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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
1

Free-Electron Laser and Synchrotron Spectroscopy of Fundamental Excitations in Ytterbium-Doped Fluoride Lattices

Hughes-Currie, Rosa January 2015 (has links)
The spectroscopy of wide-bandgap fluoride materials doped with divalent ytterbium is presented. The structure of impurity-trapped excitons is explored, vacuum ultraviolet excitation is used to investigate the transfer processes between excitations, and the effect of confinement on self-trapped excitons is studied. The excited-state structure of impurity-trapped excitons is measured in the multisite system NaMgF₃:Yb²⁺. A two-colour ultraviolet-infrared pulsed photoluminescence enhancement technique is employed to probe the interlevel transitions and dynamics of impurity-trapped excitons in doped insulating phosphor materials. NaMgF₃:Yb²⁺ exhibits emission from two charge-compensation centres with peaks at 22 300 cm⁻¹ (448 nm) and 24 000 cm⁻¹ (417 nm). The observed photoluminescence enhancement is caused by a combination of intra-excitonic excitation and electron trap liberation. The electron traps are inferred to have a depth of approximately 800 cm⁻¹. Time-resolved VUV spectroscopic studies of emission and excitation spectra of CaF₂:Yb, NaMgF₃Yb and MgF₂:Yb are presented to investigate excitation and relaxation mechanisms of both impurity-trapped excitons and intrinsic excitons in each fluoride host. Host-to-impurity energy transfer mechanisms leading to formation of impurity-trapped excitons are discussed. The 4f¹⁴ → 4f¹³5d CaF₂:Yb²⁺ absorption bands are successfully modeled with a semi-empirical effective Hamiltonian calculation for NaMgF₃:Yb²⁺ and MgF₂:Yb²⁺. The excitation and emission spectra of all studied materials are compared. Results on VUV spectroscopy of 3 and 5 monolayer CdF₂–CaF₂ superlattices show the change in optical behaviour of the self-trapped exciton in CdF₂ when it is confined and give an indication of the radius of the exciton. The decay of the emission is modeled with three components, corresponding to three self-trapped exciton states. Results on the VUV spectroscopy of CdF₂–CaF₂ superlattices show that the confinement effect seems to equally influence the energy of excitonic and bandgap absorption in 3 and 5 monolayer superlattices. At the same time, as the self-trapped exciton is more confined, the emission is blue-shifted by 1600 cm⁻¹ indicating that the effective excitonic radius is about three monolayers.

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