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PubMed2002

Effects of crystal shape on the energy levels of zero-dimensional PbS quantum dots.

Nanometer-size PbS quantum dots have been made by electrodeposition on a Au(111) substrate. The deposited nanocrystals have a flattened cubic shape. We probed the single-electron energy-level spectrum of individual quantum dots by scanning tunneling spectroscopy and found that it deviates strongly from that of spherical PbS quantum dots. The measured energy-level spectrum is successfully explained by considering strong confinement in a flattened cubic box.

Journal Article↗
PubMed2005

Turning all the lights on: quantum dots in cellular assays.

Quantum dot materials are increasingly used in cellular assays, and offer a powerful and enabling complement to existing methods of labeling proteins, such as green fluorescent protein. These materials give researchers the ability to study specificity and functional responses in cellular systems, in a highly multiplexed manner, at either a molecular or cellular level. The recent literature bears witness to the increasing use of quantum dots for the investigation of chemicals on biological systems, and paves the way to the use of these assays for high-throughput analysis of functional responses in relevant models at scales including molecular, cellular and whole animal.

Cells↗
PubMed2006

[Quantum dots and their applications in cancer research].

Quantum dots are semiconductor nanocrystals with physical dimensions smaller than the exciton Bohr radius. As their fluorescence emissions are size-tunable, we can acquire any spectrum from ultraviolet (UV) to near-infrared by changing the particles' radiuses. The large Stokes shifts of quantum dots can be used to further improve detection sensitivity. The luminescence intensity is high and stable. Single quantum dots have longer excited state lifetimes, and they appear 10-20 times brighter than organic fluorescent dyes. And they have good biocompatibility because quantum dots with appropriate shells don't interfere with physiological processes, such as growth, development, signaling and motility. With the development of optical labeling and imaging technology, many present conventional biomedical methods have limitations in microcosmic direct real-time researches of bio-molecular interactions and early diagnosis of malignant tumors. The invention of quantum dots and their biomedical applications make them as good markers for tumor cell tracing and targeting in cancer research, such as prostate cancer, mammary cancer, cervical cancer, basal cell carcinoma, liver cancer, and melanoma. The current research is focused on tumor markers imaging and molecular interaction based on tangible carriers such as cells and tissues. The next research orientation would be to tap the potential of this highly sensitive technology to image tumor biomarkers in serum and other body fluids, so as to increase the early diagnosis rate of malignant tumors.

Animals↗
PubMed2005

Dynamics within the exciton fine structure of colloidal CdSe quantum dots.

Evidence for an interaction between the quantum dot exciton fine structure states F = +/-1 is obtained by measuring the dynamics of transitions among those states, exciton spin relaxation or flipping. An ultrafast transient grating experiment based on a crossed-linear polarization grating is reported. By using the quantum dot selection rules for absorption of circularly polarized light, it is demonstrated that it is possible to detect transitions between nominally degenerate fine structure states, even in a rotationally isotropic system. The results for colloidal CdSe quantum dots reveal a strong size dependence for the exciton spin relaxation rate from one bright exciton state (F = +/-1) to the other in CdSe colloidal quantum dots at 293 K, on a time scale ranging from femtoseconds to picoseconds, depending on the quantum dot size. The results are consistent with an interaction between those states attributed to a long-range contribution to the electron-hole exchange interaction.

Journal Article↗
PubMed2004

Water-soluble silica-overcoated CdS:Mn/ZnS semiconductor quantum dots.

Highly luminescent and photostable CdS:Mn/ZnS core/shell quantum dots are not water soluble because of their hydrophobicity. To create water-soluble quantum dots by an appropriate surface functionalization, CdS:Mn/ZnS quantum dots synthesized in a water-in-oil (W/O) microemulsion system (reverse micelles) were consecutively overcoated with a very thin silica layer ( approximately 2.5 nm thick) within the same reverse micellar system. The water droplet serves as a nanosized reactor for the controlled hydrolysis and condensation of a silica precursor, tetraethyl orthosilicate (TEOS), using an ammonium hydroxide (NH4OH) catalyst. Structural characterizations with transmission electron microscopy (TEM) and x-ray photoelectron spectroscopy (XPS) indicate that the silica-quantum dot nanocomposites consist of a layered structure. Owing to the amorphous, porous nature of a silica layer, the optical and photophysical properties of silica-overcoated CdS:Mn/ZnS quantum dots are found to remain close to those of uncoated counterparts.

Journal Article↗
PubMed2005

Dark field transmission electron microscope images of III-V quantum dot structures.

Multi-layer quantum dot structures are becoming increasingly common in order to improve the efficiency of quantum dot lasers. Each layer of dots may be influenced by the preceding dot layer, and the dot density can vary from layer to layer. Characterization of such structures relies on the reliable determination of the shape, size and density of dots in each layer. Dark field transmission electron microscopy (TEM) images using the 002 diffraction condition are frequently used, viewing the layers edge-on in a cross-section sample. A simple model is used to describe the contrast as a function of dot size and shape, specimen thickness, and the composition of the dot and surrounding materials. Good agreement with experimental results is obtained. It is found that the dot size is not accurately related to the bright region seen in such images. While 002 images can be used to determine the size and shape of dots, a density per unit area cannot be calculated in the cross section geometry without either measuring--or assuming--the specimen thickness. In multilayer structures, plan-view TEM images show the layers as overlapping, losing the information from individual layers. By tilting a cross-section specimen to allow imaging with the dark field 113 diffraction condition, the density in individual layers can be measured. Additional information, such as wetting layer thickness variations and alignment of dots due to surface roughness or substrate offcut, can also be obtained.

Contrast Sensitivity↗
PubMed2006

Synthesis and application of quantum dots FRET-based protease sensors.

Preparation of FRET-based quantum dots as protease sensors-RGDC peptide molecules are bound to the surface of CdSe/ZnS quantum dots. The peptide molecules are then labeled with rhodamine dye molecules. The emission color of the quantum dots change from green to orange due to fluorescence resonance energy transfer (FRET) between the quantum dots and the bound rhodamine molecules. Cleavage of the peptide by selective proteases releases the rhodamine molecules from the quantum dots surface, which results in decreasing FRET efficiency between the quantum dots and the rhodamine molecules. The emission color of the quantum dots changes back to green.

Enzyme Activation↗
PubMed2006

The empirical correlation between size and two-photon absorption cross section of CdSe and CdTe quantum dots.

The tuning of CdSe quantum dot (QDs) sizes, and consequently their corresponding two-photon absorption (TPA) cross section, has been systematically investigated. As the size (diameter) of the quantum dots increases, the TPA cross section is found to be empirically related via a power-law proportionality of 3.5+/-0.5 and 5.6+/-0.7 to the diameters of CdSe and CdTe QDs, respectively. The results are tentatively rationalized via a theoretical model of two-photon excitation properties in a system incorporating excitons and defects.

Absorption↗
PubMed2006

Fate of micelles and quantum dots in cells.

Micelles and quantum dots have been used as experimental drug delivery systems and imaging tools both in vitro and in vivo. Investigations of their fate at the subcellular level require different surface-core modifications. Among the most common modifications are those with fluorescent probes, dense-core metals or radionucleids. Cellular fate of several fluorescent probes incorporated into poly(caprolactone)-b-copolymer micelles (PCL-b-PEO) was followed by confocal microscopy, and colloidal gold incorporated in poly 4-vinyl pyridine-PEO micelles were developed to explore micelle fate by electron microscopy. More recently, we have examined quantum dots (QDs) as the next-generation-labels for cells and nanoparticulate drug carriers amenable both to confocal and electron microscopic analyses. Effects of QDs at the cellular and subcellular levels and their integrity were studied. Results from different studies suggest that size, charge and surface manipulations of QDs may play a role in their subcellular distribution. Examples of pharmacological agents incorporated into block copolymer micelles, administered or attached to QD surfaces show how the final biological outcome (e.g. cell death, proliferation or differentiation) depends on physical properties of these nanoparticles.

Animals↗
PubMed2005

Phonon-induced exciton dephasing in quantum dot molecules.

A new microscopic approach to the optical transitions in quantum dots and quantum dot molecules, which accounts for both diagonal and nondiagonal exciton-phonon interaction, is developed. The cumulant expansion of the linear polarization is generalized to a multilevel system and is applied to calculation of the full time dependence of the polarization and the absorption spectrum. In particular, the broadening of zero-phonon lines is evaluated directly and discussed in terms of real and virtual phonon-assisted transitions. The influence of Coulomb interaction, tunneling, and structural asymmetry on the exciton dephasing in quantum dot molecules is analyzed.

Journal Article↗
PubMed2006

Electronic coupling and exciton energy transfer in CdTe quantum-dot molecules.

Stable dispersions of molecularlike aggregates of CdTe quantum dots are prepared by chemical cross-linking. Cryo-TEM images confirm the presence of cross-linked quantum dots and show that the size of the small aggregates can be controlled by the amount of cross-linker added. Optical measurements reveal two types of interdot interactions within these quantum-dot molecules: exciton energy transfer and electronic coupling. Quantitative information on the energy transfer rates in quantum-dot molecules is obtained by photoluminescence lifetime measurements. The degree of electronic coupling is dependent on the size of the quantum dots, which is supported by quantum mechanical calculations.

Journal Article↗
PubMed2005

Photoactivation of quantum dot fluorescence following endocytosis.

We studied the fluorescence of quantum dots in cells. Coating quantum dots with cationic peptides caused them to be endocytosed and transported to lysosomes. After overnight incubation, their fluorescence apparently dimmed but became markedly "photoactivatable", increasing more than 3-fold within minutes on exposure to bright light, and decaying over hours in the dark. Photoactivation was greater in the presence of water than ethanol, and UV illumination compensated for lack of water during photoactivation. Dimming and photoactivation could affect the use of quantum dots as quantitative probes in vivo and lead to new uses, such as tracking molecular movement.

Animals↗
PubMed2006

Peptide coated quantum dots for biological applications.

Quantum dots (QDOTs) have been widely recognized by the scientific community and the biotechnology industry, as witnessed by the exponential growth of this field in the past several years. We describe the synthesis and characterization of visible and near infrared QDots--a critical step for engineering organic molecules like proteins and peptides for building nanocomposite materials with multifunctional properties suitable for biological applications.

Coated Materials, Biocompatible↗
PubMed2004

Methods for labeling quantum dots to biomolecules.

Semiconductor quantum dots (QDs) are thought to be the most promising fluorescent probe for biological and biomedical applications because of their unique size-dependent optical and electronic properties. QD bioconjugates provide important advantages over conventional organic dyes. This review compares the optical properties of nanoparticles and dyes and describes the surface modification of the QDs and the methods for biomolecules conjugating to QDs. In addition, the effect of QDs on normal physiology in real biological applications is discussed.

Fluorescent Dyes↗
PubMed2006

Optical signatures of coupled quantum dots.

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.

Journal Article↗
PubMed2005

Single-molecule quantum-dot fluorescence resonance energy transfer.

Colloidal semiconductor quantum dots are promising for single-molecule biological imaging due to their outstanding brightness and photostability. As a proof of concept for single-molecule fluorescence resonance energy transfer (FRET) applications, we measured FRET between a single quantum dot and a single organic fluorophore Cy5. DNA Holliday junction dynamics measured with the quantum dot/Cy5 pair are identical to those obtained with the conventional Cy3/Cy5 pair, that is, conformational changes of individual molecules can be observed by using the quantum dot as the donor.

Biophysics↗
PubMed2004

Surface-immobilized self-assembled protein-based quantum dot nanoassemblies.

Luminescent semiconductor quantum dot (QD)-based optical biosensors have the potential to overcome many of the limitations associated with using conventional organic dyes for biodetection. We have previously demonstrated a hybrid QD-protein-based fluorescence resonance energy transfer (FRET) sensor. Although the QD acted as an energy donor and a protein scaffold in the sensor, recognition and specificity were derived from the proteins. Transitioning this hybrid prototype sensor into flow cells and integrated devices will require a surface-immobilization strategy that allows the QD-based sensor to sample the environment and still maintain a distinct protein-covered QD architecture. We demonstrate a self-assembled strategy designed to accomplish this. Using glass slides coated with a monolayer of neutravidin (NA) as the template, QDs with maltose binding protein (MBP) and avidin coordinated to their surface were attached to the glass slides in discrete patterns using an intermediary bridge of biotinylated MBP or antibody linkers. Control of the surface location and concentration of the QD-protein-based structures is demonstrated. The utility of this self-assembly strategy is further demonstrated by assembling a QD-protein structure that allows the QDs to engage in FRET with a dye located on the surface-covering protein.

Avidin↗
PubMed2006

Multipeak Kondo effect in one- and two-electron quantum dots.

We have fabricated a few-electron quantum dot that can be tuned down to zero electrons while maintaining strong coupling to the leads. Using a nearby quantum point contact as a charge sensor, we can determine the absolute number of electrons in the quantum dot. We find several sharp peaks in the differential conductance, occurring at both zero and finite source-drain bias, for the one- and two-electron quantum dot. We attribute the peaks at finite bias to a Kondo effect through excited states of the quantum dot and investigate the magnetic field dependence of these Kondo resonances.

Journal Article↗