Search Results

Scalable Methods for Electronic Excitations and Optical Responses of Nanostructures: Mathematics to Algorithms to Observables

Description: Kohn-Sham density functional theory (DFT) is a powerful, well-established tool for the study of condensed phase electronic structure. However, there are still a number of situations where its applicability is limited. The basic theme of our research is the development of first principles electronic structure approaches for condensed matter that goes beyond what can currently be done with standard implementations ofKohn-Sham DFT. Our efforts to this end have focused on two classes or' methods. The first addresses the well-lmown inability of DFT to handle strong, many-body electron correlation effects. Our approach is a DFT -based embedding theory, to treat localized features (e.g. impurity, adsorbate, vacancy, etc.) embedded in a periodic, metallic crystal. A description for the embedded region is provided by explicitly correlated, ab initio wave function methods. DFT, as a fo1n1ally ground state theory, does not give a good description of excited states; an additional feature of our approach is the ability to obtain excitations localized in this region. We apply our method to a first-principles study of the adsorption of a single magnetic Co ada tom on non-magnetic Cu( 111 ), a known Kondo system whose behavior is governed by strong electron correlation. � The second class of methods that we are developing is an orbital-free density functional theory (OFDFT), which addresses the speed limitations ofKohn-Sham DFT. OFDFT is a powerful, O(N) scaling method for electronic structure calculations. Unlike Kohn-Sham DFT, OFDFT goes back to the original Hohenberg-Kohn idea of directly optimizing an energy functional which is an explicit functional of the density, without invoking an orbital description. This eliminates the need to manipulate orbitals, which leads to O(N{sup 3}) scaling in the Kahn-Sham approach. The speed of OFDFT allows direct electronic structure calculations on large systems on the order of thousands to tens of thousands of atoms, ...
Date: February 2, 2013
Creator: Carter, Emily A
Item Type: Report
Partner: UNT Libraries Government Documents Department

Ultra-High Intensity Magnetic Field Generation in Dense Plasma

Description: I. Grant Objective The main objective of this grant proposal was to explore the efficient generation of intense currents. Whereasthefficient generation of electric current in low-­‐energy-­‐ density plasma has occupied the attention of the magnetic fusion community for several decades, scant attention has been paid to carrying over to high-­‐energy-­‐ density plasma the ideas for steady-­‐state current drive developed for low-­‐energy-­‐ density plasma, or, for that matter, to inventing new methodologies for generating electric current in high-­‐energy-­‐density plasma. What we proposed to do was to identify new mechanisms to accomplish current generation, and to assess the operation, physics, and engineering basis of new forms of current drive in regimes appropriate for new fusion concepts.
Date: January 8, 2014
Creator: Fisch, Nathaniel J
Item Type: Report
Partner: UNT Libraries Government Documents Department

Trace Metal Bioremediation: Assessment of Model Components from Laboratory and Field Studies to Identify Critical Variables

Description: The objective of this project was to gain an insight into the modeling support needed for the understanding, design, and operation of trace metal/radionuclide bioremediation. To achieve this objective, a workshop was convened to discuss the elements such a model should contain. A ''protomodel'' was developed, based on the recommendations of the workshop, and was used to perform sensitivity analysis as well as some preliminary simulations in support for bioremediation test experiments at UMTRA sites. To simulate the numerous biogeochemical processes that will occur during the bioremediation of uranium contaminated aquifers, a time-dependent one-dimensional reactive transport model has been developed. The model consists of a set of coupled, steady state mass balance equations, accounting for advection, diffusion, dispersion, and a kinetic formulation of the transformations affecting an organic substrate, electron acceptors, corresponding reduced species, and uranium. This set of equations is solved numerically, using a finite element scheme. The redox conditions of the domain are characterized by estimating the pE, based on the concentrations of the dominant terminal electron acceptor and its corresponding reduced specie. This pE and the concentrations of relevant species are passed to a modified version of MINTEQA2, which calculates the speciation and solubilities of the species of interest. Kinetics of abiotic reactions are described as being proportional to the difference between the actual and equilibrium concentration. A global uncertainty assessment, determined by Random Sampling High Dimensional Model Representation (RS-HDMR), was performed to attain a phenomenological understanding of the origins of output variability and to suggest input parameter refinements as well as to provide guidance for field experiments to improve the quality of the model predictions. Results indicated that for the usually high nitrate contents found ate many DOE sites, overall bioremediation of trace metals was highly sensitive to the formulation of the denitrification process. Simulations were ...
Date: February 14, 2003
Creator: Jaffe, Peter & Rabitz, Herschel
Item Type: Report
Partner: UNT Libraries Government Documents Department

Comprehensive Mechanisms for Combustion Chemistry: An Experimental and Numerical Study with Emphasis on Applied Sensitivity Analysis

Description: This project was an integrated experimental/numerical effort to study pyrolysis and oxidation reactions and mechanisms for small-molecule hydrocarbon structures under conditions representative of combustion environments. The experimental aspects of the work were conducted in large-diameter flow reactors, at 0.3 to 18 atm pressure, 500 to 1100 K temperature, and 10<SUP>-2</SUP> to 2 seconds reaction time. Experiments were also conducted to determine reference laminar flame speeds using a premixed laminar stagnation flame experiment and particle image velocimetry, as well as pressurized bomb experiments. Flow reactor data for oxidation experiments include: (1)adiabatic/isothermal species time-histories of a reaction under fixed initial pressure, temperature, and composition; to determine the species present after a fixed reaction time, initial pressure; (2)species distributions with varying initial reaction temperature; (3)perturbations of a well-defined reaction systems (e.g. CO/H<SUB>2</SUB>/O<SUB>2</SUB> or H<SUB>2</SUB>/O<SUB>2</SUB>)by the addition of small amounts of an additive species. Radical scavenging techniques are applied to determine unimolecular decomposition rates from pyrolysis experiments. Laminar flame speed measurements are determined as a function of equivalence ratio, dilution, and unburned gas temperature at 1 atm pressure. Hierarchical, comprehensive mechanistic construction methods were applied to develop detailed kinetic mechanisms which describe the measurements and literature kinetic data. Modeling using well-defined and validated mechanisms for the CO/H<SUB>2</SUB>/Oxidant systems and perturbations of oxidation experiments by small amounts of additives were also used to derive absolute reaction rates and to investigate the compatibility of published elementary kinetic and thermochemical information. Numerical tools were developed and applied to assess the importance of individual elementary reactions to the predictive performance of the developed mechanisms and to assess the uncertainties in elementary rate constant evaluations.
Date: April 10, 2009
Creator: Dryer, Frederick L.
Item Type: Report
Partner: UNT Libraries Government Documents Department

Algorithmic Techniques for Massive Data Sets

Description: This report describes the progress made during the Early Career Principal Investigator (ECPI) project on Algorithmic Techniques for Large Data Sets. Research was carried out in the areas of dimension reduction, clustering and finding structure in data, aggregating information from different sources and designing efficient methods for similarity search for high dimensional data. A total of nine different research results were obtained and published in leading conferences and journals.
Date: April 3, 2006
Creator: Charikar, Moses
Item Type: Report
Partner: UNT Libraries Government Documents Department

Is Geothermal Simulation a "Catastrophe"?

Description: All numerical simulators of geothermal reservoirs depend upon an accurate representation of the thermodynamics of steam-water systems. These relationships are required to render tractable the system of balance equations derived from the physics of flow through porous media. While it is generally recognized that the steam-water system (i.e. two phase) is not in thermodynamic equilibrium, equihbrium thermodynamics are employed in its description. In this paper, we present an alternative view based on non-equilibrium thermodynamics. The underpinnings of this approach are found in a branch of topology generally referred to as "catastrophe theory". [Thom, 1975]
Date: December 16, 1980
Creator: Nguyen, V.V. & Pinder, George F.
Item Type: Article
Partner: UNT Libraries Government Documents Department

Conceptual Design of Optimized Fossil Energy Systems with Capture and Sequestration of Carbon Dioxide

Description: In this final progress report, we describe research results from Phase I of a technical/economic study of fossil hydrogen energy systems with CO{sub 2} sequestration. This work was performed under NETL Award No. DE-FC26-02NT41623, during the period September 2002 through August 2005 The primary objective of the study is to better understand system design issues and economics for a large-scale fossil energy system co-producing H{sub 2} and electricity with CO{sub 2} sequestration. This is accomplished by developing analytic and simulation methods for studying the entire system in an integrated way. We examine the relationships among the different parts of a hydrogen energy system, and identify which variables are the most important in determining both the disposal cost of CO{sub 2} and the delivered cost of H{sub 2}. A second objective is to examine possible transition strategies from today's energy system toward one based on fossil-derived H{sub 2} and electricity with CO{sub 2} sequestration. We carried out a geographically specific case study of development of a fossil H{sub 2} system with CO{sub 2} sequestration, for the Midwestern United States, where there is presently substantial coal conversion capacity in place, coal resources are plentiful and potential sequestration sites in deep saline aquifers are widespread.
Date: November 29, 2005
Creator: Ogden, Joan M.
Item Type: Report
Partner: UNT Libraries Government Documents Department

Final Technical Report, Grant DE-FG02-87ER13714, "Fundamental Studies of Metastable Liquids"

Description: Grant DE-FG02-87ER13714 supported fundamental work on the physical properties of metastable liquids from 6/1/87 to 4/30/08. Renewal proposals were submitted every three years (1990, 1993, 1996, 1999, 2002, 2005), and included, in every case, a detailed Final Technical Report on the previous three years. Accordingly, the bulk of this report covers the final 2-year period 5/1/06 to 4/30/08 of this grant, which is not covered in any of the previous Final Technical Reports. This is preceded by a brief overview of the main research objectives and principal accomplishments during these very fruitful and productive 21 years of DOE-funded research.
Date: March 9, 2009
Creator: Debenedetti, Pablo G.
Item Type: Report
Partner: UNT Libraries Government Documents Department

Contaminant Organic Complexes: Their Structure and Energetics in Surface Decontamination Processes

Description: Siderophores are biological macromolecules (400-2000 Da) released by bacteria in iron limiting situations to sequester Fe from iron oxyhydroxides and silicates in the natural environment. These molecules contain hydroxamate and phenolate functional groups, and exhibit very high affinity for Fe{sup 3+}. While several studies were conducted to understand the behavior of siderophores and their application to the metal sequestration and mineral dissolution, only a few of them have examined the molecular structure of siderophores and their interactions with metals and mineral surfaces in aqueous solutions. Improved understanding of the chemical state of different functional moieties in siderophores can assist in the application of these biological molecules in actinide separation, sequestration and decontamination processes. The focus of our research group is to evaluate the (a) functional group chemistry of selected siderophores and their metal complexes in aqueous solutions, and (b) the nature of siderophore interactions at the mineral-water interfaces. We selected desferrioxamine B (desB), a hydroxamate siderophore, and its small structural analogue, acetohydroxamic acid (aHa), for this investigation. We examined the functional group chemistry of these molecules as a function of pH, and their complexation with aqueous and solid phase Fe(III). For solid phase Fe, we synthesized all naturally occurring Fe(III)-oxyhydroxides (goethite, lepidocrocite, akaganeite, feroxyhite) and hematite. We also synthesized Fe-oxides (goethite and hematite) of different sizes to evaluate the influence of particle size on mineral dissolution kinetics. We used a series of molecular techniques to explore the functional group chemistry of these molecules and their complexes. Infrared spectroscopy is used to specifically identify the variations in oxime group as a function of pH and Fe(III) complexation. Resonance Raman spectroscopy was used to evaluate the nature of hydroxamate binding in the case of Fe(III)-siderophore complexes and model ligands. Soft and hard X-ray spectroscopy techniques were used to examine the electronic structure ...
Date: December 13, 2005
Creator: Myneni, Satish C. B.
Item Type: Report
Partner: UNT Libraries Government Documents Department

On the structure, propagation, and stabilization of laminar premixed flames. Final report

Description: The primary objective of the funded program was to qualitatively understand and quantitatively determine the structure and dynamics of laminar premixed flames. The investigation was conducted using laser-based experimentation, computational simulation with detailed chemistry and transport, and activation energy asymptotic analysis. Highlights of accomplishments were discussed in the annual reports submitted to the program monitor for this project. Details are reported in the thirty journal publications cited in the journal article list which is the major component of this final report.
Date: July 1999
Creator: Law, Chung K.
Item Type: Report
Partner: UNT Libraries Government Documents Department

Biological physics

Description: Major goals of biological physics are the understanding of biological systems in physical terms and the study of concepts and laws of complex systems.
Date: September 24, 1998
Item Type: Report
Partner: UNT Libraries Government Documents Department

COARSE-GRID SIMULATION OF REACTING AND NON-REACTING GAS-PARTICLE FLOWS

Description: Many processes involved in coal utilization involve handling of fine particles, their pneumatic transport, and their reactions in fluidized beds, spouted beds and circulating fluidized beds. One of the factors limiting our ability to simulate these processes is the hydrodynamics encountered in them. Two major issues that contribute to this limitation are lack of good and computationally expedient models for frictional interaction between particles, and models to capture the consequences of mesoscale structures that are ubiquitous in gas-solid flows. This project has focused on the development of these models through a combination of computer simulations and experiments. The principal goal of this project, funded under the ''DOE Vision 21 Virtual Demonstration Initiative'' is better simulation of circulating fluidized bed performance. The principal challenge funded through this cooperative agreement is to devise sound physical models for the rheological characteristics of the gas-particle mixtures and implement them in the open-domain CFD code MFIX. During the course of this project, we have made the following specific advances. (a) We have demonstrated unequivocally that sub-grid models are essential to capture, even qualitatively correctly, the macroscale flow structures in gas-particle flows in vertical risers. To this end, we developed sub-grid models of different levels of detail and exposed the sensitivity of the results obtained in coarse-grid simulations of gas-particle flow in a riser to the level of sophistication of the sub-grid models. (b) We have demonstrated that sub-grid model for the fluid-particle drag force is the most important additional feature and that the corrections for the granular phase viscosity and pressure are of secondary importance. We have also established that sub-grid models for dispersion of heat and mass are of secondary importance only. (c) We have brought forth the general character of the sub-grid model for the drag force. (d) We have performed for the ...
Date: October 2004
Creator: Sundaresan, Sankaran
Item Type: Report
Partner: UNT Libraries Government Documents Department

Precipitation and Deposition of Aluminum-Containing Phases in Tank Wastes

Description: Aluminum-containing phases compose the bulk of solids precipitating during the processing of radioactive tank wastes. Processes designed to minimize the volume of high-level waste through conversion to glassy phases require transporting waste solutions near-saturated with aluminum-containing species from holding tank to processing center. The uncontrolled precipitation within transfer lines results in clogged pipes and lines and fouled ion exchangers, with the potential to shut down processing operations.
Date: January 12, 2005
Creator: Dabbs, Daniel M. & Aksay, Ilhan A.
Item Type: Report
Partner: UNT Libraries Government Documents Department

COARSE-GRID SIMULATION OF REACTING AND NON-REACTING GAS-PARTICLE FLOWS

Description: The principal goal of this project, funded under the ''DOE Vision 21 Virtual Demonstration Initiative'' is virtual demonstration of circulating fluidized bed performance. We had proposed a ''virtual demonstration tool'', which is based on the open-domain CFD code MFIX. The principal challenge funded through this grant is to devise and implement in this CFD code sound physical models for the rheological characteristics of the gas-particle mixtures. Within the past year, which was the third year of the project, we have made the following specific advances. (a) We have completed a study of the impact of sub-grid models of different levels of detail on the results obtained in coarse-grid simulations of gas-particle flow. (b) We have also completed a study of a model problem to understand the effect of wall friction, which was proved in our earlier work to be very important for stable operation of standpipes in a circulating fluidized bed circuit. These are described in a greater detail in this report.
Date: March 2004
Creator: Sundaresan, Sankaran
Item Type: Report
Partner: UNT Libraries Government Documents Department

Grand Challenge Problems in Environmental Modeling and Remediation: Groundwater Contaminant Transport (Partnerships in Computational Science)

Description: The over-reaching goal of the Groundwater Grand Challenge component of the Partnership in Computational Science (PICS) was to develop and establish the massively parallel approach for the description of groundwater flow and transport and to address the problem of uncertainties in the data and its interpretation. This necessitated the development of innovative algorithms and the implementation of massively parallel computational tools to provide a suite of simulators for groundwater flow and transport in heterogeneous media. This report summarizes the activities and deliverables of the Princeton University component of the Groundwater Grand Challenge project funded through the High Performance Computing grand challenge program of the Department of Energy from 1995 through 1998. Seven institutions were primarily involved in this project: Brookhaven National Laboratory, Oak Ridge National Laboratory, Princeton University, SUNY at Stony Brook, Texas A&amp;M University, The University of South Carolina, and the University of Texas at Austin, with contributing efforts from the Westinghouse Savannah River Technology Center. Each institution had primary responsibility for specific research components, but strong collaboration among all institutions was essential for the success of the project and in producing the final deliverables. PICS deliverables include source code for the suite of research simulators and auxiliary HPC tools, associated documentation, and test problems. These materials will be available as indicated from each institution's web page or from the Center for Computational Sciences Oak Ridge National Laboratory in January 1998.
Date: March 11, 1999
Creator: Celia, M. A.
Item Type: Report
Partner: UNT Libraries Government Documents Department

CONCEPTUAL DESIGN OF OPTIMIZED FOSSIL ENERGY SYSTEMS WITH CAPTURE AND SEQUESTRATION OF CARBON DIOXIDE

Description: In this third semi-annual progress report, we describe research results from an ongoing study of fossil hydrogen energy systems with CO{sub 2} sequestration. This work was performed under NETL Award No. DE-FC26-02NT41623, during the six-month period September 2003 through March 2004. The primary objective of the study is to better understand system design issues and economics for a large-scale fossil energy system co-producing H{sub 2} and electricity with CO{sub 2} sequestration. This is accomplished by developing analytic and simulation methods for studying the entire system in an integrated way. We examine the relationships among the different parts of a hydrogen energy system, and attempt to identify which variables are the most important in determining both the disposal cost of CO{sub 2} and the delivered cost of H{sub 2}. A second objective is to examine possible transition strategies from today's energy system toward one based on fossil-derived H{sub 2} and electricity with CO{sub 2} sequestration. We are carrying out a geographically specific case study of development of a fossil H{sub 2} system with CO{sub 2} sequestration, for the Midwestern United States, where there is presently substantial coal conversion capacity in place, coal resources are plentiful and potential sequestration sites in deep saline aquifers are widespread.
Date: May 1, 2004
Creator: Ogden, Joan M.
Item Type: Report
Partner: UNT Libraries Government Documents Department

CONCEPTUAL DESIGN OF OPTIMIZED FOSSIL ENERGY SYSTEMS WITH CAPTURE AND SEQUESTRATION OF CARBON DIOXIDE

Description: In this second semi-annual progress report, we describe research results from an ongoing study of fossil hydrogen energy systems with CO{sub 2} sequestration. This work was performed under NETL Award No. DE-FC26-02NT41623, during the six-month period March 2003 through September 2003. The primary objective of the study is to better understand system design issues and economics for a large-scale fossil energy system co-producing H{sub 2} and electricity with CO{sub 2} sequestration. This is accomplished by developing analytic and simulation methods for studying the entire system in an integrated way. We examine the relationships among the different parts of a hydrogen energy system, and attempt to identify which variables are the most important in determining both the disposal cost of CO{sub 2} and the delivered cost of H{sub 2}. A second objective is to examine possible transition strategies from today's energy system toward one based on fossil-derived H{sub 2} and electricity with CO{sub 2} sequestration. We are carrying out a geographically specific case study of development of a fossil H{sub 2} system with CO{sub 2} sequestration, for the Midwestern United States, where there is presently substantial coal conversion capacity in place, coal resources are plentiful and potential sequestration sites in deep saline aquifers are widespread.
Date: December 2003
Creator: Ogden, Joan M.
Item Type: Report
Partner: UNT Libraries Government Documents Department

CONCEPTUAL DESIGN OF OPTIMIZED FOSSIL ENERGY SYSTEMS WITH CAPTURE AND SEQUESTRATION OF CARBON DIOXIDE

Description: In this semi-annual progress report, we describe research results from an ongoing study of fossil hydrogen energy systems with CO{sub 2} sequestration. This work was performed under NETL Award No. DE-FC26-02NT41623, during the six-month period September 2002 through March 2003. The primary objective of the study is to better understand system design issues and economics for a large-scale fossil energy system co-producing H{sub 2} and electricity with CO{sub 2} sequestration. This is accomplished by developing analytic and simulation methods for studying the entire system in an integrated way. We examine the relationships among the different parts of a hydrogen energy system, and attempt to identify which variables are the most important in determining both the disposal cost of CO{sub 2} and the delivered cost of H{sub 2}. A second objective is to examine possible transition strategies from today's energy system toward one based on fossil-derived H{sub 2} and electricity with CO{sub 2} sequestration. We are carrying out a geographically specific case study of development of a fossil H{sub 2} system with CO{sub 2} sequestration, for the Midwestern United States, where there is presently substantial coal conversion capacity in place, coal resources are plentiful and potential sequestration sites in deep saline aquifers are widespread.
Date: June 26, 2003
Creator: Ogden, Joan M.
Item Type: Report
Partner: UNT Libraries Government Documents Department

Up-Scaling Geochemical Reaction Rates for Carbon Dioxide (CO2) in Deep Saline Aquifers

Description: Geochemical reactions in deep subsurface environments are complicated by the consolidated nature and mineralogical complexity of sedimentary rocks. Understanding the kinetics of these reactions is critical to our ability to make long-term predictions about subsurface processes such as pH buffering, alteration in rock structure, permeability changes, and formation of secondary precipitates. In this project, we used a combination of experiments and numerical simulation to bridge the gap between our knowledge of these reactions at the lab scale and rates that are meaningful for modeling reactive transport at core scales. The focus is on acid-driven mineral dissolution, which is specifically relevant in the context of CO2-water-rock interactions in geological sequestration of carbon dioxide. The project led to major findings in three areas. First, we modeled reactive transport in pore-network systems to investigate scaling effects in geochemical reaction rates. We found significant scaling effects when CO2 concentrations are high and reaction rates are fast. These findings indicate that the increased acidity associated with geological sequestration can generate conditions for which proper scaling tools are yet to be developed. Second, we used mathematical modeling to investigate the extent to which SO2, if co-injected with CO2, would acidify formation brines. We found that there exist realistic conditions in which the impact on brine acidity will be limited due to diffusion rate-limited SO2 dissolution from the CO2 phase, and the subsequent pH shift may also be limited by the lack of availability of oxidants to produce sulfuric acid. Third, for three Viking sandstones (Alberta sedimentary basin, Canada), we employed backscattered electron microscopy and energy dispersive X-ray spectroscopy to statistically characterize mineral contact with pore space. We determined that for reactive minerals in sedimentary consolidated rocks, abundance alone is not a good predictor of mineral accessible surface area, and should not be used in reactive transport ...
Date: February 28, 2013
Creator: Peters, Catherine A
Item Type: Report
Partner: UNT Libraries Government Documents Department

Integration of Carbon, Nitrogen, and Oxygen Metabolism in Escherichia coli--Final Report

Description: A key challenge for living systems is balancing utilization of multiple elemental nutrients, such as carbon, nitrogen, and oxygen, whose availability is subject to environmental fluctuations. As growth can be limited by the scarcity of any one nutrient, the rate at which each nutrient is assimilated must be sensitive not only to its own availability, but also to that of other nutrients. Remarkably, across diverse nutrient conditions, E. coli grows nearly optimally, balancing effectively the conversion of carbon into energy versus biomass. To investigate the link between the metabolism of different nutrients, we quantified metabolic responses to nutrient perturbations using LC-MS based metabolomics and built differential equation models that bridge multiple nutrient systems. We discovered that the carbonaceous substrate of nitrogen assimilation, α-ketoglutarate, directly inhibits glucose uptake and that the upstream glycolytic metabolite, fructose-1,6-bisphosphate, ultrasensitively regulates anaplerosis to allow rapid adaptation to changing carbon availability. We also showed that NADH controls the metabolic response to changing oxygen levels. Our findings support a general mechanism for nutrient integration: limitation for a nutrient other than carbon leads to build-up of the most closely related product of carbon metabolism, which in turn feedback inhibits further carbon uptake.
Date: October 22, 2012
Creator: Rabinowitz, Joshua D; Wingreen, Ned s; Rabitz, Herschel A & Xu, Yifan
Item Type: Report
Partner: UNT Libraries Government Documents Department