Germanium quantum dots: Optical properties and synthesis

Three different size distributions of Ge quantum dots (>~200, 110, and 60 Å) have been synthesized via the ultrasonic mediated reduction of mixtures of chlorogermanes and organochlorogermanes (or organochlorosilanes) by a colloidal sodium/potassium alloy in heptane, followed by annealing in a sealed pressure vessel at 270 °C. The quantum dots are characterized by transmission electron microscopy, x-ray powder diffraction, x-ray photoemission, infrared spectroscopy, and Raman spectroscopy. Colloidal suspensions of these quantum dots were prepared and their extinction spectra are measured with ultraviolet/visible (UV/Vis) and near infrared (IR) spectroscopy, in the regime from 0.6 to 5 eV. The optical spectra are correlated with a Mie theory extinction calculation utilizing bulk optical constants. This leads to an assignment of three optical features to the E(1), E(0'), and E(2) direct band gap transitions. The E(0') transitions exhibit a strong size dependence. The near IR spectra of the largest dots is dominated by E(0) direct gap absorptions. For the smallest dots the near IR spectrum is dominated by the Gamma25-->L indirect transitions

Photoluminescence of tetrahedral quantum-dot quantum wells

Taking into account the tetrahedral shape of a quantum dot quantum well (QDQW) when describing excitonic states, phonon modes and the exciton-phonon interaction in the structure, we obtain within a non-adiabatic approach a quantitative interpretation of the photoluminescence spectrum of a single CdS/HgS/CdS QDQW. We find that the exciton ground state in a tetrahedral QDQW is bright, in contrast to the dark ground state for a spherical QDQW. The position of the phonon peaks in the photoluminescence spectrum is attributed to interface optical phonons. We also show that the experimental value of the Huang-Rhys parameter can be obtained only within the nonadiabatic theory of phonon-assisted transitions.Comment: 4 pages, 4 figures, E-mail addresses: [email protected], [email protected], [email protected], [email protected], to be published in Phys. Rev. Letter

Resilient Pathways to Atomic Attachment of Quantum Dot Dimers and Artificial Solids from Faceted CdSe Quantum Dot Building Blocks.

The goal of this work is to identify favored pathways for preparation of defect-resilient attached wurtzite CdX (X = S, Se, Te) nanocrystals. We seek guidelines for oriented attachment of faceted nanocrystals that are most likely to yield pairs of nanocrystals with either few or no electronic defects or electronic defects that are in and of themselves desirable and stable. Using a combination of in situ high-resolution transmission electron microscopy (HRTEM) and electronic structure calculations, we evaluate the relative merits of atomic attachment of wurtzite CdSe nanocrystals on the {11̅00} or {112̅0} family of facets. Pairwise attachment on either facet can lead to perfect interfaces, provided the nanocrystal facets are perfectly flat and the angles between the nanocrystals can adjust during the assembly. Considering defective attachment, we observe for {11̅00} facet attachment that only one type of edge dislocation forms, creating deep hole traps. For {112̅0} facet attachment, we observe that four distinct types of extended defects form, some of which lead to deep hole traps whereas others only to shallow hole traps. HRTEM movies of the dislocation dynamics show that dislocations at {11̅00} interfaces can be removed, albeit slowly. Whereas only some extended defects at {112̅0} interfaces could be removed, others were trapped at the interface. Based on these insights, we identify the most resilient pathways to atomic attachment of pairs of wurtzite CdX nanocrystals and consider how these insights can translate to the creation of electronically useful materials from quantum dots with other crystal structures

Detection of topological transitions by transport through molecules and nanodevices

We analyze the phase transitions of an interacting electronic system weakly coupled to free-electron leads by considering its zero-bias conductance. This is expressed in terms of two effective impurity models for the cases with and without spin degeneracy. We demonstrate using the half-filled ionic Hubbard ring that the weight of the first conductance peak as a function of external flux or of the difference in gate voltages between even and odd sites allows one to identify the topological charge transition between a correlated insulator and a band insulator.Comment: 4 pages, 5 figures, to appear in Phys. Rev. Let

Faraday Rotation Spectroscopy of Quantum-Dot Quantum Wells

Time-resolved Faraday rotation studies of CdS/CdSe/CdS quantum-dot quantum wells have recently shown that the Faraday rotation angle exhibits several well-defined resonances as a function of probe energy close to the absorption edge. Here, we calculate the Faraday rotation angle from the eigenstates of the quantum-dot quantum well obtained with k.p theory. We show that the large number of narrow resonances with comparable spectral weight observed in experiment is not reproduced by the level scheme of a quantum-dot quantum well with perfect spherical symmetry. A simple model for broken spherical symmetry yields results in better qualitative agreement with experiment.Comment: 9 pages, 4 figure

Photothermal heterodyne imaging of individual nonfluorescent nanoclusters and nanocrystals

We introduce a new, highly sensitive, and simple heterodyne optical method for imaging individual nonfluorescent nanoclusters and nanocrystals. A 2 order of magnitude improvement of the signal is achieved compared to previous methods. This allows for the unprecedented detection of individual small absorptive objects such as metallic clusters (of 67 atoms) or nonluminescent semiconductor nanocrystals. The measured signals are in agreement with a calculation based on the scattering field theory from a photothermal-induced modulated index of refraction profile around the nanoparticle

Gel Electrophoresis of Gold-DNA Nanoconjugates

Gold-DNA conjugates were investigated in detail by a comprehensive gel electrophoresis study based on 1200 gels. A controlled number of single-stranded DNA of different length was attached specifically via thiol-Au bonds to phosphine-stabilized colloidal gold nanoparticles. Alternatively, the surface of the gold particles was saturated with single stranded DNA of different length either specifically via thiol-Au bonds or by nonspecific adsorption. From the experimentally determined electrophoretic mobilities, estimates for the effective diameters of the gold-DNA conjugates were derived by applying two different data treatment approaches. The first method is based on making a calibration curve for the relation between effective diameters and mobilities with gold nanoparticles of known diameter. The second method is based on Ferguson analysis which uses gold nanoparticles of known diameter as reference database. Our study shows that effective diameters derived from gel electrophoresis measurements are affected with a high error bar as the determined values strongly depend on the method of evaluation, though relative changes in size upon binding of molecules can be detected with high precision. Furthermore, in this study, the specific attachment of DNA via gold-thiol bonds to Au nanoparticles is compared to nonspecific adsorption of DNA. Also, the maximum number of DNA molecules that can be bound per particle was determined

A scalable optical detection scheme for matter wave interferometry

Imaging of surface adsorbed molecules is investigated as a novel detection method for matter wave interferometry with fluorescent particles. Mechanically magnified fluorescence imaging turns out to be an excellent tool for recording quantum interference patterns. It has a good sensitivity and yields patterns of high visibility. The spatial resolution of this technique is only determined by the Talbot gratings and can exceed the optical resolution limit by an order of magnitude. A unique advantage of this approach is its scalability: for certain classes of nano-sized objects, the detection sensitivity will even increase significantly with increasing size of the particle.Comment: 10 pages, 4 figure

An accurate description of quantum size effects in InP nanocrystallites over a wide range of sizes

We obtain an effective parametrization of the bulk electronic structure of InP within the Tight Binding scheme. Using these parameters, we calculate the electronic structure of InP clusters with the size ranging upto 7.5 nm. The calculated variations in the electronic structure as a function of the cluster size is found to be in excellent agreement with experimental results over the entire range of sizes, establishing the effectiveness and transferability of the obtained parameter strengths.Comment: 9 pages, 3 figures, pdf file available at http://sscu.iisc.ernet.in/~sampan/publications.htm