Quantum dots (QDs) based on III-nitride semiconductors are promising for single photon emission at non-cryogenic temperatures due to their large exciton binding energies. Here, we demonstrate GaN QD single photon emitters operating at 300 K with $g^{(2)}(0) = 0.17 \pm 0.08$ under continuous wave excitation. At this temperature, single photon emission rates up to $6\times10^6 \, \text{s}^{-1}$ are reached while $g^{(2)}(0) \leq 0.5$ is maintained. Our results are achieved for GaN QDs embedded in a planar AlN layer grown on silicon, representing a promising pathway for future interlinkage with optical waveguides and cavities. These samples allow exploring the limiting factors to key performance metrics for single photon sources, such as brightness and single photon purity. While high brightness is assured by large exciton binding energies, the single photon purity is mainly affected by the spectral overlap with the biexcitonic emission. Thus, the performance of a GaN QD as a single photon emitter depends on the balance between the emission linewidth and the biexciton binding energy. We identify small GaN QDs with an emission energy in excess of 4.2 eV as promising candidates for future room temperature applications, since the biexciton binding energy becomes comparable to the average emission linewidth of around 55 meV.
We investigate exciton states theoretically in strained GaN/AlN quantum dots with wurtzite (WZ) and zinc-blende (ZB) crystal structures, as well as strained WZ GaN/AlGaN quantum dots. We show that the strain field significantly modifies the conduction and valence band edges of GaN quantum dots. The piezoelectric field is found to govern excitonic properties of WZ GaN/AlN quantum dots, while it has a smaller effect on WZ GaN/AlGaN, and very little effect on ZB GaN/AlN quantum dots. As a result, the exciton ground state energy in WZ GaN/AlN quantum dots, with heights larger than 3 nm, exhibits a…
GaN and the heterostructures are attractive in condensed matter science and applications for electronic devices. We measure the electron transport in GaN/AlGaN field-effect transistors (FETs) at cryogenic temperature. We observe formation of quantum dots in the conduction channel near the depletion of the 2-dimensional electron gas (2DEG). Multiple quantum dots are formed in the disordered potential induced by impurities in the FET conduction channel. We also measure the gate insulator dependence of the transport properties. These results can be utilized for the development of quantum dot devi…
The optical emission of non-polar GaN/AlN quantum dots has been investigated. The presence of stacking faults inside these quantum dots is evidenced in the dependence of the photoluminescence with temperature and excitation power. A theoretical model for the electronic structure and optical properties of non-polar quantum dots, taking into account their realistic shapes, is presented which predicts a substantial reduction of the internal electric field but a persisting quantum confined Stark effect, comparable to that of polar GaN/AlN quantum dots. Modeling the effect of a 3 monolayer stacking…
A theoretical interpretation of the photoluminescence excitation spectra of self-organized polar GaN/(Al,Ga)N quantum dots is proposed. A numerical method assuming a realistic shape of the dots and including the built-in electric field effects is developed to calculate their energy structure and hence their optical absorption. The electron and hole spectra show the existence of a set of quasi-bound states that does not originate from the wetting layer, and plays a crucial role in the observed absorption spectrum of the GaN/(Al,Ga)N dots. Transitions involving these quasi-bound states and wetti…
Semiconductor light emitters compatible with standard Si integration technology (SIT) are of particular interest for overcoming limitations in the operating speed of microelectronic devices 1-3. Light sources based on group-IV elements would be SIT compatible but suffer from the poor optoelectronic properties of bulk Si and Ge. Here, we demonstrate that epitaxially grown Ge quantum dots (QDs) in a fully coherent Si matrix show extraordinary optical properties if partially amorphised by Ge-ion bombardment (GIB). The GIB-QDs exhibit a quasi-direct-band gap and show, in contrast to conventional S…
Two-photon transition rates are investigated in resonance to the ground state in wurtzite GaN/AlN quantum dots. The ground state transition is two-photon allowed because of the electron-hole separation inherent to polar wurtzite III-nitride heterostructures. We show that this built-in parity breaking mechanism can allow deterministic triggering of single-photon emission via coherent two-photon excitation. Radiative lifetimes obtained for single-photon relaxation are in good agreement with available time-resolved micro-photoluminescence experiments, indicating the reliability of the employed co…
We study the nature of excitons bound to I1 basal plane stacking faults in ensembles of ultrathin GaN nanowires by continuous-wave and time-resolved photoluminescence spectroscopy. These ultrathin nanowires, obtained by the thermal decomposition of spontaneously formed GaN nanowire ensembles, are tapered and have tip diameters down to 6 nm. With decreasing nanowire diameter, we observe a strong blue shift of the transition originating from the radiative decay of stacking fault-bound excitons. Moreover, the radiative lifetime of this transition in the ultrathin nanowires is independent of tempe…
Formation of excitonic states in quantum dots of nitride based III-V semiconductors GaN and AlN including coulomb and exchange interactions are investigated. Dark exciton formation is found to occur for both GaN quantum dots(QDs) with wurtzite structure having positive crystal field splitting and GaN and AlN QDs with zero crystal field splitting with a transition from dark to bright exciton at about 40Å. In wurtzite AlN QDs with negative crystal field splitting the splitting between the dark and bright excitonic states is very small and vanishes at about 15Å.
In this work we present a detailed analysis of the second-order piezoelectric effect in $c$-plane In$_{x}$Ga$_{1-x}$N/GaN quantum dots and its consequences for electronic and optical properties of these systems. Special attention is paid to the impact of increasing In content $x$ on the results. We find that in general the second-order piezoelectric effect leads to an increase of the electrostatic built-in field. Furthermore, our results show that for an In content $\geq$30\% this increase in the built-in field has a significant effect on the emission wavelength and the radiative lifetimes. Fo…
Quantum-dot-in-nanowire systems constitute building blocks for advanced photonics and sensing applications. The electronic symmetry of the emitters impacts their function capabilities. Here, we study the fine structure of gallium-rich quantum dots nested in the shell of GaAs-AlGaAs core-shell nanowires. We used optical spectroscopy to resolve the splitting resulting from the exchange terms and extract the main parameters of the emitters. Our results indicate that the quantum dots can host neutral as well as charges excitonic complexes and that the excitons exhibit a slightly elongated footprin…
We have demonstrated surface-plasmon induced change in spontaneous emission rate in the ultraviolet regime at ~ 375-380 nm, using AlN/GaN quantum dots (QD). Using time-resolved and continuous-wave photoluminescence measurements, the recombination rate in AlN/GaN QD is shown to be enhanced when spontaneous emission is resonantly coupled to a metal-surface plasmon mode. The exciton recombination process via Ag-surface plasmon modes is observed to be as much as 3-7 times faster than in normal QD spontaneous emission and depends strongly on the emission wavelength and silver thickness.
Exciton fine structures in cubic III-V semiconductor GaAs, InAs and GaN quantum dots are investigated systematically and the exciton spin relaxation in GaN quantum dots is calculated by first setting up the effective exciton Hamiltonian. The electron-hole exchange interaction Hamiltonian, which consists of the long- and short-range parts, is derived within the effective-mass approximation by taking into account the conduction, heavy- and light-hole bands, and especially the split-off band. The scheme applied in this work allows the description of excitons in both the strong and weak confinemen…
We demonstrate an in-situ technique to tune the emission energy of semiconductor quantum dots. The technique is based on laser-induced atomic intermixing applied to nanowire quantum dots grown using a site-selective process that allows for the deterministic tuning of individual emitters. A tuning range of up to 15 meV is obtained with a precision limited by the laser exposure time. A distinct saturation of the energy shift is observed, which suggests an intermixing mechanism relying on grown-in defects that are subsequently removed from the semiconductor material during annealing. The ability …
We present measurements of the second-order coherence function on emission from single GaN quantum dots. In some cases a large degree of photon antibunching is observed, demonstrating isolation of a single quantum system. For a selected quantum dot, we study the dependence of photon antibunching on excitation power and temperature. Using pulsed excitation, we demonstrate an ultraviolet triggered single-photon source operating at a wavelength of 358 nm.
Single photon emission was observed from site-controlled InGaN/GaN quantum dots. The single-photon nature of the emission was verified by the second-order correlation function up to 90 K, the highest temperature to date for site-controlled quantum dots. Micro-photoluminescence study on individual quantum dots showed linearly polarized single exciton emission with a lifetime of a few nanoseconds. The dimensions of these quantum dots were well controlled to the precision of state-of-the-art fabrication technologies, as reflected in the uniformity of their optical properties. The yield of optical…
We analyze the potential of the $c$-plane InGaN/GaN quantum dots for polarization entangled photon emission by means of an atomistic many-body framework. Special attention is paid to the impact of random alloy fluctuations on the excitonic fine structure and the excitonic binding energy. Our calculations show that $c$-plane InGaN/GaN quantum dots are ideal candidates for high temperature entangled photon emission as long as the underlying $C_{3v}$-symmetry is preserved. However, when assuming random alloy fluctuations in the dot, our atomistic calculations reveal that while the large excitonic…
We report on the carrier dynamics in InGaN/GaN disk-in-a-wire quantum dots with precisely controlled location and structural parameters, including diameter, thickness and material composition. We measured the time-integrated and time-resolved spectra and the second-order correlation function of the photoluminescence from quantum dots with diameters ranging from 19 nm to 33 nm at temperatures of 10 K to 120 K. The influence of the small fluctuations in structural parameters, most importantly the quantum dot thickness, on the optical properties are also investigated through statistical correlati…
Optical and electronic properties of symmetric InAs/InGaAlAs/InP quantum dots formed by a ripening process in molecular beam epitaxy: a promising system for broad-range single-photon telecom emitters
A source of single photons and quantum entangled photon pairs is a key element in quantum information networks. Here, we demonstrate the electrically driven generation of quantum entangled pairs using a naturally symmetric GaAs quantum dot grown by droplet epitaxy. Coincidence histograms obtained at a temperature of 10 K reveal the generation of quantum entangled pairs that have a fidelity to the Bell pairs of 0.71 +- 0.015, much beyond the classical limit. The quantum nature of the emitted pairs is conserved at temperatures of up to ~65 K, and is essentially limited by the charge carrier conf…
Chemically prepared colloidal semiconductor quantum dots have long been proposed as scalable and color-tunable single emitters in quantum optics, but they have typically suffered from prohibitively incoherent emission. We now demonstrate that individual colloidal lead halide perovskite quantum dots (PQDs) display highly efficient single photon emission with optical coherence times as long as 80 ps, an appreciable fraction of their 210 ps radiative lifetimes. These measurements suggest that PQDs should be explored as building blocks in sources of indistinguishable single photons and entangled p…
Interfacing single emitters and photonic nanostructures enables modifying their emission properties, such as enhancing individual decay rates or controlling the emission direction. To achieve full control, the single emitter must be positioned in the nanostructures deterministically. Here, we use spectroscopy to gain spectral and spatial information about individual quantum dots in order to position each emitter in a pre-determined location in a unit cell of a photonic-crystal waveguide. Depending on the spatial and spectral positioning within the structured nanophotonic mode, we observe that …
We report single-photon emission from electrically driven site-controlled InGaN/GaN quantum dots, fabricated from a planar light-emitting diode structure containing a single InGaN quantum well using a top-down approach. The location, dimension, and height of each single-photon-emitting diode are controlled lithographically, providing great flexibility for chip-scale integration.
The heteroepitaxy of III-V semiconductors on silicon is a promising approach for making silicon a photonic platform for on-chip optical interconnects and quantum optical applications. Monolithic integration of both material systems is a long-time challenge, since different material properties lead to high defect densities in the epitaxial layers. In recent years, nanostructures however have shown to be suitable for successfully realising light emitters on silicon, taking advantage of their geometry. Facet edges and sidewalls can minimise or eliminate the formation of dislocations, and due to t…
Due to their ability to strongly modify the local electromagnetic (EM) field through the excitation of surface plasmon polaritons (SPPs), plasmonic nanostructures have been often used to reshape the emission direction and enhance the radiative decay rate of quantum emitters, such as semiconductor quantum dots (QDs). These features are essential for quantum information processing, nanoscale photonic circuitry and optoelectronics. However, the modification and enhancement demonstrated thus far often drastically alter the local energy density of the emitters, and hence their intrinsic properties,…
Integrated quantum photonic circuits (IQPCs) with deterministically integrated quantum emitters are critical elements for scalable quantum information applications and have attracted significant attention in recent years. However, scaling up them towards fully functional photonic circuits with multiple deterministically integrated quantum emitters to generate photonic input states remains a great challenge. In this work, we report on a monolithic prototype IQPC consisting of two pre-selected quantum dots deterministically integrated into nanobeam cavities at the input ports of a 2x2 multimode …
High resolution coherent nonlinear optical spectroscopy of an ensemble of red-emitting InGaN quantum dots in GaN nanowires is reported. The data show a pronounced atom-like interaction between resonant laser fields and quantum dot excitons at low temperature that is difficult to observe in the linear absorption spectrum due to inhomogeneous broadening from indium fluctuation effects. We find that the nonlinear signal persists strongly at room temperature. The robust atom-like room temperature response indicates the possibility that this material could serve as the platform for proposed exciton…
We discuss the spectral lineshapes of N quantum dots in strong coupling with the single mode of a microcavity. Nontrivial features are brought by detuning the emitters or probing the direct exciton emission spectrum. We describe dark states, quantum nonlinearities, emission dips and interferences and show how these various effects may coexist, giving rise to highly peculiar lineshapes.
Highly entangled graph states of photons have applications in universal quantum computing and in quantum communications. In the latter context, they have been proposed as the key ingredient in the establishment of long-distance entanglement across quantum repeater networks. Recently, a general deterministic approach to generate repeater graph states from quantum emitters was given. However, a detailed protocol for the generation of such states from realistic systems is still needed in order to guide experiments. Here, we provide such explicit protocols for the generation of repeater graph stat…
Photonic quantum technologies call for scalable quantum light sources that can be integrated, while providing the end user with single and entangled photons on-demand. One promising candidate are strain free GaAs/AlGaAs quantum dots obtained by droplet etching. Such quantum dots exhibit ultra low multi-photon probability and an unprecedented degree of photon pair entanglement. However, different to commonly studied InGaAs/GaAs quantum dots obtained by the Stranski-Krastanow mode, photons with a near-unity indistinguishability from these quantum emitters have proven to be elusive so far. Here, …
We report on a Python-toolbox for unbiased statistical analysis of fluorescence intermittency properties of single emitters. Intermittency, i.e., step-wise temporal variations in the instantaneous emission intensity and fluorescence decay rate properties are common to organic fluorophores, II-VI quantum dots and perovskite quantum dots alike. Unbiased statistical analysis of intermittency switching time distributions, involved levels and lifetimes is important to avoid interpretation artefacts. This work provides an implementation of Bayesian changepoint analysis and level clustering applicabl…
Quantum photonics technologies like wavelength division multiplexing (WDM) for high-rate quantum key distribution require narrowband, spectrally tunable single photon emitters. Physical methods that rely on the application of large mechanical strain to epitaxial quantum dots or electric and magnetic fields to color centers in 2D metal dichalcogenides provide limited spectral tunability. Here we adopt a chemical approach to synthesize a family of colloidal mixed-cation perovskite quantum dots ($\text{Cs}_{1-x}\text{FA}_{x}\text{PbBr}_3$) that show highly photo-stable, compositionally tunable si…
Future scalable photonic quantum information processing relies on the ability of integrating multiple interacting quantum emitters into a single chip. Quantum dots provide ideal on-chip quantum light sources. However, achieving quantum interaction between multiple quantum dots on-a-chip is a challenging task due to the randomness in their frequency and position, requiring local tuning technique and long-range quantum interaction. Here, we demonstrate quantum interactions between distant two quantum dots on a nanophotonic waveguide. We achieve a photon-mediated long-range interaction by integra…
We investigate the emission directionality of electronic intraband (intersubband) transitions in stacked coupled quantum dots. Using a well-established eight-band $k \cdot p$ method, we demonstrate that the minor contributions from the valence band mixing into the conduction band govern the polarization and emission directionality of electronic $p$-to-$s$-type intraband transitions. Despite that the contribution from the central-cell part to the momentum matrix element is dominant, we find, the contribution from the matrix elements among the envelope functions cannot be neglected. With the hel…
On-chip quantum information processing requires controllable quantum light sources that can be operated on-demand at high-speeds and with the possibility of in-situ control of the photon emission wavelength and its optical polarization properties. Here, we report on the dynamic control of the optical emission from core-shell GaN/InGaN nanowire (NW) heterostructures using radio frequency surface acoustic waves (SAWs). The SAWs are excited on the surface of a piezoelectric lithium niobate crystal equipped with a SAW delay line onto which the NWs were mechanically transferred. Luminescent quantum…
Photo-induced Wavelength-tuning of Telecom-band Quantum Dot Nanowires Embedded in a Phase Change Material
CNRS, ECL, INSA Lyon, UCBL, CPE Lyon, INL, UMR 5270（法国国家科学研究中心，里昂高等师范学校，里昂国立应用科学学院，里昂第一大学，里昂高等化学物理学院，国家科研中心）；CNRS, INSA Lyon, Université Claude Bernard Lyon 1, MATEIS, UMR 5510（法国国家科学研究中心，里昂国立应用科学学院，克洛德·贝尔纳里昂第一大学）；Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière, UMR5306（克洛德·贝尔纳里昂第一大学，法国国家科学研究中心，光物质研究所）
Colloidal quantum dots have garnered active research interest as quantum emitters due to their robust synthesis process and straightforward integration with nanophotonic platforms. However, obtaining indistinguishable photons from the colloidal quantum dots at room temperature is fundamentally challenging because they suffer from an extremely large dephasing rate. Here we propose an experimentally feasible method of obtaining indistinguishable single photons from an incoherently pumped solution-processed colloidal quantum dot coupled to a system of nanocavities. We show that by coupling a coll…
Single photon emitters play a central role in many photonic quantum technologies. A promising class of single photon emitters consists of atomic color centers in wide-bandgap crystals, such as diamond silicon carbide and hexagonal boron nitride. However, it is currently not possible to grow these materials as sub-micron thick films on low-refractive index substrates, which is necessary for mature photonic integrated circuit technologies. Hence, there is great interest in identifying quantum emitters in technologically mature semiconductors that are compatible with suitable heteroepitaxies. Her…
Photonic quantum technologies are on the verge of finding applications in everyday life with quantum cryptography and the quantum internet on the horizon. Extensive research has been carried out to determine suitable quantum emitters and single epitaxial quantum dots are emerging as near-optimal sources of bright, on-demand, highly indistinguishable single photons and entangled photon pairs. In order to build up quantum networks, it is now essential to interface remote quantum emitters. However, this is still an outstanding challenge, as the quantum states of dissimilar 'artificial atoms' have…
We demonstrate single photon emission from self-assembled m-plane InGaN quantum dots (QDs) embedded on the side-walls of GaN nanowires. A combination of electron microscopy, cathodoluminescence, time-resolved micro-PL and photon autocorrelation experiments give a thorough evaluation of the QDs structural and optical properties. The QD exhibits anti-bunched emission up to 100 K, with a measured autocorrelation function of g^2(0) = 0.28 (0.03) at 5 K. Studies on a statistically significant number of QDs show that these m-plane QDs exhibit very fast radiative lifetimes (260 +/- 55 ps) suggesting …
The development of multi-node quantum optical circuits has attracted great attention in recent years. In particular, interfacing quantum-light sources, gates and detectors on a single chip is highly desirable for the realization of large networks. In this context, fabrication techniques that enable the deterministic integration of pre-selected quantum-light emitters into nanophotonic elements play a key role when moving forward to circuits containing multiple emitters. Here, we present the deterministic integration of an InAs quantum dot into a 50/50 multi-mode interference beamsplitter via in…
Current steps attributed to resonant tunneling through individual InAs quantum dots embedded in a GaAs-AlAs-GaAs tunneling device are investigated experimentally in magnetic fields up to 28 T. The steps evolve into strongly enhanced current peaks in high fields. This can be understood as a field-induced Fermi-edge singularity due to the Coulomb interaction between the tunneling electron on the quantum dot and the partly spin polarized Fermi sea in the Landau quantized three-dimensional emitter.
(In,Ga)N insertions embedded in self-assembled GaN nanowires are of current interest for applications in solid state light emitters. Such structures exhibit a notoriously broad emission band. We use cathodoluminescence spectral imaging in a scanning electron microscope and micro-photoluminescence spectroscopy on single nanowires to learn more about the mechanisms underlying this emission. We observe a shift of the emission energy along the stack of six insertions within single nanowires that may be explained by compositional pulling. Our results also corroborate reports that the localization o…
We propose a method for the optimal time-controlled generation of entangled itinerant particles, using on-demand sources in a conductor in the quantum Hall regime. This entanglement pump is realized by applying periodic, tailored voltage pulses to pairs of quantum dots or quantum point contacts. We show that the pump can produce orbital Bell pairs of both electrons and holes at the optimal rate of half a pair per pumping cycle. The entanglement can be detected by a violation of a Bell inequality formulated in terms of low-frequency current cross correlations.
Within the Floquet theory of periodically driven quantum systems, we demonstrate that a high-frequency electromagnetic field can be used as an effective tool to control excitonic properties of semiconductor quantum dots (QDs). It is shown, particularly, that the field both decreases the exciton binding energy and dynamically stabilizes the exciton, increasing its radiative lifetime. The developed theory can serve as a basis for the ultrafast method to tune spectral characteristics of the QD-based photon emitters by a high-frequency field.
The Jaynes-Cummings model provides a well established theoretical framework for single electron two level systems in a radiation field. Similar exactly solvable models for semiconductor light emitters such as quantum dots dominated by many particle interactions are not known. We access these systems by a generalized cluster expansion, the photon-probability-cluster-expansion: a reliable approach for few photon dynamics in many body electron systems. As a first application, we discuss vacuum Rabi flopping and show that their amplitude determines the number of electrons in the quantum dot.
We study theoretically the spontaneous emission from an inhomogeneous ensemble of quantum dots in the weak excitation limit. We show that collective, superradiance-like effects lead to an enhanced emission rate in the presence of sufficiently strong coupling between the dots in agreement with experimental observations, which means that the quantum dot sample cannot be treated as an ensemble of individual emitters. We demonstrate also that the collective behavior of the quantum dot system relies on short-range interactions, while long-range dipole couplings are too weak to have any impact on th…
The possibility of non-adiabatic electron pumping in the system of three coupled quantum dots attached to the leads is discussed. We have found out that periodical changing of energy level position in the middle quantum dot results in non zero mean tunneling current appeared due to non-adiabatic non-equilibrium processes. The same principle can be used for fabrication of a new class of semiconductor electronic devices based on non-stationary non-equilibrium currents. As an example we propose a nanometer quantum emitter with non-stationary inverse level occupation achieved by electron pumping.
We investigate the dynamical behavior of entanglement in a system made by two solid-state emitters, as two quantum dots, embedded in two separated micro-cavities. In these solid-state systems, in addition to the coupling with the cavity mode, the emitter is coupled to a continuum of leaky modes providing additional losses and it is also subject to a phonon-induced pure dephasing mechanism. We model this physical configuration as a multipartite system composed by two independent parts each containing a qubit embedded in a single-mode cavity, exposed to cavity losses, spontaneous emission and pu…
Monolayer transition metal dichalcogenides have recently attracted great interests because the quantum dots embedded in monolayer can serve as optically active single photon emitters. Here, we provide an interpretation of the recombination mechanisms of these quantum emitters through polarization-resolved and magneto-optical spectroscopy at low temperature. Three types of defect-related quantum emitters in monolayer tungsten diselenide (WSe$_2$) are observed, with different exciton g factors of 2.02, 9.36 and unobservable Zeeman shift, respectively. The various magnetic response of the spatial…
The electromagnetic-vacuum-field fluctuations are intimately linked to the process of spontaneous emission of light. Atomic emitters cannot probe electric- and magnetic-field fluctuations simultaneously because electric and magnetic transitions correspond to different selection rules. In this paper we show that semiconductor quantum dots are fundamentally different and are capable of mediating electric-dipole, magnetic-dipole, and electric-quadrupole transitions on a single electronic resonance. As a consequence, quantum dots can probe electric and magnetic fields simultaneously and can thus b…
