Dataset on density functional theory investigation of ternary Heusler alloys.

This paper contains data and results from Density Functional Theory (DFT) investigation of 423 distinct X2YZ ternary full Heusler alloys, where X and Y represent elements from the D-block of the periodic table and Z signifies element from main group. The study encompasses both "regular" and "inverse" Heusler phases of these alloys for a total of 846 potential materials. For each specific alloy and each phase, a range of information is provided including total energy, formation energy, lattice constant, total and site-specific magnetic moments, spin polarization as well as total and projected density of electronic states. The aim of creating this dataset is to provide fundamental theoretical insights into ternary X2YZ Heusler alloys for further theoretical and experimental analysis.

Stearic Acid as an Atomic Layer Deposition Inhibitor: Spectroscopic Insights from AFM-IR.

Modern-day chip manufacturing requires precision in placing chip materials on complex and patterned structures. Area-selective atomic layer deposition (AS-ALD) is a self-aligned manufacturing technique with high precision and control, which offers cost effectiveness compared to the traditional patterning techniques. Self-assembled monolayers (SAMs) have been explored as an avenue for realizing AS-ALD, wherein surface-active sites are modified in a specific pattern via SAMs that are inert to metal deposition, enabling ALD nucleation on the substrate selectively. However, key limitations have limited the potential of AS-ALD as a patterning method. The choice of molecules for ALD blocking SAMs is sparse; furthermore, deficiency in the proper understanding of the SAM chemistry and its changes upon metal layer deposition further adds to the challenges. In this work, we have addressed the above challenges by using nanoscale infrared spectroscopy to investigate the potential of stearic acid (SA) as an ALD inhibiting SAM. We show that SA monolayers on Co and Cu substrates can inhibit ZnO ALD growth on par with other commonly used SAMs, which demonstrates its viability towards AS-ALD. We complement these measurements with AFM-IR, which is a surface-sensitive spatially resolved technique, to obtain spectral insights into the ALD-treated SAMs. The significant insight obtained from AFM-IR is that SA SAMs do not desorb or degrade with ALD, but rather undergo a change in substrate coordination modes, which can affect ALD growth on substrates.

Determining the Thermal Properties of Buckypapers Used in Photothermal Desorption.

Volatile organic compounds (VOCs) pose an occupational exposure risk due to their commonplace usage across industrial and vocational sectors. With millions of workers annually exposed, monitoring personal VOC exposures becomes an important task. As such, there is a need to improve current monitoring techniques by increasing sensitivity and reducing analysis costs. Recently, our lab developed a novel, preanalytical technique known as photothermal desorption (PTD). PTD uses pulses of high-energy, visible light to thermally desorb analytes from carbonaceous sorbents, with single-walled carbon nanotube buckypapers (BPs) having the best overall performance. To apply this new technology most effectively for chemical analysis, a better understanding of the theoretical framework of the thermal phenomena behind PTD must be gained. The objectives of the present work were 3-fold: measure the thermal response of BPs during irradiation with light; determine the best method for conducting such measurements; and determine the thermal conductivity of BPs. BPs were exposed to four energy densities, produced by light pulses, ranging from 0.28 to 1.33 J/cm2, produced by a xenon flash lamp. The resulting temperature measurements were obtained via fast response thermocouple (T/C) mounted to BPs by three techniques (pressing, adhering, and embedding). Temperature increase measured by T/C using the adhering and pressing techniques resulted in similar values, 29.2 ± 0.8 to 56 ± 3 °C and 29.1 ± 0.9 to 50 ± 5 °C, respectively, while temperature increase measured by embedding the T/C into the BP showed statistically larger increases ranging from 35.2 ± 0.9 to 76 ± 4 °C. Peak BP temperatures for each mounting technique were also compared with the temperatures generated by the light source, which resulted in embedded BPs demonstrating the most temperature conversion among the techniques (74-86%). Based on these results, embedding T/Cs into the BP was concluded to be the best way to measure BP thermal response during PTD. Additionally, the present work modeled BP thermal conductivity using a steady-state comparative technique and found the material's conductivity to be 10.6 ± 0.6 W/m2. The present work's findings will help pave the way for future developments of the PTD method by allowing calculation of the energy density necessary to attain a desired sorbent temperature and providing a means for comparing BP fabrication techniques and evaluating BP suitability for PTD before conducting PTD trials with analytes of interest. Sorbents with greater thermal conductivity are expected to desorb more evenly and withstand higher energy density exposures.

Demonstration of nearly pinhole-free epitaxial aluminum thin films by sputter beam epitaxy.

Superconducting resonators with high quality factors have been fabricated from aluminum films, suggesting potential applications in quantum computing. Improvement of thin film crystal quality and removal of void and pinhole defects will improve quality factor and functional yield. Epitaxial aluminum films with superb crystallinity, high surface smoothness, and interface sharpness were successfully grown on the c-plane of sapphire using sputter beam epitaxy. This study assesses the effects of varying substrate preparation conditions and growth and prebake temperatures on crystallinity and smoothness. X-ray diffraction and reflectivity measurements yield extensive Laue oscillations and Kiessig thickness fringes for films grown at 200 °C under 15 mTorr Ar, indicating excellent crystallinity and surface smoothness; moreover, an additional substrate preparation procedure which involves (1) a modified substrate cleaning procedure and (2) prebake at 700 °C in 20 mTorr O2 is shown by atomic force microscopy to yield nearly pinhole-free film growth while maintaining epitaxy and high crystal quality. The modified cleaning procedure is environmentally friendly and eliminates the acid etch steps common to conventional sapphire preparation, suggesting potential industrial application both on standard epitaxial and patterned surface sapphire substrates.

Conductivitylike Gilbert Damping due to Intraband Scattering in Epitaxial Iron.

Confirming the origin of Gilbert damping by experiment has remained a challenge for many decades, even for simple ferromagnetic metals. Here, we experimentally identify Gilbert damping that increases with decreasing electronic scattering in epitaxial thin films of pure Fe. This observation of conductivitylike damping, which cannot be accounted for by classical eddy-current loss, is in excellent quantitative agreement with theoretical predictions of Gilbert damping due to intraband scattering. Our results resolve the long-standing question about a fundamental damping mechanism and offer hints for engineering low-loss magnetic metals for cryogenic spintronics and quantum devices.

Room Temperature Skyrmions in Strain-Engineered FeGe thin films.

Skyrmions hold great promise for low-energy consumption and stable high density information storage, and stabilization of the skyrmion lattice (SkX) phase at or above room temperature is greatly desired for practical use. The topological Hall effect can be used to identify candidate systems above room temperature, a challenging regime for direct observation by Lorentz electron microscopy. Atomically ordered FeGe thin films are grown epitaxially on Ge(111) substrates with ~ 4 % tensile strain. Magnetic characterization reveals enhancement of Curie temperature to 350 K due to strain, well above the bulk value of 278 K. Strong topological Hall effect was observed between 10 K and 330 K, with a significant increase in magnitude observed at 330 K. The increase in magnitude occurs just below the Curie temperature, a similar relative temperature position as the onset of Skx phase in bulk FeGe. The results suggest that strained FeGe films may host a SkX phase above room temperature when significant tensile strain is applied.

Sensing of NO2 with zirconium hydroxide via frequency-dependent electrical impedance spectroscopy.

Zirconium hydroxide has been investigated as a candidate nitrogen dioxide dielectric sensor using impedance spectroscopy analysis. Significant changes in electronic and physical properties down to our dosage minimum of 2 ppm h have been observed. Using disc-shaped pressed pellets of Zr(OH)4 in parallel plate geometry, we observe a maximum signal shift of 35% at 2 ppm h dosage, which increases six orders of magnitude as the dosage reaches 1000 ppm h. Changes in impedance correlate with nitrogen and oxygen atomic ratio increases observed via X-ray photoelectron spectroscopy (XPS) at higher NO2 dosages. In contrast to the sharp frequency-dependent features and net impedance decreases during NO2 exposures, Zr(OH)4 exhibits a large and broad impedance increase after exposure to humid air (water vapor). The results indicate that Zr(OH)4 could be used as a selective low-cost impedance-based NO2 detector by applying frequency-dependent impedance fingerprinting.

Key role of lattice symmetry in the metal-insulator transition of NdNiO3 films.

Bulk NdNiO3 exhibits a metal-to-insulator transition (MIT) as the temperature is lowered that is also seen in tensile strained films. In contrast, films that are under a large compressive strain typically remain metallic at all temperatures. To clarify the microscopic origins of this behavior, we use position averaged convergent beam electron diffraction in scanning transmission electron microscopy to characterize strained NdNiO3 films both above and below the MIT temperature. We show that a symmetry lowering structural change takes place in case of the tensile strained film, which undergoes an MIT, but is absent in the compressively strained film. Using space group symmetry arguments, we show that these results support the bond length disproportionation model of the MIT in the rare-earth nickelates. Furthermore, the results provide insights into the non-Fermi liquid phase that is observed in films for which the MIT is absent.

Tuning bad metal and non-Fermi liquid behavior in a Mott material: Rare-earth nickelate thin films.

Resistances that exceed the Mott-Ioffe-Regel limit (known as bad metal behavior) and non-Fermi liquid behavior are ubiquitous features of the normal state of many strongly correlated materials. We establish the conditions that lead to bad metal and non-Fermi liquid phases in NdNiO3, which exhibits a prototype bandwidth-controlled metal-insulator transition. We show that resistance saturation is determined by the magnitude of Ni eg orbital splitting, which can be tuned by strain in epitaxial films, causing the appearance of bad metal behavior under certain conditions. The results shed light on the nature of a crossover to a non-Fermi liquid metal phase and provide a predictive criterion for Anderson localization. They elucidate a seemingly complex phase behavior as a function of film strain and confinement and provide guidelines for orbital engineering and novel devices.

Tailoring resistive switching in Pt/SrTiO3 junctions by stoichiometry control.

Resistive switching effects in transition metal oxide-based devices offer new opportunities for information storage and computing technologies. Although it is known that resistive switching is a defect-driven phenomenon, the precise mechanisms are still poorly understood owing to the difficulty of systematically controlling specific point defects. As a result, obtaining reliable and reproducible devices remains a major challenge for this technology. Here, we demonstrate control of resistive switching based on intentional manipulation of native point defects. Oxide molecular beam epitaxy is used to systematically investigate the effect of Ti/Sr stoichiometry on resistive switching in high-quality Pt/SrTiO3 junctions. We demonstrate resistive switching with improved state retention through the introduction of Ti- and Sr-excess into the near-interface region. More broadly, the results demonstrate the utility of high quality metal/oxide interfaces and explicit control over structural defects to improve control, uniformity, and reproducibility of resistive switching processes. Unintentional interfacial contamination layers, which are present if Schottky contacts are processed at low temperature, can easily dominate the resistive switching characteristics and complicate the interpretation if nonstoichiometry is also present.

Control of magnetocrystalline anisotropy by epitaxial strain in double perovskite Sr(2)FeMoO(6) films.

We demonstrate tuning of magnetocrystalline anisotropy in high-quality Sr(2)FeMoO(6) epitaxial films over a range of several thousand Gauss using strain induced by epitaxial growth on substrates of varying lattice constants. Spectroscopic measurements reveal a striking, linear dependence of the out-of-plane anisotropy on the strain-induced tetragonal distortion of the Sr(2)FeMoO(6) lattice. This anisotropy can be tuned from +2000 to -3300 Oe, a range sufficient to rotate the easy axis from in plane to out of plane. Combined with its half-metallicity and high Curie temperature, this result implies a broad range of scientific and technological applications for this novel spintronic material.