Showing papers on "Quantum dot published in 2006"

Electronic Confinement and Coherence in Patterned Epitaxial Graphene

Abstract: Ultrathin epitaxial graphite was grown on single-crystal silicon carbide by vacuum graphitization. The material can be patterned using standard nanolithography methods. The transport properties, which are closely related to those of carbon nanotubes, are dominated by the single epitaxial graphene layer at the silicon carbide interface and reveal the Dirac nature of the charge carriers. Patterned structures show quantum confinement of electrons and phase coherence lengths beyond 1 micrometer at 4 kelvin, with mobilities exceeding 2.5 square meters per volt-second. All-graphene electronically coherent devices and device architectures are envisaged.

Quantum-sized carbon dots for bright and colorful photoluminescence.

Abstract: We report that nanoscale carbon particles (carbon dots) upon simple surface passivation are strongly photoluminescent in both solution and the solid state. The luminescence emission of the carbon dots is stable against photobleaching, and there is no blinking effect. These strongly emissive carbon dots may find applications similar to or beyond those of their widely pursued silicon counterparts.

Quantum dot solar cells. harvesting light energy with CdSe nanocrystals molecularly linked to mesoscopic TiO2 films.

Abstract: By using bifunctional surface modifiers (SH−R−COOH), CdSe quantum dots (QDs) have been assembled onto mesoscopic TiO2 films. Upon visible light excitation, CdSe QDs inject electrons into TiO2 nanocrystallites. Femtosecond transient absorption as well as emission quenching experiments confirm the injection from the excited state of CdSe QDs into TiO2 nanoparticles. Electron transfer from the thermally relaxed s-state occurs over a wide range of rate constant values between 7.3 × 109 and 1.95 × 1011 s-1. The injected charge carriers in a CdSe-modified TiO2 film can be collected at a conducting electrode to generate a photocurrent. The TiO2−CdSe composite, when employed as a photoanode in a photoelectrochemical cell, exhibits a photon-to-charge carrier generation efficiency of 12%. Significant loss of electrons occurs due to scattering as well as charge recombination at TiO2/CdSe interfaces and internal TiO2 grain boundaries.

Ultrasensitive solution-cast quantum dot photodetectors

Abstract: Solution-processed electronic and optoelectronic devices offer low cost, large device area, physical flexibility and convenient materials integration compared to conventional epitaxially grown, lattice-matched, crystalline semiconductor devices. Although the electronic or optoelectronic performance of these solution-processed devices is typically inferior to that of those fabricated by conventional routes, this can be tolerated for some applications in view of the other benefits. Here we report the fabrication of solution-processed infrared photodetectors that are superior in their normalized detectivity (D*, the figure of merit for detector sensitivity) to the best epitaxially grown devices operating at room temperature. We produced the devices in a single solution-processing step, overcoating a prefabricated planar electrode array with an unpatterned layer of PbS colloidal quantum dot nanocrystals. The devices showed large photoconductive gains with responsivities greater than 10(3) A W(-1). The best devices exhibited a normalized detectivity D* of 1.8 x 10(13) jones (1 jones = 1 cm Hz(1/2) W(-1)) at 1.3 microm at room temperature: today's highest performance infrared photodetectors are photovoltaic devices made from epitaxially grown InGaAs that exhibit peak D* in the 10(12) jones range at room temperature, whereas the previous record for D* from a photoconductive detector lies at 10(11) jones. The tailored selection of absorption onset energy through the quantum size effect, combined with deliberate engineering of the sequence of nanoparticle fusing and surface trap functionalization, underlie the superior performance achieved in this readily fabricated family of devices.

Excitons in nanoscale systems

Abstract: Nanoscale systems are forecast to be a means of integrating desirable attributes of molecular and bulk regimes into easily processed materials. Notable examples include plastic light-emitting devices and organic solar cells, the operation of which hinge on the formation of electronic excited states, excitons, in complex nanostructured materials. The spectroscopy of nanoscale materials reveals details of their collective excited states, characterized by atoms or molecules working together to capture and redistribute excitation. What is special about excitons in nanometre-sized materials? Here we present a cross-disciplinary review of the essential characteristics of excitons in nanoscience. Topics covered include confinement effects, localization versus delocalization, exciton binding energy, exchange interactions and exciton fine structure, exciton-vibration coupling and dynamics of excitons. Important examples are presented in a commentary that overviews the present understanding of excitons in quantum dots, conjugated polymers, carbon nanotubes and photosynthetic light-harvesting antenna complexes.

Cavity quantum electrodynamics

Abstract: This paper reviews the work on cavity quantum electrodynamics of free atoms. In recent years, cavity experiments have also been conducted on a variety of solid-state systems resulting in many interesting applications, of which microlasers, photon bandgap structures and quantum dot structures in cavities are outstanding examples. Although these phenomena and systems are very interesting, discussion is limited here to free atoms and mostly single atoms because these systems exhibit clean quantum phenomena and are not disturbed by a variety of other effects. At the centre of our review is the work on the one-atom maser, but we also give a survey of the entire field, using free atoms in order to show the large variety of problems dealt with. The cavity interaction can be separated into two main regimes: the weak coupling in cavity or cavity-like structures with low quality factors Q and the strong coupling when high-Q cavities are involved. The weak coupling leads to modification of spontaneous transitions and level shifts, whereas the strong coupling enables one to observe a periodic exchange of photons between atoms and the radiation field. In this case, atoms and photons are entangled, this being the basis for a variety of phenomena observed, some of them leading to interesting applications in quantum information processing. The cavity experiments with free atoms reached a new domain with the advent of experiments in the visible spectral region. A review on recent achievements in this area is also given.

Observation of strong coupling between one atom and a monolithic microresonator

Abstract: Over the past decade, strong interactions of light and matter at the single-photon level have enabled a wide set of scientific advances in quantum optics and quantum information science. This work has been performed principally within the setting of cavity quantum electrodynamics with diverse physical systems, including single atoms in Fabry–Perot resonators, quantum dots coupled to micropillars and photonic bandgap cavities and Cooper pairs interacting with superconducting resonators. Experiments with single, localized atoms have been at the forefront of these advances with the use of optical resonators in high-finesse Fabry–Perot configurations. As a result of the extreme technical challenges involved in further improving the multilayer dielectric mirror coatings of these resonators and in scaling to large numbers of devices, there has been increased interest in the development of alternative microcavity systems. Here we show strong coupling between individual caesium atoms and the fields of a high-quality toroidal microresonator. From observations of transit events for single atoms falling through the resonator's evanescent field, we determine the coherent coupling rate for interactions near the surface of the resonator. We develop a theoretical model to quantify our observations, demonstrating that strong coupling is achieved, with the rate of coherent coupling exceeding the dissipative rates of the atom and the cavity. Our work opens the way for investigations of optical processes with single atoms and photons in lithographically fabricated microresonators. Applications include the implementation of quantum networks, scalable quantum logic with photons, and quantum information processing on atom chips.

Vacuum Rabi splitting in semiconductors

Abstract: The recent development of techniques to produce optical semiconductor cavities of very high quality has prepared the stage for observing cavity quantum-electrodynamic effects in solid-state materials. Among the most promising systems for these studies are semiconductor quantum dots inside photonic crystal, micropillar or microdisk resonators. We review the progress so far in obtaining true quantum-optical strong-coupling effects in semiconductors. We discuss the recent results on vacuum Rabi splitting with a single quantum dot, emphasizing the differences from quantum-well systems. Finally, we propose nonlinear tests for the true quantum limit and speculate about applications in quantum information devices.

Self-illuminating quantum dot conjugates for in vivo imaging.

Abstract: Fluorescent semiconductor quantum dots hold great potential for molecular imaging in vivo. However, the utility of existing quantum dots for in vivo imaging is limited because they require excitation from external illumination sources to fluoresce, which results in a strong autofluorescence background and a paucity of excitation light at nonsuperficial locations. Here we present quantum dot conjugates that luminesce by bioluminescence resonance energy transfer in the absence of external excitation. The conjugates are prepared by coupling carboxylate-presenting quantum dots to a mutant of the bioluminescent protein Renilla reniformis luciferase. We show that the conjugates emit long-wavelength (from red to near-infrared) bioluminescent light in cells and in animals, even in deep tissues, and are suitable for multiplexed in vivo imaging. Compared with existing quantum dots, self-illuminating quantum dot conjugates have greatly enhanced sensitivity in small animal imaging, with an in vivo signal-to-background ratio of > 10(3) for 5 pmol of conjugate.

Self-tuned quantum dot gain in photonic crystal lasers.

Abstract: We demonstrate that very few (2\char21{}4) quantum dots as a gain medium are sufficient to realize a photonic-crystal laser based on a high-quality nanocavity. Photon correlation measurements show a transition from a thermal to a coherent light state proving that lasing action occurs at ultralow thresholds. Observation of lasing is unexpected since the cavity mode is in general not resonant with the discrete quantum dot states and emission at those frequencies is suppressed. In this situation, the quasicontinuous quantum dot states become crucial since they provide an energy-transfer channel into the lasing mode, effectively leading to a self-tuned resonance for the gain medium.

Förster resonance energy transfer investigations using quantum-dot fluorophores.

Abstract: Forster resonance energy transfer (FRET), which involves the nonradiative transfer of excitation energy from an excited donor fluorophore to a proximal ground-state acceptor fluorophore, is a well-characterized photophysical tool. It is very sensitive to nanometer-scale changes in donor-acceptor separation distance and their relative dipole orientations. It has found a wide range of applications in analytical chemistry, protein conformation studies, and biological assays. Luminescent semiconductor nanocrystals (quantum dots, QDs) are inorganic fluorophores with unique optical and spectroscopic properties that could enhance FRET as an analytical tool, due to broad excitation spectra and tunable narrow and symmetric photoemission. Recently, there have been several FRET investigations using luminescent QDs that focused on addressing basic fundamental questions, as well as developing targeted applications with potential use in biology, including sensor design and protein conformation studies. Herein, we provide a critical review of those developments. We discuss some of the basic aspects of FRET applied to QDs as both donors and acceptors, and highlight some of the advantages offered (and limitations encountered) by QDs as energy donors and acceptors compared to conventional dyes. We also review the recent developments made in using QD bioreceptor conjugates to design FRET-based assays.

The use of luminescent quantum dots for optical sensing

Abstract: Semiconductor nanocrystals, known as “quantum dots” (QDs), have demonstrated several remarkable, attractive optoelectronic characteristics especially suited to analytical applications in the (bio)chemical field. We review progress in exploiting the attractive luminescent properties of QDs in designing novel probes for chemical and biochemical optical sensing.

Efficient CdSe/CdS quantum dot light-emitting diodes using a thermally polymerized hole transport layer.

Abstract: We report multilayer nanocrystal quantum dot light-emitting diodes (QD-LEDs) fabricated by spin-coating a monolayer of colloidal CdSe/CdS nanocrystals on top of thermally polymerized solvent-resistant hole-transport layers (HTLs). We obtain high-quality QD layers of controlled thickness (down to submonolayer) simply by spin-coating QD solutions directly onto the HTL. The resulting QD-LEDs exhibit narrow ( approximately 30 nm, fwhm) electroluminescence from the QDs with virtually no emission from the organic matrix at any voltage. Using multiple spin-on HTLs improves the external quantum efficiency of the QD-LEDs to approximately 0.8% at a brightness of 100 cd/m(2) (with a maximum brightness over 1,000 cd/m(2)). We conclude that QD-LEDs could be made more efficient by further optimization of the organic semiconductors.

Quantum-Dot Spin-State Preparation with Near-Unity Fidelity

Abstract: We have demonstrated laser cooling of a single electron spin trapped in a semiconductor quantum dot. Optical coupling of electronic spin states was achieved using resonant excitation of the charged quantum dot (trion) transitions along with the heavy-light hole mixing, which leads to weak yet finite rates for spin-flip Raman scattering. With this mechanism, the electron spin can be cooled from 4.2 to 0.020 kelvin, as confirmed by the strength of the induced Pauli blockade of the trion absorption. Within the framework of quantum information processing, this corresponds to a spin-state preparation with a fidelity exceeding 99.8%.

Carbon nanotube superconducting quantum interference device.

Abstract: A superconducting quantum interference device (SQUID) with single-walled carbon nanotube (CNT) Josephson junctions is presented. Quantum confinement in each junction induces a discrete quantum dot (QD) energy level structure, which can be controlled with two lateral electrostatic gates. In addition, a backgate electrode can vary the transparency of the QD barriers, thus permitting change in the hybridization of the QD states with the superconducting contacts. The gates are also used to directly tune the quantum phase interference of the Cooper pairs circulating in the SQUID ring. Optimal modulation of the switching current with magnetic flux is achieved when both QD junctions are in the ‘on’ or ‘off’ state. In particular, the SQUID design establishes that these CNT Josephson junctions can be used as gate-controlled π-junctions; that is, the sign of the current–phase relation across the CNT junctions can be tuned with a gate voltage. The CNT-SQUIDs are sensitive local magnetometers, which are very promising for the study of magnetization reversal of an individual magnetic particle or molecule placed on one of the two CNT Josephson junctions.

Semiconductor-Metal Nanoparticle Molecules: Hybrid Excitons and the Nonlinear Fano Effect

Abstract: Modern nanotechnology opens the possibility of combining nanocrystals of various materials with very different characteristics in one superstructure. Here we study theoretically the optical properties of hybrid molecules composed of semiconductor and metal nanoparticles. Excitons and plasmons in such a hybrid molecule become strongly coupled and demonstrate novel properties. At low incident light intensity, the exciton peak in the absorption spectrum is broadened and shifted due to incoherent and coherent interactions between metal and semiconductor nanoparticles. At high light intensity, the absorption spectrum demonstrates a surprising, strongly asymmetric shape. This shape originates from the coherent internanoparticle Coulomb interaction and can be viewed as a nonlinear Fano effect which is quite different from the usual linear Fano resonance.

Quantum dots with a paramagnetic coating as a bimodal molecular imaging probe

Abstract: MRI detectable and targeted quantum dots were developed. To that aim, quantum dots were coated with paramagnetic and pegylated lipids, which resulted in a relaxivity, r(1), of nearly 2000 mM(-1)s(-1) per quantum dot. The quantum dots were functionalized by covalently linking alphavbeta3-specific RGD peptides, and the specificity was assessed and confirmed on cultured endothelial cells. The bimodal character, the high relaxivity, and the specificity of this nanoparticulate probe make it an excellent contrast agent for molecular imaging purposes.

Doped elongated semiconductors, growing such semiconductors, devices including such semiconductors, and fabricating such devices

Abstract: A bulk-doped semiconductor that is at least one of the following: a single crystal, an elongated and bulk-doped semiconductor that, at any point along its longitudinal axis, has a largest cross-sectional dimension less than 500 nanometers, and a free-standing and bulk-doped semiconductor with at least one portion having a smallest width of less than 500 nanometers. Such a semiconductor may comprise an interior core comprising a first semiconductor; and an exterior shell comprising a different material than the first semiconductor. Such a semiconductor may be elongated and may have, at any point along a longitudinal section of such a semiconductor, a ratio of the length of the section to a longest width is greater than 4:1, or greater than 10:1, or greater than 100:1, or even greater than 1000:1. At least one portion of such a semiconductor may a smallest width of less than 200 nanometers, or less than 150 nanometers, or less than 100 nanometers, or less than 80 nanometers, or less than 70 nanometers, or less than 60 nanometers, or less than 40 nanometers, or less than 20 nanometers, or less than 10 nanometers, or even less than 5 nanometers. Such a semiconductor may be a single crystal and may be free-standing. Such a semiconductor may be either lightly n-doped, heavily n-doped, lightly p-doped or heavily p-doped. Such a semiconductor may be doped during growth. Such a semiconductor may be part of a device, which may include any of a variety of devices and combinations thereof, and a variety of assembling techniques may be used to fabricate devices from such a semiconductor. Two or more of such a semiconductors, including an array of such semiconductors, may be combined to form devices, for example, to form a crossed p-n junction of a device. Such devices at certain sizes may exhibit quantum confinement and other quantum phenomena, and the wavelength of light emitted from one or more of such semiconductors may be controlled by selecting a width of such semiconductors. Such semiconductors and device made therefrom may be used for a variety of applications.

A systematic examination of surface coatings on the optical and chemical properties of semiconductor quantum dots

Abstract: A number of procedures are currently available to encapsulate and solubilize hydrophobic semiconductor Quantum Dots (QDs) for biological applications Most of these procedures are based on the use of small-molecule coordinating ligands, amphiphilic polymers, or amphiphilic lipids However, it is still not clear how these different surface coating molecules affect the optical, colloidal, and chemical properties of the solubilized QDs Here we report a systematic study to examine the effects of surface coating chemistry on the hydrodynamic size, fluorescence quantum yield, photostability, chemical stability, and biocompatibility of water-soluble QDs The results indicate that quantum dots with the smallest hydrodynamic sizes are best prepared by direct ligand exchange with hydrophilic molecules, but the resulting particles are less stable than those encapsulated in amphiphilic polymers For stability against chemical oxidation, QDs should be protected with a hydrophobic bilayer For high stability under acidic conditions, the best QDs are prepared by using hyperbranched polyethylenimine For stability in high salt buffers, it is preferable to have uncharged, sterically-stabilized QDs, like those coated with polyethylene glycol (PEG) These insights are expected to benefit the development of quantum dots and related nanoparticle probes for molecular and cellular imaging applications

Nanocrystalline TiO2 solar cells sensitized with InAs quantum dots.

Abstract: We report nanocrystalline TiO2 solar cells sensitized with InAs quantum dots. InAs quantum dots of different sizes were synthesized and incorporated in solar cell devices. Efficient charge transfer from InAs quantum dots to TiO2 particles was achieved without deliberate modification of the quantum dot capping layer. A power conversion efficiency of about 1.7% under 5 mW/cm2 was achieved; this is relatively high for a nanocrystalline metal oxide solar cell sensitized with presynthesized quantum dots, but this efficiency could only be achieved at low light intensity. At one sun, the efficiency decreased to 0.3%. The devices are stable for at least weeks under room light in air.

Counting statistics of single electron transport in a quantum dot.

Abstract: We have measured the full counting statistics of current fluctuations in a semiconductor quantum dot (QD) by real-time detection of single electron tunneling with a quantum point contact. This method gives direct access to the distribution function of current fluctuations. Suppression of the second moment (related to the shot noise) and the third moment (related to the asymmetry of the distribution) in a tunable semiconductor QD is demonstrated experimentally. With this method we demonstrate the ability to measure very low current and noise levels.

Size series of small indium arsenide-zinc selenide core-shell nanocrystals and their application to in vivo imaging.

Abstract: We have developed a size series of unusually small, water-soluble (InAs)ZnSe (core)shell quantum dots (QDs) that emit in the near-infrared and exhibit new behavior in vivo, including multiple sequential lymph node mapping and extravasation from the vasculature. The biological utility of these fluorescent probes resulted from our intentional choice to match the semiconductor material and water-soluble ligand with a desired final hydrodynamic diameter and emission wavelength.

A gallium nitride single-photon source operating at 200 K.

Abstract: Fundamentally secure quantum cryptography has still not seen widespread application owing to the difficulty of generating single photons on demand. Semiconductor quantum-dot structures have recently shown great promise as practical single-photon sources, and devices with integrated optical cavities and electrical-carrier injection have already been demonstrated. However, a significant obstacle for the application of commonly used III–V quantum dots to quantum-information-processing schemes is the requirement of liquid-helium cryogenic temperatures. Epitaxially grown gallium nitride quantum dots embedded in aluminium nitride have the potential for operation at much higher temperatures. Here, we report triggered single-photon emission from gallium nitride quantum dots at temperatures up to 200 K, a temperature easily reachable with thermo-electric cooling. Gallium nitride quantum dots also open a new wavelength region in the blue and near-ultraviolet portions of the spectrum for single-photon sources.

Optical Signatures of Coupled Quantum Dots

Abstract: An asymmetric pair of coupled InAs quantum dots is tuned into resonance by applying an electric field so that a single hole forms a coherent molecular wave function The optical spectrum shows a rich pattern of level anticrossings and crossings that can be understood as a superposition of charge and spin configurations of the two dots Coulomb interactions shift the molecular resonance of the optically excited state (charged exciton) with respect to the ground state (single charge), enabling light-induced coupling of the quantum dots This result demonstrates the possibility of optically coupling quantum dots for application in quantum information processing

Silicon nanocrystals with ensemble quantum yields exceeding 60

Abstract: Silicon nanocrystals with diameters of less than 5nm show efficient photoluminescence at room temperature. For ensembles of silicon quantum dots, previous reports of photoluminescence quantum yields have usually been in the few percent range, and generally less than 30%. Here we report the plasma synthesis of silicon quantum dots and their subsequent wet-chemical surface passivation with organic ligands under strict exclusion of oxygen. Photoluminescence quantum yields exceeding 60% have been achieved at peak wavelengths of about 789nm.

Size-dependent extinction coefficients of PbS quantum dots.

Abstract: We report here on a detailed study on PbS colloidal quantum dots. A characterization via X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) allowed us to reliably determine the diameter and the shape of the nanocrystals. These data, together with second-derivative analysis of the absorption spectra, allowed us to determine the size dependence of seven transitions in the absorption spectrum; some of these transitions were identified on the basis of their normalized confinement energy. The size dependence of the first excitonic transition was best modeled by a four-band envelope approach which considers the anisotropy of the band edges (Andreev, A. D.; Lipovskii, A. A. Phys. Rev. B: Condens. Matter Mater. Phys. 1999, 59, 15402−15404). The extinction coefficients were calculated using concentrations obtained from inductively coupled plasma atomic emission spectrometry (ICP-AES), and their size dependence was found to follow a power law with exponent equal to ∼2.5. In contra...

Electron transport through single Mn12 molecular magnets.

Abstract: We report transport measurements through a single-molecule magnet, the Mn12 derivative [Mn12O12(O2C-C6H4-SAc)16(H2O)4], in a single-molecule transistor geometry. Thiol groups connect the molecule to gold electrodes that are fabricated by electromigration. Striking observations are regions of complete current suppression and excitations of negative differential conductance on the energy scale of the anisotropy barrier of the molecule. Transport calculations, taking into account the high-spin ground state and magnetic excitations of the molecule, reveal a blocking mechanism of the current involving nondegenerate spin multiplets.

From colour fingerprinting to the control of photoluminescence in elastic photonic crystals

Abstract: In photonic crystals (PCs), strong scattering and destructive wave interference lead to a modification of the photon density of states in particular energy regions and along certain crystallographic directions1,2. The consequences of this range from suppression and enhancement of luminescence3,4,5,6,7 to narrow-band bright reflections useful for colour sensors8,9, displays10 and tuneable filters11,12,13,14. Here we demonstrate large-area films of porous elastomeric photonic crystals (EPCs) that are compressively–decompressively cycled to reversibly shift the position of the photonic band structure over a large wavelength range. Owing to their low compressive threshold, such porous EPCs can be used for imaging that is pressure and time sensitive, for example, to obtain colour fingerprints with high accuracy. Furthermore, by incorporating luminescent PbS quantum dots in the EPCs, the photonic stop-gap can be tuned through the near-infrared (NIR) quantum dot photoluminescence (PL) peak. Thereby we demonstrate a tuneable modification of photonic characteristics, including the suppression and enhancement in emission and dynamic modification of luminescence lifetimes.