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Structural relaxation and the glass transition in metal-metal glassesMao, Ming January 1993 (has links)
This thesis presents the results of a systematic study on the structural relaxation and the glass transition of ternary metal-metal glasses Zr$ sb{67}$(Ni$ sb{1-x}$Cu$ sb{x}) sb{33}$. Differential scanning calorimetry provides macroscopic evidence of structural changes from the compositional and temperature dependence of enthalpy change. Results from high precision x-ray diffraction and Mossbauer spectroscopy, performed mainly on $ rm Zr sb{67}Ni sb{10}Cu sb{23}$ (x = 0.7), complete the picture of structural changes at the atomic level. / Irreversible structural relaxation leads to densification and enthalpy release. Shear-like atomic motion enhances local atomic order, highlighting the atomic processes during the irreversible relaxation. Reversible structural relaxation involves two partly overlapping processes initiated at different temperatures, which are characterized by the solid and liquid atomic mobilities, respectively. Interatomic positional exchanges between Cu and Ni atoms change the local structure and are active during the reversible relaxation at low temperatures, which are also partly responsible for the irreversible relaxation. Above 500 K, shear-like atomic movements characterize the reversible relaxation, involving all three atomic species in a length scale of a few near-neighbor atomic shells. The overall density is unchanged during reversible relaxation. / The strong compositional dependence of the glass transition in the ternary glasses indicates an intimate association of the glass transition with interatomic bondings among different atomic species. The atomic motion from room temperature up to above the glass transition temperature, measured by the Mossbauer spectroscopy, is macroscopically tracked by the volume expansion and the enthalpy evolution. The glass transition occurs when the length scale of the atomic motion expands so rapidly that the interatomic potential can no longer maintain the on-site atomic vibration. The rapid development of translational atomic motion upon approaching the glass transition is reflected by the dramatic enhancement of the diffusive atomic motion.
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Time resolved X-ray studies of crystallization in Zr-based glassesYang, Yong Suk Tony. January 1990 (has links)
We have developed new techniques, which enable us to study the kinetics of phase transitions in situ. By resistive self heating of samples, heating rates of over 10$ sp4$ K/s have been achieved. Our methods allows us to acquire x-ray diffraction patterns as quickly as every 3 ms. / We have used these new techniques of time resolved x-ray diffraction experiments to study the crystallization kinetics of amorphous NiZr$ sb2,$ CoZr$ sb2,$ FeZr$ sb2$ and Ni$ sb{36.5}$Zr$ sb{63.5}.$ The experiments were performed at beamline X20C National Synchrotron Light Source. / We have mostly focussed on the crystallization behaviour at high temperatures and therefore faster kinetics. We have found many new results and unexpected metastable phases in these systems. Most of these phases would not be seen using conventional techniques showing the importance of in situ time resolved structural measurements to study the kinetics of phase transitions.
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Nanolithography using an atomic microscopeGagnon Morris, Alexis January 2003 (has links)
In this thesis, I study the nanolithography of gallium arsenide samples by local oxidation with an atomic force microscope (AFM). I examine the current theoretical descriptions of the reaction kinetics and compare the results to experimental data. The main goal is to characterize the AFM oxidation process such that high quality features can be routinely patterned. I also investigate the use of alternative oxidation environments in an attempt to improve the height and aspect ratio of the AFM local oxidation features. An alternative lithography technique involving scratching under a high contact force is also studied. Finally, I discuss the steps that are necessary in order to fabricate a quantum structure with the AFM local oxidation lithography technique.
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Preparation and characterization of Tungsten tips suitable for molecular electronics studiesLucier, Anne-Sophie January 2004 (has links)
A technique for preparing tips with a radius of a few nanometers from tungsten wire is investigated. The sharp shape is obtained by electrochemical etching; further tip processing and characterization is done in ultra-high vacuum. Tips are cleaned through a high temperature annealing process and their sharpness can be quickly estimated from their field emission behaviour. Sufficiently sharp tips are imaged with a field ion microscope; full atomic characterization of the tip apex can be obtained from an analysis of the resulting images and field evaporation can be used to atomically engineer the tip apex into a desired configuration. Starting from single crystal, (111) oriented tungsten wire, a sharp tip terminating in three atoms can be fabricated; due to its geometry and its stability, this apex configuration is well suited for applications as an atomically defined electrical contact in a single molecule conductivity experiment.
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Magnetic polarisation of palladium in palladiumiron multilayersCheng, Li, 1973- January 2004 (has links)
This thesis is devoted to the studies of structural and magnetic properties of Pd/Fe multilayers with the principal goal of determining the extent to which the Pd layers are polarised by the Fe atoms and the average moment induced on each Pd atom. Although Pd/Fe multilayers have been the subject of several previous studies, no consensus on the behavior of magnetically polarised Pd has emerged. This work has the novel feature of applying a wide range of characterization techniques on the same sample. These techniques included x-ray diffraction, conversion electron Mossbauer spectroscopy (CEMS), magnetometry and polarised neutron reflectometry. Ag/Fe multilayers were first characterized to confirm the validity of the analysis of the small-angle x-ray reflectivity to obtain layer thicknesses, as well as to determine the temperature dependence of the Fe moment from GEMS data. / From the intersection of the results from the complementary measurements on Pd/Fe multilayers, for the first time, an unequivocal understanding of the behavior of magnetically polarised Pd has been achieved. We find, there is a clear excess magnetisation associated with Pd polarisation. At 4.5 K, the Pd in contact with an Fe surface is polarised with an average moment of 0.32 +/- 0.02 muB to a depth of 20 +/- 4 A (9 +/- 2 atomic layers). These results indicate a large exchange splitting of the Pd d-bands for a significant distance from the Fe surface, leaving the spin-up band full, and a moment in the Pd arising from the 0.36 holes in the spin-down band. We also find that the Fe moment at the Pd/Fe interface is slightly enhanced to 2.42 +/- 0.05 muB for about 2.0 +/- 0.3 atomic layers, suggesting that the magnetic properties of Fe is less affected by Pd as compared to the influence of Fe on Pd. Neither the extent of Pd polarisation nor the interface Fe moment agree with values predicted by theoretical calculations (the calculated Pd polarisation depth is 2 atomic layers, and the interface Fe moment is 2.7 muB). The band structure calculations will have to be refined in the light of the results from current study.
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Kondo resonance in double quantum dots : a Green's function analysisJi, Tao, 1981- January 2005 (has links)
In this thesis, an overview of non-equilibrium Green's function (NEGF) technique is presented. The entire formulism is derived from the starting point of the definitions of Green's functions. The special application of NEGF to transport problems is discussed in details. A brief introduction of Kondo phenomenon and several theoretical approaches are presented. Using the knowledge of NEGF and Kondo problem in general, we investigated the Kondo phenomenon in double quantum dots (DQD) in great detail. In this application, the physical quantities are derived in terms of Green's functions and self-consistent equations determining the state of the system are solved numerically. A phase diagram is presented as the result of competition between Kondo effect and magnetic exchange interaction, and spin flipping scattering center in the DQD system is shown to have great effect as it breaks the coherence between the two QDs under certain circumstances.
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Bismuth based nanoelectronic devicesChiu, Pit Ho Patrio, 1977- January 2005 (has links)
Bismuth (Bi) is a unique electronic material with small effective mass (∼0.001me) and long carrier mean free path (100 nm at 300K). It is particularly suitable for studying nano scale related phenomena such as size effect and energy level spacing. In this thesis work, bismuth based nanoelectronic devices were studied. Devices were fabricated using a combination of electron beam (e-beam) writing and thermal evaporation techniques. Dimensions of the fabricated devices were in the order of 100 rim. All structures were optimized for individual electrical characterization. Three types of devices were studied: Bi nanowires, Bi nanowires with dual side-gate structures and Bi nanodot structures. In the study of Bi nanowires, metal-to-semiconductor transition phenomenon and size effect were observed. The conduction behavior of Bi nanowires changed from metallic to semiconductor when the device's critical dimension was reduced to below 50 nm. It is a solid experimental evidence of the quantum confinement-induced bandgap theory. Additionally, it has been found in the present work that resistivity of individual Bi nanowire increased as linewidth decreased indicating size effect occurred in the Bi nanowires. Dual side-gate structures were formed adjacent to the Bi nanowires in an attempt to modulate the current. Measurements showed a 7% of current modulation. The small current modulation suggested the high carrier density in the nanowire which has prevented the full depletion of free carriers. 100 nm-diameter Bi nanodot structures were fabricated utilizing proximity effect of e-beam writing. Precise control of electron doses and process conditions led to the successful fabrication of sub-nanometer tunneling junctions to the nanodots. Significant non-linear current-voltage (I-V) characteristic was observed at low temperatures. The step like I-V characteristic was a strong indication of energy level spacing in the zero-dimensional nanodot structure. The successful observation of energy level spacing in a relatively large nanodot is due to the small effective mass of bismuth material which leads to a measurable energy level spacing.
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Electron-phonon interactions in molecular electronic devicesSergueev, Nikolai. January 2005 (has links)
Over the past several decades, semiconductor electronic devices have been miniaturized following the remarkable "Moores law". If this trend is to continue, devices will reach physical size limit in the not too distance future. There is therefore an urgent need to understand the physics of electronic devices at nano-meter scale, and to predict how such nanoelectronics will work. In nanoelectronics theory, one of the most important and difficult problems concerns electron-phonon interactions under nonequilibrium transport conditions. Calculating phonon spectrum, electron-phonon interaction, and their effects to charge transport for nanoelectronic devices including all atomic microscopic details, is a very difficult and unsolved problem. It is the purpose of this thesis to develop a theoretical formalism and associated numerical tools for solving this problem. / In our formalism, we calculate electronic Hamiltonian via density functional theory (DFT) within the nonequilibrium Green's functions (NEGF) which takes care of nonequilibrium transport conditions and open device boundaries for the devices. From the total energy of the device scattering region, we derive the dynamic matrix in analytical form within DFT-NEGF and it gives the vibrational spectrum of the relevant atoms. The vibrational spectrum together with the vibrational eigenvector gives the electron-phonon coupling strength at nonequilibrium for various scattering states. A self-consistent Born approximation (SCBA) allows one to determine the phonon self-energy, the electron Green's function, the electronic density matrix and the electronic Hamiltonian, all self-consistently within equal footing. The main technical development of this work is the DFT-NEGF-SCBA formalism and its associated codes. / A number of important physics issues are studied in this work. We start with a detailed analysis of transport properties of C60 molecular tunnel junction. We find that charge transport is mediated by resonances due to an alignment of the Fermi level of the electrodes and the lowest unoccupied C60 molecular orbital. We then make a first step toward the problem of analyzing phonon modes of the C60 by examining the rotational and the center-of-mass motions by calculating the total energy. We obtain the characteristic frequencies of the libration and the center-of-mass modes, the latter is quantitatively consistent with recent experimental measurements. Next, we developed a DFT-NEGF theory for the general purpose of calculating any vibrational modes in molecular tunnel junctions. We derive an analytical expression for dynamic matrix within the framework of DFT-NEGF. Diagonalizing the dynamic matrix we obtain the vibrational (phonon) spectrum of the device. Using this technique we calculate the vibrational spectrum of benzenedithiolate molecule in a tunnel junction and we investigate electron-phonon coupling under an applied bias voltage during current flow. We find that the electron-phonon coupling strength for this molecular device changes drastically as the bias voltage increases, due to dominant contributions from the center-of-mass vibrational modes of the molecule. Finally, we have investigated the reverse problem, namely the effect of molecular vibrations on the tunneling current. For this purpose we developed the DFT-NEGF-SCBA formalism, and an example is given illustrating the power of this formalism.
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Development of metallic electrodes on KBrFostner, Shawn. January 2005 (has links)
A system for the deposition of metallic electrodes on KBr under ultra-high vacuum conditions has been designed and fabricated. Stencil masks and membranes 4-5 mum thick are fabricated on silicon chips have been created using wet etching in tetramethyl ammonium hydroxide (TMAH) with a boron etch stop. A holding system for UHV has been designed and built with a modified sample holder for performing electrical measurements on samples. The UHV system contains an AFM, STM, and SEM for surface examination and characterization. The growth of metals on KBr was examined using a separately constructed sample holder under high vacuum. Examination of 2.5 and 5 nm tantalum and 20 nm gold films using AFM and SEM revealed significant differences in the film growth and quality. Tantalum films appeared to be continuous, though possessing significant buckling whereas gold films have significant voids and poor edge definition around simple masks.
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Time-dependent quantum transport in mesoscopic structuresMaciejko, Joseph. January 2006 (has links)
In this thesis, we present a theory to calculate the time-dependent current flowing through an arbitrary noninteracting nanoscale phase-coherent device connected to arbitrary noninteracting external leads, in response to sharp step- and square-shaped voltage pulses. Our analysis is based on the Keldysh nonequilibrium Green's functions formalism, and provides an exact analytical solution to the transport equations in the far from equilibrium, nonlinear response regime. The essential feature of our solution is that it does not rely on the commonly used wideband approximation where the coupling between device scattering region and leads is taken to be independent of energy, and as such provides a way to perform transient transport calculations from first principles on realistic systems, taking into account the detailed electronic structure of the device scattering region and the leads. As an illustration of the general theory, we perform a toy model calculation for a quantum dot with Lorentzian linewidth and show how interesting finite-bandwidth effects arise in the time-dependent current dynamics. Finally, we describe possible generalizations of our theory to the cases of superconducting leads (an example of broken symmetry) and one-dimensional leads in the Luttinger liquid regime (an example of an interacting system).
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