Physics Commons^™

Quantum-Mechanical Evaluation Of Defects In Uranium-Bearing Materials, Megan Hoover

All Dissertations

Quantum-mechanical calculations using density functional theory with the generalized gradient approximation were employed to investigate the effects dopants have on the uranium dioxide (UO₂) structure. Uraninite is a common U⁴⁺ mineral in the Earth's crust and an important material used to produce energy and medical isotopes. Though the incorporation mechanism remains unclear, divalent cations are known to incorporate into the uranium dioxide system. Three charge-balancing mechanisms were evaluated to achieve a net neutral system, including the substitution of (1) a divalent cation for a tetravalent uranium atom and oxygen atom; (2) two divalent cations for a tetravalent …

Crystal Structure Prediction Of Materials At Extreme Conditions, Ashley S. Williams

USF Tampa Graduate Theses and Dissertations

The prediction of the structure of a crystal given only the constituent elements is one of the greatest challenges in both materials science and computational science alike. If one were to try to predict a novel crystal by brute force, meaning by arranging the atoms in every possible position of the unit cell and optimizing the geometry to find the energy minima of the potential energy surface, the amount of computer resources required to complete the calculation on the timescale of a few years would vastly exceed the currently installed computational capacity of the entire world. Fortunately, several methods have …

Multi-Scale Computational Modeling Of Metal/Ceramic Interfaces, Abu Shama Mohammad Miraz

Master's Theses

Multi-scale atomistic calculations were carried out to understand the interfacial features that dictate the mechanical integrity of the metal/ceramic nanolaminates. As such, first principles density functional theory (DFT) calculations were performed to understand the electronic and atomistic factors governing adhesion and resistance to shear for simple metal/ceramic interfaces, whereas molecular dynamics (MD) simulations were performed to observe the impact of interfacial structures, such as misfit dislocation network geometries and orientation relationships, on interfacial mechanical properties.

For the DFT investigation, we choose metals with different crystal structures, namely - Cu (fcc), Cr (bcc) and Ti (hcp) along with a variety of …

Multi-Scale Computational Modeling Of Metal/Ceramic Interfaces, Abu Shama Mohammad Miraz

Doctoral Dissertations

Multi-scale atomistic calculations were carried out to understand the interfacial features that dictate the mechanical integrity of the metal/ceramic nanolaminates. As such, first principles density functional theory (DFT) calculations were performed to understand the electronic and atomistic factors governing adhesion and resistance to shear for simple metal/ceramic interfaces, whereas molecular dynamics (MD) simulations were performed to observe the impact of interfacial structures, such as misfit dislocation network geometries and orientation relationships, on interfacial mechanical properties.

For the DFT investigation, we choose metals with different crystal structures, namely - Cu (fcc), Cr (bcc) and Ti (hcp) along with a variety of …

Parallel Algorithms For Time Dependent Density Functional Theory In Real-Space And Real-Time, James Kestyn

Doctoral Dissertations

Density functional theory (DFT) and time dependent density functional theory (TDDFT) have had great success solving for ground state and excited states properties of molecules, solids and nanostructures. However, these problems are particularly hard to scale. Both the size of the discrete system and the number of needed eigenstates increase with the number of electrons. A complete parallel framework for DFT and TDDFT calculations applied to molecules and nanostructures is presented in this dissertation. This includes the development of custom numerical algorithms for eigenvalue problems and linear systems. New functionality in the FEAST eigenvalue solver presents an additional level of …

Building Predictive Chemistry Models, Christopher Browne, Nicolas Onofrio, Alejandro Strachan

The Summer Undergraduate Research Fellowship (SURF) Symposium

Density Functional Theory (DFT) simulations allow for sophisticated modeling of chemical interactions, but the extreme computational cost makes it inviable for large scale applications. Molecular dynamics models, specifically ReaxFF, can model much larger simulations with greater speed, but with lesser accuracy. The accuracy of ReaxFF can be improved by comparing predictions of both methods and tuning ReaxFF’s parameters. Molecular capabilities of ReaxFF were gauged by simulating copper complexes in water over a 200 ps range, and comparing energy predictions against ReaxFF. To gauge solid state capabilities, volumetric strain was applied to simulated copper bulk and the strain response functions used …

Theoretical Studies Of The Growth And Functionality Of Layered Materials, Wei Chen

Doctoral Dissertations

In this thesis, we present several projects on the growth and functionality of layered materials, using density functional theory (DFT) method and phenomenological modeling approach. Beyond the understanding of growth mechanisms and exploration of properties, we propose novel avenues to realize controllable growth processes and layered materials with desirable properties. The contents have three major parts:

(1) Graphene growth on Cu(111) and Ni(111) substrates. We first demonstrate that the inherent multi-orientational degeneracy of the graphene islands on Cu(111) in the early stages of nucleation could result in the prevalence of grain boundaries (GBs). Next, we propose a possible solution to …

An Ab-Initio Study Of The Elastic Properties Of Important Group Iv Diborides At High Temperatures, Manny Gonzales

Open Access Theses & Dissertations

Presented is an ab-initio Molecular Dynamics (MD) study, employing the Density Functional Theory (DFT), of the lattice parameter, thermal expansion coefficients and elastic constants of ZrB₂, TiB₂ and HfB₂ as a function of temperature. The MD trajectories provide the equilibrium lattice parameters at finite temperatures, and the gradient of the energy from these equilibrium solutions is then used to calculate the components of the stiffness tensor. The results for ZrB₂ are shown to agree well with reported experimental results for the lattice parameters and elastic constants as a function of temperature.

Study Of The Electronic Structure Of Cafeo₃, Jinbo Yang, M. S. Kim, Qingsheng Cai, X.-D. Zhou, Harlan U. Anderson, William Joseph James, William B. Yelon

Materials Science and Engineering Faculty Research & Creative Works

We have studied the charge disproportionation phenomenon in CaFeO3 using the local-spin density approximation with the on-site Coulomb interaction parameter U and exchange parameter J. The calculation reveals that the total number of the 3d electrons is about 5.1 for both Fe(1)(Fe5+) and Fe(2)(Fe3+) atoms, and that there are about 0.25 electron holes in the O-2p band. Therefore, the charge disproportionation can be more accurately described as 2d5L(Fe4+)=d5L2(Fe5+)+d5(Fe3+), where L denotes a hole in the oxygen 2p band, instead of 2d4(Fe4+)=d3(Fe5+)+d5(Fe3+). The hybridization between the Fe-3d and O-2p orbitals is stronger for Fe(1) than for Fe(2) due to the shorter …