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Description
Fluctuation Electron Microscopy (FEM) has become an effective materials' structure characterization technique, capable of probing medium-range order (MRO) that may be present in amorphous materials. Although its sensitivity to MRO has been exercised in numerous studies, FEM is not yet a quantitative technique. The holdup has been the discrepancy between the computed kinematical variance and the experimental variance, which previously was attributed to source incoherence. Although high-brightness, high coherence, electron guns are now routinely available in modern electron microscopes, they have not eliminated this discrepancy between theory and experiment. The main objective of this thesis was to explore, and to reveal, the reasons behind this conundrum.
The study was started with an analysis of the speckle statistics of tilted dark-field TEM images obtained from an amorphous carbon sample, which confirmed that the structural ordering is sensitively detected by FEM. This analysis also revealed the inconsistency between predictions of the source incoherence model and the experimentally observed variance.
FEM of amorphous carbon, amorphous silicon and ultra nanocrystalline diamond samples was carried out in an attempt to explore the conundrum. Electron probe and sample parameters were varied to observe the scattering intensity variance behavior. Results were compared to models of probe incoherence, diffuse scattering, atom displacement damage, energy loss events and multiple scattering. Models of displacement decoherence matched the experimental results best.
Decoherence was also explored by an interferometric diffraction method using bilayer amorphous samples, and results are consistent with strong displacement decoherence in addition to temporal decoherence arising from the electron source energy spread and energy loss events in thick samples.
It is clear that decoherence plays an important role in the long-standing discrepancy between experimental FEM and its theoretical predictions.
The study was started with an analysis of the speckle statistics of tilted dark-field TEM images obtained from an amorphous carbon sample, which confirmed that the structural ordering is sensitively detected by FEM. This analysis also revealed the inconsistency between predictions of the source incoherence model and the experimentally observed variance.
FEM of amorphous carbon, amorphous silicon and ultra nanocrystalline diamond samples was carried out in an attempt to explore the conundrum. Electron probe and sample parameters were varied to observe the scattering intensity variance behavior. Results were compared to models of probe incoherence, diffuse scattering, atom displacement damage, energy loss events and multiple scattering. Models of displacement decoherence matched the experimental results best.
Decoherence was also explored by an interferometric diffraction method using bilayer amorphous samples, and results are consistent with strong displacement decoherence in addition to temporal decoherence arising from the electron source energy spread and energy loss events in thick samples.
It is clear that decoherence plays an important role in the long-standing discrepancy between experimental FEM and its theoretical predictions.
ContributorsRezikyan, Aram (Author) / Treacy, Michael M.J. (Thesis advisor) / Smith, David J. (Committee member) / McCartney, Martha R. (Committee member) / Rez, Peter (Committee member) / Arizona State University (Publisher)
Created2015
Raman spectroscopy characterization of anharmonicity and alloying effects in semiconductor materials
Description
The chemical sensitivity and spatial resolution of Raman spectroscopy, combined with the sensitivity of modern systems that can easily detect single atomic layers, have made this technique a preferred choice for the strain characterization of complex systems such as nanoscale complementary metal-oxide-semiconductor - CMOS - devices. A disadvantage of Raman spectroscopy, however, is that the shifts associated with strain are not related to the geometrical deformations in any obvious way, so that careful calibrations are needed to determine the anharmonic coefficients (p, q and r) that relate strain to Raman shifts. A new set of measurements of the Raman shift in strained Ge films grown on relaxed SiGe buffer layers deposited on Si substrates is presented, and thereby, a new consistent set of values for the parameters p and q for Ge has been proposed. In this dissertation the study of the vibrational properties of Ge1-xSnx alloys has also been reported. The temperature dependence of the Raman spectrum of Ge-rich Ge1-x Snx and Ge1-x-ySi xSny alloys has been determined in the 10 K - 450 K range. The Raman line shift and width changes as a function of temperature are found to be virtually identical to those observed in bulk Ge. This result shows that the anharmonic decay process responsible for the temperature dependence is extremely robust against the alloy perturbation.
ContributorsBagchi, Sampriti (Author) / Menéndez, Jose (Thesis advisor) / Treacy, Michael (Committee member) / Ponce, Fernando (Committee member) / Tsen, Kong-Thon (Committee member) / Rez, Peter (Committee member) / Arizona State University (Publisher)
Created2011
Description
In this work, a new method, "Nanobonding" [1,2] is conceived and researched to bond Si-based surfaces, via nucleation and growth of a 2 D silicon oxide SiOxHx interphase connecting the surfaces at the nanoscale across macroscopic domains. Nanobonding cross-bridges two smooth surfaces put into mechanical contact in an O2/H2O mixed ambient below T <200 °C via arrays of SiOxHx molecules connecting into a continuous macroscopic bonding interphase. Nano-scale surface planarization via wet chemical processing and new spin technology are compared via Tapping Mode Atomic Force Microscopy (TMAFM) , before and after nano-bonding. Nanobonding uses precursor phases, 2D nano-films of beta-cristobalite (beta-c) SiO2, nucleated on Si(100) via the Herbots-Atluri (H-A) method [1]. beta-c SiO2 on Si(100) is ordered and flat with atomic terraces over 20 nm wide, well above 2 nm found in native oxides. When contacted with SiO2 this ultra-smooth nanophase can nucleate and grow domains with cross-bridging molecular strands of hydroxylated SiOx, instead of point contacts. The high density of molecular bonds across extended terraces forms a strong bond between Si-based substrates, nano- bonding [2] the Si and silica. A new model of beta-cristobalite SiO2 with its <110> axis aligned along Si[100] direction is simulated via ab-initio methods in a nano-bonded stack with beta-c SiO2 in contact with amorphous SiO2 (a-SiO2), modelling cross-bridging molecular bonds between beta-c SiO2 on Si(100) and a-SiO2 as during nanobonding. Computed total energies are compared with those found for Si(100) and a-SiO2 and show that the presence of two lattice cells of !-c SiO2 on Si(100) and a-SiO2 lowers energy when compared to Si(100)/ a-SiO2 Shadow cone calculations on three models of beta-c SiO2 on Si(100) are compared with Ion Beam Analysis of H-A processed Si(100). Total surface energy measurements via 3 liquid contact angle analysis of Si(100) after H-A method processing are also compared. By combining nanobonding experiments, TMAFM results, surface energy data, and ab-initio calculations, an atomistic model is derived and nanobonding is optimized. [1] US Patent 6,613,677 (9/2/03), 7,851,365 (12/14/10), [2] Patent Filed: 4/30/09, 10/1/2011
ContributorsWhaley, Shawn D (Author) / Culbertson, Robert J. (Thesis advisor) / Herbots, Nicole (Committee member) / Rez, Peter (Committee member) / Marzke, Robert F (Committee member) / Lindsay, Stuart (Committee member) / Chamberlin, Ralph V (Committee member) / Arizona State University (Publisher)
Created2011
Description
Many species e.g. sea urchin form amorphous calcium carbonate (ACC) precursor phases that subsequently transform into crystalline CaCO3. It is certainly possible that the biogenic ACC might have more than 10 wt% Mg and ∼ 3 wt% of water. The structure of ACC and the mechanisms by which it transforms to crystalline phase are still poorly understood. In this dissertation our goal is to determine an atomic structure model that is consistent with diffraction and IR measurements of ACC. For this purpose a calcite supercell with 24 formula units, containing 120 atoms, was constructed. Various configurations with substitution of Ca by 6 Mg ions (6 wt.%) and insertion of 3-5 H2O molecules (2.25-3.75 wt.%) in the interstitial positions of the supercell, were relaxed using a robust density function code VASP. The most noticeable effects were the tilts of CO3 groups and the distortion of Ca sub-lattice, especially in the hydrated case. The distributions of Ca-Ca nearest neighbor distance and CO3 tilts were extracted from various configurations. The same methods were also applied to aragonite. Sampling from the calculated distortion distributions, we built models for amorphous calcite/aragonite of size ∼ 1700 nm3 based on a multi-scale modeling scheme. We used these models to generate diffraction patterns and profiles with our diffraction code. We found that the induced distortions were not enough to generate a diffraction profile typical of an amorphous material. We then studied the diffraction profiles from several nano-crystallites as recent studies suggest that ACC might be a random array of nanocryatallites. It was found that the generated diffraction profile from a nano-crystallite of size ∼ 2 nm3 is similar to that from the ACC.
ContributorsSinha, Sourabh (Author) / Rez, Peter (Thesis advisor) / Bearat, Hamdallah A. (Committee member) / Bennett, Peter A. (Committee member) / McCartney, Martha R. (Committee member) / Peng, Xihong (Committee member) / Arizona State University (Publisher)
Created2012
Description
A system for illuminating a sample in situ with visible and UV light inside a transmission electron microscope was devised to study photocatalysts. There are many factors which must be considered when designing and building such a system. These include both mechanical, optical, and electron optical considerations. Some of the restrictions posed by the electron microscope column are significant, and care must be taken not to degrade the microscope's electron optical performance, or to unduly restrict the other current capabilities of the microscope. The nature of these various design considerations is discussed in detail. A description of the system that has been added to the microscope at ASU, an FEI Tecnai F20 environmental transmission electron microscope is also given. The system includes a high brightness broadband light source with optical filters, a fiber to guide the light to the sample, and a system for precisely aligning the fiber tip. The spatial distribution and spectrum of the light reaching the sample has been characterized, and is described in detail.
ContributorsMiller, Benjamin (Author) / Crozier, Peter A. (Thesis advisor) / McCartney, Martha (Committee member) / Rez, Peter (Committee member) / Arizona State University (Publisher)
Created2012
Description
The goal of this theoretical study of infrared spectra was to ascertain to what degree molecules may be identified from their IR spectra and which spectral regions are best suited for this purpose. The frequencies considered range from the lowest frequency molecular vibrations in the far-IR, terahertz region (below ~3 THz or 100 cm-1) up to the highest frequency vibrations (~120 THz or 4000 cm-1). An emphasis was placed on the IR spectra of chemical and biological threat molecules in the interest of detection and prevention. To calculate IR spectra, the technique of normal mode analysis was applied to organic molecules ranging in size from 8 to 11,352 atoms. The IR intensities of the vibrational modes were calculated in terms of the derivative of the molecular dipole moment with respect to each normal coordinate. Three sets of molecules were studied: the organophosphorus G- and V-type nerve agents and chemically related simulants (15 molecules ranging in size from 11 to 40 atoms); 21 other small molecules ranging in size from 8 to 24 atoms; and 13 proteins ranging in size from 304 to 11,352 atoms. Spectra for the first two sets of molecules were calculated using quantum chemistry software, the last two sets using force fields. The "middle" set used both methods, allowing for comparison between them and with experimental spectra from the NIST/EPA Gas-Phase Infrared Library. The calculated spectra of proteins, for which only force field calculations are practical, reproduced the experimentally observed amide I and II bands, but they were shifted by approximately +40 cm-1 relative to experiment. Considering the entire spectrum of protein vibrations, the most promising frequency range for differentiating between proteins was approximately 600-1300 cm-1 where water has low absorption and the proteins show some differences.
ContributorsMott, Adam J (Author) / Rez, Peter (Thesis advisor) / Ozkan, Banu (Committee member) / Shumway, John (Committee member) / Thorpe, Michael (Committee member) / Vaiana, Sara (Committee member) / Arizona State University (Publisher)
Created2012
Description
In this dissertation, various characterization techniques have been used to investigate many aspects of the properties of III-nitride materials and devices for optoelectronic applications.
The first part of this work is focused on the evolution of microstructures of BAlN thin films. The films were grown by flow-modulated epitaxy at 1010 oC, with B/(B+Al) gas-flow ratios ranging from 0.06 to 0.18. The boron content obtained from X-ray diffraction (XRD) patterns ranges from x = 0.02 to 0.09, while Rutherford backscattering spectrometry (RBS) measures x = 0.06 to 0.16. Transmission electron microscopy indicates the sole presence of the wurtzite crystal structure in the BAlN films, and a tendency towards twin formation and finer microstructure for B/(B+Al) gas-flow ratios greater than 0.15. The RBS data suggest that the incorporation of B is highly efficient, while the XRD data indicate that the epitaxial growth may be limited by a solubility limit in the crystal phase at about 9%. Electron energy loss spectroscopy has been used to profile spatial variations in the composition of the films. It has also located point defects in the films with nanometer resolution. The defects are identified as B and Al interstitials and N vacancies by comparison of the observed energy thresholds with results of density functional theory calculations.
The second part of this work investigates dislocation clusters observed in thick InxGa1-xN films with 0.07 ≤ x ≤ 0.12. The clusters resemble baskets with a higher indium content at their interior. Threading dislocations at the basket boundaries are of the misfit edge type, and their separation is consistent with misfit strain relaxation due the difference in indium content between the baskets and the surrounding matrix. The base of the baskets exhibits no observable misfit dislocations connected to the threading dislocations, and often no net displacements like those due to stacking faults. It is argued that the origin of these threading dislocation arrays is associated with misfit dislocations at the basal plane that dissociate, forming stacking faults. When the stacking faults form simultaneously satisfying the crystal symmetry, the sum of their translation vectors does add up to zero, consistent with our experimental observations.
The first part of this work is focused on the evolution of microstructures of BAlN thin films. The films were grown by flow-modulated epitaxy at 1010 oC, with B/(B+Al) gas-flow ratios ranging from 0.06 to 0.18. The boron content obtained from X-ray diffraction (XRD) patterns ranges from x = 0.02 to 0.09, while Rutherford backscattering spectrometry (RBS) measures x = 0.06 to 0.16. Transmission electron microscopy indicates the sole presence of the wurtzite crystal structure in the BAlN films, and a tendency towards twin formation and finer microstructure for B/(B+Al) gas-flow ratios greater than 0.15. The RBS data suggest that the incorporation of B is highly efficient, while the XRD data indicate that the epitaxial growth may be limited by a solubility limit in the crystal phase at about 9%. Electron energy loss spectroscopy has been used to profile spatial variations in the composition of the films. It has also located point defects in the films with nanometer resolution. The defects are identified as B and Al interstitials and N vacancies by comparison of the observed energy thresholds with results of density functional theory calculations.
The second part of this work investigates dislocation clusters observed in thick InxGa1-xN films with 0.07 ≤ x ≤ 0.12. The clusters resemble baskets with a higher indium content at their interior. Threading dislocations at the basket boundaries are of the misfit edge type, and their separation is consistent with misfit strain relaxation due the difference in indium content between the baskets and the surrounding matrix. The base of the baskets exhibits no observable misfit dislocations connected to the threading dislocations, and often no net displacements like those due to stacking faults. It is argued that the origin of these threading dislocation arrays is associated with misfit dislocations at the basal plane that dissociate, forming stacking faults. When the stacking faults form simultaneously satisfying the crystal symmetry, the sum of their translation vectors does add up to zero, consistent with our experimental observations.
ContributorsWang, Shuo, Ph.D (Author) / Ponce, Fernando A. (Thesis advisor) / Menéndez, Jose (Committee member) / Rez, Peter (Committee member) / McCartney, Martha (Committee member) / Arizona State University (Publisher)
Created2018
Description
The inherent risk in testing drugs has been hotly debated since the government first started regulating the drug industry in the early 1900s. Who can assume the risks associated with trying new pharmaceuticals is unclear when looked at through society's lens. In the mid twentieth century, the US Food and Drug Administration (FDA) published several guidance documents encouraging researchers to exclude women from early clinical drug research. The motivation to publish those documents and the subsequent guidance documents in which the FDA and other regulatory offices established their standpoints on women in drug research may have been connected to current events at the time. The problem of whether women should be involved in drug research is a question of who can assume risk and who is responsible for disseminating what specific kinds of information. The problem tends to be framed as one that juxtaposes the health of women and fetuses and sets their health as in opposition. That opposition, coupled with the inherent uncertainty in testing drugs, provides for a complex set of issues surrounding consent and access to information.
ContributorsMeek, Caroline Jane (Author) / Maienschein, Jane (Thesis director) / Brian, Jennifer (Committee member) / School of Life Sciences (Contributor) / Sanford School of Social and Family Dynamics (Contributor) / Barrett, The Honors College (Contributor)
Created2018-05
Description
Social-emotional learning (SEL) methods are beginning to receive global attention in primary school education, yet the dominant emphasis on implementing these curricula is in high-income, urbanized areas. Consequently, the unique features of developing and integrating such methods in middle- or low-income rural areas are unclear. Past studies suggest that students exposed to SEL programs show an increase in academic performance, improved ability to cope with stress, and better attitudes about themselves, others, and school, but these curricula are designed with an urban focus. The purpose of this study was to conduct a needs-based analysis to investigate components specific to a SEL curriculum contextualized to rural primary schools. A promising organization committed to rural educational development is Barefoot College, located in Tilonia, Rajasthan, India. In partnership with Barefoot, we designed an ethnographic study to identify and describe what teachers and school leaders consider the highest needs related to their students' social and emotional education. To do so, we interviewed 14 teachers and school leaders individually or in a focus group to explore their present understanding of “social-emotional learning” and the perception of their students’ social and emotional intelligence. Analysis of this data uncovered common themes among classroom behaviors and prevalent opportunities to address social and emotional well-being among students. These themes translated into the three overarching topics and eight sub-topics explored throughout the curriculum, and these opportunities guided the creation of the 21 modules within it. Through a design-based research methodology, we developed a 40-hour curriculum by implementing its various modules within seven Barefoot classrooms alongside continuous reiteration based on teacher feedback and participant observation. Through this process, we found that student engagement increased during contextualized SEL lessons as opposed to traditional methods. In addition, we found that teachers and students preferred and performed better with an activities-based approach. These findings suggest that rural educators must employ particular teaching strategies when addressing SEL, including localized content and an experiential-learning approach. Teachers reported that as their approach to SEL shifted, they began to unlock the potential to build self-aware, globally-minded students. This study concludes that social and emotional education cannot be treated in a generalized manner, as curriculum development is central to the teaching-learning process.
ContributorsBucker, Delaney Sue (Author) / Carrese, Susan (Thesis director) / Barab, Sasha (Committee member) / School of Life Sciences (Contributor, Contributor) / School of Civic & Economic Thought and Leadership (Contributor) / School of International Letters and Cultures (Contributor) / Barrett, The Honors College (Contributor)
Created2020-05
Description
As of 2019, 30 US states have adopted abortion-specific informed consent laws that require state health departments to develop and disseminate written informational materials to patients seeking an abortion. Abortion is the only medical procedure for which states dictate the content of informed consent counseling. State abortion counseling materials have been criticized for containing inaccurate and misleading information, but overall, informed consent laws for abortion do not often receive national attention. The objective of this project was to determine the importance of informed consent laws to achieving the larger goal of dismantling the right to abortion. I found that informed consent counseling materials in most states contain a full timeline of fetal development, along with information about the risks of abortion, the risks of childbirth, and alternatives to abortion. In addition, informed consent laws for abortion are based on model legislation called the “Women’s Right to Know Act” developed by Americans United for Life (AUL). AUL calls itself the legal architect of the pro-life movement and works to pass laws at the state level that incrementally restrict abortion access so that it gradually becomes more difficult to exercise the right to abortion established by Roe v. Wade. The “Women’s Right to Know Act” is part of a larger package of model legislation called the “Women’s Protection Project,” a cluster of laws that place restrictions on abortion providers, purportedly to protect women, but actually to decrease abortion access. “Women’s Right to Know” counseling laws do not directly deny access to abortion, but they do reinforce key ideas important to the anti-abortion movement, like the concept of fetal personhood, distrust in medical professionals, the belief that pregnant people cannot be fully autonomous individuals, and the belief that abortion is not an ordinary medical procedure and requires special government oversight. “Women’s Right to Know” laws use the language of informed consent and the purported goal of protecting women to legitimize those ideas, and in doing so, they significantly undermine the right to abortion. The threat to abortion rights posed by laws like the “Women’s Right to Know” laws indicates the need to reevaluate and strengthen our ethical defense of the right to abortion.
ContributorsVenkatraman, Richa (Author) / Maienschein, Jane (Thesis director) / Brian, Jennifer (Thesis director) / Abboud, Carolina (Committee member) / Historical, Philosophical & Religious Studies (Contributor) / School of Life Sciences (Contributor, Contributor) / Barrett, The Honors College (Contributor)
Created2020-05