Design and synthesis of biofunctional magnetic/fluorescent glyco-nanoparticles and quantum dots and their application as specific molecular imaging probes

206 p.

Fermionic quantum systems. Part I: Phase transitions in quantum dots. Part II: Nuclear matter on a lattice

In the first part I perform Hartree-Fock calculations to show that quantum dots (i.e., two-dimensional systems of up to twenty interacting electrons in an external parabolic potential) undergo a gradual transition to a spin-polarized Wigner crystal with increasing magnetic field strength. The phase diagram and ground state energies have been determined. I tried to improve the ground state of the Wigner crystal by introducing a Jastrow ansatz for the wave function and performing a variational Monte Carlo calculation. The existence of so called magic numbers was also investigated. Finally, I also calculated the heat capacity associated with the rotational degree of freedom of deformed many-body states and suggest an experimental method to detect Wigner crystals.

The second part of the thesis investigates infinite nuclear matter on a cubic lattice. The exact thermal formalism describes nucleons with a Hamiltonian that accommodates on-site and next-neighbor parts of the central, spin-exchange and isospin-exchange interaction. Using auxiliary field Monte Carlo methods, I show that energy and basic saturation properties of nuclear matter can be reproduced. A first order phase transition from an uncorrelated Fermi gas to a clustered system is observed by computing mechanical and thermodynamical quantities such as compressibility, heat capacity, entropy and grand potential. The structure of the clusters is investigated with the help two-body correlations. I compare symmetry energy and first sound velocities with literature and find reasonable agreement. I also calculate the energy of pure neutron matter and search for a similar phase transition, but the survey is restricted by the infamous Monte Carlo sign problem. Also, a regularization scheme to extract potential parameters from scattering lengths and effective ranges is investigated.

Light absorption in silicon quantum dots embedded in silica

The photon absorption in Si quantum dots (QDs) embedded in SiO2 has been systematically investigated by varying several parameters of the QD synthesis. Plasma-enhanced chemical vapor deposition (PECVD) or magnetron cosputtering (MS) have been used to deposit, upon quartz substrates, single layer, or multilayer structures of Si-rich- SiO2 (SRO) with different Si content (43-46 at. %). SRO samples have been annealed for 1 h in the 450-1250 °C range and characterized by optical absorption measurements, photoluminescence analysis, Rutherford backscattering spectrometry and x-ray Photoelectron Spectroscopy. After annealing up to 900 °C SRO films grown by MS show a higher absorption coefficient and a lower optical bandgap (∼2.0 eV) in comparison with that of PECVD samples, due to the lower density of Si-Si bonds and to the presence of nitrogen in PECVD materials. By increasing the Si content a reduction in the optical bandgap has been recorded, pointing out the role of Si-Si bonds density in the absorption process in small amorphous Si QDs. Both the photon absorption probability and energy threshold in amorphous Si QDs are higher than in bulk amorphous Si, evidencing a quantum confinement effect. For temperatures higher than 900 °C both the materials show an increase in the optical bandgap due to the amorphous-crystalline transition of the Si QDs. Fixed the SRO stoichiometry, no difference in the optical bandgap trend of multilayer or single layer structures is evidenced. These data can be profitably used to better implement Si QDs for future PV technologies. © 2009 American Institute of Physics.

Positive Correlations in Tunneling through coupled Quantum Dots

Due to the Fermi-Dirac statistics of electrons the temporal correlations of tunneling events in a double barrier setup are typically negative. Here, we investigate the shot noise behavior of a system of two capacitively coupled quantum dot states by means of a Master equation model. In an asymmetric setup positive correlations in the tunneling current can arise due to the bunching of tunneling events. The underlying mechanism will be discussed in detail in terms of the current-current correlation function and the frequency-dependent Fano factor.

Quantum dots and nanowires for optoelectronic device applications

InGaAs quantum dots (QDs) and nanowires have been grown on GaAs by metal-organic chemical vapour deposition on GaAs (100) and (111)B substrates, respectively. InGaAs QD lasers were fabricated and characterised. Results show ground-state lasing at about 1150 nm in devices with lengths greater than 2.5 mm. We also observed a strong influence of nanowire density on nanowire height specific to nanowires with high indium composition. This dependency was attributed to the large difference of diffusion length on (111)B surfaces between In and Ga reaction species, with In being the more mobile species. Selective area epitaxy for applications in quantum-dot optoelectronic device integration is also discussed in this paper. ©2006 IEEE.

Tuning photoluminescence of single InAs quantum dot by electric field

By using photoluminescence (PL) and time-resolved PL spectra, the optical properties of single InAs quantum dot (QD) embedded in the p-1-n structure have been studied under an applied electric field With the increasing of electric field, the exciton lifetime increases due to the Stark effect. We noticed that the decrease or quenching of PL intensity with increasing the electric field is mainly due to the decrease of the carriers captured by QD.

Modification of two-photon excited fluorescence from quantum dots on SiN photonic crystals

We investigate two-photon excited fluorescence from CdSe quantum dots with a center-emitting wavelength of 655 nm on SiN photonic crystals. We find that two-photon excited fluorescence is enhanced by more than 1 order of magnitude in the vertical direction when a photonic crystal is used compared to the fluorescence spectra in the absence of photonic crystals. The spectrum of two-photon excited fluorescence from quantum dots on SiN photonic crystal is observed to shift to blue compared to that from quantum dots on SiN without photonic crystals. (C) 2010 Optical Society of America

Synthesis of MDMO-PPV capped PbS quantum dots and their application to solar cells

Poly[2-methoxy-5-(3',7'-dimethyloctyloxy)-1,4-phenylenevinylene] (MDMO-PPV) capped PbS quantum dots about 3-6 nm in diameter were synthesized with a novel method. Unlike the synthesis of oleic acid capped PbS quantum dots, the reactions were carried out in solution at room temperature, with the presence of a capping ligand species, MDMO-PPV. The quantum dots were used to fabricate bulk heterojunction solar cells with an indium tin oxide (ITO)/polyethylenedioxythiophene/polystyrenesulphonate (PEDOT: PSS)/MDMO-PPV: PbS/Al structure. Current density-voltage characterization of the devices showed that after the addition of the MDMO-PPV capped PbS quantum dots to MDMO-PPV film, the performance was dramatically improved compared with pristine MDMO-PPV solar cells. (C) 2008 Elsevier Ltd. All rights reserved.

Small SiGe quantum dots obtained by excimer laser annealing

In this paper, we obtain SiGe quantum dots with the diameters and density of 15-20 nm and 1.8 x 10(11) cm(-2), respectively, by 193 nm excimer laser annealing of Si0.77Ge0.23 strained films. Under the excimer laser annealing, only surface atoms diffusion happens. From the detailed statistical information about the size and shape of the quantum dots with different annealing time, it is shown that the as-grown self-assembled quantum dots, especially the {105}-faceted dots, are not stable and disappear before the appearance of the laser-induced quantum dots. Based on the calculation of surface energy and surface chemical potential, we show that the {103}-faceted as-grown self-assembled quantum dots are more heavily strained than the {105}-faceted ones, and the heavy strain in the dot can decrease the surface energy of the dot facets. The formation of the laser-induced quantum dots, which is also with heavy strain, is attributed to kinetic constraint. (c) 2008 Elsevier B.V. All rights reserved.

First-principles study on rutile TiO2 quantum dots

The electronic structure of rutile TiO2 quantum dots (QDs) are investigated via the first-principles band structure method. We first propose a model to passivate the rutile TiO2 surfaces for the local density approximation calculations. In this model pseudohydrogen atoms are used to passivate the surface dangling bonds, which remove the localized in-cap surface states in the TiO2 QDs. As the size of the QD decreases, the band gap evolves as E-g(dot) = E-g(bulk) + 73.70/d(1.93), where E-g(dot) and d are the band gap and diameter of the QD, and E-g(bulk) is the band gap of the bulk rutile TiO2. The valence band maximum and the conduction band minimum states of the QDs are distributed mostly in the interior of the QDs, and they well inherit the atomic characteristics of those states of the bulk rutile TiO2.

Spin-dependent current noises in transport through coupled quantum dots

Current fluctuations can provide additional insight into quantum transport in mesoscopic systems. The present work is carried out for the fluctuation properties of transport through a pair of coupled quantum dots which are connected with ferromagnetic electrodes. Based on an efficient particle-number-resolved master equation approach, we are concerned with not only fluctuations of the total charge and spin currents, but also of each individual spin-dependent component. As a result of competition among the spin polarization, Coulomb interaction, and dot-dot tunnel coupling, rich behaviors are found for the self- and mutual-correlation functions of the spin-dependent currents.

Tuning of energy levels and optical properties of graphene quantum dots

We investigate theoretically the magnetic levels and optical properties of zigzag- and armchair-edged hexagonal graphene quantum dots (GQDs) utilizing the tight-binding method. A bound edge state at zero energy appears for the zigzag GQDs in the absence of a magnetic field. The magnetic levels of GQDs exhibit a Hofstadter-butterfly spectrum and approach the Landau levels of two-dimensional graphene as the magnetic field increases. The optical properties are tuned by the size, the type of the edge, and the external magnetic field.