The performance of kilometer-scale electron accelerators, which are used for high energy physics and next-generation light sources as well as meter-scale ultra-fast electron diffraction setups is limited by the brightness of electron sources. A potential emerging candidate for such applications is the family of alkali and bi-alkali antimonides. Much of the physics of photoemission from such semiconductor photocathodes is not fully understood even today, which poses a hindrance to the complete exploration and optimization of their photoemission properties. This thesis presents the theoretical and experimental measurements which lead to advances in the understanding of the photoemission process and properties of cesium-antimonide photocathodes. First, the growth of high quantum efficiency (QE), atomically smooth and chemically homogeneous Cs$_3$Sb cathodes on lattice-matched strontium titanate substrates (STO) is demonstrated. The roughness-induced mean transverse energies (MTE) simulations indicate that the contribution to MTE from nanoscale surface roughness of Cs$_3$Sb cathodes grown on STO is inconsequential over typically used field gradients in photoinjectors. Second, the formulation of a new approach to model photoemission from cathodes with disordered surfaces is demonstrated. The model is used to explain near-threshold photoemission from thin film Cs$_3$Sb cathodes. This model suggests that the MTE values may get limited to higher values due to the defect density of states near the valence band maximum. Third, the detailed measurements of MTE and kinetic energy distribution spectra along with QE from Cs$_3$Sb cathodes using the photoemission electron microscope are presented. These measurements indicate that Cs$_3$Sb cathodes have a work function in the range of 1.5-1.6 eV. When photoemitting near this work function energy, the MTE nearly converges to the thermal limit of 26 meV. However, the QE is extremely low, of the order of 10$^{-7}$, which limits the operation of these photocathodes for high current applications. Lastly, the growth of Cs$_3$Sb cathodes using the ion beam assisted molecular beam deposition (IBA-MBE) technique is demonstrated. This technique has the potential to grow epitaxial Cs$_3$Sb cathodes in a more reproducible, easier fashion. Structural characterization of such cathodes via tools such as reflection high energy electron diffraction (RHEED) and x-ray diffraction (XRD) will be necessary to investigate the role of the IBA-MBE technique in facilitating the epitaxial, ordered growth of alkali-antimonides.

The research of this dissertation has primarily involved using transmission electron microscopy (TEM) techniques to study several semiconductor materials considered promising for future photovoltaic device applications.

Layers of gallium phosphide (GaP) grown on silicon (Si) substrates were characterized by TEM and aberration-corrected scanning transmission electron microscopy (AC-STEM). High defect densities were observed for samples with GaP layer thicknesses 250nm and above. Anti-phase boundaries (APBs) within the GaP layers were observed at interfaces with the Si surfaces which were neither atomically flat nor abrupt, contradicting conventional understanding of APB formation.

Microcrystalline-Si (μc-Si) layers grown on crystalline-Si (c-Si) substrates were investigated. Without nanoparticle seeding, an undesired amorphous-Si (a-Si) layer grew below the μc-Si layer. With seeding, the undesired a-Si layer grew above the μc-Si layer, but μc-Si growth proceeded immediately at the c-Si surface. Ellipsometry measurements of percent crystallinity did not match TEM images, but qualitative agreement was found between TEM results and Ultraviolet Raman spectroscopy.

TEM and Xray spectroscopy were used to study metal-induced crystallization and layer exchange for aluminum/ germanium (Al/Ge). Only two samples definitively exhibited both Ge crystallization and layer exchange, and neither process was complete in either sample. The results were finally considered as inconclusive since no reliable path towards layer exchange and crystallization was established.

Plan-view TEM images of indium arsenide (InAs) quantum dots with gallium arsenide antimonide (GaAsSb) spacer layers revealed the termination of some threading dislocations in a sample with spacer-layer thicknesses of 2nm, while a sample with 15-nm-thick spacer layers showed a dense, cross-hatched pattern. Cross-sectional TEM images of samples with 5-nm and 10-nm spacer-layer thicknesses showed less layer undulation in the latter sample. These observations supported photoluminescence (PL) and Xray diffraction (XRD) results, which indicated that GaAsSb spacer layers with 10-nm thickness yielded the highest quality material for photovoltaic device applications.

a-Si/c-Si samples treated by hydrogen plasma were investigated using high-resolution TEM. No obvious structural differences were observed that would account for the large differences measured in minority carrier lifetimes. This key result suggested that other factors such as point defects, hydrogen content, or interface charge must be affecting the lifetimes.

In this dissertation I studied the anomalous Hall effect in MgO/Permalloy/Nonmagnetic Metal(NM) based structure, spin polarized current in YIG/Pt based thin films and the origin of the perpendicular magnetic anisotropy(PMA) in the Ru/Co/Ru based structures.

The anomalous Hall effect is the observation of a nonzero voltage difference across a magnetic material transverse to the current that flows through the material and the external magnetic field. Unlike the ordinary Hall effect which is observed in nonmagnetic metals, the anomalous Hall effect is only observed in magnetic materials and is orders of magnitude larger than the ordinary Hall effect. Unlike quantum anomalous Hall effect which only works in low temperature and extremely large magnetic field, anomalous Hall effect can be measured at room temperature under a relatively small magnetic field. This allows the anomalous Hall effect to have great potential applications in spintronics and be a good characterization tool for ferromagnetic materials especially materials that have perpendicular magnetic anisotropy(PMA).

In my research, it is observed that a polarity change of the Hall resistance in the MgO/Permalloy/NM structure can be obtained when certain nonmagnetic metal is used as the capping layer while no polarity change is observed when some other metal is used as the capping layer. This allows us to tune the polarity of the anomalous Hall effect by changing the thickness of a component of the structure. My conclusion is that an intrinsic mechanism from Berry curvature plays an important role in the sign of anomalous Hall resistivity in the MgO/Py/HM structures. Surface and interfacial scattering also make substantial contribution to the measured Hall resistivity.

Spin polarization(P) is one of the key concepts in spintronics and is defined as the difference in the spin up and spin down electron population near the Fermi level of a conductor. It has great applications in the spintronics field such as the creation of spin transfer torques, magnetic tunnel junction(MTJ), spintronic logic devices.

In my research, spin polarization is measured on platinum layers grown on a YIG layer. Platinum is a nonmagnetic metal with strong spin orbit coupling which intrinsically has zero spin polarization. Nontrivial spin polarization measured by ARS is observed in the Pt layer when it is grown on YIG ferromagnetic insulator. This result is contrary to the zero spin polarization in the Pt layer when it is grown directly on SiO2 substrate. Magnetic proximity effect and spin current pumping from YIG into Pt is proposed as the reason of the nontrivial spin polarization induced in Pt. An even higher spin polarization in the Pt layer is observed when an ultrathin NiO layer or Cu layer is inserted between Pt and YIG which blocks the proximity effect. The spin polarization in the NiO inserted sample shows temperature dependence. This demonstrates that the spin current transmission is further enhanced in ultrathin NiO layers through magnon and spin fluctuations.

Perpendicular Magnetic Anisotropy(PMA) has important applications in spintronics and magnetic storage. In the last chapter, I study the origin of PMA in one of the structures that shows PMA: Ru/Co/Ru. By measuring the ARS curve while changing the magnetic field orientation, the origin of the PMA in this structure is determined to be the strain induced by lattice mismatch.

An electrical current with high spin polarization is desirable for the performance of novel spintronics devices, such as magnetic tunnel junction and giant magnetoresistance devices. The generation of spin polarized current can be from ferromagnetic materials or triplet superconductors.

Anomalous Hall effect (AHE) is an effective way to study the properties of magnetic structures. The scattering of electrons by the magnetic moments affects the change of resistance, which can be used to detect the magnetization. In this dissertation, AHE is used to study the perpendicular magnetic anisotropy (PMA) structures, including Co/Pt and Ta/CoFeB/MgO.

Domain walls exist in all ferromagnetic materials. This dissertation studies the domain wall movement in the Ta/CoFeB/MgO structure. A single domain is observed by measuring the anomalous Hall effect. On the other hand, a zero Hall step is successfully observed in a single layer of magnetic material for the first time, which can be used to fabricate advanced domain wall spintronics devices.

Besides the normal ferromagnetic material, the generation of spin polarized current in superconductor is also important for Spintronics. The electrons in superconductors form Cooper pairs. In this dissertation, Andreev Reflection Spectroscopy (ARS) is used to study the spin configuration in Cooper pairs.

Generally, ferromagnetism and superconductivity can not co-exist. In this dissertation, the Bi/Ni bilayer structure has been studied with ARS, and the measurement results show a triplet superconductivity below 4K. The appearance of superconductivity is believed to be attributed to the Bi-Ni interface, and the triplet Cooper pair makes it a promising candidate in superconducting spintronics.

Besides, a Bi3Ni single crystal is also studied with ARS. The measurements show a singlet superconductivity in this material, which further proves the importance of the Bi/Ni interface to achieve triplet superconductivity.

Finally, ARS is also used to study NbSe2 monolayer, a 2D superconductor. The monolayer is verified by the measurements of critical temperature and critical field, which are different from the values of multilayer or bulk. Andreev reflection results show that NbSe2 monolayer is a singlet superconductor and there is no node exist in the superconducting gap for a in plane magnetic field up to 58 kOe.

In this experiment, an attempt was made to measure the index of refraction of a thin glass microscope slide, with a known thickness of 1.01 mm. A monochromatic laser with wavelength of 532nm was employed to generate the interference pattern through the use of a Michelson interferometer. The slide was placed in the path of one of the beams. The slide could then be rotated through a series of angles, and, from the resulting changes in the interference pattern, the index of refraction of the slide could be extracted. The index of refraction was found to be 1.5±0.02.

A theoretical study of a three-dimensional (3D) N/S interface with arbitrary spin

polarization and interface geometry is presented. The 3D model gives the same intrinsic

spin polarization and superconducting gap dependence as the 1D model. This

demonstrates that the 1D model can be use to t 3D data.

Using this model, a Heusler alloy is investigated. Andreev reflection measurements

show that the spin polarization is 80% in samples sputtered on unheated MgO(100)

substrates and annealed at high temperatures. However, the spin polarization is

considerably smaller in samples deposited on heated substrates.

Ferromagnetic FexSi􀀀x alloys have been proposed as potential spin injectors into

silicon with a substantial spin polarization. Andreev Reflection Spectroscopy (ARS) is

utilized to determine the spin polarization of both amorphous and crystalline Fe65Si35

alloys. The amorphous phase has a significantly higher spin polarization than that of

the crystalline phase.

In this thesis, (1111) Fe SmO0:82F0:18FeAs and Pb superconductors are used to

measure the spin polarization of a highly spin-polarized material, La0:67Sr0:33MnO3.

Both materials yield the same intrinsic spin polarization, therefore, Fe-superconductors

can be used in ARS. Based on the behavior of the differential conductance for highly

spin polarized LSMO and small polarization of Au, it can be concluded that the Fe-Sc

is not a triplet superconductor.

Zero bias anomaly (ZBA), in point contact Andreev reflection (PCAR), has been

utilized as a characteristic feature to reveal many novel physics. Complexities at a

normal metal/superconducting interface often cause nonessential ZBA-like features,

which may be mistaken as ZBA. In this work, it is shown that an extrinsic ZBA,

which is due to the contact resistance, cannot be suppressed by a highly spin-polarized

current while a nonessential ZBA cannot be affected the contact resistance.

Finally, Cu/Cu multilayer GMR structures were fabricated and the GMR% measured

at 300 K and 4.5 K gave responses of 63% and 115% respectively. Not only

do the GMR structures have a large enhancement of resistance, but by applying an

external magnetic eld it is shown that, unlike most materials, the spin polarization

can be tuned to values of 0.386 to 0.415 from H = 0 kOe to H = 15 kOe.

Zeolites are a class of microporous materials that are immensely useful as molecular sieves and catalysts. While there exist millions of hypothetical zeolite topologies, only 206 have been recognized to exist in nature, and the question remains: What distinguishes known zeolite topologies from their hypothetical counterparts? It has been found that all 206 of the known zeolites can be represented as networks of rigid perfect tetrahedra that hinge freely at the connected corners. The range of configurations over which the corresponding geometric constraints can be met has been termed the "flexibility window". Only a small percentage of hypothetical types exhibit a flexibility window, and it is thus proposed that this simple geometric property, the existence of a flexibility window, provides a reliable benchmark for distinguishing potentially realizable hypothetical structures from their infeasible counterparts. As a first approximation of the behavior of real zeolite materials, the flexibility window provides additional useful insights into structure and composition. In this thesis, various methods for locating and exploring the flexibility window are discussed. Also examined is the assumption that the tetrahedral corners are force-free. This is a reasonable approximation in silicates for Si-O-Si angles above ~135°. However, the approximation is poor for germanates, where Ge-O-Ge angles are constrained to the range ~120°-145°. Lastly, a class of interesting low-density hypothetical zeolites is evaluated based on the feasibility criteria introduced.

The energy band gap of a semiconductor material critically influences the operating wavelength of an optoelectronic device. Realization of any desired band gap, or even spatially graded band gaps, is important for applications such as lasers, light-emitting diodes (LEDs), solar cells, and detectors. Compared to thin films, nanowires offer greater flexibility for achieving a variety of alloy compositions. Furthermore, the nanowire geometry permits simultaneous incorporation of a wide range of compositions on a single substrate. Such controllable alloy composition variation can be realized either within an individual nanowire or between distinct nanowires across a substrate. This dissertation explores the control of spatial composition variation in ternary alloy nanowires. Nanowires were grown by the vapor-liquid-solid (VLS) mechanism using chemical vapor deposition (CVD). The gas-phase supersaturation was considered in order to optimize the deposition morphology. Composition and structure were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive x-ray spectroscopy (EDS), and x-ray diffraction (XRD). Optical properties were investigated through photoluminescence (PL) measurements. The chalcogenides selected as alloy endpoints were lead sulfide (PbS), cadmium sulfide (CdS), and cadmium selenide (CdSe). Three growth modes of PbS were identified, which included contributions from spontaneously generated catalyst. The resulting wires were found capable of lasing with wavelengths over 4000 nm, representing the longest known wavelength from a sub-wavelength wire. For CdxPb1-xS nanowires, it was established that the cooling process significantly affects the alloy composition and structure. Quenching was critical to retain metastable alloys with x up to 0.14, representing a new composition in nanowire form. Alternatively, gradual cooling caused phase segregation, which created heterostructures with light emission in both the visible and mid-infrared regimes. The CdSSe alloy system was fully explored for spatial composition variation. CdSxSe1-x nanowires were grown with composition variation across the substrate. Subsequent contact printing preserved the designed composition gradient and led to the demonstration of a variable wavelength photodetector device. CdSSe axial heterostructure nanowires were also achieved. The growth process involved many variables, including a deliberate and controllable change in substrate temperature. As a result, both red and green light emission was detected from single nanowires.

Studying charge transport through single molecules tethered between two metal electrodes is of fundamental importance in molecular electronics. Over the years, a variety of methods have been developed in attempts of performing such measurements. However, the limitation of these techniques is still one of the factors that prohibit one from gaining a thorough understanding of single molecule junctions. Firstly, the time resolution of experiments is typically limited to milli to microseconds, while molecular dynamics simulations are carried out on the time scale of pico to nanoseconds. A huge gap therefore persists between the theory and the experiments. This thesis demonstrates a nanosecond scale measurement of the gold atomic contact breakdown process. A combined setup of DC and AC circuits is employed, where the AC circuit reveals interesting observations in nanosecond scale not previously seen using conventional DC circuits. The breakdown time of gold atomic contacts is determined to be faster than 0.1 ns and subtle atomic events are observed within nanoseconds. Furthermore, a new method based on the scanning tunneling microscope break junction (STM-BJ) technique is developed to rapidly record thousands of I-V curves from repeatedly formed single molecule junctions. 2-dimensional I-V and conductance-voltage (G-V) histograms constructed using the acquired data allow for more meaningful statistical analysis to single molecule I-V characteristics. The bias voltage adds an additional dimension to the conventional single molecule conductance measurement. This method also allows one to perform transition voltage spectra (TVS) for individual junctions and to study the correlation between the conductance and the tunneling barrier height. The variation of measured conductance values is found to be primarily determined by the poorly defined contact geometry between the molecule and metal electrodes, rather than the tunnel barrier height. In addition, the rapid I-V technique is also found useful in studying thermoelectric effect in single molecule junctions. When applying a temperature gradient between the STM tip and substrate in air, the offset current at zero bias in the I-V characteristics is a measure of thermoelectric current. The rapid I-V technique allows for statistical analysis of such offset current at different temperature gradients and thus the Seebeck coefficient of single molecule junctions is measured. Combining with single molecule TVS, the Seebeck coefficient is also found to be a measure of tunnel barrier height.

This research focuses on the stress and structure evolution observed in-situ during the earliest stages of thin film growth in Cu on Au(111)-reconstruction. For the research, an ultra high vacuum-scanning tunneling microscopy (UHV-STM) system was modified to have the additional capabilities of in-situ deposition and in-situ stress evolution monitoring. The design and fabrication processes for the modifications are explained in detail. The deposition source enabled imaging during the deposition of Cu thin films, while also being columnar enough to avoid negatively impacting the function of the microscope. It was found that the stress-induced changes in piezo voltage occurred over a substantially longer time scale and larger piezo scale than used during imaging, allowing for the deconvolution of the two sources of piezo voltage change. The intrinsic stress evolution observed at the onset of Cu growth was tensile in character and reached a maximum of 0.19 N/m at approximately 0.8ML, with an average tensile slope of 1.0GPa. As the film thickness increased beyond 0.8 ML, the stress became less tensile as the observation of disordered stripe and trigon patterns of misfit dislocations began to appear. The transport of atoms from the surface of enlarged Cu islands into the strained layer played an important role in this stage, because they effectively reduce the activation barrier for the formation of the observed surface structures. A rich array of structures were observed in the work presented here including stripe, disordered stripe and trigon patterns co-existing in a single Cu layer. Heteroepitaxial systems in existing literature showed a uniform structure in the single layer. The non-uniform structures in the single layer of this work may be attributed to the room temperature Cu growth, which can kinetically limit uniform pattern formation. The development of the UHV-STM system with additional capabilities for this work is expected to contribute to research for the stress and structure relationships of many other heteroepitaxial systems.