Ag colloids and arrays for plasmonic non-radiative energy transfer from quantum dots to a quantum well
Graham P. Murphy, John J. Gough, Luke J. Higgins, Vasilios D. Karanikolas, Keith M. Wilson, Jorge A. Garcia Coindreau, Vitaly Z. Zubialevich, Peter J. Parbrook, A. Louise Bradley
Ag nanoparticles in the form of colloids and ordered arrays are used to demonstrate plasmon-mediated non-radiative energy transfer from quantum dots to quantum wells with varying top barrier thicknesses. Plasmon-mediated energy transfer efficiencies of up to ~25% are observed with the Ag colloids. The distance dependence of the plasmon-mediated energy transfer is found to follow the same d^{-4} dependence as the direct quantum dot to quantum well energy transfer. There is also evidence for an increase in the characteristic distance of the interaction, thus indicating that it follows a Förster-like model with the Ag nanoparticle-quantum dot acting as an enhanced donor dipole. Ordered Ag nanoparticle arrays display plasmon-mediated energy transfer efficiencies up to ~21%. To explore the tunability of the array system, two arrays with different geometries are presented. It is demonstrated that changing the geometry of the array allows a transition from overall quenching of the acceptor quantum well emission to enhancement, as well as control of the competition between the quantum dot donor quenching and energy transfer rates.
We theoretically investigated the transmission properties of a single plasmon interacting with two-level quantum dots (QDs) and a V-type three-level QD, coupled to plasmonic waveguide, respectively. We investigated the transmission of a single plasmon by a system including a V-type three-level QD and compared it with that by a system including only two-level QDs.
Nanoparticles made of non-noble metals such as gallium have recently attracted significant attention due to promising applications in UV plasmonics. To date, experiments have mostly focused on solid and liquid pure gallium particles immobilized on solid substrates. However, for many applications, colloidal liquid-metal nanoparticle solutions are vital. Here, we experimentally demonstrate strong UV plasmonic resonances of eutectic gallium-indium (EGaIn) liquid-metal alloy nanoparticles suspended in ethanol. We rationalise experimental results through a theoretical model based on Mie theory. Our…
We use cathodoluminescence to locate droplet epitaxy quantum dots with a precision $\lesssim$ nm before fabricating nanoantennas in their vicinity by electron-beam lithography. Cathodoluminescence is further used to evidence the effect of the antennas as a function of their length on the light emitted by the dot. Experimental results are in good agreement with numerical simulations of the structures.
Strong light-matter interaction and high-efficiency optical collection of fluorescence from quantum emitters are crucial topics in quantum and nanophotonic fields. High-quality cavities, dispersive photonic crystal waveguides and even plasmonic structures have been used to enhance the interaction with quantum emitters, thus realize efficient collection of the fluorescence. In this work, a new method is proposed to collect the fluorescence of quantum dots (QDs) with a fiber-integrated multimode silver nanowire (AgNW) waveguide. Fluorescence lifetime measurement is performed to investigate the c…
We demonstrate scaffolding of plasmonic nanoparticles by topological defects induced by colloidal microspheres to match their surface boundary conditions with a uniform far-field alignment in a liquid crystal host. Displacing energetically costly liquid crystal regions of reduced order, anisotropic nanoparticles with concave or convex shapes not only stably localize in defects but also self-orient with respect to the microsphere surface. Using laser tweezers, we manipulate the ensuing nanoparticle-microsphere colloidal dimers, probing the strength of elastic binding and demonstrating self-asse…
Optical properties of colloidal plasmonic titanium nitride nanoparticles are examined with an eye on their photothermal via transmission electron microscopy and optical transmittance measurements. Single crystal titanium nitride cubic nanoparticles with an average size of 50 nm exhibit plasmon resonance in the biological transparency window. With dimensions optimized for efficient cellular uptake, the nanoparticles demonstrate a high photothermal conversion efficiency. A self-passivating native oxide at the surface of the nanoparticles provides an additional degree of freedom for surface funct…
We investigate theoretically the entanglement of two quantum dots (QDs) coupled to metallic nanowaveguide in the presence of the flip-flop interaction with the analytical solutions of eigenvalue equations of the coupled system. High entanglement of two QDs could be achieved by adjusting the direct coupling strength of the QDs, the interaction of QDs with near-zero waveguide modes, interparticle distance of the QDs, total dissipation and detuning even when two QDs are resonant with the incident single plasmon. The discussed system with the flip-flop interaction provides us rich way to realize t…
Structured light has emerged as an important tool to interrogate and manipulate matter at micron and sub-micron scale. One form of structured light is an optical vortex beam. The helical wavefront of these vortices carry orbital angular momentum which can be transferred to a Brownian colloid. When the colloid is made of metallic nanostructures, such as silver and gold, resonant optical effects play a vital role, and the interaction leads to complex dynamics and assembly. This brief review aims to discuss some recent work on trapping plasmonic colloids with optical vortices and their lattices. …
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…
Localized surface plasmon resonances have recently attracted considerable attention due to their ability to dramatically enhance near-field optical intensities and boost nanoscale light-matter interactions. Here we demonstrate unambiguously that polyhedral silver nanoparticles can be tailored to promote enhanced coherent emission from organic dye dispersions in a cavity. In particular, we observe that nanoparticles supporting resonances close to the absorption peak of the dye yield to more efficient lasing, up to one order of magnitude, which is also evidenced by the narrowing of the emission …
Fabrication and characterization of shape- and topology-optimized optical cavities with deep sub-wavelength confinement for interfacing with colloidal quantum dots
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…
We report on the deterministic coupling between single semiconducting nanowire quantum dots emitting in the visible and plasmonic Au nanoantennas. Both systems are separately carefully characterized through microphotoluminescence and cathodoluminescence. A two-step realignment process using cathodoluminescence allows for electron beam lithography of Au antennas near individual nanowire quantum dots with a precision of 50 nm. A complete set of optical properties are measured before and after antenna fabrication. They evidence both an increase of the NW absorption, and an improvement of the quan…
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…
Multiexcitonic transitions and emission of several photons per excitation comprise a very attractive feature of semiconductor quantum dots for optoelectronics applications. However, these higher-order radiative processes are usually quenched in colloidal quantum dots by Auger and other non-radiative decay channels. To increase the multiexcitonic quantum efficiency, several groups have explored plasmonic enhancement, so far with moderate results. By controlled positioning of individual quantum dots in the near field of gold nanocone antennas, we enhance the radiative decay rates of monoexcitons…
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.
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 enhancement of the photoluminescence of quantum dots induced by an optical nanoantenna has been studied considerably, but there is still significant interest in optimizing and miniaturizing such structures, especially when accompanied by an experimental demonstration. Most of the realizations use plasmonic platforms, and some also use all-dielectric nanoantennas, but hybrid dielectric-plasmonic (subwavelength) nanostructures have been very little explored. In this paper, we propose and demonstrate single subwavelength hybrid dielectric-plasmonic optical nanoantennas coupled to localized qu…
Active nanoplasmonics has recently led to the emergence of many promising applications. One of them is spaser (surface plasmons amplification by stimulated emission of radiation) that has been shown to generate coherent and intense fields of selected surface plasmon modes that are strongly localized in the nanoscale. We propose a novel nanospaser composed of metal nanoparticles-graphene nanodisks hybrid plasmonic system as its resonator and a quantum dots cascade stack as its gain medium. We derive the plasmonic fields induced by pulsed excitation through the use of the effective medium theory…
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…
It is a generally accepted idea that the particle size distribution strongly affects the optical spectra of colloidal plasmonic nanoparticles. It is often quoted as one of the main reasons while explaining the mismatch between the theoretical and experimental optical spectra of such nanoparticles. In this work, these aspects are critically analyzed by means of a bottom up statistical approach that considers variables such as mean, standard deviation and skewness of the nanoparticle size distribution independently from one another. By assuming normal and log-normal distributions of the particle…
We introduce the concept of optical control of the fluorescence yield of CdSe quantum dots through plasmon-induced structural changes in random semicontinuous nanostructured gold films. We demonstrate that the wavelength- and polarization dependent coupling between quantum dots and the semicontinuous films, and thus the fluorescent emission spectrum, can be controlled and significantly increased through the optical extinction of a selective band of eigenmodes in the films. This optical method of effecting controlled changes in the metal nanostructure allows for versatile functionality in a sin…
An integrated interference and colloid sphere lithography (IICL) is presented to produce complex plasmonic structures consisting of wavelength-scaled periodic arrays of nano-objects with arbitrary array symmetry and controllable nano-scaled sub-structure. The IICL method is based on illumination of colloid sphere monolayers by interference patterns synchronized with sphere arrays along arbitrary crystallographic directions. This nano-kaleidoscope method enables to tune four structure parameters independently: the symmetry and characteristic periodicity of the interference pattern might be vari…
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…
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…
We report an experimental study of the plasmon-assisted spontaneous emission and the Förster resonance energy transfer between organic molecules and semiconductor colloidal quantum dots. The localized plasmonic field in the nanogap between a gold nano-popcorn's tips and a 5-nm separated gold film supports high photonic density of states and provides pathways for the light-matter interaction mechanisms. We demonstrate that, besides the total spontaneous emission rate enhancement factor up to 66 for quantum dots and molecules, the Förster resonance energy transfer efficiency and rate constant ar…
We report on the growth and optical characterisation of droplet GaAs quantum dots with extremely-thin (11 nm) capping layers. To achieve such result, an internal thermal heating step is introduced during the growth and its role in the morphological properties of the quantum dots obtained is investigated via scanning electron and atomic force microscopy. Photoluminescence measurements at cryogenic temperatures show optically stable, sharp and bright emission from single quantum dots, at near-infrared wavelengths. Given the quality of their optical properties and the proximity to the surface, su…
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…
We report that hybridizing semiconductor quantum dots with plasmonic metamaterial leads to a multi-fold intensity increase and narrowing of their photoluminescence spectrum. The luminescence enhancement is a clear manifestation of the cavity quantum electrodynamics Purcell effect that can be controlled by the metamaterial's design. This observation is an essential step towards understanding loss compensation in metamaterials with gain media and for developing metamaterial-enhanced gain media.
Plasmonic nanopatch antennas that incorporate dielectric gaps hundreds of picometers to several nanometers thick have drawn increasing attention over the past decade because they confine electromagnetic fields to grossly sub-diffraction limited volumes. Substantial control over the optical properties of excitons and color centers confined within these plasmonic cavities has already been demonstrated with far-field optical spectroscopies, but near-field optical spectroscopies are essential to an improved understanding of the plasmon-emitter interaction at the nanoscale. Here, we characterize th…
Quantum dots optically excited in close proximity to a silver nanowire can launch nanowire surface plasmons. The challenge related to this promising hybrid system is to control the position of nanoemitters on the nanowire. We report on the use of two-photon photopolymerization process to strategically position quantum dots on nanowires at controlled sites. A parametric study of the distance between the quantum dots and the nanowire extremity shows that precise control of the position of the launching sites enables control of light intensity at the wire end, through surface plasmon propagation.
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…
Transport properties of a single plasmon interacting with two quantum dots (QDs) system coupled to one-dimensional surface plasmonic waveguide are investigated theoretically via the real-space approach. We mainly focus on the coupling effects of the two QDs on the transmission properties of a single incident plasmon. We demonstrated that switching of a single plasmon can be achieved by controlling the interparticle distance, the interparticle coupling strength, and the QD-waveguide coupling strength, as well as spectral detuning. We also showed that the coupling between the continuum excitatio…
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…
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…
We present optical investigations of hybrid plasmonic nanosystems consisting of lithographically defined plasmonic Au-waveguides or beamsplitters on GaAs substrates coupled to proximal self-assembled InGaAs quantum dots. We designed a sample structure that enabled us to precisely tune the distance between quantum dots and the sample surface during nano-fabrication and demonstrated that non-radiative processes do not play a major role for separations down to $\sim 10 nm$. A polarized laser beam focused on one end of the plasmonic nanostructure generates propagating surface plasmon polaritons th…
We introduce a scheme for generating entanglement between two quantum dots using a plasmonic waveguide made from an array of metal nanoparticles. We show that the scheme is robust to loss, enabling it to work over long distance plasmonic nanoparticle arrays, as well as in the presence of other imperfections such as the detuning of the energy levels of the quantum dots. The scheme represents an alternative strategy to the previously introduced dissipative driven schemes for generating entanglement in plasmonic systems. Here, the entanglement is generated by using dipole-induced interference eff…
We investigate the quantum entanglement between two quantum dots in a plasmonic waveguide with near-zero mode index, considering the dependence of concurrence on interdot distance, quantum dot-waveguide frequency detuning and coupling strength ratio. High concurrence is achieved for a wide range of interdot distance due to the near-zero mode index, which largely relaxes the strict requirement of interdot distance in conventional dielectric waveguides or metal nanowires. The proposed quantum dot-waveguide system with near-zero phase variation along the waveguide near the mode cutoff frequency s…
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 estimat…
We report single plasmon generation with a self-assembled InAs/GaAs quantum dot embedded in a plasmonic microring resonator. The plasmonic cavity based on a GaAs microring is defined on an atomically-smooth silver surface. We fabricated this structure with the help of transfer printing, which enables the pick-and-place assembly of the complicated, heterogeneous three dimensional stack. We show that a high-order surface-plasmon-polariton transverse mode mediates efficient coupling between the InAs/GaAs quantum dots and the plasmonic cavity, paving the way for developing plasmonic quantum light …
The plasmonic structures exhibiting narrowband resonances (NBR) are of a great interest for various applications. We propose to use hysteresis behavior in a 1D system of nonlinear nanoresonators in order to achieve the NRB; the nonlinearity is provided by saturation of a two-level quantum system coupled with the nanoresonators (nanolaser/spaser configuration). Quantum Dots (QD) were assumed as quantum systems; their numerical parameters have been adopted for estimations. Role of the loss compensation on the quality of the NBR is shown for below (under compensation) and above threshold (generat…
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）
By modifying the density of optical states at the location of an emitter, weak cavity-emitter coupling can enable a host of potential applications in quantum optics, from the development of low- threshold lasers to brighter single-photon sources for quantum cryptography. Although some of the first demonstrations of spontaneous emission modification occurred in metallic structures, it was only after the recent demonstration of cavity quantum electrodynamics effects in dielectric optical cavities that metal-based optical cavities were considered for quantum optics applications. Advantages of met…
Scattering properties of a single plasm on interacting with three non-equally spaced quantum dots coupled to one-dimensional surface plasmonic waveguide is investigated theoretically via the real-space approach. It is demonstrated that the transmission and reflection of a single plasmon can be switched on or off by controlling the detuning and changing the interparticle distances between the quantum dots. By controlling the transition frequencies and interparticle distances of QDs, one can construct a half-transmitting mirror with three QDs system. We also showed that controlling the transitio…
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…
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.
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…
