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At least 775 records · Page 43

Probing the Effects of the First Atomic Layer on the Dynamic Behavior of Sub-2 nm MgO/Al 2 O 3 Memristors

As electronic devices continue to scale down from the current sub-5 nm range, atomic-scale control of defects becomes increasingly crucial to suppressing their impact on the physical properties of the devices. Memristors present an excellent example as a nonlinear and dynamic device with high speed and endurance required for electronic applications ranging from neuromorphic computing to nonvolatile memories. Herein we investigate the impact of atomic defects in sub-2 nm thick MgO/Al 2 O 3 atomic layer stack (ALS) memristors that use an M1 (switching layer)/M2 (oxygen vacancy reservoir layer) bilayer structure grown using in vacuo atomic layer deposition (iALD). Intriguingly, we revealed a direct correlation of the atomic defects in the M2 layer with the memristor dynamic behavior using a combined analysis of in situ scanning tunneling spectroscopy (iSTS) on the M2 layer and ex situ characterization on the memristors. Specifically, incomplete coverage of the 1st ALD atomic layer of M2 on the electrode yields defects at the M2/electrode interface. Despite the monotonic increase of ALD coverage, by almost three-fold from ~30% to >90%, at completion of the M2 layer of ~ 0.7 nm in thickness, the impact of the defects on the M2/electrode interface has been found detrimental to both memristor switching speed and endurance. Guided by atomistic simulation, we addressed the issue of interface defects via tuning of the Al surface hydroxylation to increase the first atomic layer ALD coverage to ~75%, leading to improved memristor switching speed and endurance by several orders of magnitude. In conclusion, these findings shed light on the correlation between the atomic defects and the dynamic behavior of sub-2 nm memristors and the importance of minimizing the atomic defects in memristors for future electronic applications.

Atomic Layer Deposition↗

Early stages of plasma induced nitridation of Si (111) surface and study of interfacial band alignment

We report here a systematic study of the nitridation of the Si (111) surface by nitrogen plasma exposure. The surface and interface chemical composition and surface morphology are investigated by using RHEED, X-ray photoelectron spectroscopy, and atomic force microscopy (AFM). At the initial stage of nitridation two superstructures—“8 × 8” and “8/3 × 8/3”—form, and further nitridation leads to 1 × 1 stoichiometric silicon nitride. The interface is seen to have the Si{sup 1+} and Si{sup 3+} states of silicon bonding with nitrogen, which suggests an atomically abrupt and defect-free interface. The initial single crystalline silicon nitride layers are seen to become amorphous at higher thicknesses. The AFM image shows that the nitride nucleates at interfacial dislocations that are connected by sub-stoichiometric 2D-nitride layers, which agglomerate to form thick overlayers. The electrical properties of the interface yield a valence band offset that saturates at 1.9 eV and conduction band offset at 2.3 eV due to the evolution of the sub-stoichiometric interface and band bending.

36 MATERIALS SCIENCE↗

Using interfaces to: create strongly-coupled magnetic-ferroelectrics

Starting at the level of electrons and atoms our long-term goal is to rationally design complex oxide heterostructures and interface-materials with targeted emergent behaviors. This is not a matter of simply optimizing material parameters, but rather begins with understanding a mechanism to control the interplay between the diverse microscopic degrees of freedom prevalent in complex oxides in order to create targeted macroscopic phenomena and ends with the design of new material realizations. These realizations are in turn created with atomic-layer precision, structurally assessed to see that they are the intended realization, and finally their relevant properties are measured. During this program we have developed the scientific ideas necessary to apply this materials-by-design paradigm to the creation of materials offering electrical control of magnetism. At the heart of our approach lies a partnership between theory, synthesis, and characterization. These are the areas of expertise of the three co-PIs, who have worked closely together since their arrival at Cornell. During this project bold ideas on where to put the atoms to provide electrical control of magnetism were met with the latest methods of synthesis science and electron microscopy in an attempt create targeted new multiferroics. Our work applying this materials-by-design methodology to multiferroics has enjoyed multiple successes. The Co-PIs have invented new mechanisms for multiferroics, which provide strong coupling between polarization and magnetism, and reduced them to practice. Specifically, we pioneered multiferroics based on spin-phonon coupling, rotation-driven multiferroicity, and novel geometric multiferroics. Importantly, the latter two of these mechanisms enable the deterministic switching of magnetism by an applied electric field, which is key to the application of multiferroics to future device technologies. Most recently, we performed detailed theoretical analysis on a system involving the combination of magnetoelectric and colossal magnetoresistance behaviors and predict that electrical control of a metal-insulator transition is possible in appropriately strained SmBaMn2O6. The research enabled by this grant led to 63 publications in leading refereed journals including Nature, Nature Materials, Physical Review Letters, and Advanced Materials demonstrating a materials-by-design paradigm to the creation of materials offering electrical control of magnetism.

36 MATERIALS SCIENCE↗

Atomic Oxygen Effects on Seal Leakage

Common Berthing Mechanism (CBM) provides the structural interface between separate International Space Station (ISS) elements, such as the Laboratory and Node modules. The CBM consists of an active and a passive half that join together with structural bolts. The seal at this interface is the CBM-to-CBM molded seal. The CBM-to-CBM interface is assembled on orbit, thus the seals can be exposed to the space environment for up to 65 hours. Atomic Oxygen/Vacuum Ultraviolet radiation (AO/VUV) in space is a potential hazard to the seals. Testing was conducted to determine the effect on leakage of the CBM-to-CBM seal material exposed to AO/VUV. The sealing materials were S383 silicone and V835 fluorocarbon material. Control samples, which were not exposed to the AO/VUV environment, were used to ensure that if any changes in leakage occurred, they could be attributed to the AO/VUV exposure. After exposure to the AO/VUV environment the leakage increase was dramatic for the fluorocarbon. This testing was a major contributing factor in selecting silicone as the CBM-to-CBM seal material.

Christensen, John R.↗

Atomic Oxygen Effects on Seal Leakage

Common Berthing Mechanism (CBM provides the structural interface between separate International Space Station (ISS) elements, such as the Laboratory and Node modules. The CBM consists of an active and a passive half that join together with structural bolts. The seal at this interface is the CBM-to-CBM molded seal. The CBM-to-CBM interface is assembled on orbit, thus the seals can be exposed to the space environment for up to 65 hours. Atomic Oxygen/Vacuum Ultraviolet radiation (AO/VUV) in space is a potential hazard to the seals. Testing was conducted to determine the effect on leakage of the CBM-to-CBM seal material exposed to AO/VUV. The sealing materials were S383 silicone and V835 fluorocarbon material. Control samples, which were not exposed to the AO/VUV environment, were used to ensure that ff any changes in leakage occurred, they could be attributed to the AO/VUV exposure. After exposure to the AO/VUV environment the leakage increase was dramatic for the fluorocarbon. This testing was a major contributing factor in selecting silicone as the CBM-to-CBM seal material.

Christensen, John R.↗

First Principles Determination of the Potential-of-Zero-Charge in an Alumina-Coated Aluminum/Water Interface Model for Corrosion Applications

The surfaces of most metals immersed in aqueous electrolytes have a several-nanometer-thick oxide/hydroxide surface layer. This gives rise to the existence of both metal|oxide and oxide|liquid electrotlyte interfaces, and makes it challenging to correlate atomic length-scale structures with electrochemical properties such the potential-of-zero-charge (PZC). The PZC has been shown to be correlated the onset potential for pitting corrosion. Here, we conduct large-scale Density Functional Theory and ab initio molecular dynamics to calculate the PZC of a Al(111)| γ -Al 2 O 3 (110)| water double-interface model within the context of aluminum corrosion. By partitioning the multiple interfaces involved into binary components with additive contributions to the overall work function and voltage, we predict the PZC to be -1.53 V vs SHE for this model. Furthermore, we calculate the orbital energy levels of defects like oxygen vacancies in the oxide, which are critical parameters in theories associated with pitting corrosion. We predict that the Fermi level at the PZC lies above the impurity defect levels of the oxygen vacancies, which are therefore uncharged at the PZC. From the PZC estimate, we predict the voltage needed to create oxygen vacancies with net positive charges within a flatband approximation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tunable spin polarization and superconductivity in engineered oxide interfaces

Advances in growth technology of oxide materials allow single atomic layer control of heterostructures. In particular delta doping, a key materials’ engineering tool in today’s semiconductor technology, is now also available for oxides. Here we show that a fully electric-field-tunable spin-polarized and superconducting quasi-2D electron system (q2DES) can be artificially created by inserting a few unit cells of delta doping EuTiO 3 at the interface between LaAlO 3 and SrTiO 3 oxides. Spin polarization emerges below the ferromagnetic transition temperature of the EuTiO 3 layer (T FM = 6–8 K) and is due to the exchange interaction between the magnetic moments of Eu-4 f and of Ti-3 d electrons. Moreover, in a large region of the phase diagram, superconductivity sets in from a ferromagnetic normal state. As a result, the occurrence of magnetic interactions, superconductivity and spin–orbit coupling in the same q2DES makes the LaAlO 3 /EuTiO 3 /SrTiO 3 system an intriguing platform for the emergence of novel quantum phases in low-dimensional materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Damage initiation and evolution in Al-Si layered microstructures under shock loading conditions at atomic scales

Designing materials with microstructural features like multiphase interfaces have shown significant promise for usage in the next generation defense and nuclear applications. The dynamic response of these interfaces in extreme environments is observed to vary with the deformability of individual phases, which could subsequently alter the favored damage nucleation sites related to spall failure. Here, we investigate the role of spacing of interfaces in a nanocrystalline layered Aluminum-Silicon system on the shock wave propagation behavior, and microstructural and defect evolution using classical molecular dynamics simulations. The simulations are carried out with different hypothetical Al/Si microstructures including variations in the distribution of Si grains as layers in a nanocrystalline Al matrix. The molecular dynamics simulations suggest that spall failure is preferentially initiated at Al/Si interfaces. In addition, for the same system volume and same concentration of Si, a higher number of layers is marked by an increase in shock wave velocity and reduced resistance to spall failure.

36 MATERIALS SCIENCE↗

Mechanism of β-FeSi{sub 2} precipitates growth-and-dissolution and pyramidal defects' formation during oxidation of Fe-contaminated silicon wafers

Fe-implanted Si-wafers have been oxidized at 900 °C and 1100 °C in order to investigate the behaviour of Fe atoms at the growing SiO{sub 2}/Si interface and the impact on the integrity of microelectronic devices of an involuntary Fe contamination before or during the oxidation process. As-implanted and oxidized wafers have been characterized using secondary ion mass spectroscopy, atom probe tomography, and high-resolution transmission electron microscopy. Experimental results were compared to calculated implantation profiles and simulated images. Successive steps of iron disilicide precipitation and oxidation were evidenced during the silicon oxidation process. The formation of characteristic pyramidal-shaped defects, at the SiO{sub 2}/Si interface, was notably found to correlate with the presence of β-FeSi{sub 2} precipitates. Taking into account the competitive oxidation of these precipitates and of the surrounding silicon matrix, dynamic mechanisms are proposed to model the observed microstructural evolution of the SiO{sub 2}/Si interface, during the growth of the silicon oxide layer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Development of Corrosion Resistant Coatings for Structural Materials for Liquid Fueled Molten Salts Reactors Applications (Final Report)

Current structural alloys, code certified for the MSRs temperature ranges, contain high levels of chromium, making them highly susceptible to molten halide salt corrosion. One potential solution to circumvent the need for code certification of novel alloys, which is expensive and time consuming, is to design claddings that will protect the underlying code certified materials from corrosion damage during operation. In this work, we examined the corrosion of Ni and Cu electroplated, Ni and CuNi weld overlay, Mo-laser clad, and carburized claddings on SS316H for use in molten salt reactor environments. After characterization of the cladded materials (Task 1), static corrosion tests were used to assess corrosion resistance of the claddings in typical molten fluoride salts (Task 2). The corrosion tests were performed in molten FLiNaK at 700°C up to 1000 hours. Pre- and post-corrosion Scanning Electron Microscopy (SEM), energy-dispersive-spectroscopy (EDS), Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD) and glow-discharge-optical-emission-spectroscopy (GDOES) were performed on cladding cross-sections and surfaces to evaluate degradation. The Cu and Ni electroplated samples, as well as the carburized samples, showed excellent corrosion resistance relative to the bare SS316H. To assess high temperature cladding stability, ageing experiments were performed at temperatures up to 900 C in inert atmosphere for the electroplated and carburized samples and a diffusion model was developed to predict long term cladding behavior (Task 3). It was found that the Cu cladding was basically insensitive to the high temperature ageing, except for small secondary phases forming at the interface. On the other hand, the Ni electroplated cladding experienced significant interdiffusion. Nevertheless, the gain in corrosion resistance for a 100μm Ni electroplated cladding is phenomenal, with more than 50% reduction in chromium dissolution from the substrate material for the first 15 years of salt exposure at 700°C. To assess radiation resistance and phase stability, high-temperature 4MeV Ni heavy ion irradiation was performed across the cladding/substrate interface up to 50 displacement-per-atom (DPA) at 500°C and 700°C to assess the phase stability and irradiation behaviors of the electroplated systems (Task 4). The Ni and Cu electroplated systems did not experience void swelling at the contrary to the SS316H substrate due to their nanocrystalline nature. Some level of recrystallization was observed in the cladding, as well as radiation induced segregation and enhanced diffusion. The interface acted as a potent sink for point defects with the presence of a void denuded zone. The mechanical properties of the claddings were assessed using thermal shock, micro-indentation, nano-indentation, and four-point bend testing experiments (Task 5). These experiments were performed on the claddings in as-received, corroded, irradiated, and thermally aged states to determine the effects of typical molten salt reactor environments on cladding integrity. No significant mass loss was observed after repeated thermal shocks. While the electroplated samples softened after high-temperature ageing, irradiation hardening compensate this effect, such that there is little different with the as-received materials. The results of these experiments suggest that the electroplated (copper/nickel) show the greatest promise for application in molten salt reactor development. These claddings prevented any chromium dissolution from occurring during the static corrosion experiments. Additionally, they demonstrated favorable properties for high temperature diffusion, phase stability, interfacial mechanical properties, and irradiation resistance. Weld-overlay cladding are also of great interest and could reach properties similar to the electroplated samples upon optimization (especially with multiple weld passes). The carburized SS316H showed excellent behavior as well, but more work needs to be done to assess their long-term stability. Finally, the Mo-laser clad system was not pursued further due to the manufacturing challenges. It is also worth noting that the Ni cladding systems should behave relatively well in terms of weldability since the Ni-weld overlay microstructure and associated corrosion rate are sound. While the NiCu weld-overlay has even lower corrosion rates than the Ni-weld overlay, more studies on welding of Cu-electroplated systems are necessary since Cu clusters are known to embrittle steels.

36 MATERIALS SCIENCE↗

Characterisation of nano-scale precipitates in BOR60 irradiated T91 steel using atom probe tomography

Atom probe tomography has characterised the microstructural changes in T91 steel after BOR60 reactor irradiation at five temperatures between 376 °C and 524 °C to doses between 14.6 dpa and 35.1 dpa. Irradiation-induced precipitation and segregation to carbide/matrix interface induced by neutron irradiation has been characterised. Atom probe tomography characterisation shows that Mn, Ni, Si -rich (MNS-rich) clusters form in T91 steel irradiated in BOR60 reactor at temperatures between 376 °C and 415 °C, which is not observed at higher temperatures 460 °C and 524 °C. Additionally, the number density, volume fraction and composition of MNS-rich clusters have been characterised. Ni, Mn, Si and P is found to segregate at carbide matrix interface after irradiation at lower temperature and only P segregation is observed at 524 °C.

36 MATERIALS SCIENCE↗

Contact-induced spin polarization of monolayer hexagonal boron nitride on Ni(111)

Hexagonal boron nitride (h-BN) is a promising barrier material for graphene spintronics. In this Letter, spin-polarized metastable de-excitation spectroscopy (SPMDS) is employed to study the spin-dependent electronic structure of monolayer h-BN/Ni(111). The extreme surface sensitivity of SPMDS enables us to elucidate a partial filling of the in-gap states of h-BN without any superposition of Ni 3d signals. The in-gap states are shown to have a considerable spin polarization parallel to the majority spin of Ni. The positive spin polarization is attributed to the π-d hybridization and the effective spin transfer to the nitrogen atoms at the h-BN/Ni(111) interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Effects of Aperiodicity and Roughness on Coherent Heat Conduction in Superlattices

Coherent phonon heat conduction has recently been confirmed experimentally in superlattice structures. Such traveling coherent phonon waves in superlattices lead to a linear increase in thermal conductivity as the number of periods increases. For applications such as thermal insulation or thermoelectrics, minimization of the phonon coherent effect is desirable. In this paper, we use molecular dynamics simulations to study how to control coherent heat conduction in superlattices (SLs). It is found that either aperiodic SLs or SLs with rough interfaces can significantly disrupt coherent heat conduction when the interface densities are high. For sample thickness less than 125 nm, aperiodic SLs with perfect interfaces are found to have the lowest thermal conductivity. We use the atomic Green’s function method to examine the phonon dynamics. The impact of either aperiodicity or interface roughness is attributed to reduced transmittance. Such impact diminishes as the interface density reduces.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Grafting nanometer metal/oxide interface towards enhanced low-temperature acetylene semi-hydrogenation

Metal/oxide interface is of fundamental significance to heterogeneous catalysis because the seemingly “inert” oxide support can modulate the morphology, atomic and electronic structures of the metal catalyst through the interface. The interfacial effects are well studied over a bulk oxide support but remain elusive for nanometer-sized systems like clusters, arising from the challenges associated with chemical synthesis and structural elucidation of such hybrid clusters. We hereby demonstrate the essential catalytic roles of a nanometer metal/oxide interface constructed by a hybrid Pd/Bi 2 O 3 cluster ensemble, which is fabricated by a facile stepwise photochemical method. The Pd/Bi 2 O 3 cluster, of which the hybrid structure is elucidated by combined electron microscopy and microanalysis, features a small Pd-Pd coordination number and more importantly a Pd-Bi spatial correlation ascribed to the heterografting between Pd and Bi terminated Bi 2 O 3 clusters. The intra-cluster electron transfer towards Pd across the as-formed nanometer metal/oxide interface significantly weakens the ethylene adsorption without compromising the hydrogen activation. As a result, a 91% selectivity of ethylene and 90% conversion of acetylene can be achieved in a front-end hydrogenation process with a temperature as low as 44 °C.

36 MATERIALS SCIENCE↗

First Principles Predictions of SnO2/CdTe and SnO2/CdCl2/CdTe Interface Structures

Interfaces become increasingly the limiting factor of solar cell efficiency, raising the interest in computational models. However, explicit atomic structure models from microscopy are rare, and hypothetical assumptions about the atomic structure become ambiguous for incoherent or highly lattice mismatched interfaces. Adopting a bulk crystal structure prediction algorithm to interfacial systems enables explicit structure models for the bare and CdCl 2 treated SnO 2 /CdTe interface.

CdTe↗

The localization and crystallographic dependence of Si suboxide species at the SiO2/Si interface

X-ray photoemission spectroscopy has been used to examine the localization and crystallographic dependence of Si(+), Si(2+), and Si(3+) suboxide states at the SiO2/Si interface for (100)and (111)-oriented substrates with gate oxide quality thermal oxides. The Si(+) and Si(2+) states are localized within 6-10 A of the interface while the Si(3+) state extends about 30 A into the bulk SiO2. The distribution of Si(+) and Si(2+) states shows a strong crystallographic dependence with Si(2+) dominating on (100) substrates and Si(+) dominating on (111) substrates. This crystallographic dependence is anticipated from consideration of ideal unreconstructed (100) and (111) Si surfaces, suggesting that (1) the Si(+) and Si(2+) states are localized immediately within the first monolayer at the interface and (2) the first few monolayers of substrate Si atoms are not significantly displaced from the bulk. The total number of suboxide states observed at the SiO2/Si interface corresponds to 94 and 83 percent of a monolayer for these (100) and (111) substrates, respectively.

Grunthaner, P. J.↗

Electron Trapping and Ion Leaching at the Li-Modified Quartz–Water Interface

Electrons and ions at metal oxide-water interfaces have a critical role in many phenomena and applications, thus making their properties of considerable interest. We here investigate the behavior of a lithium impurity at the water interface with Li-doped SiO 2 using hybrid density functional based ab initio molecular dynamics simulations. We find that the excess electron donated by the lithium dopant localizes on a surface silicon atom and is partially solvated at the aqueous interface. While the position of the excess electron does not change during our ~60 ps simulation, the lithium cation diffuses from its initial position in the SiO 2 subsurface toward the interface and eventually leaches out of the oxide surface and becomes solvated by four water molecules, forming an aqueous Li+- electron complex at the interface. The degree of interaction between the localized electron and the lithium ion controls not only the energy level of the excess electron but also the extent of structural distortion and hydrogen-bonding at the interface. The results of our study can be relevant for understanding the initial stages of glass corrosion, where alkali ions are leached from the surface region by interactions with water.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interfaces Between CdTe and ALD Al 2 O 3

In this work, we present a combination of X-ray photoelectron spectroscopy (XPS) and time-resolved photoluminescence (TRPL) to probe the details of interface formation between CdTe and alumina deposited by atomic layer deposition (ALD). Alumina ALD using water as the oxygen source causes the elimination of Te oxides that are initially present on air-exposed CdTe surfaces. TRPL on the resulting CdTe interface indicates some degree of passivation. On the other hand, postgrowth treatment of Al 2 O 3 /CdTe structures with CdCl 2 and oxygen causes regrowth of Te oxides. Some of these structures show improved lifetimes, thereby pointing toward a critical role for Te oxides in interfacial CdTe passivation by Al 2 O 3 . Lastly, direct measurement of band positions with XPS indicates that the passivation is caused primarily by chemical rather than field effect mechanisms.

14 SOLAR ENERGY↗