An array of radiatively coupled emitters is an exciting new platform for generating, storing, and manipulating quantum light. However, the simultaneous positioning and tuning of multiple lifetime-limited emitters into resonance remains a significant challenge. Here we report the creation of superradiant and subradiant entangled states in pairs of lifetime-limited and sub-wavelength spaced organic molecules by permanently shifting them into resonance with laser-induced tuning. The molecules are embedded as defects in an organic nanocrystal. The pump light redistributes charges in the nanocrystal and dramatically increases the likelihood of resonant molecules. The frequency spectra, lifetimes, and second-order correlation agree with a simple quantum model. This scalable tuning approach with organic molecules provides a pathway for observing collective quantum phenomena in sub-wavelength arrays of quantum emitters.
Collectivity in ensembles of atoms gives rise to effects like super- and subradiance. While superradiance is well studied and experimentally accessible, subradiance remains elusive since it is difficult to track experimentally as well as theoretically. Here we present a new type of phase transition in the resonantly driven, open Dicke model that leads to a deterministic generation of subradiant states. At the transition the system switches from a predominantly superradiant to a predominantly subradiant state. Clear experimental signatures for the effect are presented and entanglement propertie…
The propagation of a step pulse through a thick resonant absorber with homogeneously broadened absorption line is considered. It is shown that a specific subradiant state is naturally developed in the absorber due to the formation of the spatial domains of the atomic coherence with opposite phases. It is proposed to divide the absorber into slices in accord with these domains and place the phase shifters in front of the first slice and between the other slices. If the phase shifters are switched on simultaneously at a particular moment of time, elapsed from the beginning of the step pulse, a s…
Superradiance and subradiance concerning enhanced and inhibited collective radiation of an ensemble of atoms have been a central topic in quantum optics. However, precise generation and control of these states remain challenging. Here we deterministically generate up to 10-qubit superradiant and 8-qubit subradiant states, each containing a single excitation, in a superconducting quantum circuit with multiple qubits interconnected by a cavity resonator. The $\sqrt{N}$-scaling enhancement of the coupling strength between the superradiant states and the cavity is validated. By applying appropriat…
We propose a complete superradiant and subradiant states that can be manipulated and prepared in a three-dimensional atomic array. These subradiant states can be realized by absorbing a single photon and imprinting the spatially-dependent phases on the atomic system. We find that the collective decay rates and associated cooperative Lamb shifts are highly dependent on the phases we manage to imprint, and the subradiant state of long lifetime can be found for various lattice spacings and atom numbers. We also investigate both optically thin and thick atomic arrays, which can serve for systemati…
Disordered quantum networks, as those describing light-harvesting complexes, are often characterized by the presence of peripheral ring-like structures, where the excitation is initialized, and inner reaction centers (RC), where the excitation is trapped. The peripheral rings display coherent features: their eigenstates can be separated in the two classes of superradiant and subradiant states. Both are important to optimize transfer efficiency. In the absence of disorder, superradiant states have an enhanced coupling strength to the RC, while the subradiant ones are basically decoupled from it…
We report a time-resolved study of collective emission in dense ensembles of two-level atoms. We compare, on the same sample, the build-up of superradiance and subradiance from the ensemble when driven by a strong laser. This allows us to measure the dynamics of the population of superradiant and subradiant states as a function of time. In particular we demonstrate the build up in time of subradiant states through the superradiant dynamics. This illustrates the dynamics of the many-body density matrix of superradiant ensembles of two-level atoms when departing from the ideal conditions of Dick…
Using a non-Hermitian Hamiltonian approach to open systems, we study the interplay of disorder and superradiance in a one- and three-dimensional Anderson model. Analyzing the complex eigenvalues of the non-Hermitian Hamiltonian, a transition to a superradiant regime is shown to occur. As an effect of openness the structure of eigenstates undergoes a strong change in the superradiant regime: we show that the sensitivity to disorder of the superradiant and the subradiant subspaces is very different; superradiant states remain delocalized as disorder increases, while subradiant states are sensiti…
Using a non-Hermitian Hamiltonian approach to open systems, we study the interplay of disorder and superradiance in a one-dimensional Anderson model. Analyzing the complex eigenvalues of the non-Hermitian Hamiltonian, a transition to a superradiant regime is shown to occur. As an effect of openness the structure of eigenstates undergoes a strong change in the superradiant regime: we show that the sensitivity to disorder of the superradiant and the subradiant subspaces is very different; superradiant states remain delocalized as disorder increases, while subradiant states are sensitive to the d…
Disordered quantum networks, as those describing light-harvesting complexes, are often characterized by the presence of antenna structures where the light is captured and inner structures (reaction centers) where the excitation is transferred. Antennae often display distinguished coherent features: their eigenstates can be separated, with respect to the transfer of excitation, in the two classes of superradiant and subradiant states. Both are important to optimize transfer efficiency. In absence of disorder superradiant states have an enhanced coupling strength to the RC, while subradiant ones…
We develop a rigorous theoretical approach for analyzing inelastic scattering of photon pairs in arrays of two-level qubits embedded in a waveguide. Our analysis reveals strong enhancement of the scattering when the energy of incoming photons resonates with the double-excited subradiant states. We identify the role of different double-excited states in the scattering such as superradiant, subradiant, and twilight states, being a product of single-excitation bright and subradiant states. Importantly, the N-excitation subradiant states can be engineered only if the number of qubits exceeds 2N. B…
Resonant light interacting with matter can support different phases of a polarizable medium, and optical bistability where two such phases coexist. Here we identify signatures of optical phase transitions and optical bistability mapped onto scattered light in planar arrays of cold atoms. Methods on how to explore such systems in superradiant, and extreme subradiant states existing outside the light cone, are proposed. The cooperativity threshold and intensity regimes for the intrinsic optical bistability, supported by resonant dipole-dipole interactions alone, are derived in several cases of i…
Recent work has shown that collective single photon emission from an ensemble of resonate two-level atoms, i.e. single photon superradiance, is a rich field of study. The present paper addresses the flip side of superradiance, i.e. subradiance. Single photon subradiant states are potentially stable against collective spontaneous emission and can have ultrafast readout. In particular it is shown how many atom collective effects provide a new way to control spontaneous emission by preparing and switching between subradiant and superradiant states.
In this paper we study the spontaneous emission spectra and the emission decay rates of a simplest atom system that exhibits sub- and superradiant properties: a system which consists of two artificial atoms (superconducting qubits) embedded in a one-dimensional open waveguide. The calculations are based on the method of the transition operator which was firstly introduced by R. H. Lehmberg to theoretically describe the spontaneous emission of two-level atoms in a free space. We obtain the explicit expressions for the photon radiation spectra and the emission decay rates for different initial t…
One-dimensional (1D) subwavelength atom arrays display multiply excited subradiant eigenstates which are reminiscent of free fermions. So far, these states have been associated with subradiant states with decay rates $\propto N^{-3}$, with N the number of atoms, which fundamentally prevents detection of their fermionic features by optical means. In this Letter, we show that free-fermion states generally appear whenever the band of singly excited states has a quadratic dispersion relation at the band edge and, hence, may also be obtained with radiant and even superradiant states. 1D arrays have…
Weakly bound molecules have physical properties without atomic analogues, even as the bond length approaches dissociation. In particular, the internal symmetries of homonuclear diatomic molecules result in formation of two-body superradiant and subradiant excited states. While superradiance has been demonstrated in a variety of systems, subradiance is more elusive due to the inherently weak interaction with the environment. Here we characterize the properties of deeply subradiant molecular states with intrinsic quality factors exceeding $10^{13}$ via precise optical spectroscopy with the longe…
We theoretically investigate the light scattering of the super- and subradiant states which can be prepared by the excitation of a single photon which carries an orbital angular momentum (OAM).\ With this helical phase imprinted on the stacked ring of atomic arrays, the subradiant modes show directional side scattering in the far-field, allowing for light collimation and quantum storage of light with OAM.\ For the excitations with linear polarizations, we find a discrete $C_4$ rotational symmetry in scattering for the number of atoms $N$ $=$ $4n $ with integers $n$, while for circular polariza…
In super- or subradiance, a quantum superposition of excited atoms collectively emits a photon much more or much less rapidly than an isolated atom. Superradiant and subradiant lifetimes have been derived for finite spheres of uniform media, either by simulating random samples or by expanding in spherical harmonics and analyzing Bessel functions. We introduce a simple regulator that applies to unbounded media, enabling trivial derivation and analysis of lifetimes via elementary Fourier techniques. The regulator can be interpreted as a correlation length for atomic positions; the regularized sy…
We study the cooperative optical coupling between regularly spaced atoms in a one-dimensional waveguide using decompositions to subradiant and superradiant collective excitation eigenmodes, direct numerical solutions, and analytical transfer-matrix methods. We illustrate how the spectrum of transmitted light through the waveguide including the emergence of narrow Fano resonances can be understood by the resonance features of the eigenmodes. We describe a method based on superradiant and subradiant modes to engineer the optical response of the waveguide and to store light. The stopping of light…
We investigate collective radiant properties of two separated atoms in X-type quantum states. We show that quantum correlations measured by quantum discord (QD) can induce and enhance superradiance and subradiance in the two-atom system even though in the absence of interatomic quantum entanglement. We also explore quantum statistical properties of photons in the superradiance and subradiance by addressing the second-order correlation function. In particular, when the initial state of the two separated atoms is the Werner state with non-zero QD, we find that radiation photons in the superradia…
We develop a theoretical framework for the analysis of the quantum coherence of light emitted by two independent single-photon sources in an arbitrary environment. The theory provides design rules for the control of the degree of quantum coherence, in terms of classical quantities widely used in nanophotonics. As an important example, we derive generalized conditions to generate superradiant and subradiant states of the emitters, and demonstrate the ability of a structured environment to induce long-range quantum coherence. These results should have broad applications in quantum nanophotonics,…
Scaling law for optimal excitation storage and superradiant release in waveguide QED systems
National Taiwan University（台湾大学）；Institute of Atomic and Molecular Sciences, Academia Sinica（中央研究院原子与分子科学研究所）；Center for Quantum Science and Engineering, National Taiwan University（台湾大学量子科学与工程中心）；Trapped-Ion Quantum Computing Laboratory, Hon Hai Research Institute（鸿海研究院会离子阱量子计算实验室）；Physics Division, National Center for Theoretical Sciences（国家理论科学中心物理组）；Department of Physics, National Central University（中央大学物理系）
By modeling the coupling of multiple superconducting qubits to a single cavity in the circuit-quantum electrodynamics (QED) framework we find that it should be possible to observe superradiance and phase multistability using currently available technology. Due to the exceptionally large couplings present in circuit-QED we predict that superradiant microwave pulses should be observable with only a very small number of qubits (just three or four), in the presence of energy relaxation and non-uniform qubit-field coupling strengths. This paves the way for circuit-QED implementations of superradian…
We study numerically the slow (subradiant) decay of the fluorescence of motionless atoms after a weak pulsed excitation. We show that, in the linear-optics regime and for an excitation detuned by several natural linewidths, the slow decay rate can be dominated by close pairs of atoms (dimers) forming superradiant and subradiant states. However, for a large-enough resonant optical depth and at later time, the dynamics is dominated by collective many-body effects. In this regime, we study the polarization and the spectrum of the emitted light, as well as the spatial distribution of excitation in…
Light-matter interacting quantum systems manifest strong correlations that lead to distinct cooperative spontaneous emissions of subradiance or superradiance. To demonstrate the essence of long-range correlations in such systems, we consider an atomic array under the resonant dipole-dipole interactions (RDDI) and apply an interpretable machine learning with the integrated gradients to identify the crossover between the subradiant and superradiant sectors. The machine shows that the next nearest-neighbor couplings in RDDI play as much as the roles of nearest-neighbor ones in determining the who…
Single-photon superradiance can emerge when a collection of identical emitters are spatially separated by distances much less than the wavelength of the light they emit, and is characterized by the formation of a superradiant state that spontaneously emits light with a rate that scales linearly with the number of emitters. This collective phenomena has only been demonstrated in a few nanomaterial systems, all requiring temperatures below 10K. Here, we rationally design a single colloidal nanomaterial that hosts multiple (nearly) identical emitters that are impervious to the fluctuations which …
The coherent dipole-dipole interactions of atoms in an atomic array are studied. It is found that the excitation probability of an atom in an array parallel to the direction of laser propagation ($\boldsymbol{\hat{k}}$) will either grow or decay logarithmically along $\boldsymbol{\hat{k}}$, depending on the detuning of the laser. The symmetry of the system for atomic separations of $δr = jλ/2$, where $j$ is an integer, causes the excitation distribution and scattered radiation to abruptly become symmetric about the center of the array. For atomic separations of $δr < λ/2$, the appearance of a …
Atomic arrays provide an important quantum optical platform with photon-mediated dipoledipole interactions, which can be engineered to realize key applications in quantum information processing. A major obstacle for such application is the fast decay of the excited states. By controlling two-band Bloch oscillations in an atomic array under external magnetic field, here we show that exotic subradiance can be realized and maintained at a time scale upto 12 orders of magnitude larger than the spontaneous decay time in atomic arrays with the finite size. The key finding is to show a way for preven…
We consider the radiative properties of a system of two identical correlated atoms interacting with the electromagnetic field in its vacuum state in the presence of a generic dielectric environment. We suppose that the two emitters are prepared in a symmetric or antisymmetric superposition of one ground state and one excited state and we evaluate the transition rate to the collective ground state, showing distinctive cooperative radiative features. Using a macroscopic quantum electrodynamics approach to describe the electromagnetic field, we first obtain an analytical expression for the decay …
Photon-mediated interactions between quantum systems are essential for realizing quantum networks and scalable quantum information processing. We demonstrate such interactions between pairs of silicon-vacancy (SiV) color centers strongly coupled to a diamond nanophotonic cavity. When the optical transitions of the two color centers are tuned into resonance, the coupling to the common cavity mode results in a coherent interaction between them, leading to spectrally-resolved superradiant and subradiant states. We use the electronic spin degrees of freedom of the SiV centers to control these opti…
The control and manipulation of quantum-entangled non-local states is a crucial step for the development of quantum information processing. A promising route to achieve such states on a wide scale is to couple solid-state quantum emitters through their coherent dipole-dipole interactions. Entanglement in itself is challenging, as it requires both nanometric distances between emitters and nearly degenerate electronic transitions. Implementing hyperspectral imaging to identify pairs of coupled organic molecules trapped in a low temperature matrix, we reach distinctive spectral signatures of maxi…
We derive equations for the strongly coupled system of light and dense atomic ensembles. The formalism includes an arbitrary internal level structure for the atoms and is not restricted to weak excitation of atoms by light. In the low light intensity limit for atoms with a single electronic ground state, the full quantum field-theoretical representation of the model can be solved exactly by means of classical stochastic electrodynamics simulations for stationary atoms that represent cold atomic ensembles. Simulations for the optical response of atoms in a quantum degenerate regime require one …
The interaction between anharmonic quantum emitters (e.g., molecular vibrations) and confined electromagnetic fields gives rise to quantum states with optical and chemical properties that are different from those of their precursors. The exploration of these properties has been typically constrained to the first excitation manifold, the harmonic approximation, ensembles of two-level systems [Tavis-Cummings (TC) model], or the anharmonic single-molecule case. The present work studies, for the first time, a collective ensemble of identical multi-level anharmonic emitters and their dipolar intera…
A Rydberg atom array coupled to a high-cooperativity optical cavity
University of California, Berkeley（加州大学伯克利分校）；Challenge Institute for Quantum Computation, University of California, Berkeley（加州大学伯克利分校量子计算挑战研究所）；Columbia University（哥伦比亚大学）；Oratomic
