auxiliary driving to initialize atom state, rapid generation of multi-photon Fock states can be addressed sequentially. Compared with an adiabatic counterpart, the shortcut-based operation in a shorter time contributes to enhance fidelity. The strategy could offer a promising avenue towards optimized creation of microwave photon Fock states with superconducting quantum circuits.

Electromagnetic coupling in tight-binding models for strongly correlated light and matter

We discuss the construction of low-energy tight-binding Hamiltonians for condensed matter systems with a strong coupling to the quantum electromagnetic field. Such Hamiltonians can be obtained by projecting the continuum theory on a given set of Wannier orbitals. However, different representations of the continuum theory lead to different low-energy formulations, because different representations may entangle light and matter, transforming orbitals into light-matter hybrid states before the projection. In particular, a multi-center Power-Zienau-Woolley transformation yields a dipolar Hamiltonian which incorporates the light-matter coupling via both Peierls phases and a polarization density. We compare this dipolar gauge Hamiltonian and the straightforward Coulomb gauge Hamiltonian for a one-dimensional solid, to describe sub-cycle light-driven electronic motion in the semiclassical limit, and a coupling of the solid to a quantized cavity mode which renormalizes the band-structure into electron-polariton bands. Both descriptions yield the same result when many bands are taken into account, but the dipolar Hamiltonian is more accurate when the model is restricted to few electronic bands, while the Coulomb Hamiltonian requires fewer electromagnetic modes.

Fast-generating entanglement state between a transmon qubit and cavity photons via resonant driving

Fast generation of entanglement states is of critical importance for robust quantum information processing. In this paper, we propose an efficient protocol for a rapidly generating entanglement state between a transmon qubit and microwave photons. The transmon system is coupled to a classical microwave driving and a quantized cavity mode. With the adjustable classical driving, we consider the entanglement creation by transferring the composite states via resonant driving. Compared with the non-resonant cases, the present operation can be accomplished in a shorter time, which thus contributes to mitigating the decoherence effects. Moreover, many transmons inside a common cavity field could be addressed in a scalable way. The proposed strategy could offer a promising approach to optimally prepare entanglement states with superconducting quantum systems.

Comparison of semiclassical and quantum models of a two-level atom-cavity QED system in the strong coupling regime

ABSTRACTWe present a numerical study comparing semiclassical and quantum models of a damped, strongly interacting cavity QED system composed of a single two-level atom interacting with a single quantized cavity mode driven externally by a tunable monochromatic field. We compute the steady state transmission spectrum of the coupled system under each model and show that in the strong coupling regime, the two models yield starkly different results. The fully quantum mechanical model of the system correctly yields the expected multiphoton transmission spectra while the semiclassical approach results in a bistable spectrum.

Purcell enhancement of the parametric down-conversion in two-dimensional nonlinear materials

Ultracompact nonlinear optical devices utilizing two-dimensional (2D) materials and nanostructures are emerging as important elements of photonic circuits. Integration of the nonlinear material into a subwavelength cavity or waveguide leads to a strong Purcell enhancement of the nonlinear processes and compensates for a small interaction volume. The generic feature of such devices which makes them especially challenging for analysis is strong dissipation of both the nonlinear polarization and highly confined modes of a subwavelength cavity. Here we solve a quantum-electrodynamic problem of the spontaneous and stimulated parametric down-conversion in a nonlinear quasi-2D waveguide or cavity. We develop a rigorous Heisenberg-Langevin approach which includes dissipation and fluctuations in the electron ensemble and in the electromagnetic field of a cavity on equal footing. Within a relatively simple model, we take into account the nonlinear coupling of the quantized cavity modes, their interaction with a dissipative reservoir and the outside world, amplification of thermal noise and zero-point fluctuations of the electromagnetic field, and other relevant effects. We derive closed-form analytic results for relevant quantities such as the spontaneous parametric signal power and the threshold for parametric instability. We find a strong reduction in the parametric instability threshold for 2D nonlinear materials in a subwavelength cavity and provide a comparison with conventional nonlinear photonic devices.

Photon–photon correlations with a V-type three-level system interacting with two quantized field modes

We carry out a model study on the interaction of a $V$-type three-level emitter with two quantized cavity modes which are weakly driven by two classical fields. The emitter may be an atom or a molecule with nondegenerate upper levels in general. The lifetimes of the two upper levels are assumed to be much longer than the lifetime of the cavity photons. We calculate the two-time second order coherence function, namely Hanbury Brown-Twiss function $g^{(2)}(\tau)$ where $\tau$ is the time delay between the two modes. We analyze the photon-photon correlations between the two cavity modes in terms of $g^{(2)}(\tau)$. The variation of $g^{(2)}(\tau)$ as a function of $\tau$ exhibits collapse and revival type oscillations as well as quantum beats for relatively short $\tau$ while in the limit $\tau \rightarrow \infty$, $g^{(2)}(\tau) \simeq 1$. We further show that the two cavity field modes are entangled when $g^{(2)}(0) > 2$. We develop a dressed state picture with single photon in each mode to explain the results and use the negativity of the partial transpose of the reduced field density matrix to show the entanglement between field modes. The model presented in this paper may be useful for generating entangled photon pairs, and also manipulating photon-photon correlations with a cavity QED set up.

The effect of nonadiabaticity on the efficiency of quantum memory based on an optical cavity

Quantum efficiency is an important characteristic of quantum memory devices that are aimed at recording the quantum state of light signals and its storing and reading. In the case of memory based on an ensemble of cold atoms placed in an optical cavity, the efficiency is restricted, in particular, by relaxation processes in the system of active atomic levels. We show how the effect of the relaxation on the quantum efficiency can be determined in a regime of the memory usage in which the evolution of signals in time is not arbitrarily slow on the scale of the field lifetime in the cavity and when the frequently used approximation of the adiabatic elimination of the quantized cavity mode field cannot be applied. Taking into account the effect of the nonadiabaticity on the memory quality is of interest in view of the fact that, in order to increase the field–medium coupling parameter, a higher cavity quality factor is required, whereas storing and processing of sequences of many signals in the memory implies that their duration is reduced. We consider the applicability of the well-known efficiency estimates via the system cooperativity parameter and estimate a more general form. In connection with the theoretical description of the memory of the given type, we also discuss qualitative differences in the behavior of a random source introduced into the Heisenberg–Langevin equations for atomic variables in the cases of a large and a small number of atoms.

One-step implementation of quantum comtrolled-phase gate via quantum Zeno dynamics

We propose a scheme to implement a quantum controllable-phase gate via quantum Zeno dynamics. The two qubits are asymmetrically encoded by two four-level atoms coupled via a quantized cavity mode. Under proper conditions, the desirable logic operation can be implemented in one step. Since the qubit is encoded by the ground and the metastable states of the atom and the cavity mode is not really excited, our protocol is robust against the spontaneous decays of the atoms and cavity. Specifically, the feasibility of our generic proposal is demonstrated with two nitrogen-vacancy centers coupled to whispering-gallery microresonator.

Breaking the Carnot limit without violating the second law: A thermodynamic analysis of off-resonant quantum light generation

The Carnot limit, formulated in 1824, represents the maximal efficiency of a classical heat engine. In this work we present a thermodynamical analysis of a light amplifier based on a three-level atom coupled off-resonantly to a single quantized cavity mode and to two heat reservoirs with positive temperatures. Based on standard work and heat flow equilibrium, we show that for a cavity blue-detuned with respect to the atomic resonance, the system can surpass the Carnot limit. Nevertheless, the second law of thermodynamics is still obeyed, as the total entropy always increases. By analyzing a semiclassical version of the model, we derive a formula for the critical frequency for which the Carnot limit is broken and a formula for the amplifier efficiency which agrees with its quantum counterpart. In the semiclassical regime, however, the second law is not satisfied and hence it does not offer a physically acceptable description of the system. Finally, we show that breaking the Carnot limit occurs also in a blue-detuned quantum amplifier with output coupling, which represents a realistic model of a laser or maser.

Interaction of a quantum-dot cavity system with acoustic phonons: Stronger light-matter coupling can reduce the visibility of strong coupling effects

We present a numerically complete study of the combined dynamics of a quantum dot exciton coupled to a single quantized cavity mode and a continuum of acoustic phonons. We demonstrate that acoustic phonons have a pronounced impact on effects characteristic of the strong light-matter coupling regime, such as vacuum Rabi oscillations and collapse and revival scenarios. This impact is considerable already at zero temperature, where initially no phonons are present. Counterintuitively it is found that an increase of the light-matter coupling does not necessarily enhance the visibility of strong-coupling effects. In fact, for typical experimental situations, a stronger light-matter coupling will considerably reduce the visibility.

Controllable nonlinear effects in an optomechanical resonator containing a quantum well

We study nonlinear effects in an optomechanical system containing a quantum well. The nonlinearity due to the optomechanical coupling leads to a bistable behavior in the mean intracavity photon number and substantial squeezing in the transmitted field. We show that the optical bistability and the degree of squeezing can be controlled by tuning the power and frequency of the pump laser. The transmitted field intensity spectrum consists of six distinct peaks corresponding to optomechanical, polariton, and hybrid resonances. Interestingly, even though the quantum well and the mechanical modes are not directly coupled, their interaction with the common quantized cavity mode results in appearance of hybrid resonances.

Generation of Mesoscopic Entangled States in a Cavity Coupled to an Atomic Ensemble

We propose a novel scheme for the efficient production of entangled states for N photons of the form |N>(a)|0>(b) + |0>(a)|N>(b) (NOON states) based on the resonant interaction of a pair of quantized cavity modes with an ensemble of atoms. We show that, in the strong-coupling regime, the adiabatic evolution of the system tends to a limiting state that describes mesoscopic entanglement between photons and atoms which can easily be converted to a purely photonic or atomic NOON state. We also demonstrate the remarkable property that the efficiency of this scheme increases exponentially with the cavity cooperativity factor, which gives efficient access to high number NOON states. The experimental feasibility of the scheme is discussed, and its efficiency is demonstrated numerically.

Jaynes–Cummings photonic superlattices

A classical realization of the Jaynes-Cummings (JC) model, describing the interaction of a two-level atom with a quantized cavity mode, is proposed based on light transport in engineered waveguide superlattices. The optical setting enables us to visualize in Fock space dynamical regimes not yet accessible in quantum systems, providing new physical insights into the deep strong coupling regime of the JC model. In particular, bouncing of photon number wave packets in Hilbert space and revivals of populations are explained as generalized Bloch oscillations in an inhomogeneous tight-binding lattice.

Cavity quantum electrodynamics with a Rydberg-blocked atomic ensemble

The realization of a Jaynes-Cummings model in the optical domain is proposed for an atomic ensemble. The scheme exploits the collective coupling of the atoms to a quantized cavity mode and the nonlinearity introduced by coupling to high-lying Rydberg states. A two-photon transition resonantly couples the single-atom ground state $|g\ensuremath{\rangle}$ to a Rydberg state $|e\ensuremath{\rangle}$ via a nonresonant intermediate state $|i\ensuremath{\rangle}$, but due to the interaction between Rydberg atoms only a single atom can be resonantly excited in the ensemble. This restricts the state space of the ensemble to the collective ground state $|G\ensuremath{\rangle}$ and the collectively excited state $|E\ensuremath{\rangle}$ with a single Rydberg excitation distributed evenly on all atoms. The collectively enhanced coupling of all atoms to the cavity field with coherent coupling strengths which are much larger than the decay rates in the system leads to the strong coupling regime of the resulting effective Jaynes-Cummings model. We use numerical simulations to show that the cavity transmission can be used to reveal detailed properties of the Jaynes-Cummings ladder of excited states and that the atomic nonlinearity gives rise to highly nontrivial photon emission from the cavity. Finally, we suggest that the absence of interactions between remote Rydberg atoms may, due to a combinatorial effect, induce a cavity-assisted excitation blockade whose range is larger than the typical Rydberg dipole-dipole interaction length.

Photon-Number Selective Group Delay in Cavity Induced Transparency

We show that the group velocity of a probe pulse in an ensemble of Λ-type atoms driven by a quantized cavity mode depends on the quantum state-of-the input probe pulse. In the strong-coupling regime of the atom-cavity system the probe group delay is photon-number selective. This can be used to spatially separate the single photon from higher photon-number components of a few-photon probe pulse and thus create a deterministic single-photon source.