Significant progress has been made in studying strongly correlated electronic systems with major focus on understanding high-temperature superconductivity. At the center of these studies are the so-called cuprates, which are characterized by a quasi-2D Copper-Oxide plane in which superconductivity is believed to arise. From the theoretical point of view, the complex electronic structure of these materials makes a fully ab initio many-body computation a formidable task, so we are forced to focus on minimal models that can reproduce the physics, the most well known of which is known as the Hubbard Model, which relies on the Zhang-Rice singet notion to reduce the degrees of freedom by treating the oxygen atoms implicitly. However, despite years of study, the superconducting order is still unknown. Moreover, recent experiments indicate that the oxygen p-bands play a significant role as non-trivial hole carriers, so we find it fit to study the three-band Hubbard (Emery) model, which treats the oxygen p-orbitals explicitly. We perform extensive generalized Hartree–Fock and auxiliary-field quantum Monte Carlo (AFQMC) calculations for the three-band Hubbard (Emery) model in the underdoped regime, in order to study the ground-state properties of Copper-Oxygen planes in the cuprates. Firstly, we find it important to focus on the magnetic and charge orders, and present results from generalized Hartree-Fock (GHF) calculations. The ground-state properties at the thermodynamic limit are challenging to pin down because of sensitivity to computational details, including the shapes and sizes of the supercells. We employ large-scale computations with various technical improvements to determine the orders within GHF. The ground state exhibits a rich phase diagram with hole doping as the charge transfer energy is varied, including ferromagnetic domain walls embedded in an antiferromagnetic background, spin spirals, and nematic order. Secondly, we use these results to guide and feed into exact methods by employing cutting-edge AFQMC techniques with a self-consistent gauge constraint in auxiliary-field space to control the sign problem, we reach supercells containing 500 atoms to capture collective modes in the charge and spin orders and characterize the behavior in the thermodynamic limit. The self-consistent scheme interfaced with generalized Hartree-Fock calculations allows high accuracy in AFQMC to resolve small energy scales, which is crucial for determining the complex candidate orders in such a system. We present results on the charge order, spin order, and localization properties as a function of charge-transfer energy

Vanadium Dioxide (VO2) is a strongly correlated material which has been studied for many decades. VO2 has been proposed for uses in technologies such as optical modulators, IR modulators, optical switches and Mott memory devices. These technologies are taking advantage of VO2’s insulator to metal transition (IMT) and the corresponding changes to the optical and material properties. The insulator to metal transition in VO2 can be accessed by thermal heating, applied electric field, or ultra-fast photo induced processes. Recently, thin films of VO2 grown on Titanium Dioxide doped with Niobium (TiO2:Nb), have shown promise as a possible UV photo detector with high quantum efficiency which utilizes a heterostructure between these two materials. In this work, the dynamics of the IMT on thin films of VO2 is explored. We show that surface plasmons generated in an Au thin film can induce the insulator to metal transition in a thin film of VO2 due to the enhanced electric field as well as help detect the IMT via changes in its resonance condition. Time resolved pump probe studies were also done on thin films of VO2 grown on TiO2 and TiO2:Nb, using UV photon energy of 3.1 eV (400nm wavelength). The fluence threshold of the IMT at 3.1 eV was significantly lower than published values for the 1.55 eV pump fluence. The time response of the IMT shows uncommon reflectivity dynamics in these samples. The response was partially attributed to internal interference of the reflected probe beam from the inhomogeneous layers formed inside the film by different phases of VO2, and can be elucidated by a diffusion model with respect to its optical properties. Finally, the photocurrent generation time constants for the sample with highest quantum efficiency are given and compared to its ultrafast photo induced IMT time constants.

Upon cooling past a critical temperature Tc = 340 K Vanadium dioxide (VO2) exhibits a metal-insulator transition (MIT) from a metallic rutile R to an insulating monoclinic M1 phase. Other insulating phases, a monoclinic M2 and triclinic T, have been identifed and are accessible via strain or doping. Despite decades of research, the nature of the VO2 MIT is still not fully understood. In this work we present ab-initio hybrid density functional theory (DFT) calculations on the insulating phases, compare the results to experimental measurements and discuss their implications on our understanding of the VO2 MIT. Recent measurements on M1 VO2 under high pressure found a transition to a metallic monoclinic state X at Pc = 34.3 GPa. Following this increased interest in the study of VO2 at high pressures, we will also present results of hybrid-DFT calculations on the M1 phase under increasing pressure. Our calculations predict that M1 may become metallic above ∼32 GPa, in good agreement with experiment.

Bulk niobium (Nb) superconducting radio frequency (SRF) cavities are currently the preferred method for acceleration of charged particles at accelerating facilities around the world. However, bulk Nb cavities have poor thermal conductance, impose material and design restrictions on other components of a particle accelerator, have low reproducibility and are approaching the fundamental material-dependent accelerating field limit of approximately 50MV/m. Since the SRF phenomena occurs at surfaces within a shallow depth of ~1 µm, a proposed solution to this problem has been to utilize thin film technology to deposit superconducting thin films on the interior of cavities to engineer the active SRF surface in order to achieve cavities with enhanced properties and performance. Two proposed thin film applications for SRF cavities are: 1) Nb thin films coated on bulk cavities made of suitable castable metals (such as copper or aluminum) and 2) multilayer films designed to increase the accelerating gradient and performance of SRF cavities. While Nb thin films on copper (Cu) cavities have been attempted in the past using DC magnetron sputtering (DCMS), such cavities have never performed at the bulk Nb level. However, new energetic condensation techniques for film deposition, such as High Power Impulse Magnetron Sputtering (HiPIMS), offer the opportunity to create suitably thick Nb films with improved density, microstructure and adhesion compared to traditional DCMS. Clearly use of such novel technique requires fundamental studies to assess surface evolution and growth modes during deposition and resulting microstructure and surface morphology and the correlation with RF superconducting properties. Here we present detailed structure-property correlative research studies done on Nb/Cu thin films and NbN- and NbTiN-based multilayers made using HiPIMS and DCMS, respectively.

We present results from a constrained path Monte Carlo (CPMC) study of a modified two-dimensional Hubbard model. We include more general forms of the band structure and electron interaction in order to examine their effects on ground-state properties, such as electron pairing correlations. Both next-nearest neighbor hopping, t', and third-nearest neighbor hopping, t″, are introduced in the Hamiltonian. A nearest neighbor interaction of strength V is also included. We carry out CPMC calculations on system sizes up to 16 x 16, at various electron fillings, to investigate the ground state of the model for different values of these parameters. For realistic systems, these calculations indicate that Hubbard-like models are not capable of showing enhanced pairing. The modified Hamiltonian also presents an opportunity to more closely examine the accuracy and robustness of the CPMC algorithm. Results of further benchmark calculations involving CPMC are presented. These benchmarks confirm that CPMC is able to show enhanced pairing in systems where such behavior is known to exist.

Charge transport properties of manganites can be significantly modified by temperature, chemical doping, strain, and interfacial boundaries. In this dissertation, we report studies on broadband far-field infrared spectroscopy and near-field infrared imaging of single crystalline thin films of Sr doped manganite LaMnO3 at 0.33 doping level. at this Sr-doping level, the manganite films undergo a phase transition between a ferromagnetic metallic phase at low temperatures to a paramagnetic, insulating phase at higher temperatures. The films were grown on different substrates with different thicknesses by pulsed laser deposition method. The temperature dependent far-field infrared data on 85 nm thick La0.67Sr0.33MnO3 (LSMO) film grown on (100) lanthanum aluminate substrate reveals that electron and hole free carriers behave quite similarly in the low temperature ferromagnetic metallic state of the thin film. The number densities, effective masses and relaxation response of the delocalized electrons and holes are quantified. We discover that only one-third of the doped charges are coherent and contribute to the dc transport. The temperature dependence of the relaxation rate of the free carriers at low temperatures fulfills the formula A+BT2 with anomalously large A and B coefficients compared to a conventional metal like gold. We detected some of the 8 infrared-active phonons predicted for the rhombohedral lattice. We also observed splitting of the 580 cm-1 infrared-active phonon at high temperatures which we attribute to the local Jahn-Teller distortion effect. We performed detailed scattering-type scanning near-field mid-infrared microscopy on an 18 nm thick La0.67Sr0.33MnO3 film grown on (100) strontium titanate substrate. In contrast to a percolative type first-order phase transition, a continuous homogeneous phase transition is observed within the bulk of the thin film when this sample is heated up from room temperature to 330K.The infrared near-field amplitude data is consistent with a second order phase transition from the ferromagnetic metallic phase to the paramagnetic insulating phase. We discover critical fluctuations at a fixed temperature within the bulk of the thin film near its nominal phase transition temperature. We also discover temperature independent phase segregation near the film-substrate interface which we attribute to more conducting regions with A-type antiferromagnetic order coexisting with less conducting ones with C-type antiferromagnetic structure.

We have studied the exchange bias interaction in metal bilayers IrMn/Co and FeMn/Co using the static and ultrafast pump-probe Kerr effects. Experiments conducted on wedged Co samples show that the exchange bias interaction is sensitive to the buffer layers grown beneath it when the antiferromagnetic layer is FeMn. The exchange bias strength, as measured by the shift in the magnetic hysteresis loop, follows a 1/tFM dependence as reported in the literature. The time-domain pump-probe experiments reveal coherent magnetization oscillations, whose frequencies are comparable to those measured by frequency-domain FMR measurements, and they fit well to FMR equations for the frequency. We have also been able to use the pump beam to permanently alter the exchange bias interface which leads to the launching of oscillations along new geometries, particularly along the easy axis where magnetization is aligned with the applied field. This is explained qualitatively by showing that the pump has enough energy to overcome the energy barrier in the AF, allowing it to flip and provide a torque on the magnetization that launches oscillations.

No description available.

We have developed a completely general first principles self-consistent full-potential linearized-augmented-plane-wave (LAPW) method program within the density functional formalism to calculate electronic band structure, total energy, pressure and other quantities. No symmetry assumptions are used for the crystal structure. Shape unrestricted charge densities and potentials are calculated inside muffin-tin (MT) spheres as well as in the interstitial regions. All contributions to the Hamiltonian matrix elements are completely taken into account. The core states are treated fully relativistically using the spherical part of the potential only. Scalar relativistic effects are included for the band-states, and spin-orbit coupling is included using a second variation procedure. Both core states and valence states are treated self-consistently, the frozen core approximation is not required. The fast Fourier transformation method is used wherever it is applicable, and this greatly improves the efficiency. This state-of-the-art program has been tested extensively to check the accuracy and convergence properties by comparing calculated electronic band structures, ground state properties, equations of state and cohesive energies for bulk W and GaAs with other theoretical calculations and experimental results. It has been successfully applied to calculate and predict structural and metal-insulator phase transitions for close-packed crystal BaSe and BaTe and the geometric structure of the d-band metal W(001) surface. The results are in generally good agreement with experiment.

We study light propagation in strongly scattering, random photonic materials from material synthesis, sample fabrication, characterization of light propagation and theoretical calculation. Light propagation in random photonic materials is very important not only because the study can lead to better understanding of light propagation in ordered photonic materials (photonic crystal) ( i.e., the best filling fraction in photonic crystal, the coordination number to maximize the photonic band gap, etc.); and also because the light propagation in random materials can lead to fascinating physical problems (i.e., coherent backscattering, Anderson localization, and random laser etc.). For the experiments, we synthesize the high index of refraction core-shell particles (ZnS-shell PS core, micron scale) with sonochemical methods. The smooth random films are fabricated by creating a concave meniscus from the colloidal solution. The structure (characterized by average coordination number Z) of high index particles is tuned by mixing the ZnS-PS with sacrificial PMMA spheres and followed by acetone wash. After the strongly scattering, random films are fabricated, the light propagation is characterized by measuring the coherent backscattering effect to obtain the transport mean free part of 1.06-micron wavelength light. We find a local minimum of l* (∼2.1μm) around Z∼4-5 and the scattering weakened with the increase of Z (Z>5). We show that the experimental results for porous random films disagree with the existing model for diffusive transport in random media. To explain our experimental discovery, we present a modified diffusion transport theory which incorporates the correlation of waves at strong scattering limit and Mie resonance regime to describe our experiments. The model should be useful to find the optimal conditions to enhance the scattering in random photonic materials. Furthermore, we try to enhance the scattering in random photonic materials by changing the size of scatterers, index of refraction and incident laser wavelength not only in theoretical calculation according to our modified diffusion transport theory but also in the experiments. We synthesize high index of refraction material (SnS2, n∼3.0) whose index is characterized by single scattering method. We also synthesize metallic photonic materials (such as Gallium micro-spheres) whose index of refraction can vary dramatically in visible and near infrared regime. All these studies to enhance the scattering could lead to fascinating physical phenomena (i.e. Anderson localization, and random laser etc.).