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At least 307 records · Page 17

Development of integral covers on solar cells

The electron-beam technique for evaporating a dielectric material onto solar cells is investigated. A process has been developed which will provide a highly transparent, low stress, 2 mil thick cover capable of withstanding conventional space type qualification tests including humidity, thermal shock, and thermal cycling. The covers have demonstrated the ability to withstand 10 to the 15th power 1 MeV electrons and UV irradiation with minor darkening. Investigation of the cell AR coating has produced a space qualifiable titanium oxide coating which will give an additional 6% current output over similar silicon oxide coated cells when covered by glass.

Stella, P.↗

Chemical reactivity of hydrogen, nitrogen, and oxygen atoms at temperatures below 100 k

The synthesis of unusual compounds by techniques employing cryogenic cooling to retard their very extreme reactivity was investigated. Examples of such species that were studied are diimide (N2H2), cyclobutadiene (C4H4), cyclopropanone (C3H4O), oxirene (C2H2O), and many others. Special purpose cryogenically cooled inlet arrangements were designed such that the analyses incurred no warm-up of the cold, and frequently explosively unstable, compounds. Controlled energy electron impact techniques were used to measure critical potentials and to develop the molecular energetics and thermodynamics of these molecules and to gain some insight into their kinetic characteristics as well. Three and four carbon strained ring molecules were studied. Several reactions of oxygen and hydrogen atoms with simple molecules of H, N, C, and O in hard quench configurations were studied. And the quench stabilization of BH3 was explored as a model system in cryochemistry.

Mcgee, H. A., Jr.↗

The preparation and properties of aluminum nitride films

Aluminum nitride films have been deposited on silicon substrates at 800-1200 C by the pyrolysis of an aluminum trichloride-ammonia complex, AlCl3.3NH3, in a gas flow system. The deposit was transparent, tightly adherent to the substrate, and was confirmed to be aluminum nitride by X-ray and electron diffraction techniques. The deposited aluminum nitride films were found to be polycrystalline with the crystallite size increasing with increasing temperature of deposition. Other properties of aluminum nitride films relevant to device applications, including density, refractive index, dissolution rate, dielectric constant, and masking ability, have been determined. These properties indicate that aluminum nitride films have potential as a dielectric in electronic devices.

Chu, T. L.↗

In situ sputter cleaning of thin film metal substrates for UHV-TEM corrosion studies.

A prerequisite for conducting valid corrosion experiments by in situ electron microscopy techniques is not only the achievement of UHV background pressure conditions at the site of the specimen but also the ability to clean the surface of the thin metal substrate specimen before initiation of the corrosive interaction. A miniaturized simple ion gun has been constructed for this purpose. The gun is small enough to be incorporated into an UHV electron microscope specimen chamber with hot stage in such a way as to permit bombardment of the substrate specimen while observing it by transmission electron microscopy TEM. It is shown that the ion beam generated is confined well enough to cause a sputtering removal of substrate material at a rate of approximately 5-10 A/min and to prevent the sputter deposition of contaminating material from the specimen holder.

Heinemann, K.↗

Efficient matrix partitioning for optical computing

Techniques for partitioning optical linear algebra problems to make them amenable to solution using optical processors programmed with simple algorithms are explored. Generalized methods for splitting a linear algebra matrix into a series of submatrices are reviewed, showing that simple forms can be pipelined smoothly and that parallel accumulation can be achieved by beam combining on detectors or by summing electronically. The techniques offer simplified bookkeeping, algorithmic independence, and high efficiency. The computational speed will depend on the number of multiplier-accumulators devoted to the task.

Caulfield, H. J.↗

Direct Fabrication of Atomically Defined Pores in MXenes Using Feedback-Driven STEM

Controlled fabrication of nanopores in 2D materials offer the means to create robust membranes needed for ion transport and nanofiltration. Techniques for creating nanopores have relied upon either plasma etching or direct irradiation; however, aberration-corrected scanning transmission electron microscopy (STEM) offers the advantage of combining a sub-Å sized electron beam for atomic manipulation along with atomic resolution imaging. Here, for this work, a method for automated nanopore fabrication is utilized with real-time atomic visualization to enhance the mechanistic understanding of beam-induced transformations. Additionally, an electron beam simulation technique, Electron-Beam Simulator (E-BeamSim) is developed to observe the atomic movements and interactions resulting from electron beam irradiation. Using the MXene Ti 3 C 2 T x , the influence of temperature on nanopore fabrication is explored by tracking atomic transformations and find that at room temperature the electron beam irradiation induces random displacement and results in titanium pileups at the nanopore edge, which is confirmed by E-BeamSim. At elevated temperatures, after removal of the surface functional groups and with the increased mobility of atoms results in atomic transformations that lead to the selective removal of atoms layer by layer. This work can lead to the development of defect engineering techniques within functionalized MXene layers and other 2D materials.

36 MATERIALS SCIENCE↗

Electron Microprobe Analyses of Lithic Fragments and Their Minerals from Luna 20 Fines

The bulk analyses (determined with the broad beam electron microprobe technique) of lithic fragments are given in weight percentages and are arranged according to the rock classification. Within each rock group the analyses are arranged in order of increasing FeO content. Thin section and lithic fragment numbers are given at the top of each column of analysis and correspond to the numbers recorded on photo mosaics on file in the Institute of Meteoritics. CIPW molecular norms are given for each analysis. Electron microprobe mineral analyses (given in oxide weight percentages), structural formulae and molecular end member values are presented for plagioclase, olivine, pyroxene and K-feldspar. The minerals are selected mostly from lithic fragments that were also analyzed for bulk composition. Within each mineral group the analyses are presented according to the section number and lithic fragment number. Within each lithic fragment the mineral analyses are arranged as follows: Plagioclase in order of increasing CaO; olivine and pyroexene in order of increasing FeO; and K-feldspar in order of increasing K2O. The mineral grains are identified at the top of each column of analysis by grain number and lithic fragment number.

Conrad, G. H.↗

Fe and O EELS Studies of Ion Irradiated Murchison CM2 Carbonaceous Chondrite Matrix

Introduction: The physical and chemical response of hydrated carbonaceous chondrite materials to space weathering processes is poorly understood. Improving this understanding is a key part of establishing how regoliths on primitive carbonaceous asteroids respond to space weathering processes, knowledge that supports future sample return missions (Hayabusa 2 and OSIRISREx) that are targeting objects of this type. We previously reported on He+ irradiation of Murchison matrix and showed that the irradiation resulted in amorphization of the matrix phyllosilicates, loss of OH, and surface vesiculation. Here, we report electron energy-loss spectroscopy (EELS) measurements of the irradiated material with emphasis on the Fe and O speciation. Sample and Methods: A polished thin section of the Murchison CM2 carbonaceous chondrite was irradiated with 4 kilovolts He(+) (normal incidence) to a total dose of 1 x 10(exp 18) He(+) per square centimeter. We extracted thin sections from both irradiated and unirradiated regions in matrix using focused ion beam (FIB) techniques with electron beam deposition for the protective carbon strap to minimize surface damage artifacts from the FIB milling. The FIB sections were analyzed using a JEOL 2500SE scanning and transmission electron microscope (STEM) equipped with a Gatan Tridiem imaging filter. EELS spectra were collected from 50 nanometer diameter regions with an energy resolution of 0.7 electronvolts FWHM at the zero loss. EELS spectra were collected at low electron doses to minimize possible artifacts from electron-beam irradiation damage. Results and Discussion: Fe L (sub 2,3) EELS spectra from matrix phyllosilicates in CM chondrites show mixed Fe(2+)/Fe(3+) oxidation states with Fe(3+)/Sigma Fe approximately 0.5. Fe L(sub 2,3) spectra from the irradiated/ amorphized matrix phyllosilicates show higher Fe(2+)/Fe(3+) ratios compared to spectra obtained from pristine material at depths beyond the implantation/amorphization layer. We also obtained O Ka spectra from phyllosilicates in both regions of the sample. The O Ka spectra show a pre-edge feature at approximately 530.5 electronvolts that is related to O 2p states hybridized with Fe 3d states. The intensity ratio of the O Ka pre-edge peak relative to the main part of the O Ka edge (that results from transitions of O 1s to 2p states) is lower in the irradiated layer compared to the pristine material and may reflect the loss of O (as OH) as was observed by IR spectroscopy. Conclusions: In addition to amorphization and OH loss, EELS spectra of He(+) irradiated matrix phyllosilicates in Murchison show that some of the Fe(3+) is reduced to Fe(2+). Spectral deconvolution is underway to extract quantitative ratios from the EELS spectra.

Keller, L. P.↗

Probing thermal conductivity of subsurface, amorphous layers in irradiated diamond

In this study, we report on the thermal conductivity of amorphous carbon generated in diamond via nitrogen ion implantation (N 3+ at 16.5 MeV). Here, transmission electron microscopy techniques demonstrate amorphous band formation about the longitudinal projected range, localized approximately 7 μm beneath the sample surface. While high-frequency time-domain thermoreflectance measurements provide insight into the thermal properties of the near-surface preceding the longitudinal projected range depth, a complimentary technique, steady-state thermoreflectance, is used to probe the thermal conductivity at depths which could not otherwise be resolved. Through measurements with a series of focusing objective lenses for the laser spot size, we find the thermal conductivity of the amorphous region to be approximately 1.4 W m –1 K –1 , which is comparable to that measured for amorphous carbon films fabricated through other techniques.

36 MATERIALS SCIENCE↗

Molecular modeling of polymer composite-analyte interactions in electronic nose sensors

We report a molecular modeling study to investigate the polymer-carbon black (CB) composite-analyte interactions in resistive sensors. These sensors comprise the JPL electronic nose (ENose) sensing array developed for monitoring breathing air in human habitats. The polymer in the composite is modeled based on its stereoisomerism and sequence isomerism, while the CB is modeled as uncharged naphthalene rings with no hydrogens. The Dreiding 2.21 force field is used for the polymer, solvent molecules and graphite parameters are assigned to the carbon black atoms. A combination of molecular mechanics (MM) and molecular dynamics (NPT-MD and NVT-MD) techniques are used to obtain the equilibrium composite structure by inserting naphthalene rings in the polymer matrix. Polymers considered for this work include poly(4-vinylphenol), polyethylene oxide, and ethyl cellulose. Analytes studied are representative of both inorganic and organic compounds. The results are analyzed for the composite microstructure by calculating the radial distribution profiles as well as for the sensor response by predicting the interaction energies of the analytes with the composites. c2003 Elsevier Science B.V. All rights reserved.

NASA Center JPL↗

Electronic thermal transport measurement in low-dimensional materials with graphene non-local noise thermometry

In low-dimensional systems, the combination of reduced dimensionality, strong interactions and topology has led to a growing number of many-body quantum phenomena. Thermal transport, which is sensitive to all energy-carrying degrees of freedom, provides a discriminating probe of emergent excitations in quantum materials and devices. However, thermal transport measurements in low dimensions are dominated by the phonon contribution of the lattice, requiring an experimental approach to isolate the electronic thermal conductance. In this work we measured non-local voltage fluctuations in a multi-terminal device to reveal the electronic heat transported across a mesoscopic bridge made of low-dimensional materials. Using two-dimensional graphene as a noise thermometer, we measured the quantitative electronic thermal conductance of graphene and carbon nanotubes up to 70 K, achieving a precision of ~1% of the thermal conductance quantum at 5 K. Employing linear and nonlinear thermal transport, we observed signatures of energy transport mediated by long-range interactions in one-dimensional electron systems, in agreement with a theoretical model.

36 MATERIALS SCIENCE↗

Integrally covered silicon solar cells.

The electron-beam technique for evaporating dielectric materials onto solar cells has been examined and developed. Titanium oxide cell antireflection coatings have been obtained which compare to silicon monoxide in environmental capabilities and which provide 3 to 4% improvement over SiO for glass covered cells. Evaporation processes have been obtained which provide a 50 to 100 micromil thick transparent (0.5 to 1.0% absorption per mil), low stressed integral cover capable of surviving space type qualification testing. Irradiation with 10 to the 15th power 1-MeV electrons shows 2% darkening, and long term UV irradiation incurs approximately 1.3% cover darkening for 50 micromil thick covers.

Stella, P. M.↗

Direct observation of elemental fluctuation and oxygen octahedral distortion-dependent charge distribution in high entropy oxides

The enhanced compositional flexibility to incorporate multiple-principal cations in high entropy oxides (HEOs) offers the opportunity to expand boundaries for accessible compositions and unconventional properties in oxides. Attractive functionalities have been reported in some bulk HEOs, which are attributed to the long-range compositional homogeneity, lattice distortion, and local chemical bonding characteristics in materials. However, the intricate details of local composition fluctuation, metal-oxygen bond distortion and covalency are difficult to visualize experimentally, especially on the atomic scale. Here, we study the atomic structure-chemical bonding-property correlations in a series of perovskite-HEOs utilizing the recently developed four-dimensional scanning transmission electron microscopy techniques which enables to determine the structure, chemical bonding, electric field, and charge density on the atomic scale. The existence of compositional fluctuations along with significant composition-dependent distortion of metal-oxygen bonds is observed. Consequently, distinct variations of metal-oxygen bonding covalency are shown by the real-space charge-density distribution maps with sub-ångström resolution. The observed atomic features not only provide a realistic picture of the local physico-chemistry of chemically complex HEOs but can also be directly correlated to their distinctive magneto-electronic properties.

36 MATERIALS SCIENCE↗

The Role of Pulse Radiolysis in Advanced Nuclear Fuel Cycles

The effects of ionizing radiation are ubiquitous throughout all aspects of a nuclear fuel cycle. The complexity and intensity of these effects are greatest during reactor operations and in the management of used nuclear fuel and waste. Radiation-induced processes typically promote the chemical transformation of molecules and materials with the formation of potentially detrimental degradation products and corresponding changes in physical and chemical properties, which ultimately impact the effectiveness and longevity of nuclear technologies. Consequently, a molecular-level understanding of radiation effects over multiple time, distance, and material domains is essential for the innovation and deployment of next generation nuclear technologies. Attaining this knowledge necessitates a firm grasp of radiation-induced reaction kinetics, for which pulsed electron radiolysis is the methodology of choice. Presented here are several recent studies from our group that demonstrate the critical role of pulsed electron radiolysis techniques in the advancement of our understanding of radiation-induced chemistry under advanced nuclear fuel cycle conditions. Research topics include late actinide redox chemistry, radiation robustness of used nuclear fuel reprocessing complexants, and the behavior of metal cations in high temperature molten salt media.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Demonstration of closed shell breeding of cesium ions with an electron beam ion source

An electron beam ion source serves as a charge breeder for the Californium Rare Isotope Breeder Upgrade (CARIBU) at the Argonne Tandem Linac Accelerator System (ATLAS). The source accepts radioactive beams of 1+ or 2+ ions and raises their charge state for post-acceleration by ATLAS. The efficiency of this process impacts the length of each experiment and, hence, the type and number of experiments that can be run in each program cycle. Recent efforts to improve the charge breeding efficiency for the 80 < A < 160 species typical of CARIBU have focused on utilizing the closed shell breeding technique. Here, with this technique, the electron beam energy is manipulated to take advantage of the large gap in ionization energies at shell closures and selectively populate a single charge state. Charge breeding studies with stable cesium ions have demonstrated an absolute efficiency of 72% for Cs 27+ and a total efficiency of 93%. The Cs 27+ efficiency result represents a factor of 3 improvement over the previous best charge breeding result of 23% for Cs 27+ .

Vondrasek, R. [Argonne National Laboratory (ANL), ↗

Probing Distinctive Redox Mechanism in Ni-Rich Cathode Via Real-Time Quick X-Ray Absorption Spectroscopy

X-ray radiation damage on the measuring system has been a critical issue regularly for a long-time exposure to X-ray beam during the in operando characterizations, which is particularly severe when the applied X-ray energy is near the absorption edges (M, L, K, etc.) of the interest element. Here, to minimize the negative effects raised by beam radiation, we employ quick X-ray absorption spectroscopy (QXAS) to study the electrochemical reaction mechanism of a Ni-rich layered structure cathode for lithium-ion batteries. With the advanced QXAS technique, the electronic structure and local coordination environment of the transition metals (TMs) are monitored in-operando with limited radiation damage. Compared to the conventional step-mode X-ray absorption spectroscopy, the QXAS can provide more reliable oxidation state change and more detailed local structure evolutions surrounding TMs (Ni and Co) in Ni-rich layered oxides. By leveraging these advantages of QXAS, we demonstrated that the Ni dominates the electrochemical process with the Co being almost electrochemically inactive. Reversible Ni ions movement between TMs sites and Li sites is also revealed by the time-resolved QXAS technique.

25 ENERGY STORAGE↗

Interfacial electronic states of misfit heterostructure between hexagonal ZnO and cubic NiO

The combination of materials with dissimilar symmetries can induce a large amount of stress at the interfacial layer of films, thereby promoting the appearance of novel properties in related devices. The study of the interfacial state is critical for determining the inner mechanism. In this work, the misfit heterostructure between cubic NiO films and wurtzite ZnO is investigated. A NiO film grown using molecular beam epitaxy on a ZnO substrate shows a highly (100)-oriented texture featuring three domains with a rotation angle of 30°, which is in agreement with first principles calculations. Misfit-induced dislocations and lattice distortions within the interfacial layers of the NiO film give rise to interfacial electronic states, which are different from those in bulk; these electronic states are analyzed by in situ synchrotron-based x-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, x-ray absorption spectroscopy, and ex situ electron energy loss spectroscopy. Additionally, the origin of these interfacial states is discussed. This work aims to provide insights for the integration of semiconducting hexagonal ZnO with other functional materials that have a cubic symmetry. Additionally, we investigate the integration of photon and electron-based techniques to explore the interfacial states of complex interfaces, which is an important aspect of material science.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Oxide Two‐Dimensional Electron Gas with High Mobility at Room‐Temperature

Abstract The prospect of 2‐dimensional electron gases (2DEGs) possessing high mobility at room temperature in wide‐bandgap perovskite stannates is enticing for oxide electronics, particularly to realize transparent and high‐electron mobility transistors. Nonetheless only a small number of studies to date report 2DEGs in BaSnO 3 ‐based heterostructures. Here, 2DEG formation at the LaScO 3 /BaSnO 3 (LSO/BSO) interface with a room‐temperature mobility of 60 cm 2 V −1 s −1 at a carrier concentration of 1.7 × 10 13 cm –2 is reported. This is an order of magnitude higher mobility at room temperature than achieved in SrTiO 3 ‐based 2DEGs. This is achieved by combining a thick BSO buffer layer with an ex situ high‐temperature treatment, which not only reduces the dislocation density but also produces a SnO 2 ‐terminated atomically flat surface, followed by the growth of an overlying BSO/LSO interface. Using weak beam dark‐field transmission electron microscopy imaging and in‐line electron holography technique, a reduction of the threading dislocation density is revealed, and direct evidence for the spatial confinement of a 2DEG at the BSO/LSO interface is provided. This work opens a new pathway to explore the exciting physics of stannate‐based 2DEGs at application‐relevant temperatures for oxide nanoelectronics.

2-dimensional electron gas↗