Single Quantum Dot Emission Research Articles

Single quantum dot selection and tailor-made photonic device integration using nanoscale focus pinspot.

Among the diverse platforms of quantum light sources, epitaxially grown semiconductor quantum dots (QDs) are one of the most attractive workhorses for realizing quantum photonic technologies owing to their outstanding brightness and scalability. However, the spatial and spectral randomness of most QDs severely hinders the construction of large-scale photonic platforms. In this work, we present a methodology to deterministically integrate single QDs with tailor-made photonic structures. We apply a nondestructive luminescence picking method termed as nanoscale focus pinspot (NFP) using helium ion microscopy to reduce the luminous QD density while retaining the surrounding medium. We extract only a single QD emission out of the high-density ensemble QDs. Then the tailor-made photonic structure of a circular Bragg reflectors (CBR) are designed and deterministically integrated with the selected QD. Given that the microscopy can image with nanoscale resolution and apply NFP in situ, photonic devices can be deterministically fabricated on target QDs. The extraction efficiency of the NFP-selected QD emission is improved by 25 times after the CBR integration. Since the NFP method only controls the luminescence without destroying the medium, it is applicable to various photonic structures such as photonic waveguides or photonic crystal cavities regardless of materials. This article is protected by copyright. All rights reserved.

Single SiGe quantum dot emission deterministically enhanced in a high-Q photonic crystal resonator.

We report the resonantly enhanced radiative emission from a single SiGe quantum dot (QD), which is deterministically embedded into a bichromatic photonic crystal resonator (PhCR) at the position of its largest modal electric field by a scalable method. By optimizing our molecular beam epitaxy (MBE) growth technique, we were able to reduce the amount of Ge within the whole resonator to obtain an absolute minimum of exactly one QD, accurately positioned by lithographic methods relative to the PhCR, and an otherwise flat, a few monolayer thin, Ge wetting layer (WL). With this method, record quality (Q) factors for QD-loaded PhCRs up to Q ∼ 105 are achieved. A comparison with control PhCRs on samples containing a WL but no QDs is presented, as well as a detailed analysis of the dependence of the resonator-coupled emission on temperature, excitation intensity, and emission decay after pulsed excitation. Our findings undoubtedly confirm a single QD in the center of the resonator as a potentially novel photon source in the telecom spectral range.

Bright and Polarized Fiber In-Line Single-Photon Source Based on Plasmon-Enhanced Emission into Nanofiber Guided Modes

We demonstrate a bright and polarized fiber in-line single-photon source based on plasmon-enhanced emission of colloidal single quantum dots into an optical nanofiber. We show that emission properties of single quantum dots can be strongly enhanced in the presence of single gold nanorods leading to a bright and strongly polarized single-photon emission. The single photons are efficiently coupled to guided modes of the nanofiber and eventually to a single-mode optical fiber. The brightness (fiber-coupled photon count rate) of the single-photon source is estimated to be $12.2\ifmmode\pm\else\textpm\fi{}0.6$ MHz, with high single-photon purity [${g}^{2}(0)=0.20\ifmmode\pm\else\textpm\fi{}0.04$] and degree of polarization as high as 94--97 %. The polarized and fiber-coupled single photons can be implemented for potential applications in quantum photonics.

Narrow Intrinsic Line Widths and Electron–Phonon Coupling of InP Colloidal Quantum Dots

InP quantum dots (QDs) are the material of choice for QD display applications and have been used as active layers in QD light-emitting diodes (QDLEDs) with high efficiency and color purity. Optimizing the color purity of QDs requires understanding mechanisms of spectral broadening. While ensemble-level broadening can be minimized by synthetic tuning to yield monodisperse QD sizes, single QD line widths are broadened by exciton-phonon scattering and fine-structure splitting. Here, using photon-correlation Fourier spectroscopy, we extract average single QD line widths of 50 meV at 293 K for red-emitting InP/ZnSe/ZnS QDs, among the narrowest for colloidal QDs. We measure InP/ZnSe/ZnS single QD emission line shapes at temperatures between 4 and 293 K and model the spectra using a modified independent boson model. We find that inelastic acoustic phonon scattering and fine-structure splitting are the most prominent broadening mechanisms at low temperatures, whereas pure dephasing from elastic acoustic phonon scattering is the primary broadening mechanism at elevated temperatures, and optical phonon scattering contributes minimally across all temperatures. Conversely for CdSe/CdS/ZnS QDs, we find that optical phonon scattering is a larger contributor to the line shape at elevated temperatures, leading to intrinsically broader single-dot line widths than for InP/ZnSe/ZnS. We are able to reconcile narrow low-temperature line widths and broad room-temperature line widths within a self-consistent model that enables parametrization of line width broadening, for different material classes. This can be used for the rational design of more spectrally narrow materials. Our findings reveal that red-emitting InP/ZnSe/ZnS QDs have intrinsically narrower line widths than typically synthesized CdSe QDs, suggesting that these materials could be used to realize QDLEDs with high color purity.

CdSe quantum dot formation induced by electron beam irradiation

The formation of quantum dots (QDs) induced by electron beam irradiation onto a highly strained CdSe layer on ZnSe (001) is investigated. In situ reflection high-energy electron diffraction is used for dual purposes: QD formation by electron beam irradiation and monitoring the progress of surface morphology. QD formation is confirmed by observation of nanoscale three-dimensional islands using transmission electron microscopy. It is also verified by imaging of an isolated single QD emission at room temperature by photoluminescence microscopy. Electron beam irradiation increases QD size both in height and lateral directions, resulting in the shift of emission from green to yellow spectral region.

Quantification of mRNA in Single Cells Based on Dimerization-Induced Photoluminescence Nonblinking of Quantum Dots.

Photoluminescence (PL) intermittency (or "blinking") is a unique characteristic of single quantum dot (QD) emission. Here, we report a novel single-molecule detection strategy for the intracellular mRNA of interest using the mRNA-induced nonblinking QD dimers as probes. The working principle of the method is that the DNA hybrid of the target DNA (or mRNA) with a biotin-modified ssDNA probe can induce two blinking streptavidin-modified QDs (SAV-QDs) conjugated. The formed QD dimer as a bright spot showed a nonblinking emission property, observed with total inner reflection fluorescence microscopy (TIRFM). In theory, one nonblinking spot indicated a target DNA (or mRNA). The experimental results from single-spot fluorescence trajectory analysis and single-particle brightness analysis based on TIRFM and fluorescence correlation spectroscopy (FCS) techniques verified this dimerization process of QDs or its induced nonblinking emission. Employing a target DNA with the same base sequences to Survivin mRNA as a model, the detection strategy was used to detect the target DNA concentration based on the linear relationship between the percentage of the nonblinking spots and the target DNA concentration. This single-molecule detection strategy was also successfully used for determining Survivin mRNA in a single HeLa cell. The method can simplify the hybridization steps, eliminate self-quenching and photobleaching of fluorophores, and reduce the influence of unspecific binding on the detection.

Unraveling the dual emission of single quantum-dot by single particle spectroscopy

Two-color emissive 0D–2D quantum-dot quantum-well (QD-QW) heteronanocrystals has created profound research activities. First multicolor emission in the visible region has been reported by Peng and co-workers in CdSe(core)–ZnS(barrier)-CdSe(shell) (core-barrier-shell) based heteronanostructures where the both CdSe phases (core and the shell) are emissive and tuneable as well. Owing to this enhanced and tuneable functionality, the QD-QW systems colloidal nanocrystals has fuelled their optical and imaging applications. Single particle spectroscopy has taken a giant step toward unravelling the features of individual particles and thus to provide direct information on their heterogeneity. To elucidate the dual emission characteristic of individual nanocrystals we performed energy mapped photoluminescence imaging. Surprisingly, the pseudo color PL intensity image shows that not all single particles are dual emissive in nature, few are either green emitting or red emitting. Photoluminescence spectrum of individual nanocrystals further confirms that individual nanocrystals can be dual emissive in nature. However, single color emissive dots are also present indicating the ensemble heterogeneity at single particle levels. The temporal evolution PL spectra of a single quantum shows spectral diffusion. The single dot experiments on the dual emissive QD-QW system unravels hidden photophysics which are otherwise not observed by ensemble spectroscopy.

Optical Quality of InAs/InP Quantum Dots on Distributed Bragg Reflector Emitting at 3rd Telecom Window Grown by Molecular Beam Epitaxy.

We present an experimental study on the optical quality of InAs/InP quantum dots (QDs). Investigated structures have application relevance due to emission in the 3rd telecommunication window. The nanostructures are grown by ripening-assisted molecular beam epitaxy. This leads to their unique properties, i.e., low spatial density and in-plane shape symmetry. These are advantageous for non-classical light generation for quantum technologies applications. As a measure of the internal quantum efficiency, the discrepancy between calculated and experimentally determined photon extraction efficiency is used. The investigated nanostructures exhibit close to ideal emission efficiency proving their high structural quality. The thermal stability of emission is investigated by means of microphotoluminescence. This allows to determine the maximal operation temperature of the device and reveal the main emission quenching channels. Emission quenching is predominantly caused by the transition of holes and electrons to higher QD’s levels. Additionally, these carriers could further leave the confinement potential via the dense ladder of QD states. Single QD emission is observed up to temperatures of about 100 K, comparable to the best results obtained for epitaxial QDs in this spectral range. The fundamental limit for the emission rate is the excitation radiative lifetime, which spreads from below 0.5 to almost 1.9 ns (GHz operation) without any clear spectral dispersion. Furthermore, carrier dynamics is also determined using time-correlated single-photon counting.

Optically Driven Giant Superbunching from a Single Perovskite Quantum Dot

AbstractPhoton superbunching is a signature of a strong correlation between photons, which is a crucial resource needed in quantum communication and computation. As such, a superbunched photon source based on a material with high quantum efficiency, like cesium lead halide perovskite, is highly desirable. Utilizing the large dark–bright exciton splitting in CsPbBr3quantum dot (QD), the authors achieve a superbunching with a large g(2)(0) ≈ 30 from an optically driven single CsPbBr3QD emission at cryogenic temperature. The cascaded emission is identified as the cause of this superbunching by utilizing second‐order cross‐correlation measurement and exploring the excitation power and temperature dependence of the bunching level. The findings have immediate implications on the basic understanding of a single perovskite QD emission and its application as a quantum light source.

Metal, dielectric and hybrid nanoantennas for enhancing the emission of single quantum dots: A comparative study

The confinement of electromagnetic energy to subwavelength volumes through nanoscale antennas can be used to enhance the spontaneous emission of quantum emitters. With this aim, different configurations of metallic and high refractive index dielectric nanoparticles have been explored. Here, we carry out a comparative analysis of planar metallic, high refractive index dielectric, and hybrid nanoantennas considering three different parameters: the Purcell factor enhancement, radiation efficiency, and directionality properties. We focus our study on different geometries and material combinations of a dimer of cylinders. A dimer made of two gold nanocylinders is the most promising candidate for improving the spontaneous emission. While most previous works have paid attention to the redirection of the scattered emission in the nanoparticle plane, our proposed nanostructure of two large gold cylinders (R=λ/4) emits most of the radiation upwards. This effect is due to the strong quadrupolar electric contribution to the resonant mode. With the aim to further improve the directionality properties, additional silicon nanocylinders are used as directors of the scattered radiation, increasing the directivity by a factor of 2.4 with respect to the gold dimer without directors. All in all, a hybrid structure composed of a gold dimer and silicon nanoparticles is proposed to enhance the spontaneous emission of a single quantum dot and to govern its emission pattern. The results shown in this work could be useful in fluorescence enhancement or in quantum photonics. They are particularly interesting for the development of single-photon sources based on quantum dots and other nanoscale emitters.

3D printed micro-optics for quantum technology: Optimised coupling of single quantum dot emission into a single-mode fibre

Future quantum technology relies crucially on building quantum networks with high fidelity. To achieve this challenging goal, it is of utmost importance to connect individual quantum systems such that their emitted single photons overlap with the highest possible degree of coherence. This requires perfect mode overlap of the emitted light from different emitters, which necessitates the use of single-mode fibres. Here, we present an advanced manufacturing approach to accomplish this task. We combined 3D printed complex micro-optics, such as hemispherical and Weierstrass solid immersion lenses, as well as total internal reflection solid immersion lenses, on top of individual indium arsenide quantum dots with 3D printed optics on single-mode fibres and compared their key features. We observed a systematic increase in the collection efficiency under variations of the lens geometry from roughly 2 for hemispheric solid immersion lenses up to a maximum of greater than 9 for the total internal reflection geometry. Furthermore, the temperature-induced stress was estimated for these particular lens dimensions and results to be approximately 5 meV. Interestingly, the use of solid immersion lenses further increased the localisation accuracy of the emitters to less than 1 nm when acquiring micro-photoluminescence maps. Furthermore, we show that the single-photon character of the source is preserved after device fabrication, reaching a $ g^{(2)} (0)$ value of approximately 0.19 under pulsed optical excitation. The printed lens device can be further joined with an optical fibre and permanently fixed.This integrated system can be cooled by dipping into liquid helium using a Stirling cryocooler or by a closed-cycle helium cryostat without the necessity for optical windows, as all access is through the integrated single-mode fibre. We identify the ideal optical designs and present experiments that demonstrate excellent high-rate single-photon emission.

Thermal stability of emission from single InGaAs/GaAs quantum dots at the telecom O-band

Single-photon sources are key building blocks in most of the emerging secure telecommunication and quantum information processing schemes. Semiconductor quantum dots (QD) have been proven to be the most prospective candidates. However, their practical use in fiber-based quantum communication depends heavily on the possibility of operation in the telecom bands and at temperatures not requiring extensive cryogenic systems. In this paper we present a temperature-dependent study on single QD emission and single-photon emission from metalorganic vapour-phase epitaxy-grown InGaAs/GaAs QDs emitting in the telecom O-band at 1.3 μm. Micro-photoluminescence studies reveal that trapped holes in the vicinity of a QD act as reservoir of carriers that can be exploited to enhance photoluminescence from trion states observed at elevated temperatures up to at least 80 K. The luminescence quenching is mainly related to the promotion of holes to higher states in the valence band and this aspect must be primarily addressed in order to further increase the thermal stability of emission. Photon autocorrelation measurements yield single-photon emission with a purity of {g}_{50K}^{(2)}left(0right)=0.13 up to 50 K. Our results imply that these nanostructures are very promising candidates for single-photon sources at elevated (e.g., Stirling cryocooler compatible) temperatures in the telecom O-band and highlight means for improvements in their performance.

Observation of Cooperative Purcell Enhancements in Antenna-Cavity Hybrids.

Localizing light to nanoscale volumes through nanoscale resonators that are low loss and precisely tailored in spectrum to properties of matter is crucial for classical and quantum light sources, cavity QED, molecular spectroscopy, and many other applications. To date, two opposite strategies have been identified: to use either plasmonics with deep subwavelength confinement yet high loss and very poor spectral control or instead microcavities with exquisite quality factors yet poor confinement. In this work we realize hybrid plasmonic–photonic resonators that enhance the emission of single quantum dots, profiting from both plasmonic confinement and microcavity quality factors. Our experiments directly demonstrate how cavity and antenna jointly realize large cooperative Purcell enhancements through interferences. These can be controlled to engineer arbitrary Fano lineshapes in the local density of optical states.

Quantum correlation measurement with single photon avalanche diode arrays.

Temporal photon correlation measurement, instrumental to probing the quantum properties of light, typically requires multiple single photon detectors. Progress in single photon avalanche diode (SPAD) array technology highlights their potential as high-performance detector arrays for quantum imaging and photon number-resolving (PNR) experiments. Here, we demonstrate this potential by incorporating a novel on-chip SPAD array with 42% peak photon detection efficiency, low dark count rate and crosstalk probability of 0.14% per detection in a confocal microscope. This enables reliable measurements of second and third order photon correlations from a single quantum dot emitter. Our analysis overcomes the inter-detector optical crosstalk background even though it is over an order of magnitude larger than our faint signal. To showcase the vast application space of such an approach, we implement a recently introduced super-resolution imaging method, quantum image scanning microscopy (Q-ISM).

Enhancement of Biexciton Emission Due to Long-Range Interaction of Single Quantum Dots and Gold Nanorods in a Thin-Film Hybrid Nanostructure.

Semiconductor quantum dots (QDs) are known for their ability to exhibit multiphoton emission caused by recombination of biexcitons (BX). However, the quantum yield (QY) of BX emission is low due to the fast Auger process. Plasmonic nanoparticles (PNPs) provide an attractive opportunity to accelerate BX radiative recombination. Here, we demonstrate the PNPs induced distance-controlled enhancement of BX emission of single QDs. Studying the same single QD before and after its integration with the PNPs, we observed a plasmon-mediated increase in the QY of BX emission. Remarkably, the enhancement of BX emission remains pronounced even at distances of 170 nm. We attribute this effect to efficient coupling, which results in the trade-off between resonance energy transfer from QD to gold nanorods and the Purcell effect at small QD-PNP separations and the predominant influence of the Purcell effect at longer distances. Our findings constitute a reliable approach to managing the efficiency of multiexciton emission over a wide span of distances, thus paving the way for new applications.

Models of semiconductor quantum dots blinking based on spectral diffusion -=SUP=-*-=/SUP=-

AbstractThree models of single colloidal quantum dot emission fluctuations (blinking) based on spectral diffusion were considered analytically and numerically. It was shown that the only one of them, namely the Frantsuzov and Marcus model reproduces the key properties of the phenomenon. The other two models, the Diffusion-Controlled Electron Transfer (DCET) model and the Extended DCET model predict that after an initial blinking period, most of the QDs should become permanently bright or permanently dark which is significantly different from the experimentally observed behavior.

Models of Semiconductor Quantum Dots Blinking based on Spectral Diffusion

Three models of single colloidal quantum dot emission fluctuations (blinking) based on spectral diffusion were considered analytically and numerically. It was shown that the only one of them, namely the Frantsuzov and Marcus model reproduces the key properties of the phenomenon. The other two models, the Diffusion-Controlled Electron Transfer (DCET) model and the Extended DCET model predict that after an initial blinking period, most of the QDs should become permanently bright or permanently dark which is significantly different from the experimentally observed behavior.

Tuning Single Quantum Dot Emission with a Micromirror.

The photoluminescence of single quantum dots fluctuates between bright (on) and dark (off) states, also termed fluorescence intermittency or blinking. This blinking limits the performance of quantum dot-based devices such as light-emitting diodes and solar cells. However, the origins of the blinking remain unresolved. Here, we use a movable gold micromirror to determine both the quantum yield of the bright state and the orientation of the excited state dipole of single quantum dots. We observe that the quantum yield of the bright state is close to unity for these single QDs. Furthermore, we also study the effect of a micromirror on blinking, and then evaluate excitation efficiency, biexciton quantum yield, and detection efficiency. The mirror does not modify the off-time statistics, but it does change the density of optical states available to the quantum dot and hence the on times. The duration of the on times can be lengthened due to an increase in the radiative recombination rate.

Single photon detection and circular polarized emission manipulated with individual quantum dot

Studies on quantum dots (QDs) provide great opportunities in single photon detection as well as single circular polarized photon emission, which are the key technology for future quantum information processing. For single photon detection, the quantum-dot-resonant-tunneling-diode (QD-RTD) is evaluated as one of the most promising scheme but still suffering from the ultralow working temperature (～5 K) and lack the capability to discriminate photon numbers. Here we demonstrate a photon-number-resolving detector based on quantum dot coupled resonant tunneling diodes (QD-cRTD). Individual QDs coupled closely with adjacent quantum well (QW) of resonant tunneling diode operate as photon-gated switches which turn on (off) the RTD tunneling current when they trap photon-generated holes (recombine with injected electrons). With proper decision regions defined, 1-photon and 2-photon states are resolved in 4.2 K with excellent propabilities of accuracy of 90% and 98% respectively. Further, by identifying step-like photon responses, the photon-number-resolving capability is sustained to 77 K, making the detector a promising candidate for advanced quantum information applications where photon-number-states should be accurately distinguished. On the other hand, we firstly performed the magneto-optical studies on single InGaAs/GaAs self-assembled QDs. We observed the exciton Zeeman splitting and diamagnetic shift of a single QD under magnetic field, and the exciton g factor and diamagnetic coefficient was extracted by fitting the magnetic field dependent PL energies. By comparing with theories, we discussed on the effect of QD size, shape and composition on these two parameters. Based on these work, we investigated the single QD exciton-cavity mode coupling effect under external magnetic field. By first time we observed the interaction of Zeeman splitted exciton spin states with the cavity mode and realized the selective enhancement of the SE rate of the exciton state with specific spin configuration by means of magnetic manipulation of Purcell effect. In this sense, single QD emission with higher circular polarization degree under non-polarized excitation was realized. Our results have high potential to open up a way to novel quantum light sources and quantum information processing applications based on cavity quantum electrodynamics effects.

Subminiature emitters based on a single (111) In(Ga)As quantum dot and hybrid microcavity

The results of numerical modeling and investigation of a hybrid microcavity based on a semiconductor Bragg reflector and a microlens selectively positioned above a single (111) In(Ga)As quantum dot are presented. Emitters based on the hybrid microcavity demonstrate the effective pumping of a single quantum dot and high emission output efficiency. The microcavity design can be used to implement emitters of polarization- entangled photon pairs based on single semiconductor quantum dots.