Quantum-confined stark effect in single CdSe nanocrystallite quantum dots

The quantum-confined Stark effect in single cadmium selenide (CdSe) nanocrystallite quantum dots was studied. The electric field dependence of the single-dot spectrum is characterized by a highly polarizable excited state ( approximately 10(5) cubic angstroms, compared to typical molecular values of order 10 to 100 cubic angstroms), in the presence of randomly oriented local electric fields that change over time. These local fields result in spontaneous spectral diffusion and contribute to ensemble inhomogeneous broadening. Stark shifts of the lowest excited state more than two orders of magnitude larger than the linewidth were observed, suggesting the potential use of these dots in electro-optic modulation devices.     

Capture of a single molecule in a nanocavity

We describe a heptameric protein pore that has been engineered to accommodate two different cyclodextrin adapters simultaneously within the lumen of a transmembrane beta barrel. The volume between the adapters is a cavity of approximately 4400 cubic angstroms. Analysis of single-channel recordings reveals that individual charged organic molecules can be pulled into the cavity by an electrical potential. Once trapped, an organic molecule shuttles back and forth between the adapters for hundreds of milliseconds. Such self-assembling nanostructures are of interest for the fabrication of multianalyte sensors and could provide a means to control chemical reactions.     

Electrochromic nanocrystal quantum dots

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.     

Conditional dynamics of interacting quantum dots

Conditional quantum dynamics, where the quantum state of one system controls the outcome of measurements on another quantum system, is at the heart of quantum information processing. We demonstrate conditional dynamics for two coupled quantum dots, whereby the probability that one quantum dot makes a transition to an optically excited state is controlled by the presence or absence of an optical excitation in the neighboring dot. Interaction between the dots is mediated by the tunnel coupling between optically excited states and can be optically gated by applying a laser field of the right frequency. Our results represent substantial progress toward realization of an optically effected controlled-phase gate between two solid-state qubits.     

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.     

Heavily doped semiconductor nanocrystal quantum dots

Doping of semiconductors by impurity atoms enabled their widespread technological application in microelectronics and optoelectronics. However, doping has proven elusive for strongly confined colloidal semiconductor nanocrystals because of the synthetic challenge of how to introduce single impurities, as well as a lack of fundamental understanding of this heavily doped limit under strong quantum confinement. We developed a method to dope semiconductor nanocrystals with metal impurities, enabling control of the band gap and Fermi energy. A combination of optical measurements, scanning tunneling spectroscopy, and theory revealed the emergence of a confined impurity band and band-tailing. Our method yields n- and p-doped semiconductor nanocrystals, which have potential applications in solar cells, thin-film transistors, and optoelectronic devices.     

Slow electron cooling in colloidal quantum dots

Hot electrons in semiconductors lose their energy very quickly (within picoseconds) to lattice vibrations. Slowing this energy loss could prove useful for more efficient photovoltaic or infrared devices. With their well-separated electronic states, quantum dots should display slow relaxation, but other mechanisms have made it difficult to observe. We report slow intraband relaxation (>1 nanosecond) in colloidal quantum dots. The small cadmium selenide (CdSe) dots, with an intraband energy separation of approximately 0.25 electron volts, are capped by an epitaxial zinc selenide (ZnSe) shell. The shell is terminated by a CdSe passivating layer to remove electron traps and is covered by ligands of low infrared absorbance (alkane thiols) at the intraband energy. We found that relaxation is markedly slowed with increasing ZnSe shell thickness.     

Chaotic Dirac billiard in graphene quantum dots

The exceptional electronic properties of graphene, with its charge carriers mimicking relativistic quantum particles and its formidable potential in various applications, have ensured a rapid growth of interest in this new material. We report on electron transport in quantum dot devices carved entirely from graphene. At large sizes (>100 nanometers), they behave as conventional single-electron transistors, exhibiting periodic Coulomb blockade peaks. For quantum dots smaller than 100 nanometers, the peaks become strongly nonperiodic, indicating a major contribution of quantum confinement. Random peak spacing and its statistics are well described by the theory of chaotic neutrino billiards. Short constrictions of only a few nanometers in width remain conductive and reveal a confinement gap of up to 0.5 electron volt, demonstrating the possibility of molecular-scale electronics based on graphene.     

Exciton storage in semiconductor self-assembled quantum dots

Storage and retrieval of excitons were demonstrated with semiconductor self-assembled quantum dots (QDs). The optically generated excitons were dissociated and stored as separated electron-hole pairs in coupled QD pairs. A bias voltage restored the excitons, which recombined radiatively to provide a readout optical signal. The localization of the spatially separated electron-hole pair in QDs was responsible for the ultralong storage times, which were on the order of several seconds. The present limits of this optical storage medium are discussed.     

A tunable kondo effect in quantum dots

A tunable Kondo effect has been realized in small quantum dots. A dot can be switched from a Kondo system to a non-Kondo system as the number of electrons on the dot is changed from odd to even. The Kondo temperature can be tuned by means of a gate voltage as a single-particle energy state nears the Fermi energy. Measurements of the temperature and magnetic field dependence of a Coulomb-blockaded dot show good agreement with predictions of both equilibrium and nonequilibrium Kondo effects.     

Excitation spectra of circular, few-electron quantum dots

Studies of the ground and excited states in semiconductor quantum dots containing 1 to 12 electrons showed that the quantum numbers of the states in the excitation spectra can be identified and compared with exact calculations. A magnetic field induces transitions between the ground and excited states. These transitions were analyzed in terms of crossings between single-particle states, singlet-triplet transitions, spin polarization, and Hund's rule. These impurity-free quantum dots allow "atomic physics" experiments to be performed in magnetic field regimes not accessible for atoms.     

Ordering of quantum dots using genetically engineered viruses

A liquid crystal system was used for the fabrication of a highly ordered composite material from genetically engineered M13 bacteriophage and zinc sulfide (ZnS) nanocrystals. The bacteriophage, which formed the basis of the self-ordering system, were selected to have a specific recognition moiety for ZnS crystal surfaces. The bacteriophage were coupled with ZnS solution precursors and spontaneously evolved a self-supporting hybrid film material that was ordered at the nanoscale and at the micrometer scale into approximately 72-micrometer domains, which were continuous over a centimeter length scale. In addition, suspensions were prepared in which the lyotropic liquid crystalline phase behavior of the hybrid material was controlled by solvent concentration and by the use of a magnetic field.     

量子点在食品安全检测中的应用研究

近年来,量子点由于其优异的荧光性能,被广泛地作为生物纳米探针用于食品安全分析领域。为了解量子点及其在食品安全检测中的应用研究现状,综述了量子点的组成结构、光学特性、制备方法,以及量子点在食品安全检测方面应用取得的最新进展,并对其研究方向进行展望,以期促进量子点在食品安全检测中得到进一步的推广和运用。     

Single-electron delocalization in hybrid vertical-lateral double quantum dots

We used a hybrid vertical-lateral double-dot device, consisting of laterally coupled vertical quantum dots, to measure the interdot tunnel coupling. By using nonlinear transport measurements of "Coulomb diamonds," we showed that an inherent asymmetry in the capacitances of the component dots influences the diamond slopes, thereby allowing for the determination of the dot through which the electron has passed. We used this technique to prepare a delocalized one-electron state and Heitler-London (HL) two-electron state, and we showed that the interdot tunnel coupling, which determines whether HL is the ground state, is tunable. This implies that our device may be useful for implementing two-electron spin entanglement.     

Coherent spin transfer between molecularly bridged quantum dots

Femtosecond time-resolved Faraday rotation spectroscopy reveals the instantaneous transfer of spin coherence through conjugated molecular bridges spanning quantum dots of different size over a broad range of temperature. The room-temperature spin-transfer efficiency is approximately 20%, showing that conjugated molecules can be used not only as interconnections for the hierarchical assembly of functional networks but also as efficient spin channels. The results suggest that this class of structures may be useful as two-spin quantum devices operating at ambient temperatures and may offer promising opportunities for future versatile molecule-based spintronic technologies.     

Spatially resolved visible luminescence of self-assembled semiconductor quantum dots

Ensembles of defect-free InAIAs islands of ultrasmall dimensions embedded in AIGaAs have been grown by molecular beam epitaxy. Cathodoluminescence was used to directly image the spatial distribution of the quantum dots by mapping their luminescence and to spectrally resolve very sharp peaks from small groups of dots, thus providing experimental verification for the discrete density of states in a zero-dimensional quantum structure. Visible luminescence is produced by different nominal compositions of InxAI(1-x)As-AIyGa(1-y)As.     

Quantization of multiparticle auger rates in semiconductor quantum dots

We have resolved single-exponential relaxation dynamics of the 2-, 3-, and 4-electron-hole pair states in nearly monodisperse cadmium selenide quantum dots with radii ranging from 1 to 4 nanometers. Comparison of the discrete relaxation constants measured for different multiple-pair states indicates that the carrier decay rate is cubic in carrier concentration, which is characteristic of an Auger process. We observe that in the quantum-confined regime, the Auger constant is strongly size-dependent and decreases with decreasing the quantum dot size as the radius cubed.     

Water-soluble quantum dots for multiphoton fluorescence imaging in vivo

The use of semiconductor nanocrystals (quantum dots) as fluorescent labels for multiphoton microscopy enables multicolor imaging in demanding biological environments such as living tissue. We characterized water-soluble cadmium selenide-zinc sulfide quantum dots for multiphoton imaging in live animals. These fluorescent probes have two-photon action cross sections as high as 47,000 Goeppert-Mayer units, by far the largest of any label used in multiphoton microscopy. We visualized quantum dots dynamically through the skin of living mice, in capillaries hundreds of micrometers deep. We found no evidence of blinking (fluorescence intermittency) in solution on nanosecond to millisecond time scales.     

Imaging the electron wave function in self-assembled quantum dots

Magnetotunneling spectroscopy is used as a noninvasive and nondestructive probe to produce two-dimensional spatial images of the probability density of an electron confined in a self-assembled semiconductor quantum dot. The technique exploits the effect of the classical Lorentz force on the motion of a tunneling electron and can be regarded as the momentum (k) space analog of scanning tunneling microscopy imaging. The images reveal the elliptical symmetry of the ground state and the characteristic lobes of the higher energy states.