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Structure and optical properties of natural low dimensional, semiconducting, organic inorganic hybridsBlack, Robert Shewan 06 February 2013 (has links)
The aim of investigating the 2D PbX6 inorganic organic hybrids was to study octahedral distortions, short interlayer spacing’s, and the effect of functionalized aliphatic’s terminal halogen on idealizing or destabilizing the octahedral arrangements and their effect on the band gap of the single layer 2D hybrid systems. It was found that the PbX6 metal centred distortions do display some impact on the band gap, the greater the distortion experienced in the Ieq-Pb-Ieq cis bond angles, the wider the band gap, as we suspect a decrease in I 5p antibonding character which lowers the top of the valence band. The terminal halogen interaction specifically in (BrC2)PbI4, clearly displayed some Br 4p/s character at the bottom of the conduction band, which may further explain the reduction of the band gap of this compound. This in conjunction with the shorter interlayer spacing serve to stabilize more idealized bridging angles, as seen in both the lead iodide and bromide analogues. In the short interlayer spacing compounds large idealizations of the Pb-X-Pb bridging angles are observed however display a large metal centred octahedral distortions in order accommodate the spatial occupation of the lone pair on lead.
It was generally observed that the lead bromide hybrids appear to have a greater sensitivity to exciton lattice interactions, which give rise to red shifted emissions and absorptions with decreasing temperature. Structurally this behaviour is counterintuitive; because the structures increase in inorganic distortions with decreasing temperature and therefore a blue shift in the exciton absorption is expected. It should be noted that compounds displaying this phenomenon most, (C4, C6, C7)PbBr4 do display a large amount of structural disorder in their lower temperature phases.
In the 1D systems investigated further structure to property correlations were made. Optically it was found that unlike the corner-shared perovskite type 1D wires of [NH2C(I)=NH2]3PbI5 and [CH3SC(=NH2)NH2]3PbI5 the first exciton absorption of the octahedral face sharing wires of (A)PbI3 appear to be largely insensitive to the inorganic structural distortions experienced as a result of the low temperature phase transitions. In one instance however a low temperature phase transition did result in a polaron emission which was directly related to a discontinuity in the inorganic wires. More generally experimental links between the STE luminescence emissions and the inter-wire spacing, organic dielectric constant, and the density of the crystal, were shown to influence the STE lattice interactions to a greater degree. This effect is increased through a decrease in crystal density and organic dielectric constant, with an associated increase in the inter-wire spacing. Therefore as the exciton lattice interactions increase, a red shift in the STE emissions is observed.
In another series of systems strong 1- and interactions were present in particularly two 1D charge transfer compounds. It was noted that the inorganic wires promote interactions between the organic templates as has also been established in literature. Structurally it was also observed that the CT transitions of these compounds begin to largely coincide with the STE emission arising from the inorganic wire. Even though the CT compounds structurally have strong interactions the current experiments do not ascertain to what degree this interaction assists in electron transport. It was also established that as intermolecular interactions are absent in previously published MV and Et compounds with the dominant CT interaction was the I…N interaction which functions over a large range (4.9A). This long distance is substantiated from the strong covalent character of the I…N interaction observed in IR experiments completed on (MV)Pb2I6. It was also observed in our compounds that the position of the LUMO of the organic cation relative to the valence band of the inorganic wires appears to be largely dependent on the N…I distance and largely independent of the electron accepting templates HOMO-LUMO gap.
The increased wire thickness observed in these compounds does appear to display a pronounced effect on the PL emissions as seen in three chain wide wires produced. The thicker chains begin to allow higher energy emission’s to occur i.e. the desired first exciton emission begins to become favored due to the relaxing of the wires spatial confinement on the electron-hole’s orbit. Further investigations are needed into even thicker chain wires, in order to ascertain the ideal size of the wire to obtain the desired high energy first exciton emission. To date the wire thickness that does give rise to the first exciton emission appears to still need at least six coordinated PbI6 octahedral units.
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Electronic properties of low dimensional carbon materialsSanders, Kirsty Gail January 2016 (has links)
A Dissertation submitted to the Faculty of Science, University of the Witwatersrand,
Johannesburg, in ful lment of the requirements for the degree of Master of Science. Johannesburg 2016. / Low dimensional carbon systems are of immense interest in condensed matter physics
due to their exceptional and often startling electric and magnetic properties. In this
dissertation we consider two of these materials - graphene and nanocrystalline diamond.
The effect of synthesis parameters on the quality of graphene is examined and
it is found that controlling the partial pressure of the synthesis gases plays a critical
role in determining the quality of the sample. Superconductivity in Boron doped
nanocrystalline diamond (B-NCD) is considered and weak localisation along with a
Berezinsky-Kosterlitz-Thouless (BKT) transition is identified in the samples. Furthermore
we explore theoretically the problem of electric transport through a double quantum
dot system coupled to a nanomechanical resonator. We find resonant tunnelling
when the difference between the energy levels of the dots equals an integer multiple of
the resonator frequency, and that while initially increasing the electron phonon coupling
(g) increases the current through the sample further increase in g inhibits electric
transport through the quantum dots. / LG2017
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Study of interface plasmon in low-dimensional silicon nanostructures. / 低維硅納米結構表界面等離激元之研究 / CUHK electronic theses & dissertations collection / Study of interface plasmon in low-dimensional silicon nanostructures. / Di wei gui na mi jie gou biao jie mian deng li ji yuan zhi yan jiuJanuary 2010 (has links)
In this thesis study, the surface/interface plasmon excitations in different Si nanostructures were revealed through the EELS study in TEM/STEM. In the case of the planar boundary such as the wedge-like specimen, the spatially resolved EELS results disclose the dependence of the intensity and the position of the interface plasmon peak on the sample thickness. In the case of the Si-core/ SiO2-shell nanoparticles, we found that the SP/IP peak will firstly red-shifts with the increase of the SiO2 shell thickness and eventually levels off . As the aspect ratio of the Si nanoparticles increases, (from spherical particle to nanorod and nanowire), the SP/IP will split into two branches: transverse and longitudinal modes. We also found the intensity ratio of the transverse/longitudinal mode excitations depends on the diameter of the Si core size in the nanostructures. In the one-dimensional interacting Si nanoparticle chains, the Si nanoparticles were embedded in the SiO 2 shell, the splitting of the SP excitation into transverse and longitudinal modes was also observed. As the inter-particle distance reduces to several nanometers, the coupling of the IP excitation between the adjacent particles becomes significant, and results in the local field enhancement in-between the two particles. This is directly visualized using EFTEM imaging in TEM/STEM. / Surface/interface plasmons (SP/IP) are the plasmons confined at specific boundaries, describing the surface/interface charge density oscillation. They are generated when the scattered electromagnetic wave with its scattering vector component parallel to the boundary propagates along the surface/interface. Study of surface plasmon resonance in noble metals such as gold and silver nanoparticles have started decades ago, and recent interests are focused on the plasmonic properties of individual nanoparticles, as enabled by the size/shape control in the nanostructure growth and advances made in the characterization methodologies. Besides the noble metals, semiconductor such as silicon also attracts much attention for its plasmonic behavior. The surface/interface plasmon resonance frequency of Si-based nanostructures occurs at relatively higher energies (compared to Au and Ag), making it a perfect system to be studied using electron energy loss spectroscopy (EELS) based techniques. When performed in a scanning transmission electron microscope (STEM), such a technique enjoys excellent spatial resolution, and can map the local plasmonic properties of individual nanostructures. / The plasmon excitation depends sensitively on not only the material dielectric properties but also the geometrical configurations of the material. In the present thesis work, silicon-based nanostructures with planar, spherical, and cylindrical boundaries were investigated using both experimental and theoretical approaches, with focus on the plasmon oscillation originating from the Si/SiO 2 interface. The specimens employed include silicon/silica thin films, Si-core/SiO2-shell nanoparticles with different aspect ratios and spherical-shaped nanoparticle chains, as well as Si-core/SiO2-shell nanocables. / Wang, Xiaojing = 低維硅納米結構表界面等離激元之研究 / 王笑靜. / Adviser: Li Quan. / Source: Dissertation Abstracts International, Volume: 73-01, Section: B, page: . / Thesis (Ph.D.)--Chinese University of Hong Kong, 2010. / Includes bibliographical references (leaves 118-122). / Electronic reproduction. Hong Kong : Chinese University of Hong Kong, [2012] System requirements: Adobe Acrobat Reader. Available via World Wide Web. / Electronic reproduction. [Ann Arbor, MI] : ProQuest Information and Learning, [201-] System requirements: Adobe Acrobat Reader. Available via World Wide Web. / Abstract also in Chinese. / Wang, Xiaojing = Di wei gui na mi jie gou biao jie mian deng li ji yuan zhi yan jiu / Wang Xiaojing.
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Optical Spectroscopy of Two-Dimensional Superatomic Semiconductors and Magnetic MaterialsLee, Kihong January 2019 (has links)
Since the first discovery of atomically thin sheets of carbon, two-dimensional (2D) materials have captured the interest from scientific community to expand the understanding in fundamental physics and chemistry at low dimensional systems. With extraordinary phenomena only possible at atomically thin limits, there has been high demand to reveal new and unique 2D materials and manipulate their structures and properties. Structural tunability of superatomic solids motivates us to control dimentionality of the materials and construct layered structures which could be exfoliated to 2D materials. The layered crystal [Co6Se8(PEt2phen)6][C60]5 can be used as a template to create a 2D C60-based material with an optical gap in mid-infrared. Re6Se8Cl2 and Mo6S3Br6, are presented as the first examples of covalently linked 2D superatomic solids built from nanoscale building blocks with hierarchical structures and semiconducting properties. We further demonstrate the emergence of hierarchical coherent phonons in a 2D superatomic semiconductor Re6Se8Cl2. Lastly, we explore complex magnetic phases in 2D ferromagnetic semiconductor CrSBr using second harmonic generation and Raman spectroscopy. 2D superatomic semiconductors and 2D magnetic materials provide additional sets of design principles to manipulate structural, electronic, phononic, and magnetic properties at the atomically thin limits. These materials hold promises as model systems to study fundamental physical principles as well as platform for applications with phonon engineering and magnetic optoelectronic devices.
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Electron-phonon interactions in low dimensional structuresLeadley, David Romwald January 1989 (has links)
Transport properties of the two-dimensional electron gas (2DEG) in high magnetic fields are used to investigate scattering processes affecting the resistivity of GaAs-GaAlAs and GaInAs-InP heterojunctions and quantum wells: especially coupling of electrons to acoustic and optic phonons; and transitions between electric subbands. The experiments fall into two groups: A systematic study of magnetophonon resonance (MPR) between 30K and 300K. Resonance positions indicate a coupling substantially below the LO phonon energy, expected from 3D measurements. GaAs-GaAlAs hetero junctions show amplitudes varying smoothly with electron density (n<sub>s</sub>) and closely related to the 4K mobility. On rotation in magnetic field they decrease rapidly as the resonance position returns to the LO value. In modulation doped structures the damping factor is determined by remote impurity scattering. As n<sub>s</sub> is increased in GaInAs-InP the coupling frequency decreases dramatically from the GaAs-like LO at 272cm<sup>-1</sup> to the InAs-like TO at 226cm<sup>-1</sup>. At higher electric fields the 'normal' MPR maxima invert, starting at low magnetic fields, to form 'hot electron' MPR minima, with maximum amplitude at ~60K. This is the first direct observation of HEMPR in 2D and is explained in a diffusion picture. At lower electric fields, additional resonances are identified with resonant cooling by inter-subband scattering. Comparisons are made with calculations and explanations sought including consideration of interface phonons; coupled plasmon-phonon modes; and shifts of the resonance positions due to the shape of the density of states. Low temperature magnetoresistance measurements in GaAs-GaAlAs heterojunctions with more than one occupied electric subband. Shubnikov-de Haas oscillations in perpendicular magnetic fields contain non-additive terms at electron temperatures > 2K where acoustic phonon mediated inter-subband scattering is comparable to intra-subband scattering. Subband separations and greatly enhanced g-factors [largest for electrons in the upper subband ] are deduced from the oscillations. Damping of the oscillations in field, gives values for quantum lifetimes (τ<sub>s</sub>), much smaller than τ<sub>tʼ</sub>, deduced from mobility. With two subbands occupied τ<sub>s</sub> is always largest for the upper subband, while relative sizes of τ<sub>t</sub> depend on sample quality. Study of electron energy loss rates, from thermal damping of the oscillations, shows enhancement in the region kT<sub>e</sub> ~ ħω<sub>cʼ</sub>, which is evidence for cyclotron phonon emission. Depopulating subbands in parallel fields causes the resistance to drop, by up to 60%, due to suppression of inter-subband scattering. Systematic studies show this scattering rate is independent of n<sub>s</sub>.
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Phase slip fluctuations in low-dimensional superconductors : a numerical study using the string method /Qiu, Chunyin. January 2009 (has links)
Thesis (Ph.D.)--Hong Kong University of Science and Technology, 2009. / Includes bibliographical references (p. 100-107).
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Novel properties of interacting particles in small low-dimensional systemsRomanovsky, Igor Alexandrovich. January 2006 (has links)
Thesis (Ph. D.)--Physics, Georgia Institute of Technology, 2007. / Landman, Uzi, Committee Member ; Yannouleas, Constantine, Committee Member ; Bunimovich, Leonid, Committee Member ; Chou, Mei-Yin, Committee Member ; Pustilnik, Michael, Committee Member.
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Properties of low-dimensional systemsLapilli, Cintia Mariela, January 2006 (has links)
Thesis (Ph. D.)--University of Missouri-Columbia, 2006. / The entire dissertation/thesis text is included in the research.pdf file; the official abstract appears in the short.pdf file (which also appears in the research.pdf); a non-technical general description, or public abstract, appears in the public.pdf file. Title from title screen of research.pdf file viewed on (May 2, 2007) Vita. Includes bibliographical references.
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Interaction of Plasmons and Excitons for Low-Dimension SemiconductorsLin, Jie (physicist) 12 1900 (has links)
The effects of surface plasmon for InGaN/GaN multi-quantum wells and ZnO nanoparticles optical linear and nonlinear emission efficiency had been experimentally studied. Due to the critical design for InGaN MQWs with inverted hexagonal pits based on GaN, both contribution of surface plasmon effect and image charge effect at resonant and off resonant frequencies were experimentally and theoretically investigated. With off- resonant condition, the InGaN MQWs emission significantly enhanced by metal nanoparticles. This enhancement was caused by the image charge effect, due to the accumulation of carriers to NPs region. When InGaN emission resonated with metal particles SP modes, surface Plasmon effect dominated the emission process. We also studied the surface plasmon effect for ZnO nanoparticles nonlinear optical processes, SHG and TPE. Defect level emission had more contribution at high incident intensity. Emissions are different for pumping deep into the bulk and near surface. A new assumption to increase the TPE efficiency was studied. We thought by using Au nanorods localized surface plasmon mode to couple the ZnO virtual state, the virtual state’s life time would be longer and experimentally lead the emission enhancement. We studied the TPE phenomena at high and near band gap energy. Both emission intensity and decay time results support our assumption. Theoretically, the carriers dynamic mechanism need further studies.
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Novel properties of interacting particles in small low-dimensional systems.Romanovsky, Igor Alexandrovich 11 July 2006 (has links)
This work is about the properties of several low dimensional, small systems of interacting particles. We demonstrate that interaction between particles in the low dimensional small systems can lead to many unexpected effects. We considered electrons in a Luttinger liquid, in a superconducting state, and atoms in a magneto-optical trap. Using bosonization techniques we calculated the thermopower of a Luttinger liquid wire with an impurity. We predicted the appearance of a phase dependent force and resonant phase dependent magnetization in the nanoscopic superconductor - normal metal superconductor (or superconductor - two dimensional electron gas - superconductor) junction. We also considered plasma oscillations inside thin superconducting tubes and rings and predicted that the velocities of the plasmons in these systems are periodic functions of the magnetic flux. By considering neutral atoms in a harmonic trap we discovered that strongly repelling atoms do not form Bose-Einstein condensate at zero temperature but tend to occupy different orbitals with small mutual overlap, forming crystallite structures similar to Wigner molecules of electrons inside a quantum dot.
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