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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Influence of surface relaxation on solute atoms positioning within atom probe tomography reconstructions

Highlights: • APT measurement of Al/Cu alloy is simulated with a combined electrostatics and molecular dynamics (MD) approach. • Results show segregation of dilute Cu at [111] poles in correspondence to experimental measurements. • No temperature is involved. The effect originates in both disparate evaporation field and bond-energies in the alloy. While thermal or field-induced surface migration has been invoked often in past literature to rationalize the experimental observations of solute and impurity atoms segregation to specific poles and zones lines in atom probe tomography (APT) reconstructions, it does not satisfactorily explain all experimental results. Using a combined finite-element and molecular dynamics simulation approach that models the field evaporation process from mechanically relaxed emitter structures, we show that an additional mechanism, athermal relaxation, can also drive significant solute migration. The mechanism is illustrated for Cu in solid solution in Al, which exhibits segregation of Cu to 111 poles and along [110] zone lines in reconstructed APT data. The higher bonding energy of Cu atoms on the surface, confirmed using density-functional theory calculations, causes longer retention on the surface and preferential evaporation of neighboring Al atoms with subsequent athermal relaxation of Cu into higher-neighbor-count sites left vacant by evaporating Al neighbors. This in turn results in barrier-free long-range migration of the Cu atoms by a series of relaxation events that follow the receding terrace ledges towards high-neighbor count poles and zone lines. This mechanism fundamentally limits spatial resolution in the limit of zero temperature.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Atom–by–Atom Fabrication of Single and Few Dopant Quantum Devices

Atomically precise fabrication has an important role to play in developing atom-based electronic devices for use in quantum information processing, quantum materials research, and quantum sensing. Atom-by-atom fabrication has the potential to enable precise control over tunnel coupling, exchange coupling, on-site charging energies, and other key properties of basic devices needed for solid-state quantum computing and analog quantum simulation. Using hydrogen-based scanning probe lithography, individual dopant atoms are deterministically placed relative to atomically aligned contacts and gates to build single electron transistors, single atom transistors, and gate-controlled quantum sensing devices. Here, the key steps required to fabricate and demonstrate the essential building blocks needed for spin selective initialization/readout and coherent quantum manipulation are described.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Visualizing the iron atom exchange front in the Fe(II)-catalyzed recrystallization of goethite by atom probe tomography

The autocatalytic redox interaction between aqueous Fe(II) and Fe(III)-(oxyhydr)oxide minerals such as goethite and hematite leads to rapid recrystallization marked, in principle, by an atom exchange (AE) front, according to bulk iron isotopic tracer studies. However, direct evidence for this AE front has been elusive given the analytical challenges of mass-resolved imaging at the nanoscale on individual crystallites. We report successful isolation and characterization of the AE front in goethite microrods by 3D atom probe tomography (APT). The microrods were reacted with Fe(II) enriched in tracer 57 Fe at conditions consistent with prior bulk studies. APT analyses and 3D reconstructions on cross-sections of the microrods reveal an AE front that is spatially heterogeneous, at times penetrating several nanometers into the lattice, in a manner consistent with defect-accelerated exchange. Evidence for exchange along microstructural domain boundaries was also found, suggesting another important link between exchange extent and initial defect content. The findings provide an unprecedented view into the spatial and temporal characteristics of Fe(II)-catalyzed recrystallization at the atomic scale, and substantiate speculation regarding the role of defects controlling the dynamics of electron transfer and AE interaction at this important redox interface.

Taylor, Sandra D.↗
DOE OSTI2018

Atomic-scale imaging of ultrafast materials dynamics

The advent of short-pulse electron and x-ray sources has enabled pump-probe approaches for elucidating ultrafast materials dynamics. From such studies, a comprehensive picture of the time-dependent evolution of the initial steps of energy deposition, propagation, relaxation, and conversion in a wide range of materials can be generated. In this article, we provide an overview of the capabilities of femtosecond electron and x-ray scattering for resolving structural dynamics of materials. With such approaches, time resolutions are ultimately limited by the durations of the electron and x-ray pulses, and dynamics can be studied at length scales spanning atomic to mesoscale dimensions. The articles in this issue represent a cross section of the vigorous activity occurring in the study of light-induced ultrafast materials dynamics as it relates to charge carriers, surfaces and interfaces, lattice-coupling mechanisms, coherent structural motions, and next-generation instrument development. Here, the approaches highlighted here are leading to new physical insights, new possibilities for engineering the properties of matter, and ultimately, a new understanding of materials functionality on ultrasmall and ultrashort spatiotemporal scales.

36 MATERIALS SCIENCE↗
DOE OSTI2019

A Versatile Approach for Quantification of Surface Site Fractions using Reaction Kinetics: The Case of CO Oxidation on Supported Ir Single Atoms and Nanoparticles

Supported metal single atom catalysts have shown unique activity and selectivity for several reactions. Investigating the reaction mechanism on single atom catalysts and unambiguous assignment of the activity and selectivity requires catalysts with exclusively single atoms. However, it is challenging to prepare pure single atom catalysts with conventional impregnation methods, which typically result in a mixture of single atoms and nanoparticles. Here, we show that owing to different reaction mechanisms on single atoms and nanoparticles, reaction kinetics can serve as a surface sensitive characterization technique for quantifying their surface site fractions. As a case study, we use CO oxidation kinetics on Ir/MgAl2O4 to quantify the surface site fractions of single atoms and nanoparticles and the results are consistent with aberration-corrected scanning transmission electron microscopy, X-ray absorption fine structure and infrared spectroscopies. Additionally, by carefully choosing the reaction conditions, the activity of single atoms (or nanoparticles) can be made dominant, enabling detection of a small fraction, or allowing a study of their reaction mechanism on a catalyst containing a mixture of single atoms and nanoparticles. These results are general and could be applied to other systems where two types of sites have different reaction mechanisms.

Single atom catalyst, Kinetics, CO oxidation, x-ra↗
DOE OSTI2019

Iridium Atoms Bonded to Crystalline Powder MgO: Characterization by Imaging and Spectroscopy

Samples with low loadings of metals on well-defined supports provide some of the best opportunities to determine the metal–support structure and bonding. We illustrate methods for characterizing atomically dispersed heavy metals on metal oxide supports by aberration-corrected scanning transmission electron microscopy (STEM) complemented by fluorescence detection extended X-ray absorption fine structure and infrared spectroscopies. STEM images of Ir atoms derived from Ir(C 2 H 4 ) 2 (acac) (acac = acetylacetonato) on high-surface-area MgO powder were obtained with minimized electron beam damage by quickly recording images near where the focus had been established. The images show that iridium at a loading of 1.0 wt % on MgO calcined at 1073 K was atomically dispersed, populating much of the surface of the MgO particles, which had irregular shapes—consequently the Ir atoms were bonded at various sites to two or three surface O atoms. In contrast, MgO calcined at 1273 K consisted of almost perfectly cubic crystals, and Ir atoms at a loading of only 0.01 wt % on this nearly ideal support were anchored preferentially at edges and corners of the (100) faces and bonded to three surface O atoms. The latter results indicate a path forward for the determination of precise structures of atomically dispersed metals on crystalline metal oxide supports.

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

Accelerated Cu2O Reduction by Single Pt Atoms at the Metal-Oxide Interface§

The reducibility of metal oxides, when serving as the catalyst support or the active sites themselves, plays an important role in heterogeneous catalytic reactions. Here we present an integrated experimental and theoretical study that reveals how the addition of small amounts of atomically dispersed Pt at the metal/oxide interface dramatically enhances the reducibility of a Cu2O thin film by H2. X-ray photoelectron spectroscopy (XPS) and temperature-programmed desorption (TPD) results reveal that upon oxidation, a PtCu single-atom alloy (SAA) surface is covered by a thin Cu2O film and is therefore unable to dissociate H2. Despite this, in situ studies using ambient pressure (AP) XPS reveal that the presence of a small amount of Pt under the oxide layer can, at the single-atom limit, promote the reduction of Cu2O by H2 at room temperature. We build two density functional theory based surface models to better understand these experimental findings: A Cu2O/Cu(111)-like surface oxide layer, known as the ‘29’ oxide, in which Pt is alloyed into the Cu(111) surface as well as a PtCu SAA. Our calculations suggest that the increased activity is due to the presence of atomically dispersed Pt under the surface oxide layer, which weakens the Cu-O bonds in its immediate vicinity, thus making the interface between subsurface Pt and the surface oxide a nucleation site for the formation of metallic Cu. This initial step in the reduction process results in the presence of surface Pt atoms surrounded by metallic Cu patches, and the Pt atoms become active in H2 dissociation, which consequently accelerates the reduction of the oxide layer. This work demonstrates how isolated Pt atoms at the metal/oxide interface of a Cu-based catalyst accelerate the reduction of the oxide and, therefore, helps maintain the active, reduced state of the catalyst under reaction conditions, as is required for the synthesis of methanol from CO2 hydrogenation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Casimir-Polder potential on an excited atom near an atomic array

We develop a microscopic description of the fluctuation-mediated Casimir-Polder (CP) shifts on a 'test' two-level atom placed near a two-dimensional atomic array of two-level atoms. We derive the resonant and off-resonant CP potentials experienced by the excited test atom using fourth-order perturbation theory, under the assumption that the test atom resonance is far detuned from those of the array atoms. The total potential on the test atom can be described as the sum of the pairwise resonant and off-resonant potentials resulting from its interaction with the individual atoms of the array. We analyze the asymptotic scaling of CP shifts as a function of the test atom-array separation, and its dependence on various system parameters: array spacing and size, and dipole orientation of the array atoms. Our results bridge the description of CP potential across two distinct regimes: (i) from a single-atom limit where we recover the well-known two-atom Van der Waals potential, (ii) to a macroscopic boundary limit, where we demonstrate new asymptotic scaling laws. We demonstrate that these scaling laws can be tuned via the microscopic parameters of the atomic array, establishing atomically-controlled arrays as a versatile platform for tailoring fluctuation-induced QED phenomena.

FOS: Physical sciences↗
DOE OSTI2018

Building Structures Atom by Atom via Electron Beam Manipulation

Building materials from the atom up is the pinnacle of materials fabrication. Until recently the only platform that offered single-atom manipulation was scanning tunneling microscopy. Here controlled manipulation and assembly of a few atom structures are demonstrated by bringing together single atoms using a scanning transmission electron microscope. An atomically focused electron beam is used to introduce Si substitutional defects and defect clusters in graphene with spatial control of a few nanometers and enable controlled motion of Si atoms. The Si substitutional defects are then further manipulated to form dimers, trimers, and more complex structures. The dynamics of a beam-induced atomic-scale chemical process is captured in a time-series of images at atomic resolution. In conclusion, these studies suggest that control of the e-beam-induced local processes offers the next step toward atom-by-atom nanofabrication, providing an enabling tool for the study of atomic-scale chemistry in 2D materials and fabrication of predefined structures and defects with atomic specificity.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Three-dimensional atomic packing in amorphous solids with liquid-like structure

Liquids and solids are two fundamental states of matter. However, our understanding of their three-dimensional atomic structure is mostly based on physical models. Here we use atomic electron tomography to experimentally determine the three-dimensional atomic positions of monatomic amorphous solids, namely a Ta thin film and two Pd nanoparticles. We observe that pentagonal bipyramids are the most abundant atomic motifs in these amorphous materials. Instead of forming icosahedra, the majority of pentagonal bipyramids arrange into pentagonal bipyramid networks with medium-range order. Molecular dynamics simulations further reveal that pentagonal bipyramid networks are prevalent in monatomic metallic liquids, which rapidly grow in size and form more icosahedra during the quench from the liquid to the glass state. Furthermore, these results expand our understanding of the atomic structures of amorphous solids and will encourage future studies on amorphous–crystalline phase and glass transitions in non-crystalline materials with three-dimensional atomic resolution.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Atom-by-atom fabrication with electron beams

Assembling matter atom-by-atom into functional devices is the ultimate goal of nanotechnology. The possibility of achieving this goal is intrinsically dependent on the ability to visualize matter at the atomic level, induce and control atomic-scale motion, facilitate and direct chemical reactions, and coordinate and guide fabrication processes towards desired structures atom-by-atom. In this Perspective, we summarize recent progress in chemical transformations, material alterations and atomic dynamics studies enabled by the converged, atomic-sized electron beam of an aberration-corrected scanning transmission electron microscope. We discuss how such top-down observations have led to the concept of controllable, beam-induced processes and then of bottom-up, atom-by-atom assembly via electron-beam control. Finally, the progress in this field, from electron-beam-induced material transformations to atomically precise doping and multi-atom assembly, is reviewed, as are the associated engineering, theoretical and big-data challenges.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Guided cold atom inertial sensors with membrane integrated photonics on atom trap integrated platforms

A guided cold-atom inertial sensor system comprises an atom trap integrated platform, a laser system, a magnetic field system, a control system, and a computing system. The laser system and magnetic field system are adapted to form a magneto-optical trap (MOT) about a suspended waveguide of the atom trap integrated platform made of membrane integrated photonics. After loading cold atoms from a MOT, the photonic atom trap integrated platform generates one-dimensional guided atoms with an evanescent field optical dipole trap (EF-ODT) along the optical waveguide to create guided atomic accelerometers/gyroscopes. Motion of atomic wavepackets in a superposition state is created along the guided atom geometry by way of state-dependent momentum kicks. The light-pulse sequence of guided atom interferometry splits, redirects, and recombines atomic wavepackets, which allows measurement of atom interference fringes sensitive to inertial forces via a probe laser.

Lee, Jongmin↗