The strong and distinctive excitonic interactions are among one of the most interesting aspects of the newly discovered family of two-dimensional semiconductors, monolayers of transition metal dichalcogenides (TMDC). In this dissertation, we explore two types different types of excitonic states in these materials beyond the isolated exciton in its radiative ground state. In the first part of this thesis, we examine higher-order excitonic states, involving correlations between more than a single electron and hole in the usual configuration of an exciton. In particular, we demonstrate the existence of four-body correlated or biexciton states in monolayer WSe₂. The biexciton is identified as a sharply defined state in photoluminescence spectra at high exciton density. The biexciton binding energy, i.e., the energy required to separate it into to isolated excitons, is found to be 52 meV , which is more than an order of magnitude greater than that in conventional quantum-well structures. Such high binding energy arises not only from the two-dimensional carrier confinement, but also from reduced and non-local dielectric screening. These results open the way for the creation of new correlated excitonic states linking the degenerate valleys in TMDC crystals, as well as more complex many-body states such as exciton condensates or the recently reported dropletons. In the second part of this thesis, two chapters are devoted to the identification and characterization of intrinsic lower-energy dark excitonic states in monolayer WSe₂. These optically forbidden transitions arise from the conduction band spin splitting, which was previously neglected as it only arises from higher-order spin-orbit coupling terms. First, by examining light emission using temperature-dependent photoluminescence and time-resolved photoluminescence, we indirectly probe and identify the existence of dark states that lies ~30 meV below the optically bright states. The presence of the dark state is manifest in pronounced quenching of the bright exciton emission observed at reduced temperature. To extract exact energy levels and actually utilize these dark states, as the second step, we sought direct spectroscopic identification of these states. We achieve this by applying an in-plane magnetic field, which mixes the bright and spin forbidden dark excitons. Both neutral and charged dark excitonic states have been identified in this fashion, and their energy levels are in good agreement with ab-initio calculations using GW-BSE approach. Moreover, due to the protection from their spin structure, much enhanced emission and valley lifetime were observed for these dark states. These studies directly reveal the excitonic spin manifolds in this prototypical two-dimensional semiconductor and provide a new route to control the optical and valley properties of these systems.

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Thesis (Ph. D.)--University of Washington, 2002. / Vita. Includes bibliographical references (p. 242-256).

No description available.

This thesis consists of two completely separate parts: In part I some problems related to phonons in amorphous solids are considered, whilst Part II is devoted to the study of excitons in Cuprous Oxide (Cu₂O). Part I.- A theoretical model, suitable to treat vibrations in tetrahedrally coordinated amorphous systems is developed and permits the study of a number of situations of current interest. Three of these situations are studied in detail: 1) The local response of hydrogen in amorphous silicon when a single silicon is attached to one, two or three hydrogens. The differences between these three configurations are discussed and a direct connection with experimental results is suggested. 2) The interesting case of an amorphous alloy, where both, topological and substitutional disorder are present. This is treated within the spirit of the Coherent Potential Approximation. The particular alloy chosen (Si-Ge) is readily tractable because oithe similar bond characteristics of both components, which allows the neglect of force constant changes. 3) The Raman spectrum of AX₂, glasses. The model adopted permits the investigation of the local response at the defect sites for a number of defects. In order to explain the defect lines observed in the experiments, four plausible defect configurations are considered: a missing A-X bond, a X-A double bond, an A-A bond, and a square ring (two tetrahedra sharing an edge). A simple model to calculate the Raman response in amorphous solids is also outlined. Part II.- The valence band of Cu₂0 is studied in detail to account for the deviations from the hydrogenic law of the exciton spectrum. The appearance of the two series of excitons is explained in terms of a spin-orbit splitting of the valence band in the centre of the Brillouin Zone, using a Tight-Binding Approximation. The deviations of the lowest exciton levels from their expected values are seen to arise from an admixture of the two components of the split -off valence band due to direct Coulomb and exchange interactions. The Hamiltonian used corresponds to the so called "Spherical Approximation" and the results obtained are in remarkable agreement with the experiments.

Typescript (photocopy) / 164 leaves : ill. ; 30 cm. / Title page, contents and abstract only. The complete thesis in print form is available from the University Library. / Thesis (Ph.D.)--University of Adelaide, Dept. of Physical and Inorganic Chemistry, 1982

Thesis (Ph. D.)--University of Washington, 2007. / Vita. Includes bibliographical references (p. 98-106).

Thesis (Ph. D.)--University of Canterbury, 2008. / Typescript (photocopy). Includes bibliographical references (p. 119-144). Also available via the World Wide Web.

Thesis (Ph. D.)--University of Chicago, Dept. of Chemistry, June 2000. / Includes bibliographical references. Also available on the Internet.

No description available.