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Homometallic and Heterometallic Antiferromagnetic Rings: Magnetic Properties Studied by Nuclear Magnetic Resonance

Description: The aim of the present thesis is to investigate the local magnetic properties of homometallic Cr{sub 8} antiferromagnetic (AFM) ring and the changes occurring by replacing one Cr{sup 3+} ion with diamagnetic Cd{sup 2+} (Cr{sub 7}Cd) and with Ni{sup 2+} (Cr{sub 7}Ni). In the heterometallic ring a redistribution of the local magnetic moment is expected in the low temperature ground state. We have investigated those changes by both {sup 53}Cr-NMR and {sup 19}F-NMR. We have determined the order of magnitude of the transferred hyperfine coupling constant {sup 19}F - M{sup +} where M{sup +} = Cr{sup 3+}, Ni{sup 2+} in the different rings. This latter result gives useful information about the overlapping of the electronic wavefunctions involved in the coordinative bond.
Date: May 9, 2012
Creator: Casadei, Cecilia
Partner: UNT Libraries Government Documents Department

Plasmon Mapping in Metallic Nanostructures and its Application to Single Molecule Surface Enhanced Raman Scattering: Imaging Electromagnetic Hot-Spots and Analyte Location

Description: A major component of this proposal is to elucidate the connection between optical and electron excitation of plasmon modes in metallic nanostructures. These accomplishments are reported: developed a routine protocol for obtaining spatially resolved, low energy EELS spectra, and resonance Rayleigh scattering spectra from the same nanostructures.; correlated optical scattering spectra and plasmon maps obtained using STEM/EELS.; and imaged electromagnetic hot spots responsible for single-molecule surface-enhanced Raman scattering (SMSERS).
Date: July 16, 2013
Creator: Camden, Jon P
Partner: UNT Libraries Government Documents Department

The Big Group of People Looking at How to Control Putting the Parts of the Air That Are the Same as What You Breathe Out Into Small Spaces in Rocks

Description: Representing the Nanoscale Control of Geologic CO2 (NCGC), this document is one of the entries in the Ten Hundred and One Word Challenge. As part of the challenge, the 46 Energy Frontier Research Centers were invited to represent their science in images, cartoons, photos, words and original paintings, but any descriptions or words could only use the 1000 most commonly used words in the English language, with the addition of one word important to each of the EFRCs and the mission of DOE energy. The mission of NCGC is to build a fundamental understanding of molecular-to-pore-scale processes in fluid-rock systems, and to demonstrate the ability to control critical aspects of flow, transport, and mineralization in porous rock media as applied to the injection and storage of carbon dioxide (CO2) in subsurface reservoirs.
Date: July 18, 2013
Creator: Stack, Andrew
Partner: UNT Libraries Government Documents Department

Electron Diffraction Determination of Nanoscale Structures

Description: Dominant research results on adsorption on gold clusters are reviewed, including adsorption of H{sub 2}O and O{sub 2} on gold cluster cations and anions, kinetics of CO adsorption to middle sized gold cluster cations, adsorption of CO on Au{sub n}{sup +} with induced changes in structure, and H{sub 2}O enhancement of CO adsorption.
Date: March 1, 2013
Creator: Parks, Joel H
Partner: UNT Libraries Government Documents Department

Characterization and Properties of Metallic Iron and Iron-Oxide Nanoparticles: Spectroscopy, Electrochemistry, and Kinetics

Description: There are reports that nano-sized zero-valent iron (Fe0) exhibits greater reactivity than micro-sized particles of Fe0, and it has been suggested that the higher reactivity of nano-Fe0 may impart advantages for groundwater remediation or other environmental applications. However, most of these reports are preliminary in that they leave a host of potentially significant (and often challenging) material or process variables either uncontrolled or unresolved. In an effort to better understand the reactivity of nano-Fe0, we have used a variety of complementary techniques to characterize two widely studied nano-Fe0 preparations:  one synthesized by reduction of goethite with heat and H2 (FeH2) and the other by reductive precipitation with borohydride (FeBH). FeH2 is a two-phase material consisting of 40 nm α-Fe0 (made up of crystals approximately the size of the particles) and Fe3O4 particles of similar size or larger containing reduced sulfur; whereas FeBH is mostly 20−80 nm metallic Fe particles (aggregates of <1.5 nm grains) with an oxide shell/coating that is high in oxidized boron. The FeBH particles further aggregate into chains. Both materials exhibit corrosion potentials that are more negative than nano-sized Fe2O3, Fe3O4, micro-sized Fe0, or a solid Fe0 disk, which is consistent with their rapid reduction of oxygen, benzoquinone, and carbon tetrachloride. Benzoquinonewhich presumably probes inner-sphere surface reactionsreacts more rapidly with FeBH than FeH2, whereas carbon tetrachloride reacts at similar rates with FeBH and FeH2, presumably by outer-sphere electron transfer. Both types of nano-Fe0 react more rapidly than micro-sized Fe0 based on mass-normalized rate constants, but surface area-normalized rate constants do not show a significant nano-size effect. The distribution of products from reduction of carbon tetrachloride is more favorable with FeH2, which produces less chloroform than reaction with FeBH.
Date: December 1, 2005
Creator: Nurmi, JT; Tratnyek, PG; Sarathy, V; Baer, DR; Amonette, JE; Pecher, K et al.
Partner: UNT Libraries Government Documents Department

Ion Beam Nanosculpting and Materials Science with Single Nanopores

Description: Work is reported in these areas: Nanopore studies; Ion sculpting of metals; High energy ion sculpting; Metrology of nanopores with single wall carbon nanotube probes; Capturing molecules in a nanopore; Strand separation in a nanopore; and DNA molecules and configurations in solid-state nanopores.
Date: October 3, 2009
Creator: Golovchenko, J A & Branton, D
Partner: UNT Libraries Government Documents Department

Scientific Evaluation of Nanomaterials of TiO{sub 2} and Related Derivatives in a Variety of Applications

Description: Altair Nanotechnolgies, Inc. (Altair) has performed and hereby reports on research and development of novel nanomaterials for applications in 1) advanced power storage devices, 2) sensors for chemical, biological and radiological agents and on an 3) investigation into mechanisms of living cell-nanoparticle interactions that will allow predictions of health and safety issues and potentially result in novel agents for remediation of chemical and biological hazards. The project was organized around four distinct objectives. Two of the objectives are focused on developments designed to dramatically improve the performance of rechargeable Li-Ion batteries. These efforts are based on extensions of Altair's proprietary TiO{sub 2} nanoparticles and nanoparticle aggregates in the form of lithium titanate spinel, lithium manganates and lithium cobaltates. A third objective leverages the core Altair nanomaterials technology to develop a unique (nanosensor) platform for the error-free, "lab on a chip" detection of chemical, biological and radiological agents for hazardous materials remediation and threat detection. The innovative approach taken by the Altair/Western Michigan team develops individual nanosensor elements built upon a construct that includes a target-specific receptor molecule coupled through a signal transducing nanomolecule to a gold, TiO{sub 2} or SiO{sub 2} nanoparticle coated with a high density of strongfluorescing molecules for signal amplification The final objective focuses on interaction mechanisms between cells and nanoparticles with the goal of understanding how specific chemical and physical properties of these nanoparticles influence that interaction. The effort will examine a range of microbes that have environmental or societal importance.
Date: September 30, 2008
Creator: Spitler, Timothy M; Stewart, Matthew; Pasquier, Aurelien Du; Coleman, Michael; Gunasinghe, Thushara; Manev, Veselin et al.
Partner: UNT Libraries Government Documents Department

Non-Equilibrium Nanoscale Self-Organization

Description: Self-organized one- and two-dimensional arrays of nanoscale surface features ("ripples" and "dots") sometimes form spontaneously on initially flat surfaces eroded by a directed ion beam in a process called "sputter patterning". Experiments on this sputter patterning process with focused and unfocused ion beams, combined with theoretical advances, have been responsible for a number of scientific advances. Particularly noteworthy are (i) the discovery of propagative, rather than dissipative, behavior under some ion erosion conditions, permitting a pattern to be fabricated at a large length scale and propagated over large distances while maintaining, or even sharpening, the sharpest features; (ii) the first demonstration of guided self-organization of sputter patterns, along with the observation that defect density is minimized when the spacing between boundaries is near an integer times the natural spatial period; and (iii) the discovery of metastability of smooth surfaces, which contradicts the nearly universally accepted linear stability theory that predicts that any surface is linearly unstable to sinusoidal perturbations of some wave vector.
Date: March 9, 2006
Creator: Aziz, Michael J
Partner: UNT Libraries Government Documents Department


Description: We report a class of core-shell nanomaterials that can be used as efficient surface-enhancement Raman scattering (SERS) substrates. The core consists of silver nanowires, prepared through a chemical reduction process, that are used to capture 4- mercaptobenzoic acid (4-MBA), a model analyte. The shell was prepared through a modified Stöber method and consists of patchy or full silica coats. The formation of silica coats was monitored via transmission electron microscopy, UV-visible spectroscopy and phase-analysis light scattering for measuring effective surface charge. Surprisingly, the patchy silica coated silver nanowires are better SERS substrate than silver nanowires; nanomolar concentration of 4-MBA can be detected. In addition, “nano-matryoshka” configurations were used to quantitate/explore the effect of the electromagnetic field at the tips of the nanowire (“hot spots”) in the Raman scattering experiment.
Date: March 29, 2013
Creator: Murph, S. & Murphy, C.
Partner: UNT Libraries Government Documents Department


Description: This book chapter presents an overview of research conducted in our laboratory on preparation, optical and physico-chemical properties of metallic and nanohybrid materials. Metallic nanoparticles, particularly gold, silver, platinum or a combination of those are the main focus of this review manuscript. These metallic nanoparticles were further functionalized and used as templates for creation of complex and ordered nanomaterials with tailored and tunable structural, optical, catalytic and surface properties. Controlling the surface chemistry on/off metallic nanoparticles allows production of advanced nanoarchitectures. This includes coupled or encapsulated core-shell geometries, nano-peapods, solid or hollow, monometallic/bimetallic, hybrid nanoparticles. Rational assemblies of these nanostructures into one-, two- and tridimensional nano-architectures is described and analyzed. Their sensing, environmental and energy related applications are reviewed.
Date: May 2, 2012
Creator: Murph, S.
Partner: UNT Libraries Government Documents Department

Nanorods of Silicon and Germanium with Well-Defined Shapes and Sizes

Description: We have made number of important discoveries along the major goals of the project, namely i) electrodeposition of germanium thin films from clusters, ii) synthesis of cluster-based surfactants with long hydrocarbon chains and micelles made of them, iii) grafting of Ge{sub 9}-clusters onto self assembled films of siloxanes attached to glass substrates, iv) doping of Ge{sub 9}-clusters, and v) expanding the clusters to ten-atom cages of Ge{sub 10}{sup 2-}.
Date: May 3, 2012
Creator: Sevov, Slavi C.
Partner: UNT Libraries Government Documents Department

Materials Science and Physics at Micro/Nano-Scales. FINAL REPORT

Description: The scope of this project is to study nanostructures of semiconductors and superconductors, which have been regarded as promising building blocks for nanoelectronic and nanoelectric devices. The emphasis of this project is on developing novel synthesis approaches for fabrication of nanostructures with desired physical properties. The ultimate goal is to achieve a full control of the nanostructure growth at microscopic scales. The major experimental achievements obtained are summarized
Date: September 7, 2009
Creator: Wu, Judy Z
Partner: UNT Libraries Government Documents Department

Final Report: Algorithms for Diffractive Microscopy

Description: The phenomenal coherence and brightness of x-ray free-electron laser light sources, such as the LCLS at SLAC, have the potential of revolutionizing the investigation of structure and dynamics in the nano-domain. However, this potential will go unrealized without a similar revolution in the way the data are analyzed. While it is true that the ambitious design parameters of the LCLS have been achieved, the prospects of realizing the most publicized goal of this instrument — the imaging of individual bio-particles — remains daunting. Even with 10{sup 12} photons per x-ray pulse, the feebleness of the scattering process represents a fundamental limit that no amount of engineering ingenuity can overcome. Large bio-molecules will scatter on the order of only 10{sup 3} photons per pulse into a detector with 106 pixels; the diffraction “images” will be virtually indistinguishable from noise. Averaging such noisy signals over many pulses is not possible because the particle orientation cannot be controlled. Each noisy laser snapshot is thus confounded by the unknown viewpoint of the particle. Given the heavy DOE investment in LCLS and the profound technical challenges facing single-particle imaging, the final two years of this project have concentrated on this effort. We are happy to report that we succeeded in developing an extremely efficient algorithm that can reconstruct the shapes of particles at even the extremes of noise expected in future LCLS experiments with single bio-particles. Since this is the most important outcome of this project, the major part of this report documents this accomplishment. The theoretical techniques that were developed for the single-particle imaging project have proved useful in other imaging problems that are described at the end of the report.
Date: October 8, 2010
Creator: Elser, Veit
Partner: UNT Libraries Government Documents Department

Templated synthesis of nickel nanoparticles: Toward heterostructured nanocomposites for efficient hydrogen storage

Description: The world is currently facing an energy and environmental crisis for which new technologies are needed. Development of cost-competitive materials for catalysis and hydrogen storage on-board motor vehicles is crucial to lead subsequent generations into a more sustainable and energy independent future. This thesis presents work toward the scalable synthesis of bimetallic heterostructures that can enable hydrogen to compete with carbonaceous fuels by meeting the necessary gravimetric and volumetric energy densities and by enhancing hydrogen sorption/desorption kinetics near ambient temperatures and pressures. Utilizing the well-known phenomenon of hydrogen spillover, these bimetallic heterostructures could work by lowering the activation energy for hydrogenation and dehydrogenation of metals. Herein, we report a novel method for the scalable synthesis of silica templated zero-valent nickel particles (Ni⊂SiO{sub 2}) that hold promise for the synthesis of nickel nanorods for use in bimetallic heterostructures for hydrogen storage. Our synthesis proceeds by chemical reduction of a nickel-hydrazine complex with sodium borohydride followed by calcination under hydrogen gas to yield silica encapsulated nickel particles. Transmission electron microscopy and powder X-ray diffraction were used to characterize the general morphology of the resultant nanocapsules as well as the crystalline phases of the incorporated Ni{sup 0} nanocrystals. The structures display strong magnetic behavior at room temperature and preliminary data suggests nickel particle size can be controlled by varying the amount of nickel precursor used in the synthesis. Calcination under different environments and TEM analysis provides evidence for an atomic migration mechanism of particle formation. Ni⊂SiO{sub 2} nanocapsules were used as seeds to induce heterogeneous nucleation and subsequent growth within the nanocapsule via electroless nickel plating. Nickel nanoparticle growth occurs under high temperature alkaline conditions, however silica nanocapsule integrity is not maintained due to the incompatibility of silica with the growth conditions. Silica nanocapsule integrity is maintained under low temperature neutral conditions, but ...
Date: May 7, 2013
Creator: Nelson, Nicholas Cole
Partner: UNT Libraries Government Documents Department

Cellular membrane trafficking of mesoporous silica nanoparticles

Description: This dissertation mainly focuses on the investigation of the cellular membrane trafficking of mesoporous silica nanoparticles. We are interested in the study of endocytosis and exocytosis behaviors of mesoporous silica nanoparticles with desired surface functionality. The relationship between mesoporous silica nanoparticles and membrane trafficking of cells, either cancerous cells or normal cells was examined. Since mesoporous silica nanoparticles were applied in many drug delivery cases, the endocytotic efficiency of mesoporous silica nanoparticles needs to be investigated in more details in order to design the cellular drug delivery system in the controlled way. It is well known that cells can engulf some molecules outside of the cells through a receptor-ligand associated endocytosis. We are interested to determine if those biomolecules binding to cell surface receptors can be utilized on mesoporous silica nanoparticle materials to improve the uptake efficiency or govern the mechanism of endocytosis of mesoporous silica nanoparticles. Arginine-glycine-aspartate (RGD) is a small peptide recognized by cell integrin receptors and it was reported that avidin internalization was highly promoted by tumor lectin. Both RGD and avidin were linked to the surface of mesoporous silica nanoparticle materials to investigate the effect of receptor-associated biomolecule on cellular endocytosis efficiency. The effect of ligand types, ligand conformation and ligand density were discussed in Chapter 2 and 3. Furthermore, the exocytosis of mesoporous silica nanoparticles is very attractive for biological applications. The cellular protein sequestration study of mesoporous silica nanoparticles was examined for further information of the intracellular pathway of endocytosed mesoporous silica nanoparticle materials. The surface functionality of mesoporous silica nanoparticle materials demonstrated selectivity among the materials and cancer and normal cell lines. We aimed to determine the specific organelle that mesoporous silica nanoparticles could approach via the identification of harvested proteins from exocytosis process. Based on the study of endo- and exocytosis behavior ...
Date: June 21, 2012
Creator: Fang, I-Ju
Partner: UNT Libraries Government Documents Department

Multitasking mesoporous nanomaterials for biorefinery applications

Description: Mesoporous silica nanoparticles (MSNs) have attracted great interest for last two decades due to their unique and advantageous structural properties, such as high surface area, pore volume, stable mesostructure, tunable pore size and controllable particle morphology. The robust silica framework provides sites for organic modifications, making MSNs ideal platforms for adsorbents and supported organocatalysts. In addition, the pores of MSNs provide cavities/ channels for incorporation of metal and metal oxide nanoparticle catalysts. These supported metal nanoparticle catalysts benefit from confined local environments to enhance their activity and selectivity for various reactions. Biomass is considered as a sustainable feedstock with potential to replace diminishing fossil fuels for the production of biofuels. Among several strategies, one of the promising methods of biofuel production from biomass is to reduce the oxygen content of the feedstock in order to improve the energy density. This can be achieved by creating C-C bonds between biomass derived intermediates to increase the molecular weight of the final hydrocarbon molecules. In this context, pore size and organic functionality of MSNs are varied to obtain the ideal catalyst for a C-C bond forming reaction: the aldol condensation. The mechanistic aspects of this reaction in supported heterogeneous catalysts are explored. The modification of supported organocatalyst and the effect of solvent on the reaction are rationalized. The significance of two functional surfaces of MSNs is exploited by enzyme immobilization on the external surface and organo catalyst functionalization on the internal surface. Using this bifunctional catalyst, the tandem conversion of small chain alcohols into longer chain hydrocarbon molecules is demonstrated. The ability to incorporate metal and metal oxide nanoparticles in the pores and subsequent functionalization led to develop organic modified magnetic MSNs (OM-MSNs) for applications in microalgae biorefinery. Two different integrated biorefinery systems are highlighted. (i) OM-MSNs are used to harvest microalgae and ...
Date: May 2, 2013
Creator: Kandel, Kapil
Partner: UNT Libraries Government Documents Department

Making More Light with Less Energy

Description: Representing the Center for Energy Efficient Materials (CEEM), this document is one of the entries in the Ten Hundred and One Word Challenge. As part of the challenge, the 46 Energy Frontier Research Centers were invited to represent their science in images, cartoons, photos, words and original paintings, but any descriptions or words could only use the 1000 most commonly used words in the English language, with the addition of one word important to each of the EFRCs and the mission of DOE: energy. The mission of the CEEM is to discover and develop materials that control the interactions among light, electricity, and heat at the nanoscale for improved solar energy conversion, solid-state lighting, and conversion of heat into electricity.
Date: July 18, 2013
Creator: Kuritzky, Leah & Jewell, Jason
Partner: UNT Libraries Government Documents Department

Using all of the Energy from the Sun to Make Power

Description: Representing the Center for Energy Nanoscience (CEN), this document is one of the entries in the Ten Hundred and One Word Challenge and was awarded "Overall Winner Runner-up." As part of the challenge, the 46 Energy Frontier Research Centers were invited to represent their science in images, cartoons, photos, words and original paintings, but any descriptions or words could only use the 1000 most commonly used words in the English language, with the addition of one word important to each of the EFRCs and the mission of DOE: energy. The mission of the CEN is to explore the light absorption and emission in organic and nanostructure materials and their hybrids for solar energy conversion and solid state lighting.
Date: July 18, 2013
Creator: Dapkus, P. Daniel & Povinelli, Michelle
Partner: UNT Libraries Government Documents Department

Final Report of Project Nanometer Structures for Fuel Cells and Displays, etc.

Description: Low-energy ion beam bombardment induced self-assembly has been used to form various periodic nano-size wave-ordered structures (WOS). Such WOS can be used as hard etching masks to produce nanowire arrays, trenches etc., on other materials by means of traditional etching or ion sputtering. These periodic nano-size structures have a wide range of applications, including flat panel displays, optical electronics, and clean energy technologies (solar and fuel cells, lithium batteries). In order to achieve high throughput of the above processes, a large area RF-driven multicusp nitrogen ion source has been developed for the application of nitrogen ion beam induced surface modification. An integrated ion beam system, which can house either a large area RF-driven multicusp ion source or a commercially available microwave ion source (Roth &amp; Rau AG Tamiris 400-f) have been designed, manufactured, assembled, and tested.
Date: December 15, 2011
Creator: Ji, Qing
Partner: UNT Libraries Government Documents Department

Ductility Enhancement of Molybdenum Phase by Nano-sized Oxide Dispersions

Description: The objective of this research is to understand and to remedy the impurity effects for room-temperature ductility enhancement of molybdenum (Mo) based alloys by the inclusion of nano-sized metal oxide dispersions. This research combines theoretical, computational, and experimental efforts. The results will help to formulate systematic strategies in searching for better composed Mo-based alloys with optimal mechanical properties. For this project, majority of the research effort was directed to atomistic modeling to identify the mechanisms responsible for the oxygen embrittling and ductility enhancement based on fundamental electronic structure analysis. Through first principles molecular dynamics simulations, it was found that the embrittling impurity species were attracted to the metal oxide interface, consistent with previous experiments. Further investigation on the electronic structures reveals that the presence of embrittling species degrades the quality of the metallic chemical bonds in the hosting matrix in a number of ways, the latter providing the source of ductility. For example, the spatial flexibility of the bonds is reduced, and localization of the impurity states occurs to pin the dislocation flow. Rice’s criterion has been invoked to explain the connections of electronic structure and mechanical properties. It was also found that when impurity species become attracted to the metal oxide interface, some of the detrimental effects are alleviated, thus explaining the observed ductility enhancement effects. These understandings help to develop predictive capabilities to facilitate the design and optimization of Mo and other high temperature alloys (e.g. ODS alloys) for fossil energy materials applications. Based on the theoretical and computational studies, the experimental work includes the preparation of Mo powders mixed with candidate nano-sized metal oxides, which were then vacuum hot-pressed to make the Mo alloys. Several powder mixing methods were evaluated, however, the Mo alloys produced showed little improvement of room-temperature ductility. Finally, toward the end of the ...
Date: July 18, 2008
Creator: Kang, Bruce
Partner: UNT Libraries Government Documents Department