We demonstrate a fiber in-line single photon source based on a hybrid system of colloidal single quantum dots deposited on an optical nanofiber and cooled down to cryogenic temperature (3.7 K). We show that a charged state (trion) of the single quantum dot exhibits a photo-stable emission of single photons with high quantum efficiency, narrow linewidth (3 meV FWHM) and fast decay time ($10.0\pm0.5$ ns). The single photons are efficiently coupled to the guided modes of the nanofiber and eventually to a single mode optical fiber. The brightness (efficiency) of the single photon source is estimated to be $16\pm2\%$ with a maximum photon count rate of $1.6\pm0.2$ MHz and a high single photon purity ($g^2(0)=0.11\pm0.02$). The device can be easily integrated to the fiber networks paving the way for potential applications in quantum networks.
We experimentally demonstrate the efficient channeling of fluorescence photons from single q-dots on optical nanofiber into the guided modes, by measuring the photon-count rates through the guided and radiation modes simultaneously. We obtain the maximum channeling efficiency to be 22.0 (\pm4.8)% at fiber diameter of 350 nm for the emission wavelength of 780 nm. The results may open new possibilities in quantum information technologies for generating single photons into single-mode optical-fibers.
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(0.6) MHz, with high …
We demonstrate cavity QED conditions in the Purcell regime for single quantum emitters on the surface of an optical nanofiber. The cavity is formed by combining an optical nanofiber and a nanofabricated grating to create a composite photonic crystal cavity. Using this technique, significant enhancement of the spontaneous emission rate into the nanofiber guided modes is observed for single quantum dots. Our results pave the way for enhanced on-fiber light-matter interfaces with clear applications to quantum networks.
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…
Solution processible colloidal quantum dots hold great promise for realizing single-photon sources embedded into scalable quantum technology platforms. However, the high-yield integration of large numbers of individually addressable colloidal quantum dots in a photonic circuit has remained an outstanding challenge. Here, we report on integrating individual colloidal core-shell quantum dots (CQDs) into a nanophotonic network that allows for excitation and efficient collection of single-photons via separate waveguide channels. An iterative electron beam lithography process provides a viable meth…
The coupling between single photon emitters and integrated photonic circuits is an emerging topic relevant for quantum information science and other nanophotonic applications. We investigate the coupling between a hybrid system of colloidal quantum dots and propagating gap modes of a silicon nitride waveguide system. We furthermore explore the density of optical states of the system by using a scanning probe technique and find that the quantum dots couple significantly to the photonic circuit. Our results indicate that a scalable slot-waveguide might serve as a promising platform in future dev…
The lattice mismatch strain field of core/multishell structures with spherical symmetry is modeled by a linear continuum elasticity approach. The effect of the strain on the energy structure and linear optical absorption in large core/shell/shell spherical semiconductor quantum dots is analyzed. Localization of the photoexcited carriers induced by coating is found to play an important role in explaining the optical stability of large CdSe/CdS/ZnS and ZnTe/ZnSe/ZnS quantum dots.
We demonstrate an important step towards on chip integration of single photon sources operating at room temperature fiber coupling of a directional quantum emitter with back-excitation. Directionality is achieved with a hybrid metal-dielectric bullseye antenna, while back-excitation is permitted by placement of the emitter at or in a sub-wavelength hole positioned at the bullseye center. Overall, the unique design enables a direct laser excitation from the back of the on-chip device and very efficient coupling of the highly collimated photon emission to either low numerical aperture (NA) free …
Engineering an array of precisely located cavity-coupled active media poses a major experimental challenge in the field of hybrid integrated photonics. We deterministically position solution processed colloidal quantum dots (QDs) on high quality-factor silicon nitride nanobeam cavities and demonstrate light-matter coupling. By lithographically defining a window on top of an encapsulated cavity that is cladded in a polymer resist, and spin coating QD solution, we can precisely control the placement of the QDs, which subsequently couple to the cavity. We show that the number of QDs coupled to th…
Quantum dots play a promising role in the development of novel optical and biosensing devices. In this study, we investigated steady-state and time-dependent luminescence properties of InGaP/ZnS core/shell colloidal quantum dots in a solution phase at room temperature. The steady state experiments exhibited an emission maximum at 650 nm with full width at half maximum of ~ 85 nm, and strong first-excitonic absorption peak at 600 nm. The time-resolved luminescence measurements depicted a bi-exponential decay profile with lifetimes of τ1\sim 47 ns and τ 2\sim 142 ns at the emission maximum. Addi…
Materials with optical gain in the infrared are of paramount importance for optical communications, medical diagnostics and silicon photonics. The current technology is based either on costly III-V semiconductors that are not monolithic to silicon CMOS technology or Er-doped fiber technology that does not make use of the full fiber transparency window. Colloidal quantum dots (CQD) offer a unique opportunity as an optical gain medium in view of their tunable bandgap, solution processability and CMOS compatibility. The 8-fold degeneracy of infrared CQDs based on Pb-chalcogenides has hindered the…
In-Situ Quantum Optical Measurement for Colloidal Quantum Dots Confined in an Optical Trap
State Key Laboratory of Silicon and Advanced Semiconductor Materials（硅与先进半导体材料国家重点实验室）；College of Information Science and Electronic Engineering, Zhejiang University（浙江大学信息与电子工程学院）；Department of Chemistry, Zhejiang University（浙江大学化学系）；ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University（浙江大学杭州全球科创中心）；College of Optical Science and Engineering, Zhejiang University（浙江大学光电科学与工程学院）
Fabrication and characterization of shape- and topology-optimized optical cavities with deep sub-wavelength confinement for interfacing with colloidal quantum dots
We review our recent progress in the production and characterization of tapered optical fibers with a sub-wavelength diameter waist. Such fibers exhibit a pronounced evanescent field and are therefore a useful tool for highly sensitive evanescent wave spectroscopy of adsorbates on the fiber waist or of the medium surrounding. We use a carefully designed flame pulling process that allows us to realize preset fiber diameter profiles. In order to determine the waist diameter and to verify the fiber profile, we employ scanning electron microscope measurements and a novel accurate in situ optical m…
A bright source of fiber-coupled, polarized single photons is an essential component of any realistic quantum network based on today's existing fiber infrastructure. Here, we develop a Purcell enhanced, polarized source of single photons at room temperature by coupling single colloidal quantum dots to the localized surface plasmon-polariton modes of single gold nanorods, combined on the surface of an optical nanofiber. A maximum enhancement of photon emission of 62 times was measured corresponding to a degree of polarization of 86 $\%$, and a brightness enhancement of four times in the fiber m…
Electron transfer to an individual quantum dot promotes the formation of charged excitons with enhanced recombination pathways and reduced lifetimes. Excitons with only one or two extra charges have been observed and exploited for very efficient lasing or single quantum dot LEDs. Here, by room-temperature time-resolved experiments on individual giant-shell CdSe/CdS quantum dots, we show the electrochemical formation of highly charged excitons containing more than twelve electrons and one hole. We report the control over intensity blinking, along with a deterministic manipulation of quantum dot…
Multiply-excited states in semiconductor quantum dots feature intriguing physics and play a crucial role in nanocrystal-based technologies. While photoluminescence provides a natural probe to investigate these states, room temperature single-particle spectroscopy of their emission has so far proved elusive due to the temporal and spectral overlap with emission from the singly-excited and charged states. Here we introduce biexciton heralded spectroscopy, enabled by a single-photon avalanche diode array based spectrometer. This allows us to directly observe biexciton-exciton emission cascades an…
Images of semiconductor `dot in rods' and their small clusters are studied by measuring the second-order correlation function with a spatially resolving ICCD camera. This measurement allows one to distinguish between a single dot and a cluster and, to a certain extent, to estimate the number of dots in a cluster. A more advanced measurement is proposed, based on higher-order correlations, enabling more accurate determination of the number of dots in a small cluster. Nonclassical features of the light emitted by such a cluster are analyzed.
The delivery of optical signals from an external light source to a nanoscale waveguide is highly important for the development of nanophotonic circuits. However, the efficient coupling of external light energy into nanophotonic components is difficult and still remains a challenge. Herein, we use an external silica nanofiber to light up an organic-inorganic hybrid nano-waveguide, namely a system composed of a polymer filament doped with MoS$_{2}$ quantum dots. Nanofiber-excited nano-waveguides in a crossed geometry are found to asymmetrically couple excitation signals along two opposite direct…
Colloidal quantum dots are robust, efficient, and tunable emitters now used in lighting, displays, and lasers. Consequently, when the spaser, a laser-like source of surface plasmons, was first proposed, quantum dots were specified as the ideal plasmonic gain medium. Subsequent spaser designs, however, have required a single material to simultaneously provide gain and define the plasmonic cavity, an approach ill-suited to quantum dots and other colloidal nanomaterials. Here we develop a more open architecture that decouples the gain medium from the cavity, leading to a versatile class of quantu…
We report on a temporal evolution of photoluminescence (PL) spectroscopy of CuInS$_{2}$/ZnS colloidal quantum dots (QDs) by drop-casting on SiO$_{2}$/Si substrates and high quality factor microdisks (MDs) under different atmospheric conditions. Fast PL decay, peak blueshift and linewidth broadening due to photooxidation have been observed at low excitation power. With further increasing of the excitation power, the PL peak position shows a redshift and linewidth becomes narrow, which is ascribed to the enhanced F$\ddot{o}$rster resonant energy transfer between different QDs by photoinduced agg…
In this work we develop a simple theory for the green photoluminescence of ZnO quantum dots (QDs) that allows us to understand and rationalize several experimental findings on fundamental grounds. We calculate the spectrum of light emitted in the radiative recombination of a conduction band electron with a deeply trapped hole and find that the experimental behavior of this emission band with particle size can be understood in terms of quantum size effects of the electronic states and their overlap with the deep hole.We focus the comparison of our results on detailed experiments performed for c…
Unique optical properties of colloidal semiconductor quantum dots (QDs), arising from quantum mechanical confinement of charge within these structures, present a versatile testbed for the study of how high electric fields affect the electronic structure of nanostructured solids. Earlier studies of quasi-DC electric field modulation of QD properties have been limited by the electrostatic breakdown processes under the high externally applied electric fields, which have restricted the range of modulation of QD properties. In contrast, in the present work we drive CdSe:CdS core:shell QD films with…
Optical and X-ray Photo-emission Spectroscopies of Core/Shell Colloidal CdSe/CdS Quantum Dots: Modeling and Experimental Determination of Band Alignment
Individual colloidal quantum dots can be optically trapped and manipulated by a single infrared laser beam operated at low laser powers. If the absorption spectrum and the emission wavelength of the trapping laser are appropriately chosen, the trapping laser light can act as a source for two-photon excitation of the trapped quantum dot. This eliminates the need for an additional excitation laser in experiments where individual quantum dots are used both as force transducers and for visualization of the system. To use quantum dots as handles for quantitative optical force transduction, it is cr…
Nanoantenna enhanced ultrafast emission from colloidal quantum dots as quantum emitters is required for fast quantum communications. On chip integration of such devices require a scalable and high throughput technology. We report self-assembly lithography technique of preparing hybrid of gold-nanorods antenna over a com- pact CdSe quantum dot monolayer. We demonstrate resonant and off resonant gold nanorod antenna enhanced radiative and anisotropic decay. Extensive simulations explain the mechanism of the decay rates and the role of antenna in both random and a compact monolayer of quantum dot…
Two-photon excitation in the near-infrared (NIR) of colloidal nanocrystalline silicon quantum dots (nc-SiQDs) with photoluminescence also in the NIR has the potential to open up new opportunities in the field of deep biological imaging. Spectra of the degenerate two-photon absorption (2PA) cross section of colloidal nc-SiQDs are measured using two-photon excitation over a spectral range $1.46 < \hbar ω< 1.91$ eV (wavelength $850 > λ> 650$ nm) above the two-photon band gap $E_g^{(QD)}/2$, and at a representative photon energy $\hbar ω= 0.99$ eV ($λ= 1250$ nm) below this gap. Two-photon excited …
Pb-chalcogenide colloidal quantum dots (CQDs) are attractive materials to be used as tuneable laser media across the infrared spectrum. However, excessive nonradiative Auger recombination due to the presence of trap states outcompetes light amplification by rapidly annihilating the exciton population, leading to high gain thresholds. Here, we employ a binary blend of CQDs and ZnO nanocrystals in order to passivate the in-gap trap states of PbS-CQD gain medium. Using transient absorption, we measure a five-fold increase in Auger lifetime demonstrating the suppression of trap-assisted Auger reco…
We investigate the fluorescence properties of colloidal quantum dots attached to gold rod nanoantennas. These structures are fabricated by a two step electron beam lithography process in combination with a chemical linking method. By varying the nanoantenna length, the plasmon modes of the nanoantennas are successively tuned through the emission band of the quantum dots. We observe a pronounced fluorescence enhancement both for short and long nanoantennas. These findings can be attributed to the coupling of the quantum dots to bright and dark plasmon modes, respectively.
We use an optical fiber taper waveguide to probe PbS quantum dots (QDs) dried on Si photonic crystal cavities near 1.55 $μ$m. We demonstrate that a low density ($\lesssim 100 μ$m$^{-2}$) of QDs does not significantly degrade cavity quality factors as high as $\approx3\times10^4$. We also show that the tapered fiber can be used to excite the QDs and collect the subsequent cavity-filtered photoluminescence, and present measurements of reversible photodarkening and QD saturation. This method represents an important step towards spectroscopy of single colloidal QDs in the telecommunications band.
Optical gain in solution, which provides high photostability as a result of continuous regeneration of the gain medium, is extremely attractive for optoelectronic applications. Here, we propose and demonstrate amplified spontaneous emission (ASE) in solution with ultralow thresholds of 30 mikroJ/cm2 in red and of 44 mikroJ/cm2 in green from engineered colloidal quantum well (CQW) heterostructures. For this purpose, CdSe/CdS core/crown CQWs, designed to hit the green region, and CdSe/CdS/CdxZn1-xS core/crown/gradient-alloyed shell CQWs, further tuned to reach the red region by shell alloying, w…
Deterministic coupling between photonic nodes in a quantum network is an essential step towards implementing various quantum technologies. The omnidirectionality of free-standing emitters, however, makes this coupling highly inefficient, in particular if the distant nodes are coupled via low numerical aperture (NA) channels such as optical fibers. This limitation requires placing quantum emitters in nanoantennas that can direct the photons into the channels with very high efficiency. Moreover, to be able to scale such technologies to a large number of channels, the placing of the emitters shou…
We report the broadband (~ 25 nm) enhancement of radiative decay rate of colloidal quantum dots by exploiting the hyperbolic dispersion of a one-dimensional nonmagnetic metamaterial structure.
Colloidal quantum dots (cQDs) are now a mature nanomaterial with optical properties customizable through varying size and composition. However, their use in optical devices is limited as they are not widely available in convenient forms such as optical fibers. With advances in polymerization methods incorporating nanocrystals, nanocomposite materials suitable for processing into high quality hybrid active fibers can be achieved. We demonstrate a plastic optical fiber fabrication method which ensures homogeneous dispersion of cQDs within a polymer core matrix. Loading concentrations between 10$…
Optical near-field interactions between nanostructured matter, such as quantum dots, result in unidirectional optical excitation transfer when energy dissipation is induced. This results in versatile spatiotemporal dynamics of the optical excitation, which can be controlled by engineering the dissipation processes and exploited to realize intelligent capabilities such as solution searching and decision making. Here we experimentally demonstrate the ability to solve a decision making problem on the basis of optical excitation transfer via near-field interactions by using colloidal quantum dots …
Upon photo- or electrical-excitation, colloidal quantum dots (QDs) are often found in multi-carrier states due to multi-photon absorption and photo-charging of the QDs. While many of these multi-carrier states are observed in single-dot spectroscopy, their properties are not well studied due to random charging/discharging, emission intensity intermittency, and uncontrolled surface defects of single QD. Here we report in-situ deciphering the charging status, and precisely assessing the absorption cross section, and determining the absolute emission quantum yield of mono-exciton and biexciton st…
All-inorganic CsPbBr3 perovskite colloidal quantum dots have recently emerged as promising material for a variety of optoelectronic applications, among others for multi-photon-pumped lasing. Nevertheless, high irradiance levels are generally required for such multi-photon processes. One strategy to enhance the multi-photon absorption is taking advantage of high local light intensities using photonic nanostructures. Here, we investigate two-photon-excited photoluminescence of CsPbBr3 perovskite quantum dots on a silicon photonic crystal slab. By systematic excitation of optical resonances using…
Spontaneous emission (SE) rate of any light emitters directly scales with the locally available modes for photons. The emission rate can be modified, by changing the dielectric environment of light emitters. Generally cavities with modes in resonance to light emission frequency, are used to amplify the light emission rate. The Fermi golden rule predicts that if the cavity modes are offresonant to the emission frequency, then the SE rate is suppressed. In this study, we demonstrate that the SE of colloidal alloyed quantum dots is inhibited by coupling them to chemically synthesized Silver nanow…
