acase@tulane.edu / 1 / Fang Sun

Graduation date: 1997

This dissertation presents a serial study on optical properties of different semiconductor materials. Three main types of studies are addressed: The role of doping levels of N and Al atoms in the room-temperature photoluminescence (PL) of 4H-SiC films for optoelectronic applications; the use of a basic Monte Carlo method combined with probability calculations of the time-dependent Schroedinger equation to manifest multi-photon absorption and emission of II-VI compound quantum dots (QDs) for bioimaging; a theoretical quantum chemistry approach to study of structure and optical properties of InGaAsN and GaAs clusters for laser technology applications. 4H-SiC films were grown on AlN/SiC(100) substrates by a chemical vapour deposition (CVD) system. Three well-defined room-temperature PL peaks close to the band-gap energy were observed. By a detailed theoretical analysis of optical transitions in the samples, it was found that the PL peaks are most probably due to the optical transitions between impurity levels and band edges, and the transition between the second minimum of the conduction band and the top of the valance band. Special attention has been paid to effects of doping levels of N and Al impurities. Optical transitions in several II-VI semiconductor QDs have been studied by a quantum Monte Carlo method. We model the QD energy band structure by a spherical square quantum well and the electrons in the conduction band and holes in the valence band by the effective mass approximation. The optical probabilities of optical transitions induced by ultrafast and ultraintense laser pulses are calculated from the time-dependent Schroedinger equation. With the inclusion of the nonradiative electron-phonon processes, the calculated absorption and emission spectra are in agreement with experimental work. The dynamic processes and up-conversion luminescence of the QDs, required for many applications including bio-imaging, are demonstrated. Quantum chemistry is used to study InGaAsN and GaAs nano systems. The molecular structures of a series of dilute-nitride zinc blende InGaNAs clusters are examined from the energy point of view with a semi-empirical method. The optimum cluster configurations are identified by which we can identify the detailed bonding structures and the effects of In mole fraction. After proper geometry construction, an effective central insertion scheme has been implemented to study the electronic band structures of GaAs at the first-principles level. The formation of energy bands and quantum confinement effects have been revealed, thus providing theoretical support for laser design. / QC 20100730

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Within the family of transition metal oxochlorides/bromides containing lone pair elements, the transition metal cations often adopt a low-dimensional arrangement such as 2D layers, 1D chains or 0D clusters. The reduced dimensionality is attributed to the presence of stereochemically active lone pairs which are positioned in the non-bonding orbital and will not participate in bond formation and instead act as structural spacers that help to separate coordination polyhedra around transition metal cations from forming three dimensional networks. On the other hand, the chlorine and bromine ions also play an important role to open up the crystal structure because of their low coordination number. However, fluorine has been rarely used in this concept due to the difficulties in synthesis. This thesis is focused on finding new compounds in the M-L-O-F system (M = transition metal cation, L= p-block lone pair elements such as Te4+, Se4+, or Sb3+) in order to study the structural character of fluorine. Hydrothermal reactions have been adopted instead of conventional chemical transport reactions that are commonly used for synthesizing compounds in the M-L-O-(Cl, Br) family. A total of 8 new transition metal oxofluorides containing lone pair elements have been synthesized and their structures have been determined via single crystal X-ray diffraction. Bond valence sum calculations are used to distinguish in between fluorine and oxygen due to their very similar X-ray scattering factors. / <p>At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 4: Manuscript. Paper 5: Manuscript.</p>

<p> Low dimensional quantum magnets which display a collective singlet ground state and a gap in their magnetic excitation spectrum provide a framework for much exotic phase behavior in new materials, with high temperature superconductivity being the best appreciated example. Neutron scattering techniques can be applied to study a wide variety of problems in condensed matter physics. These techniques are particularly useful as applied to understanding the magnetic properties of quantum magnets that display exotic phases.</p> <p> SrCu2(BO3)2, is a rare example of a two-dimensional quantum magnet for which an exact theoretical solution describing its ground state is known to be a collective singlet. Previous high resolution neutron scattering measurements identified the most prominent features of the spin excitation spectrum in SrCu2(BO3)2, including the presence of one and two triplet excitations and weak dispersion characteristic of subleading terms in the spin Hamiltonian.</p> <p> The resemblance between the spin gap behavior in the Mott insulator SrCu2(BO3)2 and that associated with high temperature superconductors motivated the consideration of the significance of doping in order to understand the properties of this quantum magnetic system. For this reason, a series of neutron scattering studies on doped SrCu2(BO3)2 were initiated.</p> <p> These series of investigations began with the performance of neutron scattering measurements on a SrCu(2-x)Mgx(BO3)2 single crystal in order to introduce magnetic vacancies to the system. These results revealed the presence of new spin excitations within the singlet-triplet gap of this system. Application of a magnetic field induces Zeeman-split states associated with un-paired spins which exist as a consequence of doping with quenched non-magnetic impurities. Additional substantial broadening of both the one and two triplet excitations is observed in the doped system as compared to the pure system. Theoretical calculations are shown to qualitatively account for these features.</p> <p> These studies were extended to neutron scattering measurements on Sr(1-x)LaxCu2(BO3)2, with an aim of introducing charged carriers into this system. The broadening of the one and two triplet excitations is observed and compared to the thermally induced finite lifetime of the pure system. The temperature dependence of this broadening in Sr(1-x)LaxCu2(BO3)2 is different compared to that observed in both SrCu2(BO3)2 and SrCu(2-x)Mgx(BO3)2.</p> <p> It has also been suggested that there is a relation between the spin-lattice interaction in SrCu2(BO3)2 and the magnetic dynamics at low temperatures and high magnetic fields. For this reason there has been increased interest in the study of the crystalline structure and vibrational modes of SrCu2(BO3)2. In order to investigate the role of the lattice in the formation of the singlet ground state in SrCu2(BO3)2, a series of low and high energy neutron scattering measurements were carried out on this system to study both the crystalline structure as well as the normal modes of vibration of the lattice, the transverse acoustic and optical phonons. Transverse acoustic phonons with energies comparable to and higher than the onset of the two triplet continuum show substantially increased lifetimes on entering the singlet ground state below ~ 10 K. This may indicate the removal of the decay channel for the phonons due to the gapping of the spin excitation spectrum in SrCu2(BO3)2 at low temperatures. In high energy inelastic neutron scattering we observe broadening of optic phonons in the ~ 52 to 65 meV region on entering the low temperature singlet ground state.</p> <p> Additionally, the magnetic properties of CuMoO4, which is a triclinic quantum magnet system based on S=1/2 moments at the Cu2+ site, were studied using elastic and inelastic neutron scattering experiments. This material exhibits a first order structural phase transition at ~ 190 K as well as a magnetic phase transition at ~ 1.75 K. We were primarily interested in the low temperature magnetic properties of this material. Magnetization and heat capacity measurements as well as elastic and inelastic neutron scattering measurements were conducted on this system within the low temperature ordered phase. These studies confirm that this material has a magnetic phase transition at ~ 1.7 K. Neutron scattering results indicate that this magnetically ordered phase is characterized by a doubling of the a axis. Inelastic neutron scattering measurements revealed a gapped magnetic excitation spectrum in zero magnetic field, which could be filled in by the application of magnetic fields approaching 7 T.</p> / Thesis / Doctor of Philosophy (PhD)

Thesis advisor: Joshua E. Greene / We study ribbon cobordisms between 3-manifolds, i.e. rational homology cobordisms that admit a handle decomposition without 3-handles. We first define and study the more general notion of quasi-ribbon cobordisms, and analyze how lattice-theoretic methods may be used to obstruct the existence of a quasi-ribbon cobordism between two given 3-manifolds. Building on this and on previous work of Lisca, we then determine when there exists such a cobordism between two connected sums of lens spaces. In particular, we show that if an oriented rational homology sphere Y admitsa quasi-ribbon cobordism to a lens space, then Y must be homeomorphic to L(n, 1), up to orientation-reversal. As an application, we classify ribbon χ-concordances between connected sums of 2-bridge links. Lastly, we show that the notion of ribbon rational homology cobordisms yields a partial order on the set consisting of aspherical 3-manifolds and lens spaces, thus providing evidence towards a conjecture formulated by Daemi, Lidman, Vela-Vick and Wong. / Thesis (PhD) — Boston College, 2022. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Mathematics.

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Photocatalysis is a process to convert light energy into chemical energies. This advanced process has been extensively applied in different areas, such as water splitting to evolve hydrogen, organic/ inorganic pollutants decomposition, artificial photosynthesis (CO2 reduction), disinfection, heavy metal recovery, organic synthesis and nitrogen fixation (reduction). The difficulty for photocatalysis applied in practical is primarily due to the low quantum yield as for the high recombination of photogenerated charge carriers. Various strategies have been implemented to overcome these challenges. As recently developed advanced materials, two dimensional materials have attracted lots of attentions as for their superiorities such as large specific surface area and high conductivity. These advantages for two dimensional materials make them be promising cocatalysts in enhance catalytic activity. In this thesis, various two dimensional materials (such as MoS2, SnS, BN as well as C3N4) other than graphene were prepared and investigated in the promotion of photocatalytic activity. Specifically, the focus of present work is on two dimensional materials enhanced photocatalysis in environmental remediation, including organic pollutants detoxification as well as bacteria inactivation. It was found that two dimensional materials, including MoS2, SnS, BN, may be excellent candidates as cocatalysts to enhanced visible-light-driven photocatalytic activity. And g-C3N4 as an effective photocatalyst exhibited excellent photocatalytic oxidation activity, and its activity can be further enhanced with surface modification by hydroxyl functional groups (a modification method reported in the thesis). Suggestions for future work were also proposed in this thesis.