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Semantic Search for: "quantum dots"

  1. In this paper, a system of two or more quantum dots interacting with a dissipative plasmonic nanostructure is investigated in detail by using a cavity quantum electrodynamics approach with a model Hamiltonian. We focus on determining and understanding system configurations that generate multiple bipartite quantum entanglements between the occupation states of the quantum dots. These configurations include allowing for the quantum dots to be asymmetrically coupled to the plasmonic system. Analytical solution of a simplified limit for an arbitrary number of quantum dots and numerical simulations and optimization for the two- and three-dot cases are used to develop guidelines formore » maximizing the bipartite entanglements. For any number of quantum dots, we show that through simple starting states and parameter guidelines, one quantum dot can be made to share a strong amount of bipartite entanglement with all other quantum dots in the system, while entangling all other pairs to a lesser degree.« less
  2. We have investigated a nanostructured material known as sub-monolayer type-II QDs, made from wide bandgap II-VI semiconductors. Our goal is to understand and exploit their tunable optical and electrical properties by taking advantage of the type-II band alignment and quantum confinement effects. Type-II ZnTe quantum dots (QDs) in a ZnSe host are particularly interesting because of their relatively large valence band and conduction band offsets. In the current award we have developed new materials based on sub-monolayer type-II QDs that may be advantageous for photovoltaic and spintronics applications. We have also expanded the structural characterization of these materials by refiningmore » the X-ray diffraction methodologies needed to investigate them. In particular, we have 1) demonstrated ZnCdTe/ZnCdSe type-II QDs materials that have ideal properties for the development of novel high efficiency “intermediate band solar cells”, 2) we developed a comprehensive approach to describe and model the growth of these ultra-small type-II QDs, 3) analysis of the evolution of the photoluminescence (PL) emission, combined with other characterization probes allowed us to predict the size and density of the QDs as a function of the growth conditions, 4) we developed and implemented novel sophisticated X-ray diffraction techniques from which accurate size and shape of the buried type-II QDs could be extracted, 5) a correlation of the shape anisotropy with polarization dependent PL was observed, confirming the QDs detailed shape and providing insight about the effects of this shape anisotropy on the physical properties of the type-II QD systems, and 6) a detailed “time-resolved Kerr rotation” investigation has led to the demonstration of enhanced electron spin lifetimes for the samples with large densities of type-II QDs and an understanding of the interplay between the QDs and Te-isoelectroic centers, a defect that forms in the spacer layers that separate the QDs.« less
  3. Organic–inorganic lead-halide perovskites have been the subject of recent intense interest due to their unusually strong photovoltaic performance. A new addition to the perovskite family is all-inorganic Cs–Pb-halide perovskite nanocrystals, or quantum dots, fabricated via a moderate-temperature colloidal synthesis. While being only recently introduced to the research community, these nanomaterials have already shown promise for a range of applications from color-converting phosphors and light-emitting diodes to lasers, and even room-temperature single-photon sources. Knowledge of the optical properties of perovskite quantum dots still remains vastly incomplete. Here we apply various time-resolved spectroscopic techniques to conduct a comprehensive study of spectral andmore » dynamical characteristics of single- and multiexciton states in CsPbX3 nanocrystals with X being either Br, I, or their mixture. Specifically, we measure exciton radiative lifetimes, absorption cross-sections, and derive the degeneracies of the band-edge electron and hole states. We also characterize the rates of intraband cooling and nonradiative Auger recombination and evaluate the strength of exciton–exciton coupling. The overall conclusion of this work is that spectroscopic properties of Cs–Pb-halide quantum dots are largely similar to those of quantum dots of more traditional semiconductors such as CdSe and PbSe. At the same time, we observe some distinctions including, for example, an appreciable effect of the halide identity on radiative lifetimes, considerably shorter biexciton Auger lifetimes, and apparent deviation of their size dependence from the “universal volume scaling” previously observed for many traditional nanocrystal systems. The high efficiency of Auger decay in perovskite quantum dots is detrimental to their prospective applications in light-emitting devices and lasers. Furthermore, this points toward the need for the development of approaches for effective suppression of Auger recombination in these nanomaterials, using perhaps insights gained from previous studies of II–VI nanocrystals.« less
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  4. Enhancement-mode Si/SiGe electron quantum dots have been pursued extensively by many groups for their potential in quantum computing. Most of the reported dot designs utilize multiple metal-gate layers and use Si/SiGe heterostructures with Ge concentration close to 30%. Here, we report the fabrication and low-temperature characterization of quantum dots in the Si/Si0.8Ge0.2 heterostructures using only one metal-gate layer. We find that the threshold voltage of a channel narrower than 1 μm increases as the width decreases. The higher threshold can be attributed to the combination of quantum confinement and disorder. We also find that the lower Ge ratio used heremore » leads to a narrower operational gate bias range. The higher threshold combined with the limited gate bias range constrains the device design of lithographic quantum dots. We incorporate such considerations in our device design and demonstrate a quantum dot that can be tuned from a single dot to a double dot. Furthermore, the device uses only a single metal-gate layer, greatly simplifying device design and fabrication.« less
  5. Infrared (IR) light sources with high modulation rates are critical components for on-chip optical communications. Lead-based colloidal quantum dots are promising nonepitaxial materials for use in IR light-emitting diodes, but their slow photoluminescence lifetime is a serious limitation. Here we demonstrate coupling of PbS quantum dots to colloidal plasmonic nanoantennas based on film-coupled metal nanocubes, resulting in a dramatic 1300-fold reduction in the emission lifetime from the microsecond to the nanosecond regime. This lifetime reduction is primarily due to a 1100-fold increase in the radiative decay rate owing to the high quantum yield (65%) of the antenna. The short emissionmore » lifetime is accompanied by high antenna quantum efficiency and directionality. Lastly, this nonepitaxial platform points toward GHz frequency, electrically modulated, telecommunication wavelength light-emitting diodes and single-photon sources.« less
  6. In this study, luminescent solar concentrators (LSCs) can be utilized as both large-area collectors of solar radiation supplementing traditional photovoltaic cells as well as semitransparent “solar windows” that provide a desired degree of shading and simultaneously serve as power-generation units. An important characteristic of an LSC is a concentration factor (C) that can be thought of as a coefficient of effective enlargement (or contraction) of the area of a solar cell when it is coupled to the LSC. Here we use analytical and numerical Monte Carlo modeling in addition to experimental studies of quantum-dot-based LSCs to analyze the factors thatmore » influence optical concentration in practical devices. Our theoretical model indicates that the maximum value of C achievable with a given fluorophore is directly linked to the LSC quality factor (QLSC) defined as the ratio of absorption coefficients at the wavelengths of incident and reemitted light. In fact, we demonstrate that the ultimate concentration limit (C0) realized in large-area devices scales linearly with the LSC quality factor and in the case of perfect emitters and devices without back reflectors is approximately equal to QLSC. To test the predictions of this model, we conduct experimental studies of LSCs based on visible-light emitting II–VI core/shell quantum dots with two distinct LSC quality factors. We also investigate devices based on near-infrared emitting CuInSexS2–x quantum dots for which the large emission bandwidth allows us to assess the impact of varied QLSC on the concentration factor by simply varying the detection wavelength. In all cases, we find an excellent agreement between the model and the experimental observations, suggesting that the developed formalism can be utilized for express evaluation of prospective LSC performance based on the optical spectra of LSC fluorophores, which should facilitate future efforts on the development of high-performance devices based on quantum dots as well as other types of emitters.« less
  7. We study the combination of zero-dimensional (0D) colloidal CdSe/ZnS quantum dots with tin disulfide (SnS2), a two-dimensional (2D)-layered metal dichalcogenide, results in 0D–2D hybrids with enhanced light absorption properties. These 0D–2D hybrids, when exposed to light, exhibit intrahybrid nonradiative energy transfer from photoexcited CdSe/ZnS quantum dots to SnS2. Using single nanocrystal spectroscopy, we find that the rate for energy transfer in 0D–2D hybrids increases with added number of SnS2 layers, a positive manifestation toward the potential functionality of such 2D-based hybrids in applications such as photovoltaics and photon sensing.
  8. This final report describes the activities undertaken under grant "Optical Two-Dimensional Spectroscopy of Disordered Semiconductor Quantum Wells and Quantum Dots". The goal of this program was to implement optical 2-dimensional Fourier transform spectroscopy and apply it to electronic excitations, including excitons, in semiconductors. Specifically of interest are quantum wells that exhibit disorder due to well width fluctuations and quantum dots. In both cases, 2-D spectroscopy will provide information regarding coupling among excitonic localization sites.
  9. Here, we consider a droplet of electrons confined within an external harmonic potential well of elliptical or ellipsoidal shape, a geometry commonly encountered in work with semiconductor quantum dots and other nanoscale or mesoscale structures. For droplet sizes exceeding the effective Bohr radius, the dominant contribution to average system parameters in the Thomas– Fermi approximation comes from the potential energy terms, which allows us to derive expressions describing the electron droplet’s shape and dimensions, its density, total and capacitive energy, and chemical potential. Our analytical results are in very good agreement with experimental data and numerical calculations, and make itmore » possible to follow the dependence of the properties of the system on its parameters (the total number of electrons, the axial ratios and curvatures of the confinement potential, and the dielectric constant of the material). One interesting feature is that the eccentricity of the electron droplet is not the same as that of its confining potential well.« less
  10. In carrier multiplication, the absorption of a single photon results in two or more electron–hole pairs. Quantum dots are promising materials for implementing carrier multiplication principles in real-life technologies. So far, however, most of research in this area has focused on optical studies of solution samples with yet to be proven relevance to practical devices. We report ultra-fast electro-optical studies of device-grade films of electronically coupled quantum dots that allow us to observe multiplication directly in the photocurrent. Our studies help rationalize previous results from both optical spectroscopy and steady-state photocurrent measurements and also provide new insights into effects ofmore » electric field and ligand treatments on multiexciton yields. Importantly, we demonstrate that using appropriate chemical treatments of the films, extra charges produced by carrier multiplication can be extracted from the quantum dots before they are lost to Auger recombination and hence can contribute to photocurrent of practical devices.« less
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