The recent discovery of a two-dimensional electron (2DEG) gas at interfaces between nonpolar SrTiO₃ (STO) with other polar perovskites has lead to an enormous amount of research. Among this 2DEGs most interesting properties are two-dimensional superconductivity and ferromagnetism, sometimes concurrent. This study provides a starting point in understanding the reconstruction of bulk perovskite t₂[subscript g] bands near a surface or polar interface. First a symmetry constrained [k arrow] · [p arrow] model is developed for an arbitrary pseudocubic bulk perovskite. This [k arrow] · [p arrow] model is applied to studies of bulk STO under external strain and to the Shubnikov - de Haas effect in lightly doped STO to high magnetic fields. Then a simplified electronic structure model is developed for surfaces and interfaces. This model includes non-linear and non-local screening effects by a single polar lattice mode. Generalization of the lattice screening model is discussed. Bonding within a single perovskite layer is then investigated further to understand Rashba interactions and their connection with microscopic material parameters. Next the optical conductivity of quantum confined t₂[subscript g] bands is investigated. Finally some possible future work based on the ideas developed in this thesis are explained. / text

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High harmonic generation (HHG) in solids has two main applications. First, HHG is an all-solid-state source of coherent attosecond very ultraviolet (VUV) radiation. As such, it presents a promising source for attosecond science. The ultimate goal of attosecond science is to make spatially and temporally resolved movies of microscopic processes, such as the making and breaking of molecular bonds. Second, the HHG process itself can be used to spatially and temporally resolve fast processes in the condensed matter phase, such as charge shielding, multi-electron interactions, and the dynamics and decay of collective excitations. The main obstacles to realize these goals are: the very low efficiency of HHG in solids and incomplete understanding of the ultrafast dynamics of the complex many-body processes occurring in the condensed matter phase. The theoretical analysis developed in this thesis promises progress along both directions. First, it is demonstrated that nanoengineering by using lower-dimensional solids can drastically enhance the efficiency of HHG. The effect of quantum confinement on HHG in semiconductor materials is studied by systematically varying the confinement width along one and two directions transverse to the laser polarization. Our analysis shows growth in high harmonic efficiency concurrent with a reduction of ionization. This decrease in ionization comes as a consequence of an increased band gap resulting from the confinement. The increase in harmonic efficiency results from a restriction of wave packet spreading, leading to greater re-collision probability. Consequently, nanoengineering of one and two-dimensional nanosystems may prove to be a viable means to increase harmonic yield and photon energy in semiconductor materials driven by intense laser fields. Thus, it will contribute towards the development of reliable, all-solid-state, small-scale, and laboratory attosecond pulse sources. Second, it is shown that HHG from impurities can be used to tomographically reconstruct impurity orbitals. A quasi-classical three-step model is developed that builds a basis for impurity tomography. HHG from impurities is found to be similar to the high harmonic generation in atomic and molecular gases with the main difference coming from the non-parabolic nature of the bands. This opens a new avenue for strong field atomic and molecular physics in the condensed matter phase and allows many of the processes developed for gas-phase attosecond science to be applied to the condensed matter phase. As a first application, my conceptual study demonstrates the feasibility of tomographic measurement of impurity orbitals. Ultimately, this could result in temporally and spatially resolved measurements of electronic processes in impurities with potential relevance to quantum information sciences, where impurities are prime candidates for realizing qubits and single photon sources. Although scanning tunneling microscope (STMs) can measure electron charge distributions in impurities, measurements are limited to the first few surface layers and ultrafast time resolution is not possible yet. As a result, HHG tomography can add complementary capacities to the study of impurities.

acase@tulane.edu / Ever since the successful isolation of graphene, plenty of researches have been pursued to study fundamental physics in low-dimensional van der Waals materials, referred to as materials with the existence of out of plane vdW force. Not only graphene but also many other novel vdW materials start to emerge and play important roles in quantum physics. Due to the highly preserved crystal quality of the nanostructures achieved by micromechanical exfoliation, a variety of new phenomenon have been discovered in these novel materials. This dissertation focuses on the discovery and electronic properties study of new vdW materials both in 2D and 1D systems. Semiconducting transition metal dichalcogenides with layered structure have been viewed as the promising channel materials for field-effect transistors (FETs) in modern electronics. To characterize the performance, we have fabricated FETs based on multilayer WS2 thin crystals. By using gold as the contact metal and varying the thickness of the crystal, high-performance FETs with on/off ratio of 108 and mobility up to 234 cm2V-1s-1 at room temperature have been realized. The high performance is associated with the minimized Schottky barrier and a shallow impurity level below the conduction band. Elementary substance and binary compound crystals have limited members belong to 2D or 1D family. Thus, expanding the research to ternary compound materials is necessary. In this regard, we focused on a novel ternary compound 2D material Nb3SiTe6 and studied its magneto-transport. We have discovered that by using such a high crystalline 2D metal, we could study the inelastic electron-phonon (e-ph) interactions involved with reducing dimensions. From 3D bulk to 2D films with a rigid substrate, the weak antilocalization (WAL) signature is gradually enhanced according to our magnetoresistance (MR) measurements. Systematic studies of the temperature dependence of the dephasing rate in the crystal with various thicknesses suggest the suppression of electron-phonon interaction due to quantum confinement of the phonon spectrum. Our work shows great consistency with the long-standing predicted theory. We have successfully expanded the mechanical exfoliation method to 1D material group. As demonstrated by semiconducting quasi-1D materials, Ta2Pd3Se8 (TPdS) and Ta2Pt3Se8 (TPtS), the external force can efficiently break the weak vdW interactions between ribbons. In our work, we have produced ultrathin 1D TPdS and TPtS nanowires, and fabricated 1D FETs showing p-type and n-type transistor behavior respectively. Moreover, we have successfully built the functional logic NOT gate using these two different 1D FETs. / 1 / Xue Liu

The major difference between semiconductor quantum dots and bulk semiconductors is in the quantum confinement effect. It results the controllable exciton¡¦s absorption and emission spectra by tuning the size of the quantum dot. Moreover, multi-exciton states are reported to be observed in the highly symmetric quantum dot systems. In this dissertation, we use the single molecule fluorescence measurement to study the power dependence of multi-exciton state in single CdSe/ZnS semiconductor quantum dots. At low excitation fluence, anti-bunching behavior, and nearly single exponential relaxation dynamics are observed. By increasing the laser power, bi-exponential fluorescence decay dynamics as well as bunching behaviors from the same QD indicate the fast PL dynamics due to the relaxation from multi-exciton. The results indicate certain threshold energy level for multi-exciton generation. In addition, the multiple step cascade radiative relaxation processes are observed. Besides, we modulate linear polarization light to study the excitation orientation dependence. The results indicate the emission dipole of multi-exciton is similar to the single exciton, having a two dimensional transition dipole plane with c-axis symmetry. However, the absorption dipole of multi-exciton exhibits different orientation dependence from the single exciton.

Nanostructures often possess unique properties, which may lead to the development of new microelectronic and optoelectronic devices. They also provide an opportunity to test fundamental quantum mechanical concepts such as the role of quantum confinement. Considerable effort has been made to understand the electronic and structural properties of nanostructures, but many fundamental issues remain. In this work, the electronic and structural properties of nanostructures are examined using several new computational methods. The effect of dimensional confinement on quantum levels is investigated for hydrogenated Ge <110> using the plane-wave density-functional-theory pseudopotential method. We present a real-space pseudopotential method for calculating the electronic structure of one-dimensional periodic systems such as nanowires. As an application of this method, we examine H-passivated Si nanowires. The band structure and heat of formation of the Si nanowires are presented and compared to plane wave methods. Our method is able to offer the same accuracy as the traditional plane wave methods, but offers a number of computational advantages such as the ability to handle large systems and a better ease of implementation for highly parallel platforms. Doping is important to many potential applications of nano-regime semiconductors. A series of first-principles studies are conducted on the P-doped Si <110> nanowires by the real-space pseudopotential methods. Nanowires of varied sizes and different doping positions are investigated. We calculate the binding energies of P atoms, band gaps of the wires, energetics of P atoms in different doping positions and core-level shift of P atoms. Defect wave functions of P atoms are also analyzed. In addition, we study the electronic properties of phosphorus-doped silicon <111> nanofilms using the real-space pseudopotential method. Nanofilms with varied sizes and different doping positions are investigated. We calculate the binding energies of P atoms, band gaps of the films, and energetics of P atoms in different doping positions. Quantum confinement effects are compared with P-doped Si nanocrystals and as well as nanowires. We simulate the nanofilm STM images with P defects in varied film depths, and make a comparison with the experimental measurement. / text

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Cette thèse, réalisée dans l'équipe OPTO-PV du laboratoire IM2NP, porte sur l'étude des propriétés particulières des nanostructures de petites dimensions pour des application optoélectroniques. Pour le solaire photovoltaïque, leur utilisation permet d'augmenter l'efficacité et de réduire les coûts. Après avoir étudié les différentes technologies et phénomènes photovoltaïques, nous avons choisi les cellules hybrides organiques - nanosphères semiconductrices comme structures d'étude. Nous avons alors développé une approche numérique de détermination des propriétés intrinsèques des boîtes quantiques. Notre méthode est rapide et nécessite peu de paramètres pour une utilisation à la fois prédictive et explicative. Nous déterminons les propriétés électronique avec l'approximation de la masse effective en la modifiant pour tenir compte de la non-parabolicité des bandes électroniques. Nous utilisons ces résultats pour évaluer les propriétés optiques, particulièrement l'absorption qui joue un rôle important dans le processus photovoltaïque. Nous prenons en compte des effets de couplages diélectriques sur ces propriétés ainsi que des aspects thermodynamiques. Ces outils nous permettent d'étudier l'effet du confinement quantique des charges sur le comportement optoélectroniques de nanostructures de différents types: multipuits couplés, fils de section circulaire et boîtes sphériques. La réalisation et la caractérisation de couches minces de PMMA incorporant des nanosphères homogènes et (cœur)coquille composées de différents semiconducteurs valident notre approche et posent les bases de l'étude de couches actives hybrides pour la réalisation de cellules solaires performantes. / This thesis was conducted in the OPTO-PV team of the IM2NP laboratory. Its aim is to study the peculiar properties of low-dimensional nanostructures for use in optoelectronic applications. For photovoltaics in particular, they can be used for the realization of innovative devices with theoretical hight efficiencies at low costs. After we evaluated the various technologies and phenomena that can be used in nanostructured photovoltaics, we decided to choose an hybrid organic polymer - inorganic quantum dots solar cell as study structure. We then developed a numerical approach to determine the intrinsic properties of quantum dots. Our method is fast and requires few parameters so that we can conduct predictive and explicative studies. We start with the evaluation of the electronic properties under the effective mass approximation that we modify to take into account the non-parabolicity of the energy bands. We use the results to derive the optical properties with emphasis on absorption that plays an important role in the photovoltaic process. We take dielectric coupling effects and also thermodynamic effects into account. Those tools allow the study of the effect of quantum confinement on the optoelectronic behavior of various nanostructures: coupled quantum wells, circular cross-section quantum wires and spherical dots. The fabrication and characterization of PMMA thin-films containing homogeneous and (core)shell quantum dots of different semiconductors, validate our approach and constitute the first step towards the study of hybrid active layers for efficient solar cells.

Esta tese de doutorado tem por objetivo aprofundar as pesquisas realizadas no mestrado, a saber, da caracterização e estudo das propriedades estruturais e ópticas de filmes de oxinitreto de silício (SiOxNy:H) ricos em silício depositados pela técnica de deposição química a vapor assistida por plasma a baixa temperatura (PECVD). Os resultados obtidos no mestrado indicaram que os filmes de SiOxNy:H ricos em silício apresentam emissão luminescente na faixa do visível cuja intensidade e freqüência de emissão estão em correlação com o excesso de silício. Os resultados sugeriram que o excesso de silício na matriz do SiOxNy:H estava disposto na forma de aglomerados de silício de dimensões nanométricas responsáveis por efeitos de tamanho quântico bem como a estados radiativos na interface dos aglomerados com a matriz isolante. Neste trabalho a fim de avaliar o efeito da separação de fases, do tamanho quântico, e da interface, foram produzidos sistemas nanoestruturados a base de silício com total e parcial separação de fases para caracterizar e analisar suas propriedades ópticas e estruturais e compará-las com as dos filmes ricos em silício. Assim foram produzidas multicamadas de a-Si:H de poucos nanômetros de espessura com materiais dielétricos. Em algumas destas multicamadas foi promovida a mistura parcial das camadas por meio de bombardeamento iônico. O estudo nas estruturas de multicamadas permitiu caracterizar e analisar as propriedades estruturais e ópticas de materiais nanoestruturados com total e parcial separação de fases para posteriormente contrastá-los com as características dos filmes de oxinitreto de silício ricos em silício. A fim de analisar a influência da interface nas propriedades ópticas destes sistemas as multicamadas foram fabricadas com dois dielétricos diferentes: o óxido de silício e o ni treto de silício. A espessura das camadas dielétricas foi mantida fixa entanto que a das camadas de silício foi variada para avaliar efeitos de confinamento no silício. A caracterização foi feita utilizando técnicas de absorção óptica no UV-Vis, absorção no infravermelho (FTIR), espectroscopia Raman, fotoluminescência (PL), espectroscopia de absorção de raios X próximos 7 à borda do silício (XANES), e microscopia eletrônica de transmissão de alta resolução (HRTEM). Da análise dos resultados concluiu-se que o confinamento é fundamental para a existência da emissão luminescente embora o tipo de interface influencie a energia e a intensidade da emissão. A análise comparativa com as multicamadas permitiu verificar que os filmes de oxinitreto de silício ricos em silício apresentam, separação parcial de fases já como depositados, os tratamentos térmicos promovem a segregação do silício aumentando conseqüentemente a separação de fases. / The aim of this doctorate thesis is to enhance the knowledge in the research conducted along the Master degree based on the characterization and study of the structural and luminescent properties of silicon rich silicon oxynitride films (SiOxNy:H) deposited at low temperature by Plasma Enhanced Chemical Vapor Deposition (PECVD). The results of this study indicated that silicon rich SiOxNy:H films present luminescence in the visible spectra range with intensity and frequency in correlation with the silicon excess. The results suggested that the silicon excess in the SiOxNy:H matrix is confined in nanometric silicon clusters responsible for the to quantum size effects as well as for radiactive states at the interface of the silicon clusters with the insulating matrix. In the present work in order to evaluate the effect of phase separation, quantum size and interface effects si licon based nanostructured systems presenting total and partial phase separation were produced and their structural and optical properties were characterized in order to correlate them with the silicon rich films ones. In this way multilayers with few nanometers thick a-Si layers with dielectric materials were produced. The mixture of the layers was promoted by ion bombardment in some of these multilayers. The study of these structures permitted the characterization of structural and optical properties of materials with total and partial phase separation with the purpose of comparing them to the silicon-rich silicon oxynitride films characteristics. In order to analyze the interface influence in the optical properties, multilayers systems with two different dielectric materials, silicon oxide and silicon nitride, were fabricated. The dielectric layer thickness was kept constant while the silicon layer was varied in order to study the confinement effect. The characterization was done utilizing UV-Vis optical absorption, infrared absorption (FTIR), Raman spectroscopy, Photoluminescence (PL), X-ray absorption near edge spectroscopy (XANES) and high-resolution transmission electron microscopy (HRTEM) techniques. From the results analysis it was concluded that confinement is essent ial for the existence of luminescent 9 emission although the type of interface also influences the energy and intensity of the emission. The comparative analysis with the multilayers permitted to verify that the silicon-rich silicon oxynitride films present, as deposited, partial phase separation and that the thermal treatments promotes silicon aggregation thus increasing the phase separation.