The collective spontaneous emission of two point-dipole emitters near a plasmonic core-shell nanosphere is theoretically investigated. Based on the expansion of mode functions in vector spherical harmonics, we derive closed analytical expressions for both the cooperative decay rate and the dipole-dipole interaction strength associated with two point dipoles close to a sphere. Considering a plasmonic nanoshell containing a linearly amplifying medium inside the core, the second-order correlation function for the two emitters shows that it is possible to tune the photon emission, selecting either photon bunching or antibunching as a function of the polarization and position of the sphere. This result opens vistas to applications involving tunable single-photon sources in engineered artificial media.
Starting from a fully quantized Hamiltonian for an ensemble of identical emitters coupled to the modes of an optical cavity, we determine analytically regimes of thermal, collective anti-bunching and laser emission that depend explicitly on the number of emitters. The lasing regime is reached for a number of emitters above a critical number (which depends on the light-matter coupling, detuning and the dissipation rates) via a universal transition from thermal emission to collective anti-bunching to lasing as the pump increases. Cases where the second order intensity correlation fails to predic…
In a recent Letter [Phys. Rev. Lett. 126, 063902 (2021)], M. A. Carroll et al. derived a model to analytically determine regimes of thermal, collective anti-bunching, and laser emission for emitters in a cavity. According to their model, nanolasers exhibit a distinct threshold at which the coherent laser field emerges from a bifurcation at a finite pump rate. The amplitude of this coherent field increases with a further increase in the pump rate. Such a behavior contrasts the usual view of the transition to lasing in single-mode high-$β$ nanolasers, according to which strong spontaneous emissi…
We deconstruct and address a comment to Carroll et al. [Phys Rev Lett 126, 063902 (2021)] (PRL) that has been posted on arXiv appearing as two versions [arXiv:2106.15242v1] and [arXiv:2106.15242v2]. This comment claimed that a term in the model presented in the PRL had been incorrectly omitted and that, hence, the laser threshold predicted by the model in the PRL is unattainable. We show that the term in question was correctly neglected because it represents collective effects that are not observable in the devices modelled in the PRL. Moreover, even if this term were to be included, the laser…
In general, the typical approach to discriminate antibunching, bunching or superbunching categories make use of calculating the second-order coherence function ${g^{(2)}}(τ)$ of light. Although the classical light sources correspond to the specific degree of second-order coherence ${g^{(2)}}(0)$, it does not alone constitute a distinguishable metric to characterize and determine light sources. Here we propose a new mechanism to directly classify and generate antibunching, bunching or superbunching categories of light, as well as the classical light sources such as thermal and coherent light, b…
Photon-number statistics of the emitted photons from a quantum dot placed in the vicinity of a metallic nanoparticle (with either shell or solid-sphere geometry) in the non-Markovian regime is investigated theoretically. In the model scheme, the quantum dot is considered as a InAs three- level system in Lambda-type configuration with two transition channels. One of channels is driven by a polarized classical field while the two channels are coupled to the plasmon modes. Plasmon resonance modes of a nanoshell, in contrast of a nanosphere, are tunable at demand frequency by controlling the thick…
The impulsive excitation of ensembles of excitons or color centers by a high-energy electron beam results in the observation of photon bunching in the second-order correlation function of the cathodoluminescence generated by those emitters. Photon bunching in cathodoluminescence microscopy can be used to resolve the excited-state dynamics and the excitation and emission efficiency of nanoscale materials, and it can be used to probe interactions between emitters and nanophotonic cavities. Here, we report substantial changes in the measured bunching induced by indirect electron interactions (wit…
We report the observation of an anomalous antibunching dip in intensity autocorrelation function with photon correlation measurements on a single-photon emitter (SPE). We show that the anomalous dip observed is a manifestation of quantum nature of SPEs. Taking population dynamics in a quantum two-level system into account correctly, we redefine intensity autocorrelation function. This is of primary importance for precisely evaluating the lowest-level probability of multiphoton generation in SPEs toward realizing versatile pure SPEs for quantum information and communication.
One of the main characteristics of optical imaging systems is the spatial resolution, which is restricted by the diffraction limit to approximately half the wavelength of the incident light. Along with the recently developed classical super-resolution techniques, which aim at breaking the diffraction limit in classical systems, there is a class of quantum super-resolution techniques which leverage the non-classical nature of the optical signals radiated by quantum emitters, the so-called antibunching super-resolution microscopy. This approach can ensure a factor of $\sqrt{n}$ improvement in th…
Single photon sources (SPS), especially those based on solid state quantum emitters, are key elements in future quantum technologies. What is required is the development of broadband, high quantum efficiency, room temperature SPS which can also be tunably coupled to optical cavities which could lead to development of all-optical quantum communication platforms. In this regard deterministic coupling of SPS to plasmonic nanocavity arrays has great advantage due to long propagation length and delocalized nature of surface lattice resonances (SLRs). Guided by these considerations, we report experi…
We analyze the second-order photon autocorrelation function $g^{(2)}$ with respect to the photon probability distribution and discuss the generic features of a distribution that result in superthermal photon bunching ($g^{(2)}>2$). Superthermal photon bunching has been reported for a number of optical microcavity systems that exhibit processes like superradiance or mode competition. We show that a superthermal photon number distribution cannot be constructed from the principle of maximum entropy, if only the intensity and the second-order autocorrelation are given. However, for bimodal systems…
A robust process for fabricating intrinsic single-photon emitters in silicon nitride has been recently established. These emitters show promise for quantum applications due to room-temperature operation and monolithic integration with the technologically mature silicon nitride photonics platform. Here, the fundamental photophysical properties of these emitters are probed through measurements of optical transition wavelengths, linewidths, and photon antibunching as a function of temperature from 4.2K to 300K. Important insight into the potential for lifetime-limited linewidths is provided throu…
We analyze the process of simultaneous photon pair generation and quantum walks realized by spontaneous parametric down conversion of a pump beam in a quadratic nonlinear waveguide array. We demonstrate that this flexible platform allows for creating quantum states with different spatial correlations. In particular, we predict that the output photon correlations can be switched from photon bunching to antibunching controlled entirely classically by varying the temperature of the array or the spatial profile of the pump beam.
We propose the use of weakly nonlinear passive materials for prospective applications in integrated quantum photonics. It is shown that strong enhancement of native optical nonlinearities by electromagnetic field confinement in photonic crystal resonators can lead to single-photon generation only exploiting the quantum interference of two coupled modes and the effect of photon blockade under resonant coherent driving. For realistic system parameters in state of the art microcavities, the efficiency of such single-photon source is theoretically characterized by means of the second-order correla…
We introduce a scheme of single photon emission based on four-wave mixing in a three mode system with weak Kerr-type nonlinearity. A highly populated lower energy mode results in strong stimulated scattering of particle pairs out of the central mode, which consequently limits the central mode occupation. Thus, the system can be reduced to a $χ^{(2)}$ nonlinear medium with greatly enhanced interaction constant. As a model setup we consider dipolaritons in semiconductor microcavities. Using the master equation approach we show strong antibunching under continuous wave pump, which largely exceeds…
We report a new way to slow down the spontaneous emission rate of excitons in the wetting layer (WL) through radiative field coupling between the exciton emissions and the dipole field of metal islands. As a result, a long-lifetime decay process is detected in the emission of InAs/GaAs single quantum dots (QDs). It is found that when the separation distance from WL layer (QD layer) to the metal islands is around 20 nm and the islands have an average size of approximately 50 nm, QD lifetime may change from approximately 1 to 160 ns. The corresponding second-order autocorrelation function g(2) (…
The implementation of non-classical light sources is becoming increasingly important for various quantum applications. A particularly interesting approach is to integrate such functionalities on a single chip as this could pave the way towards fully scalable quantum photonic devices. Several approaches using dielectric systems have been investigated in the past. However, it is still not understood how on-chip nanoplasmonic antennas, interacting with a single quantum emitter, affect the quantum statistics of photons reflected or transmitted in the guided mode of a waveguide. Here we investigate…
We derive the statistics of scattered photons from a $Λ$- or ladder-type three-level emitter (3LE) embedded in a 1D open waveguide. The weak probe photons in the waveguide are coupled to one of the two allowed transitions of the 3LE, and the other transition is driven by a control beam. This system shows electromagnetically induced transparency (EIT) which is accompanied with the Autler-Townes splitting (ATS) at a strong driving by the control beam, and some of these effects have been observed recently. We show that the nature of second-order coherence of the transmitted probe photons near two…
We study the correlated transport of photons through a chain of three-level emitters that are coupled chirally to a photonic mode of a waveguide. It is found that this system can transfer a classical input into a strongly correlated state of light in a unitary manner, i.e. without the necessity of nonlinear photon losses. In particular, we shows that the collective interaction with the emitter ensemble leads to the emergence of highly antibunched light with long-range correlations upon crossing a critical length of the chain. By operating close to conditions of electromagnetically induced tran…
Single photon sources with high brightness and subnanosecond lifetimes are key components for quantum technologies. Optical nanoantennas can enhance the emission properties of single quantum emitters, but this approach requires accurate nanoscale positioning of the source at the plasmonic hotspot. Here, we use plasmonic nanoantennas to simultaneously trap single colloidal quantum dots and enhance their photoluminescence. The nano-optical trapping automatically locates the quantum emitter at the nanoantenna hotspot without further processing. Our dedicated nanoantenna design achieves a high tra…
We develop a general theoretical framework to dynamically engineer quantum correlations in the frequency-comb emission from an array of superconducting qubits in a waveguide, rigorously accounting for the temporal modulation of the qubit resonance frequencies. We demonstrate, that when the resonance frequencies of the two qubits are periodically modulated with a $π$ phase shift, it is possible to realize simultaneous bunching and antibunching in cross-correlations of the scattered photons from different sidebands. Our approach, based on the dynamical conversion between the quantum excitations …
The two-photon Hong-Ou-Mandel (HOM) interference is a pure quantum effect which indicates the degree of indistinguishability of photons. The four-photon HOM interference exhibits richer dynamics in comparison to the two-photon interference and simultaneously is more sensitive to the input photon states. We demonstrate theoretically and experimentally an explicit dependency of the four-photon interference to the number of temporal modes, created in the process of parametric down-conversion. Moreover, we exploit the splitting ratio of the beam splitter to manipulate the interference between bunc…
We show that strongly correlated photon transport can be observed in waveguides containing optically dense ensembles of emitters. Remarkably, this occurs even for weak coupling efficiencies. Specifically, we compute the photon transport properties through a chirally coupled system of $N$ two-level systems driven by a weak coherent field, where each emitter can also scatter photons out of the waveguide. The photon correlations arise due to an interplay of nonlinearity and coupling to a loss reservoir, which creates a strong effective interaction between transmitted photons. The highly correlate…
Room Temperature Collective Blinking and Photon Bunching from CsPbBr3 Quantum Dot Superlattice
Institute of Science Tokyo（东京科学大学）；Katholieke Universiteit Leuven（荷语鲁汶大学）；Lingnan Normal University（岭南师范学院）；Max Planck Institute for Polymer Research（马克斯·普朗克聚合物研究所）
Quantum frequency conversion (QFC), a nonlinear optical process in which the frequency of a quantum light field is altered while conserving its non-classical correlations, was first demonstrated 20 years ago. Meanwhile, it is considered an essential tool for the implementation of quantum repeaters since it allows for interfacing quantum memories with telecom-wavelength photons as quantum information carriers. Here we demonstrate efficient (>30%) QFC of visible single photons (711 nm) emitted by a quantum dot (QD) to a telecom wavelength (1,313 nm). Analysis of the first and second-order cohere…
Electron-beam Writing of Spectrally Uniform Green Single-photon Emitters in Hexagonal Boron Nitride
Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences（中国科学院大学杭州高等研究院）；Zhejiang University（浙江大学）；University of Science and Technology of China（中国科学技术大学）；Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences（中国科学院上海光学精密机械研究所）
This thesis is devoted to the study of the coupling of single-photon emitters with photonic nanostructures by using the properties of the near field of a photonic structure in view of the realization of a compact integrated single-photon source for quantum applications. The first part of my thesis work was consecrated to the optimization of perovskites nanocrystals. Although perovskites nanocrystals are very promising single-photon sources, they still need improvements: in this work, I review the main properties of these emitters and present a full characterization of perovskite nanocrystals w…
The interest in perovskite nanocrystals (NCs) such as CsPbBr$_3$ for quantum applications is rapidly raising, as it has been demonstrated that they can behave as very efficient single photon emitters. The main problem to tackle in this context is their photo-stability under optical excitation. In this article, we present a full analysis of the optical and quantum properties of highly efficient perovskite nanocubes synthesized with an established method, which is used for the first time to produce quantum emitters, and is shown to ensure an increased photostability. These emitters exhibit reduc…
Photon bunching in incoherent cathodoluminescence (CL) spectroscopy originates from the fact that a single high-energy electron can generate multiple photons when interacting with a material, thus revealing key properties of electron-matter excitation. Contrary to previous works based on Monte-Carlo modelling, here we present a fully analytical model describing the amplitude and shape of the second order autocorrelation function ($g^{(2)}(τ)$) for continuous and pulsed electron beams. Moreover, we extend the analysis of photon bunching to ultrashort electron pulses, in which up to 500 electron…
The present dissertation covers two related research projects. The first topic was initiated with the ultimate goal of observing quantum degeneracy in ultrashort free electron pulses. This constitutes a thorough theoretical analysis of the problem involving partial quantum coherence and spin polarization of the source in light of a path-integral treatment of the phenomenon of matter-wave diffraction-in-time. Subsequently, results of a trailblazing experiment, to be superseded by a Hanbury Brown-Twiss type conclusive test of free fermion antibunching with electrons, is reported. In this experim…
We investigate two-photon quantum interference in an opaque scattering medium that intrinsically supports $10^6$ transmission channels. By adaptive spatial phase-modulation of the incident wavefronts, the photons are directed at targeted speckle spots or output channels. From $10^3$ experimentally available coupled channels, we select two channels and enhance their transmission, to realize the equivalent of a fully programmable $2\times2$ beam splitter. By sending pairs of single photons from a parametric down-conversion source through the opaque scattering medium, we observe two-photon quantu…
Quantum walk represents one of the most promising resources for the simulation of physical quantum systems, and has also emerged as an alternative to the standard circuit model for quantum computing. Up to now the experimental implementations have been restricted to single particle quantum walk, while very recently the quantum walks of two identical photons have been reported. Here, for the first time, we investigate how the particle statistics, either bosonic or fermionic, influences a two-particle discrete quantum walk. Such experiment has been realized by adopting two-photon entangled state…
We report on experimental study into the effects of surface acoustic waves on the optical emission of dot-in-a-nanowire heterostructures in III-V material systems. Under direct optical excitation, the excitonic energy levels in III-nitride dot-in-a-nanowire heterostructures oscillate at the acoustic frequency, producing a characteristic splitting of the emission lines in the time-integrated photoluminescence spectra. This acoustically induced periodic tuning of the excitonic transition energies is combined with spectral detection filtering and employed as a tool to regulate the temporal output…
Optical non-linearities at the single-photon level are key ingredients for future photonic quantum technologies. Prime candidates for the realization of strong photon-photon interactions necessary for implementing quantum information processing tasks as well as for studying strongly correlated photons in an integrated photonic device setting are quantum dots embedded in photonic crystal nanocavities. Here, we report strong quantum correlations between photons on picosecond timescales. We observe (a) photon antibunching upon resonant excitation of the lowest-energy polariton state, proving that…
Bloch Oscillations (BOs) of quantum particles manifest themselves as periodic spreading and re-localization of the associated wave functions when traversing lattice potentials subject to external gradient forces. Albeit BOs are deeply rooted into the very foundations of quantum mechanics, all experimental observations of this phenomenon so far have only contemplated dynamics of one or two particles initially prepared in separable local states, which is well described by classical wave physics. Evidently, a more general description of genuinely quantum BOs will be achieved upon excitation of a …
