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Showing papers on "Quantum dot published in 2004"


Journal ArticleDOI
TL;DR: This work found that CdSe-core QDs were indeed acutely toxic under certain conditions and modulated by processing parameters during synthesis, exposure to ultraviolet light, and surface coatings, and suggests that cytotoxicity correlates with the liberation of free Cd2+ ions due to deterioration of the Cd Se lattice.
Abstract: With their bright, photostable fluorescence, semiconductor quantum dots (QDs) show promise as alternatives to organic dyes for biological labeling. Questions about their potential cytotoxicity, however, remain unanswered. While cytotoxicity of bulk cadmium selenide (CdSe) is well documented, a number of groups have suggested that CdSe QDs are cytocompatible, at least with some immortalized cell lines. Using primary hepatocytes as a liver model, we found that CdSe-core QDs were indeed acutely toxic under certain conditions. Specifically, we found that the cytotoxicity of QDs was modulated by processing parameters during synthesis, exposure to ultraviolet light, and surface coatings. Our data further suggest that cytotoxicity correlates with the liberation of free Cd2+ ions due to deterioration of the CdSe lattice. When appropriately coated, CdSe-core QDs can be rendered nontoxic and used to track cell migration and reorganization in vitro. Our results provide information for design criteria for the use of ...

3,236 citations


Journal ArticleDOI
11 Nov 2004-Nature
TL;DR: The experimental realization of a strongly coupled system in the solid state is reported: a single quantum dot embedded in the spacer of a nanocavity, showing vacuum-field Rabi splitting exceeding the decoherence linewidths of both the nanoc Cavity and the quantum dot.
Abstract: Cavity quantum electrodynamics (QED) systems allow the study of a variety of fundamental quantum-optics phenomena, such as entanglement, quantum decoherence and the quantum–classical boundary. Such systems also provide test beds for quantum information science. Nearly all strongly coupled cavity QED experiments have used a single atom in a high-quality-factor (high-Q) cavity. Here we report the experimental realization of a strongly coupled system in the solid state: a single quantum dot embedded in the spacer of a nanocavity, showing vacuum-field Rabi splitting exceeding the decoherence linewidths of both the nanocavity and the quantum dot. This requires a small-volume cavity and an atomic-like two-level system. The photonic crystal slab nanocavity—which traps photons when a defect is introduced inside the two-dimensional photonic bandgap by leaving out one or more holes—has both high Q and small modal volume V, as required for strong light–matter interactions. The quantum dot has two discrete energy levels with a transition dipole moment much larger than that of an atom, and it is fixed in the nanocavity during growth.

2,135 citations


Journal ArticleDOI
TL;DR: It is demonstrated that the fluorescence emission of type II quantum dots can be tuned into the near infrared while preserving absorption cross-section, and that a polydentate phosphine coating renders them soluble, disperse and stable in serum.
Abstract: The use of near-infrared or infrared photons is a promising approach for biomedical imaging in living tissue. This technology often requires exogenous contrast agents with combinations of hydrodynamic diameter, absorption, quantum yield and stability that are not possible with conventional organic fluorophores. Here we show that the fluorescence emission of type II quantum dots can be tuned into the near infrared while preserving absorption cross-section, and that a polydentate phosphine coating renders them soluble, disperse and stable in serum. We then demonstrate that these quantum dots allow a major cancer surgery, sentinel lymph node mapping, to be performed in large animals under complete image guidance. Injection of only 400 pmol of near-infrared quantum dots permits sentinel lymph nodes 1 cm deep to be imaged easily in real time using excitation fluence rates of only 5 mW/cm(2). Taken together, the chemical, optical and in vivo data presented in this study demonstrate the potential of near-infrared quantum dots for biomedical imaging.

2,053 citations


Journal ArticleDOI
11 Nov 2004-Nature
TL;DR: The observation of strong coupling of a single two-level solid-state system with a photon, as realized by a single quantum dot in a semiconductor microcavity, may provide a basis for future applications in quantum information processing or schemes for coherent control.
Abstract: Cavity quantum electrodynamics, a central research field in optics and solid-state physics, addresses properties of atom-like emitters in cavities and can be divided into a weak and a strong coupling regime. For weak coupling, the spontaneous emission can be enhanced or reduced compared with its vacuum level by tuning discrete cavity modes in and out of resonance with the emitter. However, the most striking change of emission properties occurs when the conditions for strong coupling are fulfilled. In this case there is a change from the usual irreversible spontaneous emission to a reversible exchange of energy between the emitter and the cavity mode. This coherent coupling may provide a basis for future applications in quantum information processing or schemes for coherent control. Until now, strong coupling of individual two-level systems has been observed only for atoms in large cavities. Here we report the observation of strong coupling of a single two-level solid-state system with a photon, as realized by a single quantum dot in a semiconductor microcavity. The strong coupling is manifest in photoluminescence data that display anti-crossings between the quantum dot exciton and cavity-mode dispersion relations, characterized by a vacuum Rabi splitting of about 140 microeV.

1,809 citations


Journal ArticleDOI
TL;DR: Long-term experiments demonstrated that these quantum dots remain fluorescent after at least four months in vivo, using only quantum dots for detection.

1,153 citations


Journal ArticleDOI
08 Jul 2004-Nature
TL;DR: A general approach for fabricating inorganically coupled colloidal quantum dots and rods, connected epitaxially at branched and linear junctions within single nanocrystal heterostructures, which allows investigation of potential applications ranging from quantum information processing to artificial photosynthesis.
Abstract: The development of colloidal quantum dots has led to practical applications of quantum confinement, such as in solution-processed solar cells1, lasers2 and as biological labels3. Further scientific and technological advances should be achievable if these colloidal quantum systems could be electronically coupled in a general way. For example, this was the case when it became possible to couple solid-state embedded quantum dots into quantum dot molecules4,5. Similarly, the preparation of nanowires with linear alternating compositions—another form of coupled quantum dots—has led to the rapid development of single-nanowire light-emitting diodes6 and single-electron transistors7. Current strategies to connect colloidal quantum dots use organic coupling agents8,9, which suffer from limited control over coupling parameters and over the geometry and complexity of assemblies. Here we demonstrate a general approach for fabricating inorganically coupled colloidal quantum dots and rods, connected epitaxially at branched and linear junctions within single nanocrystals. We achieve control over branching and composition throughout the growth of nanocrystal heterostructures to independently tune the properties of each component and the nature of their interactions. Distinct dots and rods are coupled through potential barriers of tuneable height and width, and arranged in three-dimensional space at well-defined angles and distances. Such control allows investigation of potential applications ranging from quantum information processing to artificial photosynthesis.

1,149 citations


Journal ArticleDOI
05 Aug 2004-Nature
TL;DR: In this paper, the spectral distribution and time-dependent decay of light emitted from excitons confined in the quantum dots are controlled by the host photonic crystal, and both inhibited and enhanced decay rates are observed depending on the optical emission frequency.
Abstract: Control of spontaneously emitted light lies at the heart of quantum optics. It is essential for diverse applications ranging from miniature lasers and light-emitting diodes, to single-photon sources for quantum information, and to solar energy harvesting. To explore such new quantum optics applications, a suitably tailored dielectric environment is required in which the vacuum fluctuations that control spontaneous emission can be manipulated. Photonic crystals provide such an environment: they strongly modify the vacuum fluctuations, causing the decay of emitted light to be accelerated or slowed down, to reveal unusual statistics, or to be completely inhibited in the ideal case of a photonic bandgap. Here we study spontaneous emission from semiconductor quantum dots embedded in inverse opal photonic crystals. We show that the spectral distribution and time-dependent decay of light emitted from excitons confined in the quantum dots are controlled by the host photonic crystal. Modified emission is observed over large frequency bandwidths of 10%, orders of magnitude larger than reported for resonant optical microcavities. Both inhibited and enhanced decay rates are observed depending on the optical emission frequency, and they are controlled by the crystals’ lattice parameter. Our experimental results provide a basis for all-solid-state dynamic control of optical quantum systems.

1,046 citations


Journal Article
TL;DR: This work shows that the spectral distribution and time-dependent decay of light emitted from excitons confined in the quantum dots are controlled by the host photonic crystal, providing a basis for all-solid-state dynamic control of optical quantum systems.
Abstract: Control of spontaneously emitted light lies at the heart of quantum optics. It is essential for diverse applications ranging from miniature lasers and light-emitting diodes, to single-photon sources for quantum information, and to solar energy harvesting. To explore such new quantum optics applications, a suitably tailored dielectric environment is required in which the vacuum fluctuations that control spontaneous emission can be manipulated. Photonic crystals provide such an environment: they strongly modify the vacuum fluctuations, causing the decay of emitted light to be accelerated or slowed down, to reveal unusual statistics, or to be completely inhibited in the ideal case of a photonic bandgap. Here we study spontaneous emission from semiconductor quantum dots embedded in inverse opal photonic crystals. We show that the spectral distribution and time-dependent decay of light emitted from excitons confined in the quantum dots are controlled by the host photonic crystal. Modified emission is observed over large frequency bandwidths of 10%, orders of magnitude larger than reported for resonant optical microcavities. Both inhibited and enhanced decay rates are observed depending on the optical emission frequency, and they are controlled by the crystals’ lattice parameter. Our experimental results provide a basis for all-solid-state dynamic control of optical quantum systems.

1,019 citations


Journal ArticleDOI
TL;DR: Highly fluorescent, water-soluble, few-atom Au quantum dots have been created that behave as multielectron artificial atoms with discrete, size-tunable electronic transitions throughout the visible and near IR.
Abstract: Highly fluorescent, water-soluble, few-atom Au quantum dots have been created that behave as multielectron artificial atoms with discrete, size-tunable electronic transitions throughout the visible and near IR. Correlation of nanodot sizes with emission energies fits the simple relation, ${E}_{\mathrm{F}\mathrm{e}\mathrm{r}\mathrm{m}\mathrm{i}}/{N}^{1/3}$, predicted by the jellium model. Providing the ``missing link'' between atomic and nanoparticle behavior in noble metals, these emissive, water-soluble Au nanoclusters open new opportunities for biological labels, energy transfer pairs, and light emitting sources in nanoscale optoelectronics.

1,001 citations


Journal ArticleDOI
TL;DR: The potential cytotoxicity of characterized QDs modified with various molecules suggested that the properties of QDs are not related to those of QD-core materials but to molecules covering the surface ofQDs.
Abstract: Nanocrystal quantum dots (QDs) have been applied to molecular biology because of their greater and longer fluorescence. Here we report the potential cytotoxicity of our characterized QDs modified with various molecules. Surface modification of QDs changed their physicochemical properties. In addition, the cytotoxicity of QDs was dependent on their surface molecules. These results suggested that the properties of QDs are not related to those of QD-core materials but to molecules covering the surface of QDs.

926 citations


Journal ArticleDOI
04 Nov 2004-Nature
TL;DR: This work demonstrates a single electron spin memory device in which the electron spin can be programmed by frequency selective optical excitation, and directly measure the intrinsic spin flip time and its dependence on magnetic field.
Abstract: The spin of a single electron subject to a static magnetic field provides a natural two-level system that is suitable for use as a quantum bit, the fundamental logical unit in a quantum computer. Semiconductor quantum dots fabricated by strain driven self-assembly are particularly attractive for the realization of spin quantum bits, as they can be controllably positioned, electronically coupled and embedded into active devices. It has been predicted that the atomic-like electronic structure of such quantum dots suppresses coupling of the spin to the solid-state quantum dot environment, thus protecting the 'spin' quantum information against decoherence. Here we demonstrate a single electron spin memory device in which the electron spin can be programmed by frequency selective optical excitation. We use the device to prepare single electron spins in semiconductor quantum dots with a well defined orientation, and directly measure the intrinsic spin flip time and its dependence on magnetic field. A very long spin lifetime is obtained, with a lower limit of about 20 milliseconds at a magnetic field of 4 tesla and at 1 kelvin.

Journal ArticleDOI
TL;DR: In this paper, the authors discuss the calculation of strain fields, which play an important role in the formation of such nanostructures and also influence their structural and optoelectronic properties.
Abstract: Instabilities in semiconductor heterostructure growth can be exploited for the self-organized formation of nanostructures, allowing for carrier confinement in all three spatial dimensions. Beside the description of various growth modes, the experimental characterization of structural properties, such as size and shape, chemical composition, and strain distribution is presented. The authors discuss the calculation of strain fields, which play an important role in the formation of such nanostructures and also influence their structural and optoelectronic properties. Several specific materials systems are surveyed together with important applications.

Journal ArticleDOI
TL;DR: In this paper, the synthesis of new nanocomposite nanoparticles that consist of polymer coated γ-Fe2O3 superparamagnetic cores and CdSe/ZnS quantum dots (QDs) shell was described.
Abstract: This paper describes the synthesis of new nanocomposite nanoparticles that consist of polymer coated γ-Fe2O3 superparamagnetic cores and CdSe/ZnS quantum dots (QDs) shell. A single layer of QDs was bound to the surface of thiol-modified magnetic beads through the formation of thiol−metal bonds to form luminescent/magnetic nanocomposite particles. Transmission electron microscopy (TEM) and energy disperse spectroscopy (EDS) were used to characterize the size, size distribution, and composition of the luminescent/magnetic nanoparticles. Their average diameter was 30 nm with a size variation of ±15%. The nanoparticles were modified with carboxylic groups to increase their miscibility in aqueous solution. A 3-fold decrease in the luminescence quantum yield of the luminescent/magnetic particles and a slight blue shift in their emission peaks compared to individual luminescent QDs were observed. However, the particles were bright and were easily observed using a conventional fluorescence microscope. Additionall...

Journal ArticleDOI
TL;DR: In this paper, the influence of exchange of the capping molecules with different types of thiol molecules (amino ethanethiol, (3-mercaptopropyl)trimethoxysilane, hexanetholis, 2-propenethiol and 4mercaptophenol) is investigated for both CdSe and CdTe QDs.
Abstract: Highly luminescent CdSe and CdTe quantum dots (QDs) are prepared in a hot solvent of capping molecules (TOP/TOPO/HDA for CdSe and TOP/DDA for CdTe). The influence of exchange of the capping molecules with different types of thiol molecules (amino ethanethiol, (3-mercaptopropyl)trimethoxysilane, hexanethiol, 2-propenethiol, and 4-mercaptophenol) is investigated for both CdSe and CdTe QDs. A remarkable difference is observed: capping exchange with thiol molecules results in an increased luminescence efficiency for CdTe QDs but induces quenching of the excitonic emission of CdSe QDs. The striking difference between the two types of II-VI QDs is explained by the difference in the energy of the valence band top. The lower energetic position of the valence band for CdSe results in hole trapping of the photogenerated hole on the thiol molecule, thus quenching the luminescence. For CdTe the valence band is situated at higher energies with respect to the redox level of most thiols, thus inhibiting hole trapping a...

Journal ArticleDOI
TL;DR: It is shown that the quantum dot blinking can be suppressed with the emission duty cycle approaching 100% while maintaining biocompatibility.
Abstract: Colloidal semiconductor quantum dots are attractive fluorophores for multicolor imaging because of broad absorption and narrow emission spectra, and they are brighter and far more photostable than organic dyes. However, severe intermittence in emission (also known as blinking) has been universally observed from single dots and has been considered an intrinsic limitation difficult to overcome. This is unfortunate because growing applications in spectroscopy of single biological molecules and quantum information processing using single photon sources could greatly benefit from long-lasting and nonblinking single-molecule emitters. For instance, in a recent application of single-dot imaging, the tracking of membrane receptors was interrupted frequently due to the stroboscopic nature of recording. Blinking can also reduce the brightness in ensemble imaging via signal saturation. Here we show that the quantum dot blinking can be suppressed with the emission duty cycle approaching 100% while maintaining biocomp...

Journal ArticleDOI
TL;DR: In this article, the decay rate of single colloidal CdSe quantum dots is measured by selecting only those photons collected while the single quantum dot emission intensity was near its maximum.
Abstract: We present measurements of photoluminescence decay dynamics from single colloidal CdSe quantum dots. We find that the decays fluctuate in time with decay rates that correlate with time-averaged emission intensities. Moreover, the decays measured by selecting only those photons collected while the single quantum dot emission intensity was near its maximum yields single-exponential dynamics. We find that the “maximum-intensity” decays are nearly identical across different independently synthesized samples of nearly the same size. The combination of single-exponential kinetics and decays that are reproducible across samples leads us to speculate that it is the radiative lifetime that is measured and that the quantum yield of a single dot near its maximum emission intensity is close to unity. The variations in decay rates with time and their correlation with emission intensity indicate these intensity time trajectories primarily reflect fluctuations in nonradiative relaxation pathways.

Journal ArticleDOI
TL;DR: In this article, the structural, electronic, and optical properties of hydrogen-passivated silicon nanowires along [110] and [111] directions with diameter d up to 4.2 nm from first principles were investigated.
Abstract: We investigate the structural, electronic, and optical properties of hydrogen-passivated silicon nanowires along [110] and [111] directions with diameter d up to 4.2 nm from first principles. The size and orientation dependence of the band gap is investigated and the local-density gap is corrected with the GW approximation. Quantum confinement becomes significant for d<2.2 nm, where the dielectric function exhibits strong anisotropy and new low-energy absorption peaks start to appear in the imaginary part of the dielectric function for polarization along the wire axis.

Journal ArticleDOI
TL;DR: The synthesis of the first colloidal QDs having photoluminescence (PL) in the mid-infrared is reported, allowing the first systematic correlation of QD size with PL energy for PbSe QDs emitting at wavelengths longer than 2 mum, results which are compared with a literature model.
Abstract: Efficient mid-infrared sources are of considerable general interest for gas analysis, remote sensing, and atmospheric monitoring, but existing technologies are limited. Here, we report the synthesis of the first colloidal QDs having photoluminescence (PL) in the mid-infrared. We show particle-size-tunable mid-infrared emission for large (10−17 nm), but quantum-confined, colloidal PbSe QDs, with efficient, narrow-bandwidth PL at energies as low as 0.30 eV (4.1 μm). Applying two new synthetic routes, we have achieved fine control of QD size and size distribution, allowing us to provide the first systematic correlation of QD size with PL energy for PbSe QDs emitting at wavelengths longer than 2 μm, results which are compared with a literature model. For the entire spectral range reported, we provide measured quantum yields in emission, showing a marked decrease with increasing QD size, for which we include a possible explanation. Finally, we present very promising preliminary results for overcoating PbSe wit...

Journal ArticleDOI
TL;DR: UV-Vis DRS and photoluminescence (PL) spectroscopy, combined with excitation selective Raman spectroscopic, allow us to understand the main optical and vibrational properties of a metal-organic MOF-5 framework.

Journal ArticleDOI
TL;DR: In this article, the effect of surface-capping ligands has been investigated on the photoluminescence emission intensity, leading to the conclusion that the room-temperature emission originates in donor−acceptor defects.
Abstract: Thermal decomposition of the molecular single-source precursor (PPh3)2CuIn(SEt)4 in the presence of hexanethiol in dioctylphthalate forms colloidal CuInS2 at 200 °C. The colloidal solution displays size-dependent quantum confinement behavior in the absorption and photoluminescence spectra. The average size of the nanocrystals can be increased from 2 to 4 nm by raising the reaction temperature from 200 °C to 250 °C. The nanoparticles are capped with hexanethiol ligands; these ligands can be exchanged with trioctylphosphine oxide or pyridine. The nature of the surface-capping ligands has a significant effect on the photoluminescence emission intensity. Investigation of the effect of synthesis parameters and postsynthesis treatments on the optical properties of the nanocrystals leads to the conclusion that the room-temperature emission originates in donor−acceptor defects.

Journal ArticleDOI
TL;DR: In this article, the authors focus on electronic transport through semiconductor nanostructures which are driven by ac fields and give many examples which demonstrate the possibility of using appropriate ac fields to control/manipulate coherent quantum states.



Journal ArticleDOI
TL;DR: Semiconductor quantum dots (QDs) as discussed by the authors are nanometer-sized crystals with unique photochemical and photophysical properties that are not available from either isolated molecules or bulk solids.
Abstract: Semiconductor quantum dots (QDs) are nanometer-sized crystals with unique photochemical and photophysical properties that are not available from either isolated molecules or bulk solids. In comparison with organic dyes and fluorescent proteins, these quantum-confined nanoparticles are brighter, more stable against photobleaching, and can be excited for multicolor emission with a single light source. Recent advances have shown that nanometer-sized semiconductor particles can be covalently linked with biorecognition molecules such as peptides, antibodies, nucleic acids, or small-molecule ligands for use as biological labels. High-quality QDs are also well suited for optical encoding and multiplexing applications due to their broad excitation profiles and narrow/symmetric emission spectra. In this article, we discuss recent developments in QD synthesis and bioconjugation, their applications in molecular and cellular imaging, as well as promising directions for future research.

Posted Content
TL;DR: Simulations of the highly resolved X- and Q-band nanocrystal EPR spectra confirmed that the manganese is substitutionally incorporated into the ZnO nanocrystals as Mn( 2+) with very homogeneous speciation, differing from bulk Mn(2+):ZnO only in the magnitude of D-strain.
Abstract: We report the synthesis of colloidal Mn2+-doped ZnO (Mn2+:ZnO) quantum dots and the preparation of room-temperature ferromagnetic nanocrystalline thin films. Mn2+:ZnO nanocrystals were prepared by a hydrolysis and condensation reaction in DMSO under atmospheric conditions. Synthesis was monitored by electronic absorption and electron paramagnetic resonance (EPR) spectroscopies. Zn(OAc)2 was found to strongly inhibit oxidation of Mn2+ by O2, allowing the synthesis of Mn2+:ZnO to be performed aerobically. Mn2+ ions were removed from the surfaces of as-prepared nanocrystals using dodecylamine to yield high-quality internally doped Mn2+:ZnO colloids of nearly spherical shape and uniform diameter (6.1 +/- 0.7 nm). Simulations of the highly resolved X- and Q-band nanocrystal EPR spectra, combined with quantitative analysis of magnetic susceptibilities, confirmed that the manganese is substitutionally incorporated into the ZnO nanocrystals as Mn2+ with very homogeneous speciation, differing from bulk Mn2+:ZnO only in the magnitude of D-strain. Robust ferromagnetism was observed in spin-coated thin films of the nanocrystals, with 300 K saturation moments as large as 1.35 Bohr magneton/Mn2+ and TC > 350 K. A distinct ferromagnetic resonance signal was observed in the EPR spectra of the ferromagnetic films. The occurrence of ferromagnetism in Mn2+:ZnO and its dependence on synthetic variables are discussed in the context of these and previous theoretical and experimental results.

Journal ArticleDOI
TL;DR: In this article, cavity-assisted spin-flip Raman transitions in a single electron charged quantum dot embedded in a microcavity are proposed to obtain arbitrarily high collection efficiency and indistinguishability of the generated photons.
Abstract: An optical source that produces single-photon pulses on demand has potential applications in linear optics quantum computation, provided that stringent requirements on indistinguishability and collection efficiency of the generated photons are met. We show that these are conflicting requirements for anharmonic emitters that are incoherently pumped via reservoirs. As a model for a coherently pumped single photon source, we propose cavity-assisted spin-flip Raman transitions in a single electron charged quantum dot embedded in a microcavity. We demonstrate that using such a source, arbitrarily high collection efficiency and indistinguishability of the generated photons can be obtained simultaneously with increased cavity coupling. We analyze the role of errors that arise from distinguishability of the single-photon pulses in linear optics quantum gates by relating the gate fidelity to the strength of the two-photon interference dip in photon cross-correlation measurements. We find that performing controlled phase operations with error $l1\phantom{\rule{0.2em}{0ex}}%$ requires nanocavities with Purcell factors ${F}_{P}\ensuremath{\geqslant}40$ in the absence of dephasing, without necessitating the strong coupling limit.

Journal ArticleDOI
TL;DR: In this article, the authors demonstrate transport spectroscopy on bottom-up grown few-electron quantum dots in semiconductor nanowires, defined by InP double barrier heterostructures.
Abstract: We demonstrate transport spectroscopy on bottom-up grown few-electron quantum dots in semiconductor nanowires The dots are defined by InP double barrier heterostructures in InAs nanowires catalytically grown from nanoparticles By changing the dot size, we can design devices ranging from single-electron transistors to few-electron quantum dots In the latter case, electrons can be added one by one to the dots from 0 to ∼50 electrons while maintaining an almost constant charging energy, with addition spectra of the devices displaying shell structures as a result of spin and orbital degeneracies The reduced dimensionality of the nanowire emitter gives rise to pronounced resonant tunneling peaks, where a gate can be used to control the peak positions

Journal ArticleDOI
TL;DR: Using both absolute intensity and ratiometric fluorescence coding, it is shown that the encoded porous beads can be identified with a standard flow cytometer at 1000 beads/s, indicating that the multiple excited-state lifetimes and relaxation pathways of quantum dots do not limit their applications in high-speed optical detection and imaging.
Abstract: A new generation of optically encoded beads has been prepared by using mesoporous polystyrene beads and surfactant-coated semiconductor quantum dots. In comparison with nonporous beads of similar sizes and chemical compositions, the encoded porous beads are approximately 1000 times brighter and 5 times more uniform in fluorescence intensities. Using both absolute intensity and ratiometric fluorescence coding, we show that the beads can be identified with a standard flow cytometer at 1000 beads/s. This result indicates that the multiple excited-state lifetimes and relaxation pathways of quantum dots do not limit their applications in high-speed optical detection and imaging.

Journal ArticleDOI
TL;DR: This is the first structural model of a hybrid luminescent QD-protein receptor assembly elucidated by using spectroscopic measurements in conjunction with crystallographic and other data and indicates that MBP has a preferred orientation on the QD surface.
Abstract: The first generation of luminescent semiconductor quantum dot (QD)-based hybrid inorganic biomaterials and sensors is now being developed. It is crucial to understand how bioreceptors, especially proteins, interact with these inorganic nanomaterials. As a model system for study, we use Rhodamine red-labeled engineered variants of Escherichia coli maltose-binding protein (MBP) coordinated to the surface of 555-nm emitting CdSe-ZnS core–shell QDs. Fluorescence resonance energy transfer studies were performed to determine the distance from each of six unique MBP-Rhodamine red dye-acceptor locations to the center of the energy-donating QD. In a strategy analogous to a nanoscale global positioning system determination, we use the intraassembly distances determined from the fluorescence resonance energy transfer measurements, the MBP crystallographic coordinates, and a least-squares approach to determine the orientation of the MBP relative to the QD surface. Results indicate that MBP has a preferred orientation on the QD surface. The refined model is in agreement with other evidence, which indicates coordination of the protein to the QD occurs by means of its C-terminal pentahistidine tail, and the size of the QD estimated from the model is in good agreement with physical measurements of QD size. The approach detailed here may be useful in determining the orientation of proteins in other hybrid protein–nanoparticle materials. To our knowledge, this is the first structural model of a hybrid luminescent QD-protein receptor assembly elucidated by using spectroscopic measurements in conjunction with crystallographic and other data.

Journal ArticleDOI
23 Apr 2004-Science
TL;DR: Nonlocal spin control is demonstrated by suppressing and splitting Kondo resonances in one quantum dot by changing the electron number and coupling of the other dot, suggesting an approach to non local spin control that may be relevant to quantum information processing.
Abstract: The effective interaction between magnetic impurities in metals that can lead to various magnetic ground states often competes with a tendency for electrons near impurities to screen the local moment (known as the Kondo effect). The simplest system exhibiting the richness of this competition, the two-impurity Kondo system, was realized experimentally in the form of two quantum dots coupled through an open conducting region. We demonstrate nonlocal spin control by suppressing and splitting Kondo resonances in one quantum dot by changing the electron number and coupling of the other dot. The results suggest an approach to nonlocal spin control that may be relevant to quantum information processing.