Showing papers on "Quantum dot published in 2001"

Quantum-dot-tagged microbeads for multiplexed optical coding of biomolecules.

Abstract: Multicolor optical coding for biological assays has been achieved by embedding different-sized quantum dots (zinc sulfide-capped cadmium selenide nanocrystals) into polymeric microbeads at precisely controlled ratios. Their novel optical properties (e.g., size-tunable emission and simultaneous excitation) render these highly luminescent quantum dots (QDs) ideal fluorophores for wavelength-and-intensity multiplexing. The use of 10 intensity levels and 6 colors could theoretically code one million nucleic acid or protein sequences. Imaging and spectroscopic measurements indicate that the QD-tagged beads are highly uniform and reproducible, yielding bead identification accuracies as high as 99.99% under favorable conditions. DNA hybridization studies demonstrate that the coding and target signals can be simultaneously read at the single-bead level. This spectral coding technology is expected to open new opportunities in gene expression studies, high-throughput screening, and medical diagnostics.

Highly polarized photoluminescence and photodetection from single indium phosphide nanowires.

Abstract: We have characterized the fundamental photoluminescence (PL) properties of individual, isolated indium phosphide (InP) nanowires to define their potential for optoelectronics. Polarization-sensitive measurements reveal a striking anisotropy in the PL intensity recorded parallel and perpendicular to the long axis of a nanowire. The order-of-magnitude polarization anisotropy was quantitatively explained in terms of the large dielectric contrast between these free-standing nanowires and surrounding environment, as opposed to quantum confinement effects. This intrinsic anisotropy was used to create polarization-sensitive nanoscale photodetectors that may prove useful in integrated photonic circuits, optical switches and interconnects, near-field imaging, and high-resolution detectors.

Linearly Polarized Emission from Colloidal Semiconductor Quantum Rods

Abstract: Colloidal quantum rods of cadmium selenide (CdSe) exhibit linearly polarized emission. Empirical pseudopotential calculations predict that slightly elongated CdSe nanocrystals have polarized emission along the long axis, unlike spherical dots, which emit plane-polarized light. Single-molecule luminescence spectroscopy measurements on CdSe quantum rods with an aspect ratio between 1 and 30 confirm a sharp transition from nonpolarized to purely linearly polarized emission at an aspect ratio of 2. Linearly polarized luminescent chromophores are highly desirable in a variety of applications.

Few-electron quantum dots

Abstract: We review some electron transport experiments on few-electron, vertical quantum dot devices. The measurement of current versus source–drain voltage and gate voltage is used as a spectroscopic tool to investigate the energy characteristics of interacting electrons confined to a small region in a semiconducting material. Three energy scales are distinguished: the single-particle states, which are discrete due to the confinement involved; the direct Coulomb interaction between electron charges on the dot; and the exchange interaction between electrons with parallel spins. To disentangle these energies, a magnetic field is used to reorganize the occupation of electrons over the single-particle states and to induce changes in the spin states. We discuss the interactions between small numbers of electrons (between 1 and 20) using the simplest possible models. Nevertheless, these models consistently describe a large set of experiments. Some of the observations resemble similar phenomena in atomic physics, such as shell structure and periodic table characteristics, Hund’s rule, and spin singlet and triplet states. The experimental control, however, is much larger than for atoms: with one device all the artificial elements can be studied by adding electrons to the quantum dot when changing the gate voltage.

Semiconductor quantum dots and related systems: Electronic, optical, luminescence and related properties of low dimensional systems

Abstract: This review seeks to extend the scope of both the experimental and theoreticalwork carried out since I completed my 1993 review on the electronic, optical, andto a lesser extent, the transport properties of a variety of semiconductor quantumdots (QDs). In addition to the many advances that have been made on topics suchas quantum confinement effects (QCE), optical and luminescence properties,energy levels, and theoretical models that were dealt with in outline then, anumber of new themes have emerged. These include detailed studies on singleQDs such as InAs, InP, CuCl, etc, and this became possible due to thedevelopment of several microtechniques such as scanning near field opticalmicroscopy, SNOM or NSOM, as well as the use of improved growth proceduressuch as those involving MBE and the Stranski-Krastanow (SK) growth method, orby better chemical processing. By concentrating on single dots, it has provedpossible to limit the extent of the line broadening for the optical absorption andluminescence peaks du...

Ultralong Dephasing Time in InGaAs Quantum Dots

Abstract: We measure a dephasing time of several hundred picoseconds at low temperature in the ground-state transition of strongly confined InGaAs quantum dots, using a highly sensitive four-wave mixing technique. Between 7 and 100 K the polarization decay has two distinct components resulting in a non-Lorentzian line shape with a lifetime-limited zero-phonon line and a broadband from elastic exciton-acoustic phonon interactions.

Triggered single photons from a quantum dot.

Abstract: We demonstrate a new method for generating triggered single photons. After a laser pulse generates excitons inside a single quantum dot, electrostatic interactions between them and the resulting spectral shifts allow a single emitted photon to be isolated. Correlation measurements show a reduction of the two-photon probability to 0.12 times the value for Poisson light. Strong antibunching persists when the emission is saturated. The emitted photons are also polarized.

High-Quality Manganese-Doped ZnSe Nanocrystals

Abstract: We demonstrate high-quality, highly fluorescent, ZnSe colloidal nanocrystals (or quantum dots) that are doped with paramagnetic Mn2+ impurities. We present luminescence, magnetic circular dichroism (MCD), and electron paramagnetic resonance (EPR) measurements to confirm that the Mn impurities are embedded inside the nanocrystal. Optical measurements show that by exciting the nanocrystal, efficient emission from Mn is obtained, with a quantum yield of 22% at 295 K and 75% below 50 K (relative to Stilbene 420). MCD spectra reveal an experimental Zeeman splitting in the first excited state that is large (28 meV at 2.5 T), depends on doping concentration, and saturates at modest fields. In the low field limit, the magnitude of the effective g factor is 430 times larger than in undoped nanocrystals. EPR experiments exhibit a six-line spectrum with a hyperfine splitting of 60.4 × 10-4 cm-1, consistent with Mn substituted at Zn sites in the cubic ZnSe lattice.

Coupling and Entangling of Quantum States in Quantum Dot Molecules

Abstract: We demonstrate coupling and entangling of quantum states in a pair of vertically aligned, self-assembled quantum dots by studying the emission of an interacting electron-hole pair (exciton) in a single dot molecule as a function of the separation between the dots. An interaction-induced energy splitting of the exciton is observed that exceeds 30 millielectron volts for a dot layer separation of 4 nanometers. The results are interpreted by mapping the tunneling of a particle in a double dot to the problem of a single spin. The electron-hole complex is shown to be equivalent to entangled states of two interacting spins.

Spectroscopy and hot electron relaxation dynamics in semiconductor quantum wells and quantum dots.

Abstract: ▪ Abstract Photoexcitation of a semiconductor with photons above the semiconductor band gap creates electrons and holes that are out of equilibrium. The rates at which the photogenerated charge carriers return to equilibrium via thermalization through carrier scattering, cooling by phonon emission, and radiative and nonradiative recombination are important issues. The relaxation processes can be greatly affected by quantization effects that arise when the carriers are confined to regions of space that are small compared with their deBroglie wavelength or the Bohr radius of bulk excitons. The effects of size quantization in semiconductor quantum wells (carrier confinement in one dimension) and quantum dots (carrier confinement in three dimensions) on the respective carrier relaxation processes are reviewed, with emphasis on electron cooling dynamics. The implications of these effects for applications involving radiant energy conversion are also discussed.

Rabi oscillations of excitons in single quantum dots.

Abstract: Transient nonlinear optical spectroscopy, performed on excitons confined to single GaAs quantum dots, shows oscillations that are analogous to Rabi oscillations in two-level atomic systems. This demonstration corresponds to a one-qubit rotation in a single quantum dot which is important for proposals using quantum dot excitons for quantum computing. The dipole moment inferred from the data is consistent with that directly obtained from linear absorption studies. The measurement extends the artificial atom model of quantum dot excitonic transitions into the strong-field limit, and makes possible full coherent optical control of the quantum state of single excitons using optical pi pulses.

Band Gap Variation of Size- and Shape-Controlled Colloidal CdSe Quantum Rods

Abstract: We report the band gaps of rodlike CdSe quantum dots with diameter varying from 3.0 to 6.5 nm and length from 7.5 to 40 nm. A qualitative explanation for the dependence of band gap on width and length is presented.

Blinking statistics in single semiconductor nanocrystal quantum dots

Abstract: Statistical studies of fluorescence intermittency in single CdSe nanocrystal quantum dots (QD's) reveal a temperature-independent power-law distribution in the histogram of on and off times---the time periods before the QD turns from emitting to nonemitting (bright to dark) and vice versa. Every QD shows a similar power-law behavior for the off-time distribution regardless of temperature, excitation intensity, surface morphology or size. We propose a dynamic model of tunneling between core and trapped charged states to explain the universal power-law statistics of the blinking events observed. The on-time probability distributions show evidence of both a tunneling mechanism similar to the off-time statistics and a secondary, photoinduced process that leads to a truncation of the power law. The same blinking statistics are also observed for single CdTe nanocrystal QD's.

Fermi Level Equilibration in Quantum Dot−Metal Nanojunctions†

Abstract: The process of Fermi level equilibration in 5 nm ZnO quantum dot−metal nanojunctions has been monitored using changes to both the surface plasmon band of the metal island and the sharp exciton band of the ZnO nanocrystals following photoinduced electron accumulation. In the cases of silver, copper, and gold islands, excess electrons reside on both the quantum dot and the metal, whereas for Pt islands, the excess electrons reside exclusively on the Pt island. Electrons are transferred rapidly from Pt to the solvent ethanol, preventing accumulation on the quantum dots. The combination of exciton bleaching and surface plasmon shifts provides a simple way of probing the efficiency of small metal islands as redox catalysts on semiconductor particles.

``On''/``off'' fluorescence intermittency of single semiconductor quantum dots

Abstract: Single molecule confocal microscopy is used to investigate the detailed kinetics of fluorescence intermittency in colloidal II–VI (CdSe) semiconductor quantum dots. Two distinct modes of behavior are observed corresponding to (i) sustained “on” episodes (τon) of rapid laser absorption/fluorescence cycling, followed by (ii) sustained “off” episodes (τoff) where essentially no light is emitted despite continuous laser excitation. Both on-time and off-time probability densities follow an inverse power law, P(τon/off)∝1/τon/offm, over more than seven decades in probability density and five decades in time. Such inverse power law behavior is an unambiguous signature of highly distributed kinetics with rates varying over 105-fold, in contrast with models for switching between “on” and “off” configurations of the system via single rate constant processes. The unprecedented dynamic range of the current data permits several kinetic models of fluorescence intermittency to be evaluated at the single molecule level a...

CdSe−ZnS Quantum Dots as Resonance Energy Transfer Donors in a Model Protein−Protein Binding Assay

Abstract: Specific binding of biotinilated bovine serum albumin (bBSA) and tetramethylrhodamine-labeled streptavidin (SAv−TMR) was observed by conjugating bBSA to CdSe−ZnS core−shell quantum dots (QDs) and observing enhanced TMR fluorescence caused by fluorescence resonance energy transfer (FRET) from the QD donors to the TMR acceptors. Because of the broad absorption spectrum of the QDs, efficient donor excitation could occur at a wavelength that was well resolved from the absorption spectrum of the acceptor, thereby minimizing direct acceptor excitation. Appreciable overlap of the donor emission and acceptor absorption spectra was achieved by size-tuning the QD emission spectrum into resonance with the acceptor absorption spectrum, and cross-talk between the donor and acceptor emission was minimized because of the narrow, symmetrically shaped QD emission spectrum. Evidence for an additional, nonspecific QD−TMR energy transfer mechanism that caused quenching of the QD emission without a corresponding TMR fluoresce...

Single-mode solid-state single photon source based on isolated quantum dots in pillar microcavities

Abstract: We report the fabrication of a single-mode solid-state single photon source, based on an isolated InAs quantum dot (QD) on resonance with the fundamental mode of a pillar microcavity. Photon correlation experiments under pulsed excitation reveal a clear antibunching behavior. We show that a preparation of the single photons in a given quantum state (same spatial mode, same polarization) can be obtained by placing a QD in resonance with the nondegenerate fundamental mode of an elliptical micropillar.

Highly luminescent silicon nanocrystals with discrete optical transitions.

Abstract: A new synthetic method was developed to produce robust, highly crystalline, organic-monolayer passivated silicon (Si) nanocrystals in a supercritical fluid. By thermally degrading the Si precursor, diphenylsilane, in the presence of octanol at 500 °C and 345 bar, relatively size-monodisperse sterically stabilized Si nanocrystals ranging from 15 to 40 A in diameter could be obtained in significant quantities. Octanol binds to the Si nanocrystal surface through an alkoxide linkage and provides steric stabilization through the hydrocarbon chain. The absorbance and photoluminescence excitation (PLE) spectra of the nanocrystals exhibit a significant blue shift in optical properties from the bulk band gap energy of 1.2 eV due to quantum confinement effects. The stable Si clusters show efficient blue (15 A) or green (25−40 A) band-edge photoemission with luminescence quantum yields up to 23% at room temperature, and electronic structure characteristic of a predominantly indirect transition, despite the extremely...

Acoustic phonon broadening mechanism in single quantum dot emission

Abstract: We study the effect of the exciton-acoustic-phonon coupling on the optical homogeneous line shape of confined zero-dimensional excitons and discuss the connection with the so-called pure dephasing effect. On increasing the temperature, the line shape progressively deviates from the expected Lorentzian profile, with the appearance of low energy acoustic-phonon sidebands. The non-Lorentzian line shape and its temperature dependence are theoretically modeled on the basis of the lattice relaxation due to the exciton-acoustic-phonon coupling. This gives a precise description of the underlying mechanism which controls the exciton dephasing.

Biological applications of quantum dots

Abstract: The present invention provides a composition comprising fluorescent semiconductor nanocrystals associated to a compound, wherein the nanocrystals have a characteristic spectral emission, wherein said spectral emission is tunable to a desired wavelength by controlling the size of the nanocrystal, and wherein said emission provides information about a biological state or event.

Electrochromic Nanocrystal Quantum Dots

Abstract: Incorporating nanocrystals into future electronic or optoelectronic devices will require a means of controlling charge-injection processes and an understanding of how the injected charges affect the properties of nanocrystals. We show that the optical properties of colloidal semiconductor nanocrystal quantum dots can be tuned by an electrochemical potential. The injection of electrons into the quantum-confined states of the nanocrystal leads to an electrochromic response, including a strong, size-tunable, midinfrared absorption corresponding to an intraband transition, a bleach of the visible interband exciton transitions, and a quench of the narrow band-edge photoluminescence.

Exciton rabi oscillation in a single quantum dot

Abstract: A spectroscopic method, which enables characterization of a single isolated quantum dot and a quantum wave function interferometry, is applied to an exciton discrete excited state in an InGaAs quantum dot. Long coherence of zero-dimensional excitonic states made possible the observation of coherent population flopping in a 0D excitonic two-level system in a time-domain interferometric measurement. Corresponding energy splitting is also manifested in an energy-domain measurement.

Spin-flip transitions between Zeeman sublevels in semiconductor quantum dots

Abstract: We have studied spin-flip transitions between Zeeman sublevels in GaAs electron quantum dots. Several different mechanisms which originate from spin-orbit coupling are shown to be responsible for such processes. It is shown that spin-lattice relaxation for the electron localized in a quantum dot is much less effective than for the free electron. The spin-flip rates due to several other mechanisms not related to the spin-orbit interaction are also estimated.

Resonant electron scattering by defects in single-walled carbon nanotubes.

Abstract: We report the characterization of defects in individual metallic single-walled carbon nanotubes by transport measurements and scanned gate microscopy. A sizable fraction of metallic nanotubes grown by chemical vapor deposition exhibits strongly gate voltage-dependent resistance at room temperature. Scanned gate measurements reveal that this behavior originates from resonant electron scattering by defects in the nanotube as the Fermi level is varied by the gate voltage. The reflection coefficient at the peak of a scattering resonance was determined to be about 0.5 at room temperature. An intratube quantum dot device formed by two defects is demonstrated by low-temperature transport measurements.

Photooxidation and Photobleaching of Single CdSe/ZnS Quantum Dots Probed by Room-Temperature Time-Resolved Spectroscopy

Abstract: The room-temperature luminescence of single CdSe/ZnS core−shell quantum dots is investigated by spectrally and temporally resolved confocal microscopy. A large (30 nm) blue shift is observed in the emission wavelength during illumination in air. In nitrogen, no blue shift is observed. The blue shift in air is ascribed to a 1 nm shrinkage of the CdSe core by photooxidation. Photobleaching occurs about 4 times faster in air than in nitrogen, indicating the formation of nonradiative recombination centers during photooxidation. The initial light output is higher in air than in nitrogen, which may be due to a reduction of the defect state lifetime by oxygen.

Properties of Fluorescent Semiconductor Nanocrystals and their Application to Biological Labeling

Abstract: We review recent advances in the development of colloidal fluorescent semiconductor nanocrystals (a class of quantum dots) for biological labeling. Although some of the photophysical properties of nanocrystals are not fully understood and are still actively investigated, researchers have begun developing bioconjugation schemes and applying such probes to biological assays. Nanocrystals possess several qualities that make them very attractive for fluorescent tagging: broad excitation spectrum, narrow emission spectrum, precise tunability of their emission peak, longer fluorescence lifetime than organic fluorophores and negligible photobleaching. On the down side, their emission is strongly intermittent ("blinking”) and their size is relatively large for many biological uses. We describe how to take advantage of nanocrystals’ spectral properties to increase the resolution of fluorescence microscopy measurements down to the nanometer level. We also show how their long fluorescence lifetime can be used to observe molecules and organelles in living cells without interference from background autofluorescence, a pre-requisite for single molecule detectability. Finally, their availability in multicolor species and their single molecule sensitivity open up interesting possibilities for genomics applications.

Energy spectra of quantum rings

Abstract: Ring geometries have fascinated experimental and theoretical physicists over many years. Open rings connected to leads allow the observation of the Aharonov-Bohm effect, a paradigm of quantum mechanical phase coherence. The phase coherence of transport through a quantum dot embedded in one arm of an open ring has been demonstrated. The energy spectrum of closed rings has only recently been analysed by optical experiments and is the basis for the prediction of persistent currents and related experiments. Here we report magnetotransport experiments on a ring-shaped semiconductor quantum dot in the Coulomb blockade regime. The measurements allow us to extract the discrete energy levels of a realistic ring, which are found to agree well with theoretical expectations. Such an agreement, so far only found for few-electron quantum dots, is here extended to a many-electron system. In a semiclassical language our results indicate that electron motion is governed by regular rather than chaotic motion, an unexplored regime in many-electron quantum dots.

Band gap engineering of amorphous silicon quantum dots for light-emitting diodes

Abstract: Amorphous silicon quantum dots (a-Si QDs), which show a quantum confinement effect were grown in a silicon nitride film by plasma-enhanced chemical vapor deposition. Red, green, blue, and white photoluminescence were observed from the a-Si QD structures by controlling the dot size. An orange light-emitting diode (LED) was fabricated using a-Si QDs with a mean size of 2.0 nm. The turn-on voltage was less than 5 V. An external quantum efficiency of 2×10−3% was also demonstrated. These results show that a LED using a-Si QDs embedded in the silicon nitride film is superior in terms of electrical and optical properties to other Si-based LEDs.

Coherent branched flow in a two-dimensional electron gas

Abstract: Semiconductor nanostructures based on two-dimensional electron gases (2DEGs) could form the basis of future devices for sensing, information processing and quantum computation. Although electron transport in 2DEG nanostructures has been well studied, and many remarkable phenomena have already been discovered (for example, weak localization, quantum chaos, universal conductance fluctuations), fundamental aspects of the electron flow through these structures have so far not been clarified. However, it has recently become possible to image current directly through 2DEG devices using scanning probe microscope techniques. Here, we use such a technique to observe electron flow through a narrow constriction in a 2DEG-a quantum point contact. The images show that the electron flow from the point contact forms narrow, branching strands instead of smoothly spreading fans. Our theoretical study of this flow indicates that this branching of current flux is due to focusing of the electron paths by ripples in the background potential. The strands are decorated by interference fringes separated by half the Fermi wavelength, indicating the persistence of quantum mechanical phase coherence in the electron flow. These findings may have important implications for a better understanding of electron transport in 2DEGs and for the design of future nanostructure devices.