Browsing by Subject "STM"
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Item Alignment of micro-crystals of Mn12-acetate and direct observation of single molecules thereof(2009-05-15) Seo, DongminThis dissertation focuses on three separate studies. First, magnetization of the Mn12- acetate was studied by low temperature hysteresis loops and DC magnetization data on magnetically aligned Mn12-acetate micro-crystals. Secondly, Mn12-acetate thin films were fabricated and characterized by AFM and STM. Finally, magnetization of the film material was also studied. Enhanced alignment of Mn12-acetate micro-crystals as compared to prior studies was verified by observation of several sharp steps in low temperature hysteresis loops. It was found that ~ 0.5 T is sufficient to orient the micro-crystals in an organic solvent to a degree comparable to a single crystal. The degree of the alignment was controlled by varying the magnetic field at room temperature and during the cooling process. Subsequently, low temperature hysteresis loops and DC magnetizations were measured for each prepared orientation state of a sample. The high temperature magnetic anisotropy responsible for the alignment could not be measured, possibly due to its small magnitude. Mn12-acetate was deposited onto Si/SiO2 by a solution evaporation method. Atomic force microscopy studies revealed that 2 nm thick films of molecular level smoothness were formed. Mn12-acetate was also deposited onto a Highly Ordered Pyrolytic Graphite (HOPG) surface for scanning tunneling microscopy (STM) studies. A self-assembled triangular lattice was observed in the Mn12-acetate thin films by STM at room temperature under ambient conditions. These STM images show typical center to center intermolecular separations of about 6.3 nm and height corrugation of less than 0.5 nm. Magnetization measurements were not successful in Mn12-acetate thin films due to the small amount of material in the film and the large background signal from the substrate. Therefore, a sample for the magnetization measurements, called ?film material?, was made by evaporating a dilute solution of Mn12-acetate powder in acetonitrile. Significant changes in magnetic properties of the film material were observed from magnetization measurements. The blocking temperature of the film material was found to increase to TB > 10 K at low magnetic fields.Item An Experimental Study of Mn12-Family Molecular Magnets in Isolation with High Spatial Resolution(2014-12-17) Reaves, Kelley ThomasI report my studies of Mn12O12(C6H5COO)16(H2O)4, which will be referred to as Mn12-Ph, a single molecule magnet, on Cu(111) and HOPG (highly oriented pyrolytic graphite) surfaces by scanning tunneling microscopy (STM). A technique of vacuum spray injection for room temperature deposition of films of a tunable density, between very diffuse isolated molecules and complete surface coverage, onto sample substrates was developed and used to create sub-monolayer films of Mn12-Ph on Cu(111) for low temperature observation. Scanning tunneling spectroscopy (STS) of samples at low temperatures produced insights into the local density of states (LDOS) with a high degree of precision with spatial location (X,Y,Z) and energy (eV).These spectroscopic data were analyzed and compared to results in the literature from competing groups. A theoretical model of spinstability in an interacting graph of spins was developed and simulations were carried out to find a weak topological invariant to perturbation of a given spinstate for a class of ferromagnetically interacting spingraphs. A phenomenological (post hoc) model built upon poor coupling between the molecule's wave function and the Cu surface wave function is proposed to explain the spectroscopic data. Normalized (to the Cu background) junction impedance is calculated and compared in different regions of the molecular interior to form a better view of the evolution of the tunnel junction current with respect to applied bias voltage.Item Charge Transport through Organized Organic Assemblies in Confined Geometries(2012-07-16) Schuckman, Amanda EileenOrganic molecules such as porphyrins and alkanethiols are currently being investigated for applications such as sensors, light-emitting diodes and single electron transistors. Porphyrins are stable, highly conjugated compounds and the choice of metal ion and substituents bound to the macrocycle as well as other effects such as chemical surrounding and cluster size modulate the electronic and photonic properties of the molecule. Porphyrins and their derivatives are relatively non-toxic and their very rich photo- and electro-chemistry, and small HOMO-LUMO gaps make them outstanding candidates for use in molecularly-enhanced electronic applications. For these studies, self-assembled tri-pyridyl porphyrin thiol derivatives have been fully characterized on Au(111) surfaces. A variety of surface characterization techniques such as Atomic Force Microscopy (AFM), Scanning Tunneling Microscopy (STM), FT-IR spectroscopy and X-ray photoelectron spectroscopy (XPS) have been implemented in order to obtain information regarding the attachment orientation based on the angle and physical height of the molecule, conductivity which is determined based on the apparent height and current-voltage (I-V) measurements of the molecule, conductance switching behavior due to conformational or other effects as well as the stability of the molecular ensembles. Specifically, the transport properties of free base and zinc coordinated tri-pyridyl porphyrin thiol molecular islands inserted into a dodecanethiol matrix on Au(111) were investigated using STM and cross-wire inelastic electron tunneling spectroscopy (IETS). The zinc porphyrin thiol islands observed by STM exhibited reversible bias induced switching at high surface coverage due to the formation of Coulomb islands of ca. 10 nm diameter driven by porphyrin aggregation. Low temperature measurements (~ 4 K) from crossed-wire junctions verified the appearance of a Coulomb staircase and blockade which was not observed for single molecules of this compound or for the analogous free base. Scanning probe lithography via nanografting has been implemented to directly assemble nanoscale patterns of zinc porphyrin thiols and 16-mercapotohexadecanoic acid on Au surfaces. Matrix effects during nanopatterning including solvent and background SAMs have been investigated and ultimately ~ 10 nm islands of zinc porphyrins have been fabricated which is the optimal size for the observed switching effect.Item Construction and assembly of a scanning tunneling microscope(2011-08) Ponath, Patrick; Demkov, Alexander A.; de Lozanne, Alejandro L.In the scope of this master thesis, a home-made brass scanning tunneling microscope (STM) was machined, assembled and tested for its functionality. For this microscope, a new approach-technique was used which follows the design suggested by Pan. The difference to Pan's design is the use of piezoplates, instead of piezostacks. Hence, the approach is still based on the stick and slip motion, but it allows the microscope to be more compact. A new and simple electronic circuit, in order to control the approach, is presented and was put together. This circuit is based on mechanical relays, which provide a sufficient long time gap between the single moving steps, due to their mechanical functional principle. Subsequently the approach-technique and the scanning was successfully tested. Finally, first images of HOPG were taken under ambient conditions.Item Design and Construction of a Low Temperature Scanning Tunneling Microscope(2010-10-12) Chen, ChiA low temperature scanning tunneling microscope (LTSTM) was built that we could use in an ultra high vacuum (UHV) system. The scanning tunneling microscope (STM) was tested on an existing 3He cryostat and calibrated at room, liquid nitrogen and helium temperatures. We analyzed the operational electronic and vibration noises and made some effective improvements. To demonstrate the capabilities of the STM, we obtained atomically resolved images of the Au (111) and graphite surfaces. In addition, we showed that the stable tunneling junctions can be formed between the Pt/Ir tip and a superconducting thin film PbBi. We observed the atomic corrugation on Au (111) and measured the height of the atomic steps to be approximately2.53?, which agrees with published values. In our images of the graphite surface, we found both the ? atoms triangular structure, as well as the complete ?-? hexagonal unit cell, using the same tip and the same bias voltage of 0.2V. The successful observation of the hidden ? atoms of graphite is encouraging in regards to the possibility of imaging other materials with atomic resolution using our STM. We also demonstrated that stable tunneling junctions can be formed at various temperatures. To demonstrate this, the superconducting current-voltage and differential conductance-voltage characteristics of a PbBi film were measured from 1.1K to 9K From this data, the temperature dependent energy gap of the superconductor was shown to be consistent with the predictions of the Bardeen, Cooper, and Schrieffer (BCS) theory.Item Quantum tunneling, quantum computing, and high temperature superconductivity(Texas A&M University, 2005-02-17) Wang, QianIn this dissertation, I have studied four theoretical problems in quantum tunneling, quantum computing, and high-temperature superconductivity. I have developed a generally-useful numerical tool for analyzing impurity-induced resonant-state images observed with scanning tunneling microscope (STM) in high temperature superconductors. The integrated tunneling intensities on all predominant sites have been estimated. The results can be used to test the predictions of any tight-binding model calculation. I have numerically simulated two-dimensional time-dependent tunneling of a Gaussian wave packet through a barrier, which contains charged ions. We have found that a negative ion in the barrier directly below the tunneling tip can deflect the tunneling electrons and drastically reduce the probability for them to reach the point in the target plane directly below the tunneling tip. I have studied an infinite family of sure-success quantum algorithms, which are introduced by C.-R. Hu [Phys. Rev. A {\bf 66}, 042301 (2002)], for solving a generalized Grover search problem. Rigorous proofs are found for several conjectures made by Hu and explicit equations are obtained for finding the values of two phase parameters which make the algorithms sure success. Using self-consistent Hartree-Fock theory, I have studied an extended Hubbard model which includes quasi-long-range Coulomb interaction between the holes (characterized by parameter V). I have found that for sufficiently large V/t, doubly-charged-antiphase-island do become energetically favored localized objects in this system for moderate values of U/t, thus supporting a recent conjecture by C.-R. Hu [Int. J. Mod. Phys. B {\bf 17}, 3284 (2003)].Item Scanning tunneling microscopy of Bi₂Se₃ and CuxBi₂Se₃(2013-08) Mann, Christopher William; Shih, Chih-KangRecently, Bi₂Se₃ was added to a new class of materials known as topological insulators. While several studies have provided tantalizing hints towards novel physical properties, such as backscatter suppression and spin-polarized transport, several concerns remain in actual materials. In particular, high defect densities, strong surface band bending, and potential fluctuations have been observed. Here, scanning tunneling microscopy and spectroscopy are used to reveal surface effects in Bi₂Se₃ and CuxBi₂Se₃. First, a detailed examination of defects in bulk-grown samples is described. Then, I provide an analysis of molecular beam epitaxy results, done in collaboration with colleague Yuxuan Chen. Following this, I provide a detailed study of individual point defects in Cu-doped Bi₂Se₃ and examine how Cu is incorporated into the Bi₂Se₃ lattice. Finally, through spectroscopic analysis, a novel depth-sensitive measurement of the local band bending field is developed. Furthermore, for the first time, fluctuations of the Dirac point can be correlated to specific near-surface defects, namely Se vacancies. These analyses provide valuable insights into the preparation of future samples for the investigation of topological insulators.Item Scanning Tunneling Microscopy Studies of Metal Clusters Supported on Graphene and Silica Thin Film(2012-10-19) Zhou, ZihaoThe understanding of nucleation and growth of metals on a planar support at the atomic level is critical for both surface science research and heterogeneous catalysis studies. In this dissertation, two planar substrates, including graphene and ultra-thin silica film were employed for supported model catalysts studies. The structure and stability of several catalytically important metals supported on these two substrates were thoroughly investigated using scanning tunneling microscopy (STM) coupled with other traditional surface science techniques. In the study of the graphene/Ru(0001) system, the key factors that govern the growth and distribution of metals on the graphene have been studied based on different behaviors of five transition metals, namely Pt, Rh, Pd, Co, and Au supported on the template of a graphene moire pattern formed on Ru(0001). Both metal-carbon (M-C) bond strength and metal cohesive energies play significant roles in the cluster formation process and the M-C bond strength is the most important factor that affects the morphology of clusters at the initial stages of growth. Interestingly, Au exhibits two-dimensional (2-D) structures that span several moire unit cells. Preliminary data obtained by dosing molecular oxygen onto CO pre-covered Au islands suggest that the 2-D Au islands catalyze the oxidation of CO. Moreover, graphene/Ru(0001) system was modified by introducing transition metals, oxygen or carbon at the interface between the graphene and Ru(0001). Our STM results reveal that the geometric and/or electronic structure of graphene can be adjusted correspondingly. In the study of the silica thin film system, the structure of silica was carefully investigated and our STM images favor for the [SiO4] cluster model rather than the network structure. The nucleation and adsorption of three metals, namely Rh, Pt and Pd show that the bond strength between the metal atom and Si is the key factor that determines the nucleation sites at the initial stages of metal deposition. The annealing effect studies reveal that Rh and Pt atoms diffuse beneath the silica film and form the 2-D islands that are covered with a silica thin film. In contrast, the formation of Pd silicide was observed upon annealing to high temperatures.Item Scanning tunneling microscopy studies on the structure and stability of model catalysts(2009-05-15) Yang, FanAn atomic level understanding of the structure and stability of model catalysts is essential for surface science studies in heterogeneous catalysis. Scanning tunneling microscopy (STM) can operate both in UHV and under realistic pressure conditions with a wide temperature span while providing atomic resolution images. Taking advantage of the ability of STM, our research focuses on 1) investigating the structure and stability of supported Au catalysts, especially under CO oxidation conditions, and 2) synthesizing and characterizing a series of alloy model catalysts for future model catalytic studies. In our study, Au clusters supported on TiO2(110) have been used to model supported Au catalysts. Our STM studies in UHV reveal surface structures of TiO2(110) and show undercoordinated Ti cations play a critical role in the nucleation and stabilization of Au clusters on TiO2(110). Exposing the TiO2(110) surface to water vapor causes the formation of surface hydroxyl groups and subsequently alters the growth kinetics of Au clusters on TiO2(110). STM studies on Au/TiO2(110) during CO oxidation demonstrate the real surface of a working catalyst. Au clusters supported on TiO2(110) sinter rapidly during CO oxidation, but are mostly stable in the single component reactant gas, either CO or O2. The sintering kinetics of supported Au clusters has been measured during CO oxidation and gives an activation energy, which supports the mechanism of CO oxidation induced sintering. CO oxidation was also found to accelerate the surface diffusion of Rh(110). Our results show a direct correlation between the reaction rate of CO oxidation and the diffusion rate of surface metal atoms. Synthesis of alloy model catalysts have also been attempted in our study with their structures successfully characterized. Planar Au-Pd alloy films has been prepared on a Rh(100) surface with surface Au and Pd atoms distinguished by STM. The growth of Au-Ag alloy clusters have been studied by in-situ STM on a cluster-to-cluster basis. Moreover, the atomic structure of a solution-prepared Ru3Sn3 cluster has been resolved on an ultra-thin silica film surface. The atomic structure and adsorption sites of the ultrathin silica film have also been well characterized in our study.