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Near-Monodisperse Ni-Cu Bimetallic Nanocrystals of Variable Composition: Controlled Synthesis and Catalytic Activity for H2 Generation

Description: Near-monodisperse Ni{sub 1-x}Cu{sub x} (x = 0.2-0.8) bimetallic nanocrystals were synthesized by a one-pot thermolysis approach in oleylamine/1-octadecene, using metal acetylacetonates as precursors. The nanocrystals form large-area 2D superlattices, and display a catalytic synergistic effect in the hydrolysis of NaBH{sub 4} to generate H{sub 2} at x = 0.5 in a strongly basic medium. The Ni{sub 0.5}Cu{sub 0.5} nanocrystals show the lowest activation energy, and also exhibit the highest H{sub 2} generation rate at 298 K.
Date: July 22, 2008
Creator: Zhang, Yawen; Huang, Wenyu; Habas, Susan E.; Kuhn, John N.; Grass, Michael E.; Yamada, Yusuke et al.
Partner: UNT Libraries Government Documents Department

Formation mechanism and properties of CdS-Ag2S nanorod superlattices

Description: The mechanism of formation of recently fabricated CdS-Ag{sub 2}S nanorod superlattices is considered and their elastic properties are predicted theoretically based on experimental structural data. We consider different possible mechanisms for the spontaneous ordering observed in these 1D nanostructures, such as diffusion-limited growth and ordering due to epitaxial strain. A simplified model suggests that diffusion-limited growth partially contributes to the observed ordering, but cannot account for the full extent of the ordering alone. The elastic properties of bulk Ag{sub 2}S are predicted using a first principles method and are fed into a classical valence force field (VFF) model of the nanostructure. The VFF results show significant repulsion between Ag{sub 2}S segments, strongly suggesting that the interplay between the chemical interface energy and strain due to the lattice mismatch between the two materials drives the spontaneous pattern formation.
Date: August 11, 2008
Creator: Wang, Lin-Wang; Demchenko, Denis O.; Robinson, Richard D.; Sadtler, Bryce; Erdonmez, Can K.; Alivisatos, A. Paul et al.
Partner: UNT Libraries Government Documents Department

Spin-density-wave antiferromagnetism of Cr in Fe/Cr(001) superlattices

Description: The antiferromagnetic spin-density-wave (SDW) order of Cr layers in Fe/Cr(001) superlattices was investigated by neutron scattering. For Cr thickness 51-190 {Angstrom}, a transverse SDW is formed for all temperatures below Neel temperature with a single wavevector Q normal to the layers. A coherent magnetic structure forms with the nodes of the SDW near the Fe-Cr interfaces. For thinner Cr layers, the magnetic scattering can be described by commensurate antiferromagnetic order.
Date: October 1, 1996
Creator: Fullerton, E.E.; Bader, S.D. & Robertson, J.L.
Partner: UNT Libraries Government Documents Department

Monte-Carlo simulation of surface growth. Final report for period September 15, 1997-September 14, 2001

Description: We have carried out simulations using various methods on models of epitaxial growth. We have investigated both homoepitaxial as well as heteroepitaxial growth. We have studied the effects of evaporation, island coarsening, strain due to lattice mismatch, three dimensional islands submonolayer growth, and self-organization in quantum dot superlattices. The results of our investigations are of significance to the understanding of material properties at the nanoscale.
Date: December 1, 2000
Creator: Lam, Pui-Man
Partner: UNT Libraries Government Documents Department

Self-Organized Vertical Superlattices in Epitaxial GaInAsSb

Description: Self-organized superlattices are observed in GaInAsSb epilayers grown nominally lattice matched to vicinal GaSb substrates. The natural superlattice (NSL) is detected at the onset of growth; is continuous over the lateral extent of over several microns; and persists vertically throughout several microns of the epilayer. Furthermore, the NSL is inclined by an additional 4{sup o} with respect to the vicinal (001) GaSb substrate. The tilted NSL intersects the surface of the epilayer, and the NSL period is geometrically correlated with surface undulations. While the principle driving force for this type of phase separation arises from solution thermodyamics, the mechanism for the self-organized microstructure is related to local strains associated with surface undulations. By using a substrate with surface undulations, the tilted NSL can be induced in layers with alloy compositions that normally do not exhibit this self-organized microstructure under typical growth conditions. These results underscore the complex interactions between compositional modulations and morphological perturbations.
Date: February 9, 2004
Creator: Wand, CA; Vineis, CJ & Calawa, DR
Partner: UNT Libraries Government Documents Department

Self-assembly of uniform polyhedral silver nanocrystals into densest packings and exotic superlattices

Description: Understanding how polyhedra pack into extended arrangements is integral to the design and discovery of crystalline materials at all length scales. Much progress has been made in enumerating and characterizing the packing of polyhedral shapes, and the self-assembly of polyhedral nanocrystals into ordered superstructures. However, directing the self-assembly of polyhedral nanocrystals into densest packings requires precise control of particle shape, polydispersity,interactions and driving forces. Here we show with experiment and computer simulation that a range of nanoscale Ag polyhedra can self-assemble into their conjectured densest packings. When passivated with adsorbing polymer, the polyhedra behave as quasi-hard particles and assemble into millimetre-sized three-dimensional supercrystals by sedimentation.We also show, by inducing depletion attraction through excess polymer in solution, that octahedra form an exotic superstructure with complex helical motifs rather than the densest Minkowski lattice. Such large-scale Ag supercrystals may facilitate the design of scalable three-dimensional plasmonic metamaterials for sensing, nanophotonics, and photocatalysis.
Date: March 1, 2011
Creator: Henzie, Joel; Grunwald, Michael; Widmer-Cooper, Asaph; Geissler, Phillip L. & Yang, Peidong
Partner: UNT Libraries Government Documents Department

A Study of Quantum Electron Dynamics in Periodic Superlattices under Electric Fields

Description: This thesis examines the quantum dynamics of electrons in periodic semiconductor superlattices in the presence of electric fields, especially uniform static fields. Chapter 1 is an introduction to this vast and active field of research, with an analysis and suggested solutions to the fundamental theoretical difficulties. Chapter 2 is a detailed historical review of relevant theories, and Chapter 3 is a historical review of experiments. Chapter 4 is devoted to the time-independent quantum mechanical study of the electric-field-induced changes in the transmission properties of ballistic electrons, using the transfer matrix method. In Chapter 5, a new time-dependent quantum mechanical model free from the fundamental theoretical difficulties is introduced, with its validity tested at various limiting cases. A simplified method for calculating field-free bands of various potential models is designed. In Chapter 6, the general features of "Shifting Periodicity", a distinctive feature of this new model, is discussed, and a "Bloch-Floquet Theorem" is rigorously proven. Numerical evidences for the existence of Wannier-Stark-Ladders are presented, and the conditions for its experimental observability is also discussed. In Chapter 7, an analytical solution is found for Bloch Oscillations and Wannier-Stark-Ladders at low electric fields. In Chapter 8, a new quantum mechanical interpretation for Bloch Oscillations and Wannier-Stark-Ladders is derived from the analytical result. The extension of this work to the cases of time-dependent electric fields is also discussed.
Date: May 1996
Creator: Yuan, Daiqing
Partner: UNT Libraries

Synthesis of a photoresponsive polymer and its incorporation into an organic superlattice.

Description: The synthesis of a photoswitchable polymer by grafting an azobenzene dye to methacrylate followed by polymerization is presented. The azobenzene dye undergoes a trans-cis photoisomerization that causes a persistent change in the refractive index of cast polymer films. This novel polymer was incorporated into superlattices prepared by spin casting and the optical activity of the polymer was maintained. A modified coextruder that allows the rapid production of soft matter superlattices was designed and fabricated.
Date: January 1, 2005
Creator: Morales, Alfredo Martin; Rondeau, Chris J. (Sandia National Laboratories, Albuquerque, NM); McElhanon, James Ross & Cole, Phillip James (Sandia National Laboratories, Albuquerque, NM)
Partner: UNT Libraries Government Documents Department

Magnetic phase transitions in epitaxial Fe/Cr superlattices

Description: The surface spin-flop and Neel transitions are examined in Fe/Cr superlattices. The surface spin-flop, originally predicted by Mills [Phys. Rev. Lett. 20, 18 (1968)], is observed in Fe/Cr(211) superlattices with antiferromagnetic interlayer coupling and uniaxial in-plane-anisotropy. The Neel transition (T{sub N}) of Cr is observed in Fe/Cr(001) superlattices, for which the onset of antiferromagnetism is at a thickness t{sub Cr} of 42{angstrom}. The bulk value of T{sub N} is approached asymptotically as t{sub Cr} increases and is characterized by a three-dimensional shift exponent. These T{sub N} results are attributed to finite-size effects and spin-frustration near rough Fe-Cr interfaces.
Date: December 31, 1995
Creator: Fullerton, E.E.; Sowers, C.H.; Bader, S.D.; Riggs, K.T. & Berger, A.
Partner: UNT Libraries Government Documents Department

Characterizing Composition Modulations in InAs/AIAs Short-Period Superlattices

Description: The formation of quantum wires has much interest due to their novel electronic properties which may lead to enhanced optoelectronic device performance and greater photovoltaic efficiencies. One method of forming these structures is through spontaneous lateral modulation found during the epitaxial growth of III/V alloys. In this paper, we report and summarize our investigations on the formation of lateral moduation in the MBE grown InAlAs/InP(001) system. This system was grown as a short-period superlattice where n-monolayers of InAs are deposited followed by m-Monolayers of AlAs (with n and m~2) and this sequence is repeated to grown a low strain InAlAs ternary alloy on InP(001) that exhibits lateral modulation. Films were grown under a variety of condition (growth temperature, effective alloy composition, superlattice period, and growth rate). These films have been extensively analyzed using X-ray diffraction, atomic force microscopy, and transmission electron microscopy (TEM) and microcharacterization, in addition to photon-based spectroscopes. Here we present results of several microstructural characterizations using a wide range of TEM-based techniques, and compare them to results from the other methods to obtain a unified understanding of composition modulation. Two strong points consistently emerge: 1) The lateral modulation wavelength is insensitive to growth temperature and effective alloy composition, but the strength of the lateral modulation is greatest near an effective alloy composition of In(0.46)Al(0.54)As, which corresponds to a slightly tensile global strain with respect to InP. 2) The composition variation for the strongly modulated films is as much as 0.38 InAs mole fraction. In addition, for these strongly modulated films, the modulation wave is asymmetric showing strongly peaked, narrower InAs-rich regions separated by flat AlAs-rich regions. We discuss these results and their possible implications in addition to detailing the techniques used to obtain them.
Date: April 26, 1999
Creator: Ahrenkiel, S.P.; Follstaedt, D.M.; Jones, E.D.; Lee, S.R.; Mascarenhas, A.; Millunchick, J. Mirecki et al.
Partner: UNT Libraries Government Documents Department

Large GMR values of sputtered Co/Cu multilayer structures with Co-Cu buffer layers

Description: We demonstrate large giant magnetoresistance (GMR) values of Co/Cu multilayers (MLs) sputtered on combined Co18{angstrom}/Cu48{angstrom} buffer layer. GMR values at room temperature reach 62% at the first antiferromagnetically (AF) coupling peak and 33% at the 2nd AF coupled peak, which are very close to those found in Co/Cu MLs sputtered on a Fe buffer layer. The large GMR effect is attributed to the superior superlattice structure of these samples, as evidenced by the x-ray reflectivity data as well as the TEM micrographs. In particular, the role of thin Co initial layer deposited beneath the Cu buffer layer on improved ML structure has been clarified from cross-sectional micrographs of high-resolution TEM.
Date: February 29, 1996
Creator: Huai, Y.; Vernon, S.P.; Stearns, D.G.; Cerjan, C. & Kania, D.R.
Partner: UNT Libraries Government Documents Department

Linear, Nonlinear Optical and Transport Properties of Quantum Wells Composed of Short Period Strained InAs/GaAs Superlattices

Description: In this work, ordered all-binary short-period strained InAs/GaAs superlattice quantum wells were studied as an alternative to strained ternary alloy InGaAs/GaAs quantum wells. InGaAs quantum wells QWs have been of great interest in recent years due to the great potential applications of these materials in future generations of electronic and optoelectronic devices. The all binary structures are expected to have all the advantages of their ternary counterparts, plus several additional benefits related to growth, to the elimination of alloy disorder scattering and to the presence of a higher average indium content.
Date: December 1993
Creator: Huang, Xuren
Partner: UNT Libraries

Self-Organized Growth of Alloy Superlattices

Description: We predict theoretically and demonstrate experimentally the spontaneous formation of a superlattice during crystal growth. When a strained alloy grows by "step flow", the steps at the surface form periodic bunches. The resulting modulated strain biases the incorporation of the respective alloy components at different steps in the bunch, leading to the formation of a superlattice. X-ray diffraction and electron microscopy for SiGe grown on Si give clear evidence for such spontaneous superlattice formation.
Date: October 19, 1998
Creator: Chason, E.; Floro, J.A.; Follstaedt, D.M.; Lagally, M.G.; Liu, F.; Tersoff, J. et al.
Partner: UNT Libraries Government Documents Department

Self-Organized Superlattices in GaInAsSb Grown on Vicinal Substrates

Description: Self-organized superlattices are observed in GaInAsSb epilayers grown lattice matched to vicinal GaSb substrates. The natural superlattice (NSL) is oriented at a slight angle of about 4{sup o} with respect to the vicinal (001) GaSb substrate. This vertical composition modulation is detected at the onset of growth. Layers in the NSL are continuous over the lateral extent of the substrate. Furthermore, the NSL persists throughout several microns of deposition. The NSLs have a period ranging from 10 to 30 nm, which is dependent on deposition temperature and GaInAsSb alloy composition. While the principle driving force for this type of phase separation is chemical, the mechanism for the self-organized microstructure is related to local strains associated with surface undulations. By using a substrate with surface undulations, the tilted NSL can be induced in layers with alloy compositions that normally do not exhibit this self-organized microstructure under typical growth conditions. These results underscore the complex interactions between compositional and morphological perturbations.
Date: June 9, 2003
Creator: Wang, C.A.; Vineis, C.J. & Calawa, D.R.
Partner: UNT Libraries Government Documents Department

LDRD final report on Bloch Oscillations in two-dimensional nanostructure arrays for high frequency applications.

Description: We have investigated the physics of Bloch oscillations (BO) of electrons, engineered in high mobility quantum wells patterned into lateral periodic arrays of nanostructures, i.e. two-dimensional (2D) quantum dot superlattices (QDSLs). A BO occurs when an electron moves out of the Brillouin zone (BZ) in response to a DC electric field, passing back into the BZ on the opposite side. This results in quantum oscillations of the electron--i.e., a high frequency AC current in response to a DC voltage. Thus, engineering a BO will yield continuously electrically tunable high-frequency sources (and detectors) for sensor applications, and be a physics tour-de-force. More than a decade ago, Bloch oscillation (BO) was observed in a quantum well superlattice (QWSL) in short-pulse optical experiments. However, its potential as electrically biased high frequency source and detector so far has not been realized. This is partially due to fast damping of BO in QWSLs. In this project, we have investigated the possibility of improving the stability of BO by fabricating lateral superlattices of periodic coupled nanostructures, such as metal grid, quantum (anti)dots arrays, in high quality GaAs/Al{sub x}Ga{sub 1-x}As heterostructures. In these nanostructures, the lateral quantum confinement has been shown theoretically to suppress the optical-phonon scattering, believed to be the main mechanism for fast damping of BO in QWSLs. Over the last three years, we have made great progress toward demonstrating Bloch oscillations in QDSLs. In the first two years of this project, we studied the negative differential conductance and the Bloch radiation induced edge-magnetoplasmon resonance. Recently, in collaboration with Prof. Kono's group at Rice University, we investigated the time-domain THz magneto-spectroscopy measurements in QDSLs and two-dimensional electron systems. A surprising DC electrical field induced THz phase flip was observed. More measurements are planned to investigate this phenomenon. In addition to their potential device applications, periodic ...
Date: September 1, 2008
Creator: Lyo, Sungkwun Kenneth; Pan, Wei; Reno, John Louis; Wendt, Joel Robert & Barton, Daniel Lee
Partner: UNT Libraries Government Documents Department

Tunable plasmonic lattices of silver nanocrystals

Description: Silver nanocrystals are ideal building blocks for plasmonicmaterials that exhibit a wide range of unique and potentially usefuloptical phenomena. Individual nanocrystals display distinct opticalscattering spectra and can be assembled into hierarchical structures thatcouple strongly to external electromagnetic fields. This coupling, whichis mediated by surface plasmons, depends on their shape and arrangement.Here we demonstrate the bottom-up assembly of polyhedral silvernanocrystals into macroscopic two-dimensional superlattices using theLangmuir-Blodgett technique. Our ability to control interparticlespacing, density, and packing symmetry allows for tunability of theoptical response over the entire visible range. This assembly strategyoffers a new, practical approach to making novel plasmonic materials forapplication in spectroscopic sensors, sub-wavelength optics, andintegrated devices that utilize field enhancement effects.
Date: February 18, 2008
Creator: Tao, Andrea; Sinsermsuksakul, Prasert & Yang, Peidong
Partner: UNT Libraries Government Documents Department

Electric Field Assisted Assembly of Perpendicular Oriented NanorodSuperlattices

Description: We observe the assembly of CdS nanorod superlattices by thecombination of a DC electric field and solvent evaporation. In eachelectric field (1 V/um) assisted assembly, CdS nanorods (5 x 30 nm)suspended initially in toluene were observed to align perpendicularly tothe substrate. Azimuthal alignment along the nanorod crystal faces andthe presence of stacking faults indicate that both 2D and 3D assemblieswere formed by a process of controlled super crystal growth.
Date: April 10, 2006
Creator: Ryan, Kevin M.; Mastroianni, Alex; Stancil, Kimani A.; Liu,Haitao & Alivisatos, Paul A.
Partner: UNT Libraries Government Documents Department

Ultrafast electron dynamics in silver nanoparticle arrays

Description: We present the results of ultrafast optical experiments on silver quantum dot superlattices. Dramatic changes in the electron dynamics occur as a function of interparticle spacing due to enhanced dipolar coupling and, most importantly, electron delocalization.
Date: January 1, 2002
Creator: Averitt, R. D. (Richard D.); Demsar, J. (Jure); Woode, E. K. (Ebenezer K.); Taylor, Antoinette J.,; Beverly, K. C. & Heath, J. R.
Partner: UNT Libraries Government Documents Department

Magnetic structure of La0.7Sr0.3MnO3/La0.7Sr0.3FeO3 superlattices

Description: Using x-ray magnetic dichroism we characterize the magnetic order in La{sub 0.7}Sr{sub 0.3}MnO{sub 3} (LSMO)/La{sub 0.7}Sr{sub 0.3}FeO{sub 3} (LSFO) superlattices with 6 unit cell thick sublayers. The LSMO layers exhibit a reduced Curie temperature compared to the bulk while antiferromagnetic order in the LSFO layers persists up to the bulk Neel temperature. Moreover, we find that aligning the LSMO magnetization by a magnetic field within the (001) surface plane leads to a reorientation of the Fe moments as well maintaining a perpendicular orientation of Fe and Mn moments. This perpendicular alignment is due to the frustrated exchange coupling at the LSMO/LSFO interface.
Date: January 10, 2009
Creator: Arenholz, E.; van der Laan, G.; Yang, F.; Kemik, N.; Biegalski, M.D.; Christen, H.M. et al.
Partner: UNT Libraries Government Documents Department

Spin-polarized ballistic transport channel in a thin superlattice composed of zincblende half-metallic compounds

Description: The authors examine theoretically conduction processes near the Fermi energy of thin layers of zincblende structure half metals, using as an example a superlattice consisting of monolayers of GaAs and MnAs, a bilayer of CrAs, and a bilayer of GaAs. By artificially separating bilayers, they show that non-fourfold coordinated Cr states thwart half metallicity. However, capping the metal-As bilayers restores half metallicity and ballistic conduction of electrons around 0.3 eV above the Fermi level will give nearly 100% spin-polarized transmission in the direction of the thin superlattice. Recent developments suggest atomic layer epitaxy can be used to produce such thin layers for spintronics applications.
Date: May 11, 2004
Creator: Qian, M C; Fong, C Y; Pickett, W E; Yang, L H; Pask, J E & Dag, S
Partner: UNT Libraries Government Documents Department

Spinodal Decomposition and Ordering Transformation in U-6 wt% Nb

Description: Phase stability and aging mechanisms in a water-quenched (WQ) U-6wt% Nb (WQ-U6Nb) alloy artificially aged at 200 C (16 hours) and naturally aged at room temperature for 15 years have been investigated. Age hardening/softening phenomenon is recorded from the artificially aged samples by microhardness measurement. The age hardening can be readily rationalized by the occurrence of spinodal decomposition (or fine-scaled Nb segregation), which results in the formation of a modulated structure in the aged samples. Prolonged aging leads to age softening of the alloy by coarsening of the modulated structure. Disorder-order or chemical ordering transformation is found within the naturally aged alloy according to TEM observations of antiphase domain boundaries (APBs) and superlattice diffraction patterns. The formation of a partially ordered phase in the naturally aged alloy is proposed and identified.
Date: August 15, 2005
Creator: Hsiung, L M
Partner: UNT Libraries Government Documents Department

Magnetic profiles in ferromagnetic/superconducting superlattices.

Description: The interplay between ferromagnetism and superconductivity has been of longstanding fundamental research interest to scientists, as the competition between these generally mutually exclusive types of long-range order gives rise to a rich variety of physical phenomena. A method of studying these exciting effects is by investigating artificially layered systems, i.e. alternating deposition of superconducting and ferromagnetic thin films on a substrate, which enables a straight-forward combination of the two types of long-range order and allows the study of how they compete at the interface over nanometer length scales. While originally studies focused on low temperature superconductors interchanged with metallic ferromagnets, in recent years the scope has broadened to include superlattices of high T{sub c} superconductors and colossal magnetoresistance oxides. Creating films where both the superconducting as well as the ferromagnetic layers are complex oxide materials with similar crystal structures (Figure 1), allows the creation of epitaxial superlattices, with potentially atomically flat and ordered interfaces.
Date: February 28, 2007
Creator: te Velthuis, S. G. E.; Hoffmann, A.; Santamaria, J.; Division, Materials Science & Madrid, Univ. Complutense de
Partner: UNT Libraries Government Documents Department