The objective of the present dissertation is to advance the science and engineering of metal-dielectric thin-film structures for ultrafast all-optical applications. The research presented consists of three parts: first, the linear and nonlinear optical (NLO) properties of Au and Ag/Au bilayer metallic thin films are comprehensively studied; then the design and properties of a novel nonlinear device structure are presented and finally an ultrafast all-optical shutter is developed and applications are discussed. In the first part, this study describes the linear and NLO properties of bilayer metallic films and shows that they can be tuned by controlling the mass-thickness ratio between Au and Ag. The combined properties of these bilayers are attractive for active plasmonic applications and nonlinear optical filters. Detailed physical models describing the linear and NLO response of Au and Ag/Au bilayers are presented and compared with experiments. In the second part, these models are used to optimize the NLO response of a novel Au-based NLO device. With only four layers, this novel device strongly amplifies the NLO response of the component Au thin film. NLO devices with broad spectral and angular bandwidths in the visible spectral region are demonstrated. The narrow band dependent NLO response of the NLO device is shown to lead to all-optical controls of high peak-power optical signal pulses. Finally, the NLO device technology is integrated into a novel ultrafast all-optical shutter, which allows temporal opening windows (the time shutter remains open) as short as a few ps. Ultrafast all-optical shutter potentially can temporally shape high peak-power nanosecond optical pulses, which could benefit biomedical and micromachining applications. Other possible optical applications such as short electron, X-ray pulse generations, ultrafast photography, and biomedical imaging will also be discussed.

Thesis (Ph. D.)--University of Alabama at Birmingham, 2008. / Additional advisors: Yogesh K. Vohra, Xu Feng, Jack E. Lemons, Timothy M. Wick. Description based on contents viewed July 8, 2009; title from PDF t.p. Includes bibliographical references.

In the present thesis, we have explored multiple aspects concerning the stochasticity of magnetic domain wall motion during magnetization reversal, all of which originated from our initial study of magnetic field sensing using planar Hall effect. Magnetic field sensors occupy a very important and indispensable position in modern technology. They can be found everywhere, from cellphones to automobiles, electric motors to computer hard disks. At present there are several emerging areas of technology, including biotechnology, which require magnetic field sensors which are at the same time simple to use, highly sensitive, robust under environmental conditions and sufficiently low cost to be deployed on a large scale. Magnetic field sensing using planar Hall effect is one such feasible technology, which we have explored in the course of the thesis. The work was subsequently expanded to cover some fundamental aspects of the stochasticity of domain wall motion, studied with planar Hall effect, which forms the main body of work in the present study. In Chapter 1, we give an introduction to the phenomenology of planar Hall effect, which is the most important measurement technique used for all the subsequent studies. Some early calculations, which had first led to the understanding of anisotropic magnetoresistance and planar Hall effect as being caused by spin-orbit interaction are discussed. In Chapter 2, we discuss briefly the experimental techniques used in the present study for sample growth and fabrication, structural and magnetic characterization, and measurement. We discuss pulsed laser ablation, which is the main technique used for our sample growth. Particular emphasis is given to the instrumentation that was carried out in-house for MOKE and low field magnetotransport (AMR and PHE) measurement. This includes an attempt at domain wall imaging through MOKE microscopy. Some of the standard equipments used for this work, such as the SQUID magnetometer and the acsusceptometer are also discussed in detail. In Chapter 3 we discuss our work on planar Hall sensors that led to the fabrication of a device with a very simple architecture, having transfer characteristics of 650V/A.T in a range of _2Oe. The sensing material was permalloy (Ni81Fe19), and the value had been obtained without using an exchange biased pinning layer. Field trials showed that the devices were capable of geomagnetic field sensing, as well as vehicle detection by sensing the anomaly in Earth's magnetic field caused by their motion. Its estimated detection threshold of 2.5nT made it well suited for several other applications needing high sensitivity in a small area, the most prominent of them being the detection of macromolecules of bio-medical significance. Chapter 4: The work on Barkhausen noise was prompted by reproducibility problems faced during the sensor construction, both between devices as well as within the same device. Study of the stochastic properties led us to the conclusion that the devices could be grouped into two classes: one where the magnetization reversal occurred in a single step, and the other where it took a 0staircase0 like path with multiple steps. This led us to simulations of Barkhausen noise using nucleation models like the RFIM whence it became apparent that the two different groups of samples could be mapped into two regimes of the RFIM distinguished by their magnetization reversal mode. In the RFIM, the nature of the hysteresis loop depends on the degree of disorder, with a crossover happening from single-step switching to multi-step switching at a critical disorder level. Appropriate changes also appear in the Barkhausen noise statistics due to this disorder-induced crossover. By studying the Barkhausen noise statistics for our permalloy samples and comparing them with simulations of the RFIM, we found nearly exact correspondence between the two experimental groups with the two classes resulting from crossing the critical disorder. What remained was to quantify the 0disorder0 level of our samples, which was done through XRD, residual resistivity and a study of electron-electron interaction effects in the resistivity. All these studies led to the conclusion that the samples reversing in multiple steps were more 0defective0 than the other group, at par with the model predictions. This completed the picture with respect to the modeling of the noise. In experiments, it was found that a high rate of film deposition yielded less 0defective0 samples, which severed as an important input for the sensor construction. These results can be viewed from a somewhat broader perspective if we consider the present scenario in the experimental study of Barkhausen noise, or crackling noise in general. Two classes of models exist for such phenomena: front propagation models and nucleation models. Both appear to be very successful when it comes to experiments with bulk materials, while the comparison with experiments on thin films is rather disappointing. It is still not clear whether the models are at fault or the experiments themselves. Through our study, we could demonstrate that there can be considerable variation in the Barkhausen noise character of the same material deposited in the same way, and what was important was the degree of order at the microscopic level. This may be a relevant factor when experimental papers report non-universality of Barkhausen noise in thin films, which can now be interpreted as either insufficient defects or a sample area too small for the study. Chapter 5: Defects in a sample are not the only cause for stochastic behavior during magnetization. In most cases, random thermal 0events0 are also an important factor determining the path to magnetization reversal, which was also true for our permalloy samples. We studied the distribution of the external fields at which magnetization reversal took place in our samples, and tried to explain it in terms of the popular Neel-Brown model of thermal excitation over the anisotropy barrier. The analysis showed that even though the coercivity behaved 0correctly0 in terms of the model predictions, the behavior of the distribution width was anomalous. Such anomalies were common in the literature on switching field distributions, but there seemed to be no unified explanation, with different authors coming up with their own 0exotic0 explanations. We decided to investigate the simplest situations that could result in such a behavior, and through some model-based calculations, came to the conclusion that one of the causes of the anomalies could be the different magnitudes of barrier heights/anisotropy fields experienced by the magnetic domain wall when the reversal occurs along different paths. Though an exact match for the behavior of the distribution width could not be obtained, the extended Neel-Brown model was able to produce qualitative agreement. Chapter 6 contains a study of some interesting 0geometrical0 effects on Barkhausen noise of iron thin films. By rotating the applied magnetic field out-of plane, we could observe the same single-step to multi-step crossover in hysteresis loop nature that was brought about by varying disorder in Chapter 4. We could explain this through simulations of a random anisotropy Ising model, which, apart from exhibiting the usual disorder induced crossover, showed a transition from sub-critical to critical hysteresis loops when the external field direction was rotated away form the average anisotropy direction. Once again, simulation and experiment showed very good agreement in terms of the qualitative behavior. In the second part of this chapter, a study of exchange biased Fe-FeMn system was carried out, where it was observed that the reversal mode has been changed from domain wall motion to coherent rotation. Barkhausen noise was also suppressed. Though many single-domain models existed for this type of reversal, our system was not found to be strictly compatible with them. The disagreement was with regard to the nature of the hysteresis, which, if present, had to be a single step process for a single domain model. The disagreement was naturally attributed to interaction with the nearby magnetic moments, to verify which, simulations were done with a simplified micromagnetic code, which produced excellent agreement with experiment. In Chapter 7, we have studied the temporal properties of Barkhausen avalanches, to compare the duration distributions with simulation. We had used a permalloy sample that was sub-critical according to avalanche size distributions, and our measurement was based on magneto-optic Kerr effect. We measured duration distributions which showed a similar manifestation of finite-size effects as were shown by the size distributions. The power law exponent was calculated, which was deemed 0reasonable0 upon comparison simulations of the sub-critical RFIM. Appendix A contains a study of high-field magnetoresistance of permalloy, which shows that the dominant contribution to magnetoresistance is the suppression of electron-magnon scattering. An interesting correlation is observed between the magnetization of samples and an exchange stiffness parameter d1, that was extracted from magnetoresistance measurements. Here we also re-visit our earlier observation of permalloy thin films possessing a resistance minimum at low temperature. The origin of this minimum is attributed to electron-electron interaction. Appendix B contains the source codes for most of the important programs used for simulation and data analysis. The programs are written in MATLAB and FORTRAN 95. LabView programs used for data acquisition and analysis are not included due to space requirements to display their graphical source codes. Appendix C discusses the studies on a disordered rare-earth oxide LaMnO3. The re-entrant glassy phase is characterized with ac susceptibility and magnetization measurements to extract information about the nature of interactions between the magnetic 0macrospins0 in the system. Appendix D deals with electron scattering experiments performed with spinpolarized electrons (SPLEED) from clean metal surfaces in UHV. A study of the scattering cross sections as a function of energy and scattering angle provides information about spin-orbit and exchange interactions of the electrons with the surface atoms, and can answer important questions pertaining to the electronic and magnetic structure of surfaces. In the course of this study, planar Hall effect is seen to emerge as a powerful tool to study the magnetic state of a thin film, so that it is interesting to apply it to thin films of other materials such as oxides, where magnetization noise studies are next to nonexistent. What also emerged is that there is still a lot of richness present in the details of supposedly well-understood magnetization phenomena, some of which we have explored in this thesis in the context of stochastic magnetization processes.

O caráter aleatório e não homogêneo do crescimento de filmes finos, por processo de deposição, leva à formação de uma superfície rugosa que obedece, em geral, a uma geometria fractal. A dinâmica de crescimento da superfície do filme pode ser descrita por meio de modelos de crescimento discretos, simulações numéricas e equações diferenciais estocásticas. Os modelos e as equações nos fornecem os expoentes críticos, que descrevem o comportamento da rugosidade com a escala de observação e tempo de deposição. Crescemos filmes de platina e ouro através da técnica de implantação e deposição de íons por imersão em plasma metálico. Determinamos experimentalmente os expoentes críticos por meio de microscopia de tunelamento. Comparamos os nossos resultados experimentais com previsões dadas por alguns modelos teóricos. Verificamos que há um bom acordo entre eles e as previsões dadas pela equação estocástica de Kardar, Parisi e Zhang. A estrutura cristalina dos materiais também foi analisada por meio de difração de raios x. / The randomness and inhomogeneities in the growth of thin films generate a rough surface obeying, in general, fractal geometry. The growth dynamics of film surface can be described by theoretical discrete models, numerical simulations and stochastic differential equations. Models and equations give the critical exponents that describe the behavior of roughness with the observation scale and deposition time. We have synthesized platinum and gold films by metal plasma immersion ion implantation and deposition. We have measured the critical exponents by Scanning Tunneling Microscopy. Our experimental results were compared with some theoretical models predictions. We verified that there is a good agreement between them and the theoretical predictions given by the Kardar, Parisi and Zhang stochastic equation. The crystallographic structure was also analyzed by X-ray diffraction.

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The scaling down of Complementary Metal Oxide Semiconductor (CMOS) transistors to sub-100nm requires replacement of conventional Silicon dioxide layer with high dielectric constant (K) material for gate dielectric. Among the various high-K dielectrics that have been studied, HfO2 is found to be a promising candidate because of its high dielectric constant (~25), large band gap (5.68 eV), thermodynamic stability and good interface with Si. The HfO2 films have already been deposited using different growth techniques such as Atomic layer Deposition (ALD), Metalorgonic Chemical Vapor Deposition (MOCVD) and Pulsed Laser Deposition (PLD). Ion Assisted Deposition (IAD) is a novel technique that has been successfully employed to produce optical coatings of required quality. This growth technique presents many advantages over the other techniques such as formation from solid oxide sources, low growth temperatures (25-3000C) and film densification by ion bombardment. Hence this technique has been used to prepare HfO2 films in the present investigations. This thesis presents the structural, optical and electrical properties of HfO2 thin films prepared by Ion assisted deposition (IAD). The suitability of Ion assisted deposition process and the importance of investigations on the influence of process parameters on the film characteristics have been brought out in the process parameters-structure-composition and properties correlation presented in this thesis. The aim of this work is to process and characterize HfO2 films and investigate the influence of process parameters on the structure, composition and properties of the films to identify their suitability for CMOS gate applications. HfO2 films were deposited on p-type Si (100) wafers by Ion assisted deposition in an electron beam evaporation (Leybold,L-560) system. Pre-bombardment of the substrates with Argon ions has been done to remove any native oxide layer formation on Silicon by using a hallow cathode ion source (DENTON VACUUM CC103). During the film deposition a collimated oxygen ion beam, generated from the ion source is directed towards the substrate. The oxygen ion current is controlled by adjusting the voltage applied to the ion source and the oxygen flow through the ion source. The oxygen ions bombard the film as it grows and in that process improves its packing density as well as its stoichiometry. Keeping the deposition rate and thickness constant, HfO2 films have been deposited by varying Ion Current, Ion energy and substrate temperature. MOS capacitors were fabricated with Aluminum as gate electrode deposited by thermal evaporation. Ellipsometry techniques have been used to measure the optical thickness of the films. The interfacial layer (IL) formed at the HfO2/ Si interface was investigated by using Fourier transform Infrared spectroscopy (FT-IR). The structural characterization was carried out by X-ray diffraction technique. The high frequency capacitance-voltage and DC leakage current characteristics were measured to analyze the electrical characteristics of MOS capacitors. The effect of post deposition annealing (PDA) of the films at 600°C and 700ºC in Forming Gas (15%H2+85%N2) ambient and Post metallization annealing (PMA) at 400ºC in the same ambient was also investigated to observe the changes in electrical characteristics. The initial step of this work was to compare the characteristics of the films deposited by reactive evaporation and Ion assisted deposition which confirmed the superiority of the quality of IAD coatings and justified the need to proceed further with a more detailed study on the influence of various parameters on the properties of IAD coatings. HfO2 films deposited on substrates maintained at 1000C exhibited better structural, Optical and Electrical properties. The leakage current in these films were lower which has been attributed to silicate free interface as confirmed by XRD studies. Investigations on films deposited with oxygen ion beams of different currents in the range 20 to 40mA indicated that the films deposited at 20mA ion current showed better electrical properties. Better stoichiometry of these films as indicated by FT IR studies was one of the reasons for their improved performance. Annealing of these films at 6000C and 7000C in FGA medium resulted in creation of silicates and silicides at the interface thereby increasing the leakage currents and degraded the film properties. The films deposited with oxygen ion beams generated with a driving voltage 265V showed better structural and optical properties with silicate free interface compared with low and high driving voltages. Among all the films, the maximum dielectric constant of about 21.9 with a minimum EOT of 5.5 nm corresponding to a film deposited at ion current 20mA with PMA 400°C in FG ambient for 20minites is achieved. The lowest value of interface charge density achieved is 2.7 x1012 per cm-2 eV-1 corresponding to the sample deposited at substrate temperature 100°C with deposition rate of 0.5Å/sec followed by post metallization annealing at 400°C in forming gas for 20minutes. The range of Dit values that were obtained are varying from 2.7x 1012 – 16.7x1012 cm-2eV-1.It was also found that, the samples deposited at higher ion currents show lower Dit values than the samples deposited at lower ion currents. From the I−V analysis, the leakage current density is found to be comparatively less in IAD than in reactive evaporation. Leakage current increases with increase in substrate temperature and the same trend is observed with annealed films also. The lowest leakage current density of 1.05x10–8 A/cm2 at a gate bias of 1V was observed in the films deposited at substrate temperature 1000C. The present thesis focused on the suitability of the Ion Assisted deposition process for the preparation of HfO2 films for high-K gate dielectric application and the importance of investigations on the influence of process parameters on the film characteristics.

Ce travail de thèse porte sur l'étude et la réalisation de micro-capteurs d'accélération à détection thermique. Ils sont basés sur la modification des échanges thermiques par convection naturelle dans un fluide chauffé localement lorsque le dispositif est soumis à une accélération.L'utilisation d'un fluide comme masse sismique est en rupture avec les concepts d'accéléromètres dits traditionnels. Cet avantage a pour conséquence directe leur tenue aux fortes accélérations.Un des objectifs de ce travail consiste à développer et à caractériser des accéléromètres à grande étendue de mesures (> 10 000 g). D'autre part, des études fondamentales menées en parallèle nous ont permis de mieux comprendre les phénomènes thermiques intervenant dans la cavité ainsi que d'en déduire l'effet des paramètres thermo-physiques du fluide, des conditions expérimentales et des dimensions géométriques du capteur sur la sensibilité et la bande passante.Par ailleurs, l'étude de nouveaux concepts de détection thermique basés sur l'utilisation de matériaux pyroélectriques a été entreprise pour aboutir à une amélioration de la sensibilité comme de la bande passante. Après la maîtrise des dépôts en couches minces, ce nouveau mode de détection a été mis en œuvre et le principe validé. / This PhD thesis deals with both study and fabrication of micro-accelerometers based on thermal convection. Under acceleration, convective heat transfer in a locally heated fluid is modified and induces a change in temperature profile. Using a fluid as seismic mass enhances better performances than traditional accelerometers in term of high shock reliability.One goal is to develop and characterize high-g accelerometers (> 10,000 g). Besides, analytical studies carried out in parallel have allowed us to improve our understanding of fluid thermal behaviour. Effects of thermo-physical parameters, experimental set-up and sensor size on both sensitivity and bandwidth were deduced.On the other hand, a new concept of thermal detection based on the use of pyroelectric material was undertaken to improve sensor sensitivity as well as bandwidth. First the thin-film sputtering process is developed. Then the pyroelectric thermal accelerometer principle is confirmed.

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Doctor of Philosophy / Department of Chemistry / Takashi Ito / We have investigated the orientation of cylindrical domains in thin films of a polystyrene–poly(methylmethacrylate) diblock copolymer (PS-b-PMMA) on planar substrates having different surface roughnesses and hydrophilicities. The research in this dissertation covers the substrate surface modifications, the enhancement of the diblock copolymer film coating, and the refinement of the treatments leading to nanoporous material. Treatment of the substrate with organic mercaptans forming self-assembled-monolayer (SAM), leading to various hydrophilicities of the surfaces, was inconclusive as far as orienting the PMMA domains in the PS matrix due to thermal instability of some thiols. This directed us to a different approach involving substrate roughness. PS-b-PMMA films of 20~200 nm thick were prepared via spin-coating on silicon, gold or indium tin oxide (ITO) substrates, and annealed in vacuum at 170 °C for 60 hours to induce the formation of cylindrical PMMA domains. Atomic force microscopy (AFM) images indicated the domain orientation at the free surface. In PS-b-PMMA films much thicker than the domain periodicity (L0), the domains were oriented perpendicularly to the free surface regardless of underlying substrates, reflecting the balanced interactions of PS and PMMA blocks at the polymer–vacuum interface. In films having thickness similar to L0, vertically oriented domains were observed on the Au and ITO surfaces that are covered with nanoscale grains, whereas horizontal domains were observed on the smooth Si substrates. In particular, the cylindrical PMMA domains were efficiently perpendicularly aligned when the grain size nearly was equal to L0. The perpendicular domain alignment induced by the substrate roughness was corroborated using cyclic voltammetry (CV) for gold substrates coated with PS-b-PMMA films whose PMMA domains were removed by UV and subsequent acetic acid treatments. The CV data also suggested that the PMMA domains were successfully removed, leaving a nanoporous stable PS matrix on the substrate.