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AbstractAbstract
[en] The material system of choice for the investigations performed in the frame of this Thesis were self-assembled CdSe/ZnSe QDs. The reason for this choice is twofold. First, CdSe/ZnSe QDs can be grown with excellent optical quality, which is a prerequiste for optical studies. Second, due to the polar nature of II-VI compound semiconductors, optical anisotropies induced by various asymmetries are more pronounced than in their IIIV or element IV counterparts. Unlike in the III-V materials, where the self-organization of QDs is well described by the Stranski-Krastanow growth mode, the peculiarities of the QD formation are not entirely clear in II-VI alloys. For the purposes of the current work QDs emerging from two variants of Molecular Beam Epitaxy (MBE) growth were studied. In order to establish a clear connection between the optically observed anisotropies and the growth induced asymmetries in the QDs we start out by summarizing all available structural and morphological studies that were performed on the resultant QDs, including x-ray diffraction, atomic force microscopy, high resolution transmission electron microscopy and resonant Raman scattering. Extensive investigations by Photoluminescence (PL) and Photoluminescence Excitation (PLE) spectroscopy hence detail the resultant electronic structure of excitons confined to the above QDs as well as their energy relaxation across the latter. We find that for these small-sized strongly confining QDs k-vector conservation is entirely relaxed, which enables interaction of the excitons with a continuum of phonons and explains fast and efficient exciton capture by the QDs, even for excitation conditions far above the ground state. We demonstrate how this provides an alternative fast relaxation channel to Auger-like electron-hole scattering, that may also explain fast hole relaxation and adds to the understanding of the absence of a phonon bottleneck in the energy relaxation in these type of QDs. With the above analysis as a backbone we turn to the investigation of the optical anisotropy of the radiative recombination of excitons confined to CdSe/ZnSe QDs. This is done by angle-dependent polarization-resolved PL. We demonstrate experimentally that the electron-hole exchange interaction in asymmetric QDs gives rise to an effective conversion of the optical polarization from linear to circular and vice versa. The experiment is succesfully modeled in the frame of an exciton pseudospin-formalism that is based on the exchange induced finestructure splitting of the radiative excitonic states and unambiguously proves that the observed polarization conversion is the continuous-wave equivalent to quantum beats between the exchange split states in the time domain. These results indicate that QDs may offer extended functionality beyond non-classical light sources in highly integrated all-optical device schemes, such as polarization converters or modulators. In a further extension we apply the exciton pseudospin-formalism to optical alignment studies and demonstrate how these can be used to directly measure the otherwise hidden symmetry distribution over an ensemble of QDs. This kind of measurement may be used on future optical studies in order to link optical data more directly to structural investigations, as it yields valuable information on capped QDs that cannot be looked at directly by topological methods. In the last part of this work we study the influence of an in-plane magnetic field on the optical anisotropy. We find that the optical axis of the linear polarization component of the photoluminescence signal either rotates in the opposite direction to that of the magnetic field or remains fixed to a given crystalline direction. A qualitative theoretical analysis based on the exciton pseudospin Hamiltonian unambiguously demonstrates that these effects are induced by isotropic and anisotropic contributions to the heavy-hole Zeeman term, respectively. The latter is shown to be compensated by a built-in uniaxial anisotropy in a magnetic field BC=0.4 T, resulting in an optical response that would be expected for highly symmetric QDs. For a comprehensive quantitative analysis the full heavy-hole exciton k.p-Hamiltonian is numerically calculated and the resulting optical polarization is modeled. The model is able to quantitatively describe all experimental results using a single set of parameters. From this model it is explicitly seen that a optical response characteristic for high symmetry QDs may be obtained from an ensemble of asymmetric QDs without a crossing of the zero-field bright exciton states, which was required for application of QDs in non-classical light sources. It is clearly demonstrated that any scheme using in-plane magnetic fields to symmetrize the optical response has to take into account at least four optically active states instead of the two observed in the absence of magnetic fields. These findings may explain some of the major disagreement on recent entanglement studies in asymmetric QDs [Ste06b, Lin06, Gil07], as models that do not take the above result into account cannot be a priori expected to provide reliable results on excitonic Bell states. (orig.)
Secondary Subject
Source
29 Oct 2009; 144 p; Diss. (Dr.rer.nat.)
Record Type
Miscellaneous
Literature Type
Thesis/Dissertation
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ABSORPTION SPECTRA, ALIGNMENT, ANISOTROPY, CADMIUM SELENIDES, ELECTRONIC STRUCTURE, EXCITED STATES, EXCITONS, FINE STRUCTURE, HAMILTONIANS, MAGNETIC FIELDS, MAGNETO-OPTICAL EFFECTS, MOLECULAR BEAM EPITAXY, OPTICAL PROPERTIES, PHOTOLUMINESCENCE, POLARIZATION, QUANTUM DOTS, RECOMBINATION, RESPONSE FUNCTIONS, SEMICONDUCTOR MATERIALS, SPIN ORIENTATION, ZEEMAN EFFECT, ZINC SELENIDES
CADMIUM COMPOUNDS, CHALCOGENIDES, CRYSTAL GROWTH METHODS, EMISSION, ENERGY LEVELS, EPITAXY, FUNCTIONS, LUMINESCENCE, MATERIALS, MATHEMATICAL OPERATORS, NANOSTRUCTURES, ORIENTATION, PHOTON EMISSION, PHYSICAL PROPERTIES, QUANTUM OPERATORS, QUASI PARTICLES, SELENIDES, SELENIUM COMPOUNDS, SPECTRA, ZINC COMPOUNDS
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