Multiple Quantum Dots Research Articles

In-plane commensurate GaN/AlN junctions: Single-layer composite structures, single and multiple quantum wells and quantum dots

In-plane commensurate GaN/AlN junctions: Single-layer composite structures, single and multiple quantum wells and quantum dots

A novel “top‐down” strategy for preparing organosilica micelle encapsulating multiple hydrophobic quantum dots as efficient fluorescent label

Organosilica micelle incorporating multiple hydrophobic CdSe/ZnS quantum dots (QDs) was prepared by a surfactant free microemulsion approach assisted by ultrasonication. The size of emulsion droplets along with their QDs loading amount was controlled and determined by QDs concentration in alkylsilane. Sodium silicate deposition was important in transforming the amorphous micelles into spherical beads with well defined QDs/SiO2 structure. These QD micelles were subsequently modified with epoxy group by silane coupling and covalently conjugated to transferrin. After incubated with Hela cells, these fluorescent micelles were detected as bright clusters in cells, which demonstrated the efficient cell internalization of these functionalized particles.

Electronic Nose Technology Based on Quantum Dot Filters

The electronic nose with chemical dyes as sensor can react with target gas and have specific color changes. In general, RGB camera collects a group of images to record these changes used for pattern recognition. RGB filters are not sensitive to the slight color changes, which limits the performance of this kind of electronic nose. This paper demonstrates using quantum dot spec-troscopy technology to solve this problem. Multiple quantum dot filters are placed on the surface of image sensor. When capturing images, there are more response channels of the same incident light than RGB filters. Simulation and experiment both prove that quantum dot filters with appropriate processing are more sensitive to color changes than RGB filters.

A novel electrochemiluminescence immunosensor based on Mn doped Ag2S quantum dots probe for laminin detection

In recent years, quantum dots (QDs) have been widely used as biological probes, however, most of the QDs used in electrochemiluminescence (ECL) studies have toxic heavy metals, which was an important road-block for QDs in bio-application. A novel low-toxic, water-dispersed Mn doped Ag2S quantum dots (Ag2S:Mn QDs) were firstly served as a kind of ECL materials, and applied to construct ECL biosensor for the detection of laminin (LN). Here, the Ag2S QDs were simply synthesized with 3-Mercaptopropionic acid (3-MPA) as growth template, and then Mn was doped into Ag2S QDs to improve the optical and electrical properties. Herein, the energy levels and electron transfer path were studied in detail to explain the ECL performance of Ag2S:Mn QDs with K2S2O8 as coreactant. Furthermore, the bovine serum albumin (BSA) containing amino groups (-NH2) could easily combine with Ag2S:Mn QDs via amide bond, and multiple QDs gathered to form a unit (BSA-Ag2S:Mn bioconjugates), which provided mass active area to immobilize antibody and possessed strong ECL emission to improve the detection sensitivity. Based on a sandwiched immunoassay method, this proposed immunosensor achieved a linear range from 10pg/mL to 100ng/mL with a relatively low detection limit of 3.2pg/mL for LN detection. Compared with traditional luminescent reagents, the Ag2S:Mn QDs could be served as a kind of promising luminescent materials for new types of ECL biosensors in the future due to its low toxicity, well photo-stability and easy surface functionalization.

Detection and control of charge states in a quintuple quantum dot.

A semiconductor quintuple quantum dot with two charge sensors and an additional contact to the center dot from an electron reservoir is fabricated to demonstrate the concept of scalable architecture. This design enables formation of the five dots as confirmed by measurements of the charge states of the three nearest dots to the respective charge sensor. The gate performance of the measured stability diagram is well reproduced by a capacitance model. These results provide an important step towards realizing controllable large scale multiple quantum dot systems.

Fluorescence Blinking as an Output Signal for Biosensing.

We demonstrate the first biosensing strategy that relies on quantum dot (QD) fluorescence blinking to report the presence of a target molecule. Unlike other biosensors that utilize QDs, our method does not require the analyte to induce any fluorescence intensity or color changes, making it readily applicable to a wide range of target species. Instead, our approach relies on the understanding that blinking, a single particle phenomenon, is obscured when several QDs lie within the detection volume of a confocal microscope. If QDs are engineered to aggregate when they encounter a particular target molecule, the observation of quasi-continuous emission should indicate its presence. As proof of concept, we programmed DNAs to drive rapid isothermal assembly of QDs in the presence of a target strand (oncogene K-ras). The assemblies, confirmed by various gel techniques, contained multiple QDs and were readily distinguished from free QDs by the absence of blinking.

Control of coherence transfer via tunneling in quadruple and multiple quantum dots

Transfer and manipulation of coherence among the ground state and indirect exciton states via tunneling in quadruple and multiple quantum dots is analyzed. By applying suitable amplitudes and sequences of the pump and tunneling pulses, a complete transfer of coherence or an arbitrary distribution of coherence of multiple states can be realized. The method, which is an adiabatic passage process, is different from previous works on quantum dot molecules in the way that the population can transfer from the ground state to the indirect exciton states without populating the direct exciton state, and thus no spontaneous emission occurs. This investigation can provide further insight to help the experimental development of coherence transfer in semiconductor structures, and may have potential applications in quantum information processing.

Tunneling-assisted coherent population transfer and creation of coherent superposition states in triple quantum dots

A scheme is proposed for coherent population transfer and creation of coherent superposition states assisted by one time-dependent tunneling pulse and one time-independent tunneling pulse in triple quantum dots. Time-dependent tunneling, which is similar to the Stokes laser pulse used in traditional stimulated Raman adiabatic passage, can lead to complete population transfer from the ground state to the indirect exciton states. Time-independent tunneling can also create double dark states, resulting in the distribution of the population and arbitrary coherent superposition states. Such a scheme can also be extended to multiple quantum dots assisted by one time-dependent tunneling pulse and more time-independent tunneling pulses.

Quantum Dots-Ligand Complex as Ratiometric Fluorescent Nanoprobe for Visual and Specific Detection of G-Quadruplex.

By complexing a nonionic G-quadruplex ligand with hybrid dual-emission quantum dots (QDs), a ratiometric fluorescent nanoprobe is developed for G-quadruplex detection in a sensitive and specific manner. The QDs nanohybrid comprised of a green-emission QD (gQD) and multiple red-emission QDs (rQDs) inside and outside of a silica shell, respectively, is utilized as the signal displaying unit. Only the presence of G-quadruplex can displace the ligand from QDs, breaking up the QDs-ligand complexation, and inducing the restoration of the rQDs fluorescence. Since the fluorescence of embedded gQD stays constant, variations of the dual-emission intensity ratios display continuous color changes from green to bright orange, which can be clearly observed by the naked eye. Furthermore, by utilizing competitive binding of a cationic ligand versus the nonionic ligand toward G-quadruplex, the nanoprobe is demonstrated to be applicable for assessing the affinity of a G-quadruplex-targeted anticancer drug candidate, exhibiting ratiometric fluorescence signals (reverse of that for G-quadruplex detection). By making use of the specificity of the ligand binding with G-quadruplex against a double helix, this nanoprobe is also demonstrated to be capable of sensitive detection of one-base mutation, exhibiting sequence-specific ratiometric fluorescence signals. By functionalizing with a nuclear localization peptide, the nanoprobe can be used for visualization of G-quadruplex in the nucleus of human cells.

Theory of photovoltaic characteristics of semiconductor quantum dot solar cells

We develop a comprehensive rate equations model for semiconductor quantum dot solar cells (QDSCs). The model is based on the continuity equations with a proper account for quantum dots (QDs). A general analytical expression for the total current density is obtained, and the current-voltage characteristic is studied for several specific situations. The degradation in the open circuit voltage of the QDSC is shown to be due to strong spontaneous radiative recombination in QDs. Due to small absorption coefficient of the QD ensemble, the improvement in the short circuit current density is negligible if only one QD layer is used. If spontaneous radiative recombination would be suppressed in QDs, a QDSC with multiple QD layers would have significantly higher short circuit current density and power conversion efficiency than its conventional counterpart. The effects of photoexcitation of carriers from discrete-energy states in QDs to continuum-energy states are discussed. An extended model, which includes excited states in QDs, is also introduced.

Theory of multiple quantum dot formation in strained-layer heteroepitaxy

We develop a theory for the experimentally observed formation of multiple quantum dots (QDs) in strained-layer heteroepitaxy based on surface morphological stability analysis of a coherently strained epitaxial thin film on a crystalline substrate. Using a fully nonlinear model of surface morphological evolution that accounts for a wetting potential contribution to the epitaxial film's free energy as well as surface diffusional anisotropy, we demonstrate the formation of multiple QD patterns in self-consistent dynamical simulations of the evolution of the epitaxial film surface perturbed from its planar state. The simulation predictions are supported by weakly nonlinear analysis of the epitaxial film surface morphological stability. We find that, in addition to the Stranski-Krastanow instability, long-wavelength perturbations from the planar film surface morphology can trigger a nonlinear instability, resulting in the splitting of a single QD into multiple QDs of smaller sizes, and predict the critical wavelength of the film surface perturbation for the onset of the nonlinear tip-splitting instability. The theory provides a fundamental interpretation for the observations of “QD pairs” or “double QDs” and other multiple QDs reported in experimental studies of epitaxial growth of semiconductor strained layers and sets the stage for precise engineering of tunable-size nanoscale surface features in strained-layer heteroepitaxy by exploiting film surface nonlinear, pattern forming phenomena.

Facile synthesis of wormlike quantum dots-encapsulated nanoparticles and their controlled surface functionalization for effective bioapplications

Semiconductor quantum dots (QDs) are considered as ideal fluorescent probes owing to their intrinsic optical properties. It has been demonstrated that the size and shape of nanoparticles significantly influence their behaviors in biological systems. In particular, one-dimensional (1D) nanoparticles with larger aspect ratios are desirable for cellular uptake. Here, we explore a facile and green method to prepare novel 1D wormlike QDs@SiO2 nanoparticles with controlled aspect ratios, wherein multiple QDs are arranged in the centerline of the nanoparticles. Then, an excellent cationic gene carrier, ethanolamine-functionalized poly(glycidyl methacrylate) (denoted by BUCT-PGEA), was in-situ produced via atom transfer radical polymerization on the surface of the QDs@SiO2 nanoparticles to achieve stable surfaces (QDs@SiO2-PGEA) for effective bioapplications. We found that the wormlike QDs@SiO2-PGEA nanoparticles demonstrated much higher gene transfection performance than ordinary spherical counterparts. In addition, the wormlike nanoparticles with larger aspect ratio performed better than those with smaller ratio. Furthermore, the gene delivery processes including cell entry and plasmid DNA (pDNA) escape and transport were also tracked in real time by the QDs@SiO2-PGEA/pDNA complexes. This work realized the integration of efficient gene delivery and real-time imaging within one controlled 1D nanostructure. These constructs will likely provide useful information regarding the interaction of nanoparticles with biological systems.

Electrical and Thermoelectric Transport by Variable Range Hopping in Thin Black Phosphorus Devices.

The moderate band gap of black phosphorus (BP) in the range of 0.3-2 eV, along a high mobility of a few hundred cm(2) V(-1) s(-1) provides a bridge between the gapless graphene and relatively low-mobility transition metal dichalcogenides. Here, we study the mechanism of electrical and thermoelectric transport in 10-30 nm thick BP devices by measurements of electrical conductance and thermopower (S) with various temperatures (T) and gate-electric fields. The T dependences of S and the sheet conductance (σ□) of the BP devices show behaviors of T(1/3) and exp[-(1/T)(1/3)], respectively, where S reaches ∼0.4 mV/K near room T. This result indicates that two-dimensional (2D) Mott's variable range hopping (VRH) is a dominant mechanism in the thermoelectric and electrical transport in our examined thin BP devices. We consider the origin of the 2D Mott's VRH transport in our BPs as trapped charges at the surface of the underlying SiO2 based on the analysis with observed multiple quantum dots.

Computer-automated tuning of semiconductor double quantum dots into the single-electron regime

We report the computer-automated tuning of gate-defined semiconductor double quantum dots in GaAs heterostructures. We benchmark the algorithm by creating three double quantum dots inside a linear array of four quantum dots. The algorithm sets the correct gate voltages for all the gates to tune the double quantum dots into the single-electron regime. The algorithm only requires (1) prior knowledge of the gate design and (2) the pinch-off value of the single gate T that is shared by all the quantum dots. This work significantly alleviates the user effort required to tune multiple quantum dot devices.

Entanglement properties of quantum polaritons

Exciton polaritons are coupled states of matter and light, originated by the strong interaction between an optical mode and semiconductor excitons. This interaction can be obtained also at a single-particle level, in which case it has been shown that a quantum treatment is mandatory. In this work we study the light-matter entanglement of polaritons from a fully quantum formalism including pumping and dissipation. We find that the entanglement is completely destroyed if the exciton and photon are tuned at the resonance condition, even under very low pumping rates. Instead, the best condition for maximizing entanglement and purity of the steady state is when the exciton and photon are out of resonance and when incoherent pumping exactly compensates the dissipation rate. In the presence of multiple quantum dots coupled to the light mode, matter-light entanglement survives only at larger detuning for a higher number of quantum dots considered.

Molecular Layer Deposition (MLD): Monomolecular‐Step Growth of Polymers with Designated Sequences

SummaryTailored organic thin films with designated molecular arrangements are expected to provide a variety of photonic/electronic devices due to their ability to optimize the performance or to generate new functions by controlling the electron wavefunction shapes. Molecular Layer Deposition (MLD), which enables monomolecular‐step organic film growth, is one of the promising fabrication processes of tailored organic thin films. In the present report, first, the concept and an experimental demonstration of MLD are described. Next, after three featured capabilities of MLD, namely, ultra‐thin/conformal, tailored, and selective organic film growth are presented, applications of MLD based on these capabilities are reviewed, emphasizing polymer multiple quantum dots we have developed. Finally, conceptual proposal of MLD for the molecular targeted drug delivery for cancer therapy is suggested.

High performance red-emitting multiple layer InGaN/GaN quantum dot lasers

InGaN/GaN self-organized quantum dots can provide useful advantages over quantum wells for the realization of long-wavelength visible light sources because the dots are formed by strain relaxation. A III–nitride based laser emitting in the red (λ ∼ 630 nm), which has not been demonstrated with quantum wells, would be useful for a host of applications. We have investigated the epitaxy and characteristics of self-organized InGaN/GaN multiple layer quantum dots grown by plasma-assisted molecular beam epitaxy and have optimized their properties by tuning the growth parameters. Red-emitting (λ ∼ 630 nm) quantum dots have radiative lifetime ∼2.5 ns and internal quantum efficiency greater than 50%. Edge-emitting red-lasers with multi-dot layers in the active region exhibit an extremely low threshold current density of 1.6 kA/cm2, a high temperature coefficient T0 = 240 K, and a large differential gain dg/dn = 9 × 10−17 cm2.

Design and development of high bioluminescent resonance energy transfer efficiency hybrid-imaging constructs

Here we describe the design and construction of an imaging construct with high bioluminescent resonance energy transfer (BRET) efficiency that is composed of multiple quantum dots (QDs; λem = 655 nm) self-assembled onto a bioluminescent protein, Renilla luciferase (Rluc). This is facilitated by the streptavidin–biotin interaction, allowing the facile formation of a hybrid-imaging construct (HIC) comprising up to six QDs (acceptor) grafted onto a light-emitting Rluc (donor) core. The resulting assembly of multiple acceptors surrounding a donor permits this construct to exhibit high resonance energy transfer efficiency (∼64.8%). The HIC was characterized using fluorescence excitation anisotropy measurements and high-resolution transmission electron microscopy. To demonstrate the application of our construct, a generation-5 (G5) polyamidoamine dendrimer (PAMAM) nanocarrier was loaded with our HIC for in vitro and in vivo imaging. We envision that this design of multiple acceptors and bioluminescent donor will lead to the development of new BRET-based systems useful in sensing, imaging, and other bioanalytical applications.

Engineered nanoconstructs for the multiplexed and sensitive detection of high-risk pathogens.

Many countries categorize the causative agents of severe infectious diseases as high-risk pathogens. Given their extreme infectivity and potential to be used as biological weapons, a rapid and sensitive method for detection of high-risk pathogens (e.g., Bacillus anthracis, Francisella tularensis, Yersinia pestis, and Vaccinia virus) is highly desirable. Here, we report the construction of a novel detection platform comprising two units: (1) magnetic beads separately conjugated with multiple capturing antibodies against four different high-risk pathogens for simple and rapid isolation, and (2) genetically engineered apoferritin nanoparticles conjugated with multiple quantum dots and detection antibodies against four different high-risk pathogens for signal amplification. For each high-risk pathogen, we demonstrated at least 10-fold increase in sensitivity compared to traditional lateral flow devices that utilize enzyme-based detection methods. Multiplexed detection of high-risk pathogens in a sample was also successful by using the nanoconstructs harboring the dye molecules with fluorescence at different wavelengths. We ultimately envision the use of this novel nanoprobe detection platform in future applications that require highly sensitive on-site detection of high-risk pathogens.

Fabrication of photoactive heterostructures based on quantum dots decorated with Au nanoparticles

Silica based multifunctional heterostructures, exhibiting near infrared (NIR) absorption (650–1200 nm) and luminescence in the visible region, represent innovative nanosystems useful for diagnostic or theranostic applications. Herein, colloidal synthetic procedures are applied to design a photoactive multifunctional nanosystem. Luminescent silica (SiO2) coated quantum dots (QDs) have been used as versatile nanoplatforms to assemble on their surface gold (Au) seeds, further grown into Au spackled structures. The synthesized nanostructures combine the QD emission in the visible region, and, concomitantly, the distinctive NIR absorption of Au nanodomains. The possibility of having multiple QDs in a single heterostructure, the SiO2 shell thickness, and the extent of Au deposition onto SiO2 surface have been carefully controlled. The work shows that a single QD entrapped in 16 nm thick SiO2 shell, coated with Au speckles, represents the most suitable geometry to preserve the QD emission in the visible region and to generate NIR absorption from metal NPs. The resulting architectures present a biomedical potential as an effective optical multimodal probes and as promising therapeutic agents due to the Au NP mediated photothermal effect.