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At least 955 records · Page 53
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Atomically Precise Single Metal Oxide Cluster Catalyst with Oxygen–Controlled Activity

Single cluster catalysts (SCCs) consisting of atomically precise metal nanoclusters dispersed on supports represent a new frontier of heterogeneous catalysis. However, the ability to synthesize SCCs with high loading and to precisely introduce non-metal atoms to further tune their catalytic activity and reaction scope of SCCs have been longstanding challenges. In this work, a new interface confinement strategy is developed for the synthesis of a high density of atomically precise Ru oxide nanoclusters (Ru 3 O 2 ) on reduced graphene oxide (rGO), attributed to the suppression of diffusion-induced metal cluster aggregation. Ru 3 O 2 /rGO exhibits a significantly enhanced activity for oxidative dehydrogenation of 1,2,3,4-tetrahydroquinoline (THQ) to quinoline with a high yield (≈86%) and selectivity (≈99%), superior to Ru and RuO 2 nanoparticles, and homogeneous single/multiple-site Ru catalysts. In addition, Ru 3 O 2 /rGO is also capable of efficiently catalyzing more complex oxidative reactions involving three reactants. The theoretical calculations reveal that the presence of two oxygen atoms in the Ru 3 O 2 motif not only leads to a weak hydrogen bonding interaction between the THQ reactant and the active site, but also dramatically depletes the density of states near the Fermi level, which is attributed to the increased positive valence state of Ru and the enhanced oxidative activity of the Ru 3 O 2 cluster for hydrogen abstraction.

36 MATERIALS SCIENCE↗
NASA NTRS1982

XPS Study of SiO2 and the Si/SiO2 Interface

X-ray photoelectron spectroscopy (XPS) is analytical technique for understanding electronic structure of atoms close to surface in solids, in preference to bulk structure of material. Study found evidence for core-level chemical shifts arising from changes in local structural environment in amorphous SiO2 and at Si/SiO2 interface. Observed XPS spectra may be understood as sequential convolution of several functions, each with well-defined physical interpretation.

Grunthaner, F. J.↗
DOE OSTI2015

Growing LaAlO{sub 3}/SrTiO{sub 3} interfaces by sputter deposition

Sputter deposition of oxide materials in a high-pressure oxygen atmosphere is a well-known technique to produce thin films of perovskite oxides in particular. Also interfaces can be fabricated, which we demonstrated recently by growing LaAlO{sub 3} on SrTiO{sub 3} substrates and showing that the interface showed the same high degree of epitaxy and atomic order as is made by pulsed laser deposition. However, the high pressure sputtering of oxides is not trivial and number of parameters are needed to be optimized for epitaxial growth. Here we elaborate on the earlier work to show that only a relatively small parameter window exists with respect to oxygen pressure, growth temperature, radiofrequency power supply and target to substrate distance. In particular the sensitivity to oxygen pressure makes it more difficult to vary the oxygen stoichiometry at the interface, yielding it insulating rather than conducting.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Highly strained AlAs-type interfaces in InAs/AlSb heterostructures

Spontaneously formed Al-As type interfaces of the InAs/AlSb system grown by molecular beam epitaxy for quantum cascade lasers were investigated by atomic resolution scanning transmission electron microscopy. Experimental strain profiles were compared to those coming from a model structure. High negative out-of-plane strains with the same order of magnitude as perfect Al-As interfaces were observed. The effects of the geometrical phase analysis used for strain determination were evidenced and discussed in the case of abrupt and huge variations of both atomic composition and bond length as observed in these interfaces. Intensity profiles performed on the same images confirmed that changes of chemical composition are the source of high strain fields at interfaces. The results show that spontaneously assembled interfaces are not perfect but extend over 2 or 3 monolayers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2013

Enhanced heat transfer through filler-polymer interface by surface-coupling agent in heat-dissipation material: A non-equilibrium molecular dynamics study

Developing a composite material of polymers and micrometer-sized fillers with higher heat conductance is crucial to realize modular packaging of electronic components at higher densities. Enhancement mechanisms of the heat conductance of the polymer-filler interfaces by adding the surface-coupling agent in such a polymer composite material are investigated through the non-equilibrium molecular dynamics (MD) simulation. A simulation system is composed of α-alumina as the filler, bisphenol-A epoxy molecules as the polymers, and model molecules for the surface-coupling agent. The inter-atomic potential between the α-alumina and surface-coupling molecule, which is essential in the present MD simulation, is constructed to reproduce the calculated energies with the electronic density-functional theory. Through the non-equilibrium MD simulation runs, we find that the thermal resistance at the interface decreases significantly by increasing either number or lengths of the surface-coupling molecules and that the effective thermal conductivity of the system approaches to the theoretical value corresponding to zero thermal-resistance at the interface. Detailed analyses about the atomic configurations and local temperatures around the interface are performed to identify heat-transfer routes through the interface.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2013

Power law and exponential ejecta size distributions from the dynamic fragmentation of shock-loaded Cu and Sn metals under melt conditions

Large scale molecular dynamics (MD) simulations are performed to study and to model the ejecta production from the dynamic fragmentation of shock-loaded metals under melt conditions. A generic 3D crystal in contact with vacuum containing about 10{sup 8} atoms and with a sinusoidal free surface roughness is shock loaded so as to undergo a solid-liquid phase change on shock. The reflection of the shock wave at the interface metal/vacuum gives rise to the ejection of 2D jets/sheets of atoms (Richtmyer-Meshkov instabilities in the continuum limit), which develop and break up, forming ejecta (fragments) of different volumes (or mass). The fragmentation process is investigated by analyzing the evolution of the resulting volume distribution of the ejecta as a function of time. Two metals are studied (Cu and Sn) and the amplitude of the roughness is varied. The simulations show that the associated distributions exhibit a generic behavior with the sum of two distinct terms of varying weight, following the expansion rate of the jets: in the small size limit, the distribution obeys a power law dependence with an exponent equal to 1.15 ± 0.08; and in the large size limit, it obeys an exponential form. These two components are interpreted, with the help of additional simple simulations, as the signature of two different basic mechanisms of fragmentation. The power law dependence results from the fragmentation of a 2D network of ligaments arranged following a fractal (scale free) geometry and generated when the sheets of liquid metal expand and tear. The exponential distribution results from a 1D Poisson fragmentation process of the largest ligaments previously generated. Unlike the power law distribution, it is governed by a characteristic length scale, which may be provided by energy balance principle.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Silicon Surface Tethered Polymer as Artificial Solid Electrolyte Interface

Here, we have developed a proof of concept electrode design to covalently graft poly(methyl methacrylate) brushes directly to silicon thin film electrodes via surface-initiated atom transfer radical polymerization. This polymer layer acts as a stable artificial solid electrolyte interface that enables surface passivation despite large volume changes during cycling. Thin polymer layers (75 nm) improve average first cycle coulombic efficiency from 62.4% in bare silicon electrodes to 76.3%. Average first cycle reversible capacity was improved from 3157 to 3935 mAh g -1 , and average irreversible capacity was reduced from 2011 to 1020 mAh g -1 . Electrochemical impedance spectroscopy performed on silicon electrodes showed that resistance from solid electrolyte interface formation increased from 79 to 1508 Ω in untreated silicon thin films over 26 cycles, while resistance growth was lower – from 98 to 498 Ω – in silicon films functionalized with PMMA brushes. The lower increase suggests enhanced surface passivation and lower electrolyte degradation. This work provides a pathway to develop artificial solid electrolyte interfaces synthesized under controlled reaction conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Voltage-Dependent First-Principles Simulation of Insertion of Chloride Ions into Al/Al 2 O 3 Interfaces Using the Quantum Continuum Approximation

Experiments have shown that pitting corrosion can develop in aluminum surfaces at potentials > − 0.5 V relative to the standard hydrogen electrode (SHE). Until recently, the onset of pitting corrosion in aluminum has not been rigorously explored at an atomistic scale because of the difficulty of incorporating a voltage into density functional theory (DFT) calculations. We introduce the Quantum Continuum Approximation (QCA) which self-consistently couples explicit DFT calculations of the metal-insulator and insulator-solution interfaces to continuum Poisson-Boltzmann electrostatic distributions describing the bulk of the insulating region. By decreasing the number of atoms necessary to explicitly simulate with DFT by an order of magnitude, QCA makes the first-principles prediction of the voltage of realistic electrochemical interfaces feasible. After developing this technique, we apply QCA to predict the formation energy of chloride atoms inserting into oxygen vacancies in Al(111)/α-Al 2 O 3 (0001) interfaces as a function of applied voltage. We predict that chloride insertion is only favorable in systems with a grain boundary in the Al 2 O 3 for voltages > − 0.2 V (SHE). Here our results roughly agree with the experimentally demonstrated onset of corrosion, demonstrating QCA's utility in modeling realistic electrochemical systems at reasonable computational cost.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Efficient Intermolecular Energy Exchange and Soft-ionization of Water at Nanoplatelet Interfaces

X-ray, energetic photon and electron irradiation can ionize and electronically excite target atoms and molecules. These excitations undergo complicated relaxation and energy transfer processes that ultimately determine the manifold of system responses to the deposited excess energy. In weakly bound gas- and solution-phase samples, intermolecular Coulomb decay (ICD) and electron-transfer mediated decay (ETMD) can occur with neighboring atoms or molecules leading to efficient transfer of the excess energy to the surroundings. In ionic solids such as metal-oxides, intra- and inter-atomic Auger decay produces localized final states that lead to lattice damage and typically removal of cations from the substrate. The relative importance of Auger stimulated damage (ASD) versus ICD and ETMD in micro-solvated nanoparticle interfaces is not known. Though ASD is generally expected, essentially no lattice damage and very efficient ICD and ETMD resulting from ionization and electronic excitation of micro-solvated boehmite (AlOOH) nanoplatelets has been observed. Efficient energy transfer and soft ionization of interfacial molecules is likely a general phenomenon at gas-oxyhydroxide nanoparticle interfaces where the density of states of the ionized chemisorbed species significantly overlap the core hole states of the solid.

Jones, Brant M.↗
DOE OSTI2014

Anomalous magnetic behavior at the graphene/Co interface

An intensive theoretical study on the interaction between graphene and transition metal atom has been carried out; however, its experimental verification is still lacking. To explore the theoretical prediction of antiferromagnetic coupling due to charge transfer between graphene and cobalt, epitaxial layer of cobalt is grown on graphene surface. Predicted antiferromagnetic interaction with Neel temperature (T{sub N} ∼ 32 K) which anomalously shifts to higher temperature (34 K) and becomes more prominent under application of magnetic field of 1 T is reported. Lowering of magnetoresistance as a consequence of this antiferromagnetic coupling at the interface is also observed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Acoustically enhanced heat transport

We investigate the enhancement of heat transfer in the nucleate boiling regime by inducing high frequency acoustic waves (f ∼ 10{sup 6} Hz) on the heated surface. In the experiments, liquid droplets (deionized water) are dispensed directly onto a heated, vibrating substrate. At lower vibration amplitudes (ξ{sub s} ∼ 10{sup −9} m), the improved heat transfer is mainly due to the detachment of vapor bubbles from the heated surface and the induced thermal mixing. Upon increasing the vibration amplitude (ξ{sub s} ∼ 10{sup −8} m), the heat transfer becomes more substantial due to the rapid bursting of vapor bubbles happening at the liquid-air interface as a consequence of capillary waves travelling in the thin liquid film between the vapor bubble and the air. Further increases then lead to rapid atomization that continues to enhance the heat transfer. An acoustic wave displacement amplitude on the order of 10{sup −8} m with 10{sup 6} Hz order frequencies is observed to produce an improvement of up to 50% reduction in the surface temperature over the case without acoustic excitation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Properties of Ti/TiC Interfaces from Molecular Dynamics Simulations

Titanium carbide is used as a primary component in coating materials, thin films for electronic devices, and composites. Here, the structure of coherent and semicoherent interfaces formed between close-packed TiC (111) and Ti (0001) is investigated in classical molecular dynamics simulations. The forces on the atoms in the simulations are determined using a newly developed TiC potential under the framework of the third-generation charge optimized many-body (COMB 3 ) suite of potentials. The work of adhesion energies for the coherent interfaces is calculated and compared with the predictions of density functional theory calculations. In the case of relaxed semicoherent interfaces, a two-dimensional (2D) misfit dislocation network is predicted to form that separates the interface into different regions in which the positions of the atoms are similar to the positions at the corresponding coherent interfaces. After the interface is annealed at an elevated temperature, the climb of edge dislocations is activated which modifies the 2D misfit dislocation network and increases the work of adhesion. These findings can be used as inputs for sequential larger simulation models to understand and predict the macroscopic properties of TiC/Ti interfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2015

In situ measurement of fixed charge evolution at silicon surfaces during atomic layer deposition

Interfacial fixed charge or interfacial dipoles are present at many semiconductor-dielectric interfaces and have important effects upon device behavior, yet the chemical origins of these electrostatic phenomena are not fully understood. We report the measurement of changes in Si channel conduction in situ during atomic layer deposition (ALD) of aluminum oxide using trimethylaluminum and water to probe changes in surface electrostatics. Current-voltage data were acquired continually before, during, and after the self-limiting chemical reactions that result in film growth. Our measurements indicated an increase in conductance on p-type samples with p{sup +} ohmic contacts and a decrease in conductance on analogous n-type samples. Further, p{sup +} contacted samples with n-type channels exhibited an increase in measured current and n{sup +} contacted p-type samples exhibited a decrease in current under applied voltage. Device physics simulations, where a fixed surface charge was parameterized on the channel surface, connect the surface charge to changes in current-voltage behavior. The simulations and analogous analytical relationships for near-surface conductance were used to explain the experimental results. Specifically, the changes in current-voltage behavior can be attributed to the formation of a fixed negative charge or the modification of a surface dipole upon chemisorption of trimethylaluminum. These measurements allow for the observation of fixed charge or dipole formation during ALD and provide further insight into the electrostatic behavior at semiconductor-dielectric interfaces during film nucleation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Li-atoms-induced structure changes of Guinier–Preston–Bagaryatsky zones in AlCuLiMg alloys

Guinier–Preston–Bagaryatsky (GPB) zones are the well-known strengthening precipitates of AlCuMg alloys formed upon thermal ageing. Here we report that when formed in AlCuLiMg alloys the GPB zones can change significantly in morphology and structure. It is shown that though they do still consist of Al, Cu and Mg elements fundamentally, the GPB zones in AlCuLiMg alloys have a rather different structure due to a featured Li-segregation at their interfaces with the matrix and possible Li-replacement of partial Mg atoms in the structure. As such the Li-containing GPB zones often develop from one-dimensional to quasi-two-dimensional precipitates. - Highlights: • We observe Guinier–Preston–Bagaryatsky zone variants in AlCuLiMg alloys. • We obtain atomic-resolution images of the precipitates and model their structures. • Li-atoms play a key role in modifying the structure of these precipitate variants.

36 MATERIALS SCIENCE↗
DOE OSTI2014

First Observations of Nonhydrodynamic Mix at the Fuel-Shell Interface in Shock-Driven Inertial Confinement Implosions

A strong nonhydrodynamic mechanism generating atomic fuel-shell mix has been observed in strongly shocked inertial confinement fusion implosions of thin deuterated-plastic shells filled with 3 He gas. These implosions were found to produce D 3 He-proton shock yields comparable to implosions of identical shells filled with a hydroequivalent 50:50 D 3 He gas mixture. Standard hydrodynamic mixing cannot explain this observation, as hydrodynamic modeling including mix predicts a yield an order of magnitude lower than was observed. Instead, these results can be attributed to ion diffusive mix at the fuel-shell interface.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2014

Lattice Dynamical Properties of Ferroelectric Thin Films at the Nanoscale

In this project, we have successfully demonstrated atomic layer-by-layer growth by laser MBE from separate targets by depositing SrTiO 3 films from SrO and TiO 2 targets. The RHEED intensity oscillation was used to monitor and control the growth of each SrO and TiO 2 layer. We have shown that by using separate oxide targets, laser MBE can achieve the same level of stoichiometry control as the reactive MBE. We have also studied strain relaxation in LaAlO 3 films and its effect on the 2D electron gas at LaAlO 3 /SrTiO 3 interface. We found that there are two layers of different in-plane lattice constants in the LaAlO 3 films, one next to the SrTiO 3 substrate nearly coherently strained, while the top part relaxed as the film thickness increases above 20 unit cells. This strain relaxation significantly affect the transport properties of the LaAlO 3 /SrTiO 3 interface.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2026

Phase-field model of freeze casting

Directional solidification of water-based solutions has emerged as a versatile technique for templating hierarchical porous materials. However, the underlying mechanisms of pattern formation remain incompletely understood. In this work, we present a detailed derivation and analysis of a quantitative phase-field model for simulating this nonequilibrium process. The phase-field model extends the thin-interface formulation of dilute binary alloy solidification with antitrapping to incorporate the highly anisotropic energetic and kinetic properties of the partially faceted ice-water interface. This interface is faceted in the basal plane normal to the ⟨0001⟩ directions and atomically rough in other directions within the basal plane. On the basal plane, the model reproduces a linear or nonlinear relationship between the interface growth rate and the kinetic undercooling that can be linked to experimental measurements. In both cases, spontaneous parity breaking of the solidification front is observed when the preferred growth direction is aligned with the temperature gradient. This phenomenon leads to the formation of partially faceted ice lamellae that drift laterally in one of the ⟨0001⟩ directions. Here, we demonstrate that the drifting velocity of the ice lamellae is controlled by the kinetics on the basal plane and converges as the thickness of the diffuse solid-liquid interface decreases. Furthermore, we examine the effect of the form of the kinetic anisotropy, which is chosen here such that the inverse of the kinetic coefficient varies linearly from a finite value in the ⟨0001⟩ directions to zero in all other directions within the basal plane, consistent with the assumption that the interface grows in local thermodynamic equilibrium in this plane. Our results indicate that the drifting velocity of ice lamellae is not affected by the slope of this linear relation, and the radius and undercooling at the tip of an ice lamella converge at relatively small slope values. Consequently, the phase-field simulations remain quantitative with computationally tractable choices of both the interface thickness and the slope assumed in the form of the kinetic anisotropy.

Materials science↗
DOE OSTI2016

First-principles based calculation of the macroscopic α/β interface in titanium

The macroscopic α/β interface in titanium and titanium alloys consists of a ledge interface (112){sub β}/(01-10){sub α} and a side interface (11-1){sub β}/(2-1-10){sub α} in a zig-zag arrangement. Here, we report a first-principles study for predicting the atomic structure and the formation energy of the α/β-Ti interface. Both component interfaces were calculated using supercell models within a restrictive relaxation approach, with various staking sequences and high-symmetry parallel translations being considered. The ledge interface energy was predicted as 0.098 J/m{sup 2} and the side interface energy as 0.811 J/m{sup 2}. By projecting the zig-zag interface area onto the macroscopic broad face, the macroscopic α/β interface energy was estimated to be as low as ∼0.12 J/m{sup 2}, which, however, is almost double the ad hoc value used in previous phase-field simulations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗