Ensemble Of Emitters Research Articles

Large Scale Simulations of Photosynthetic Antenna Systems: Interplay of Cooperativity and Disorder.

Large-scale simulations of light-matter interaction in natural photosynthetic antenna complexes containing more than one hundred thousands of chlorophyll molecules, comparable with natural size, have been performed. Photosynthetic antenna complexes present in Green sulfur bacteria and Purple bacteria have been analyzed using a radiative non-Hermitian Hamiltonian, well-known in the field of quantum optics, instead of the widely used dipole-dipole Frenkel Hamiltonian. This approach allows us to study ensembles of emitters beyond the small volume limit (system size much smaller than the absorbed wavelength), where the Frenkel Hamiltonian fails. When analyzed on a large scale, such structures display superradiant states much brighter than their single components. An analysis of the robustness to static disorder and dynamical (thermal) noise shows that exciton coherence in the whole photosynthetic complex is larger than the coherence found in its parts. This provides evidence that the photosynthetic complex as a whole plays a predominant role in sustaining coherences in the system even at room temperature. Our results allow a better understanding of natural photosynthetic antennae and could drive experiments to verify how the response to electromagnetic radiation depends on the size of the photosynthetic antenna.

How Single-Photon Switching Is Quenched with Multiple Λ-Level Atoms.

Single-photon nonlinearity, namely, the change in the response of the system as the result of the interaction with a single photon, is generally considered an inherent property of a single quantum emitter. Although the dependence on the number of emitters is well understood for the case of two-level systems, deterministic operations such as single-photon switching or photon-atom gates inherently require more complex level structures. Here, we theoretically consider single-photon switching in ensembles of emitters with a Λ-level scheme and show that the switching efficiency vanishes with the number of emitters. Interestingly, the mechanism behind this behavior is the quantum Zeno effect, manifested in a slowdown of the photon-controlled dynamics of the atomic ground states.

Reducing Effective System Dimensionality with Long-Range Collective Dipole-Dipole Interactions.

Dimensionality plays a crucial role in long-range dipole-dipole interactions (DDIs). We demonstrate that a resonant nanophotonic structure modifies the apparent dimensionality in an interacting ensemble of emitters, as revealed by population decay dynamics. Our measurements on a dense ensemble of interacting quantum emitters in a resonant nanophotonic structure with long-range DDIs reveal an effective dimensionality reduction to d[over ¯]=2.20(12), despite the emitters being distributed in 3D. This contrasts with the homogeneous environment, where the apparent dimension is d[over ¯]=3.00. Our work presents a promising avenue to manipulate dimensionality in an ensemble of interacting emitters.

Selective Generation of Luminescent Defects in Hexagonal Boron Nitride

AbstractSingle photon emitters from atomic defects in crystals like hexagonal boron nitride (hBN) are vital for quantum technologies. Although various techniques are devised to obtain defects emission in hBN, simultaneous control over defects position, type, and emission spectrum has not been achieved yet. Here, ion implantation with 12C, 20Ne, and 69Ga are used to create a composite defects population with emission ≈820 nm. The correlation of Raman and photoluminescence (PL) spectroscopy helps to identify the defects’ type. After selecting Ga as the ion species yielding the maximum emitter brightness, a strategy based on thermal annealing is developed to modify the composition of the induced defects. This results in an emitter ensemble with selected spectral properties, even when starting from different implantation conditions. Specifically, thermal annealing induces a defect transmutation from one type to another, shifting the emission wavelength from 820 to 625 nm. Moreover, sample patterning is combined with focused ion beam implantation and subsequent annealing in an efficient method to deterministically set the defects position as well as the PL spectral composition. These results offer a practical avenue to achieve in situ positioning and tuning of ensembles of emitters in hBN, promising for quantum information and sensing applications.

Modified dipole-dipole interactions in the presence of a nanophotonic waveguide

When an emitter ensemble interacts with the electromagnetic field, dipole-dipole interactions are induced between the emitters. The magnitude and shape of these interactions are fully determined by the specific form of the electromagnetic field modes. If the emitters are placed in the vicinity of a nanophotonic waveguide, such as a cylindrical nanofiber, the complex functional form of these modes makes the analytical evaluation of the dipole-dipole interaction cumbersome and numerically costly. In this work, we provide a full detailed description of how to successfully calculate these interactions, outlining a method that can be easily extended to other environments and boundary conditions. Such exact evaluation is of importance as, due to the collective character of the interactions and dissipation in this kind of systems, any small modification of the interactions may lead to dramatic changes in experimental observables, particularly as the number of emitters increases. We illustrate this by calculating the transmission signal of the light guided by a cylindrical nanofiber in the presence of a nearby chain of emitters.

INCLUDING THE OWN FIELDS OF QUANTUM EMITTERS IN DESCRIBING GENERATION REGIMES

The paper discusses three different modes of electromagnetic field generation by an ensemble of quantum emitters placed at the radiation wavelength in the one-dimensional case. The excitation of the resonator field is considered, which, as a rule, is determined by the geometry of the system, with and without taking into account the eigenfields of the emitters. The superradiance mode of the same ensemble of emitters is also analyzed. Since the main indicator of generation is the level of energy output from the system, the position of the maximum of this indicator determines the operating point of the device. Taking into account the intrinsic field of the emitters enhances the generation intensity and significantly changes the position of the operating point.

Interplay between disorder, local relaxation, and collective behavior for an ensemble of emitters outside versus inside a cavity

Interplay between disorder, local relaxation, and collective behavior for an ensemble of emitters outside versus inside a cavity

Dicke Superradiance Requires Interactions beyond Nearest Neighbors.

Photon-mediated interactions within an excited ensemble of emitters can result in Dicke superradiance, where the emission rate is greatly enhanced, manifesting as a high-intensity burst at short times. The superradiant burst is most commonly observed in systems with long-range interactions between the emitters, although the minimal interaction range remains unknown. Here, we put forward a new theoretical method to bound the maximum emission rate by upper bounding the spectral radius of an auxiliary Hamiltonian. We harness this tool to prove that for an arbitrary ordered array with only nearest-neighbor interactions in all dimensions, a superradiant burst is not physically observable. We show that Dicke superradiance requires minimally the inclusion of next-nearest-neighbor interactions. For exponentially decaying interactions, the critical coupling is found to be asymptotically independent of the number of emitters in all dimensions, thereby defining the threshold interaction range where the collective enhancement balances out the decoherence effects. Our findings provide key physical insights to the understanding of collective decay in many-body quantum systems, and the designing of superradiant emission in physical systems for applications such as energy harvesting and quantum sensing.

Simulating molecular polaritons in the collective regime using few-molecule models.

The study of molecular polaritons beyond simple quantum emitter ensemble models (e.g., Tavis-Cummings) is challenging due to the large dimensionality of these systems and the complex interplay of molecular electronic and nuclear degrees of freedom. This complexity constrains existing models to either coarse-grain the rich physics and chemistry of the molecular degrees of freedom or artificially limit the description to a small number of molecules. In this work, we exploit permutational symmetries to drastically reduce the computational cost of ab initio quantum dynamics simulations for large N. Furthermore, we discover an emergent hierarchy of timescales present in these systems, that justifies the use of an effective single molecule to approximately capture the dynamics of the entire ensemble, an approximation that becomes exact as N → ∞. We also systematically derive finite N corrections to the dynamics and show that addition of k extra effective molecules is enough to account for phenomena whose rates scale as 𝒪(N-k). Based on this result, we discuss how to seamlessly modify existing single-molecule strong coupling models to describe the dynamics of the corresponding ensemble. We call this approach collective dynamics using truncated equations (CUT-E), benchmark it against well-known results of polariton relaxation rates, and apply it to describe a universal cavity-assisted energy funneling mechanism between different molecular species. Beyond being a computationally efficient tool, this formalism provides an intuitive picture for understanding the role of bright and dark states in chemical reactivity, necessary to generate robust strategies for polariton chemistry.

Superradiance-Mediated Photon Storage for Broadband Quantum Memory

Superradiance, characterized by the collective, coherent emission of light from an excited ensemble of emitters, generates photonic signals on timescales faster than the natural lifetime of an individual atom. The rapid exchange of coherence between atomic emitters and photonic fields in the superradiant regime enables a fast, broadband quantum memory. We demonstrate this superradiance memory mechanism in an ensemble of cold rubidium atoms and verify that this protocol is suitable for pulses on timescales shorter than the atoms' natural lifetime. Our simulations show that the superradiance memory protocol yields the highest bandwidth storage among protocols in the same system. These high-bandwidth quantum memories provide unique opportunities for fast processing of optical and microwave photonic signals, with applications in large-scale quantum communication and quantum computing technologies.

Cavity spectral-hole-burning to boost coherence in plasmon-emitter strong coupling systems

Significant decoherence of the plasmon-emitter (i.e., plexcitonic) strong coupling systems hinders the progress towards their applications in quantum technology due to the unavoidable lossy nature of the plasmons. Inspired by the concept of spectral-hole-burning (SHB) for frequency-selective bleaching of the emitter ensemble, we propose ‘cavity SHB’ by introducing cavity modes with moderate quality factors to the plexcitonic system to boost its coherence. We show that the detuning of the introduced cavity mode with respect to the original plexcitonic system, which defines the location of the cavity SHB, is the most critical parameter. Simultaneously introducing two cavity modes of opposite detunings, the excited-state population of the emitter can be enhanced by 4.5 orders of magnitude within 300 fs, and the attenuation of the emitter’s population can be slowed down by about 56 times. This theoretical proposal provides a new approach of cavity engineering to enhance the plasmon-emitter strong coupling systems’ coherence, which is important for realistic hybrid-cavity design for applications in quantum technology.

Plasmon-induced coherence, exciton-induced transparency, and Fano interference for hybrid plasmonic systems in strong coupling regime.

We present an analytical model describing the transition to a strong coupling regime for an ensemble of emitters resonantly coupled to a localized surface plasmon in a metal-dielectric structure. The response of a hybrid system to an external field is determined by two distinct mechanisms involving collective states of emitters interacting with the plasmon mode. The first mechanism is the near-field coupling between the bright collective state and the plasmon mode, which underpins the energy exchange between the system components and gives rise to exciton-induced transparency minimum in scattering spectra in the weak coupling regime and to emergence of polaritonic bands as the system transitions to the strong coupling regime. The second mechanism is the Fano interference between the plasmon dipole moment and the plasmon-induced dipole moment of the bright collective state as the hybrid system interacts with the radiation field. The latter mechanism is greatly facilitated by plasmon-induced coherence in a system with the characteristic size below the diffraction limit as the individual emitters comprising the collective state are driven by the same alternating plasmon near field and, therefore, all oscillate in phase. This cooperative effect leads to scaling of the Fano asymmetry parameter and of the Fano function amplitude with the ensemble size, and therefore, it strongly affects the shape of scattering spectra for large ensembles. Specifically, with increasing emitter numbers, the Fano interference leads to a spectral weight shift toward the lower energy polaritonic band.

En route to nanoscopic quantum optical imaging: counting emitters with photon-number-resolving detectors.

The fundamental understanding of biological pathways requires minimally invasive nanoscopic optical resolution imaging. Many approaches to high-resolution imaging rely on localization of single emitters, such as fluorescent molecules or quantum dots. Additionally, the exact determination of the number of such emitters in an imaging volume is essential for a number of applications; however, in standard intensity-based microscopy it is not possible to determine the number of individual emitters within a diffraction limited spot without initial knowledge of system parameters. Here we explore how quantum measurements of the emitted photons using photon number resolving detectors can be used to address this challenging task. In the proposed new approach, the problem of counting emitters reduces to the task of determining differences between the emitted photon distribution and the Poisson limit. We show that quantum measurements of the number of photons emitted from an ensemble of emitters enable the determination of both the number of emitters and the probability of emission. This method can be applied for any type of single-photon emitters. The scaling laws of this new approach are presented by the Cramer-Rao Lower Bounds, and this technique has great potential in quantum optical imaging with nanoscopic resolution.

Experimental investigation of light-matter interaction when transitioning from cavity QED to waveguide QED

Cavity quantum electrodynamics (cavity QED) is conventionally described by the Jaynes- or Tavis-Cummings model, where quantum emitters couple to a single-mode cavity. The opposite scenario, in which an ensemble of emitters couples to a single spatial mode of a propagating light field, is described by waveguide QED, where emitters interact with a continuum of frequency modes. Here we present an experiment where an ensemble of cold atoms strongly couples to a fiber-ring resonator with variable length containing an optical nanofiber. By changing the length of the resonator we can tailor the density of frequency modes and thus explore the transition from cavity QED to waveguide QED. We analyse the response of the ensemble–cavity system after the sudden switch-on of resonant laser light and find that for progressively longer resonators, the Rabi oscillations typical of cavity QED disappear and the single-pass dynamics of waveguide QED appear. Our measurements shed light on the interplay between the single-pass collective response of the atoms to the propagating cavity field and the ensemble–cavity dynamics.

Bright CdSe/CdS Quantum Dot Light-Emitting Diodes with Modulated Carrier Dynamics via the Local Kirchhoff Law.

Addressing the interactions between optical antennas and ensembles of emitters is particularly challenging. Charge transfer and Coulomb interactions complicate the understanding of the carrier dynamics coupled by antennas. Here, we show how Au antennas enhance the luminescence of CdSe/CdS quantum dot assemblies through carrier dynamics control within the framework of the local Kirchhoff law. The Au antennas inject hot electrons into quantum dot assemblies via plasmon-induced hot electron transfer that increases the carrier concentration. Also, the localized surface plasmon resonances of Au antennas favorably tilt the balance between nonradiative Auger processes and radiative recombination in the CdSe core. Eventually, a high bright (125,091.6 cd/m2) deep-red quantum dot light-emitting diode is obtained by combining with Au antennas. Our findings suggest a new understanding of light emission of assembled emitters coupled by antennas, which is of essential interest for the description of light-matter interaction in advanced optoelectronics.

Long-Range Dipole-Dipole Interactions in a Plasmonic Lattice.

Spontaneous emission of quantum emitters can be enhanced by increasing the local density of optical states, whereas engineering dipole-dipole interactions requires modifying the two-point spectral density function. Here, we experimentally demonstrate long-range dipole-dipole interactions (DDIs) mediated by surface lattice resonances in a plasmonic nanoparticle lattice. Using angle-resolved spectral measurements and fluorescence lifetime studies, we show that unique nanophotonic modes mediate long-range DDI between donor and acceptor molecules. We observe significant and persistent DDI strengths for a range of densities that map to ∼800 nm mean nearest-neighbor separation distance between donor and acceptor dipoles, a factor of ∼100 larger than free space. Our results pave the way to engineer and control long-range DDIs between an ensemble of emitters at room temperature.

Dynamical Phases and Quantum Correlations in an Emitter-Waveguide System with Feedback.

We investigate the creation and control of emergent collective behavior and quantum correlations using feedback in an emitter-waveguide system using a minimal model. Employing homodyne detection of photons emitted from a laser-driven emitter ensemble into the modes of a waveguide allows for the generation of intricate dynamical phases. In particular, we show the emergence of a time-crystal phase, the transition to which is controlled by the feedback strength. Feedback enables furthermore the control of many-body quantum correlations, which become manifest in spin squeezing in the emitter ensemble. Developing a theory for the dynamics of fluctuation operators we discuss how the feedback strength controls the squeezing and investigate its temporal dynamics and dependence on system size. The largely analytical results allow to quantify spin squeezing and fluctuations in the limit of large number of emitters, revealing critical scaling of the squeezing close to the transition to the time crystal. Our study corroborates the potential of integrated emitter-waveguide systems-which feature highly controllable photon emission channels-for the exploration of collective quantum phenomena and the generation of resources, such as squeezed states, for quantum enhanced metrology.

Spatial coherence of light emitted by thermalized ensembles of emitters coupled to surface waves

The authors propose a general absorption-coherence relation to show that spatial coherence emission by molecules on a metallic film is due to the excitation of surface plasmon polaritons and is reduced in the presence of strong coupling.

Suppressing decoherence in quantum plasmonic systems by the spectral-hole-burning effect

Quantum plasmonic systems suffer from significant decoherence due to the intrinsically large dissipative and radiative dampings. Based on our quantum simulations via a quantum tensor network algorithm, we numerically demonstrate the mitigation of this restrictive drawback by hybridizing a plasmonic nanocavity with an emitter ensemble with inhomogeneously-broadened transition frequencies. By burning two narrow spectral holes in the spectral density of the emitter ensemble, the coherent time of Rabi oscillation for the hybrid system is increased tenfold. With the suppressed decoherence, we move one step further in bringing plasmonic systems into practical quantum applications.

Disorder-Enhanced and Disorder-Independent Transport with Long-Range Hopping: Application to Molecular Chains in Optical Cavities.

Overcoming the detrimental effect of disorder at the nanoscale is very hard since disorder induces localization and an exponential suppression of transport efficiency. Here we unveil novel and robust quantum transport regimes achievable in nanosystems by exploiting long-range hopping. We demonstrate that in a 1D disordered nanostructure in the presence of long-range hopping, transport efficiency, after decreasing exponentially with disorder at first, is then enhanced by disorder [disorder-enhanced transport (DET) regime] until, counterintuitively, it reaches a disorder-independent transport (DIT) regime, persisting over several orders of disorder magnitude in realistic systems. To enlighten the relevance of our results, we demonstrate that an ensemble of emitters in a cavity can be described by an effective long-range Hamiltonian. The specific case of a disordered molecular wire placed in an optical cavity is discussed, showing that the DIT and DET regimes can be reached with state-of-the-art experimental setups.