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The growth and nanothermite reaction of 2Al/3NiO multilayer thin films

Journal of Applied Physics

Abere, Michael J.; Beason, Matthew T.; Reeves, Robert V.; Rodriguez, Mark A.; Kotula, Paul G.; Sobczak, Catherine E.; Son, Steven F.; Yarrington, Cole D.; Adams, David P.

Nanothermite NiO–Al is a promising material system for low gas emission heat sources; yet, its reactive properties are highly dependent on material processing conditions. In the current study, sputter deposition is used to fabricate highly controlled nanolaminates comprised of alternating NiO and Al layers. Films having an overall stoichiometry of 2Al to 3NiO were produced with different bilayer thicknesses to investigate how ignition and self-sustained, high temperature reactions vary with changes to nanometer-scale periodicity and preheat conditions. Ignition studies were carried out with both hot plate and laser irradiation and compared to slow heating studies in hot-stage x-ray diffraction. Ignition behavior has bilayer thickness and heating rate dependencies. The 2Al/3NiO with λ ≤ 300 nm ignited via solid/solid diffusion mixing (activation energy, E a  = 49 ± 3 kJ/mole). Multilayers having λ ≥ 500 nm required a more favorable mixing kinetics of solid/liquid dissolution into molten Al ( E a  = 30 ± 4 kJ/mole). This solid/liquid dissolution E a is a factor of 5 lower than that of the previously reported powder compacts due to the elimination of a passivating Al oxide layer present on the powder. The reactant mixing mechanism between 300 and 500 nm bilayer thicknesses was dependent on the ignition source's heating rate. The self-propagating reaction velocities of 2Al/3NiO multilayers varied from 0.4 to 2.5 m/s. Pre-heating nanolaminates to temperatures below the onset reaction temperatures associated with forming intermediate nickel aluminides at multilayer interfaces led to increased propagation velocities, whereas pre-heating samples above the onset temperatures inhibited subsequent attempts at laser ignition.

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Irradiation-induced grain boundary facet motion: In situ observations and atomic-scale mechanisms

Science Advances

Barr, Christopher M.; Chen, Elton Y.; Nathaniel, James E.; Lu, Ping L.; Adams, David P.; Dingreville, Remi P.; Boyce, Brad B.; Hattar, Khalid M.; Medlin, Douglas L.

Metals subjected to irradiation environments undergo microstructural evolution and concomitant degradation, yet the nanoscale mechanisms for such evolution remain elusive. Here, we combine in situ heavy ion irradiation, atomic resolution microscopy, and atomistic simulation to elucidate how radiation damage and interfacial defects interplay to control grain boundary (GB) motion. While classical notions of boundary evolution under irradiation rest on simple ideas of curvature-driven motion, the reality is far more complex. Focusing on an ion-irradiated Pt Σ3 GB, we show how this boundary evolves by the motion of 120° facet junctions separating nanoscale {112} facets. Our analysis considers the short- and mid-range ion interactions, which roughen the facets and induce local motion, and longer-range interactions associated with interfacial disconnections, which accommodate the intergranular misorientation. We suggest how climb of these disconnections could drive coordinated facet junction motion. These findings emphasize that both local and longer-range, collective interactions are important to understanding irradiation-induced interfacial evolution.

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3D simulations of spinlike flames in Co/Al multilayers with enhanced conduction losses

Combustion and Flame

Kittell, David E.; Abere, Michael J.; Yarrington, Cole Y.; Adams, David P.

Reactive Co/Al multilayers are uniformly structured materials that may be ignited to produce rapid and localized heating. Prior studies varying the bilayer thickness (i.e., sum of two individual layers of Co and Al) have revealed different types of flame morphologies, including: (a) steady/planar, (b) wavy/periodic, and (c) transverse bands, originating in the flame front. These instabilities resemble the “spin waves” first observed in the early studies of solid combustion (i.e., Ti cylinder in a N2 atmosphere), and are likewise thought to be due to the balance of heat released by reaction and heat conduction forward into the unreacted multilayer. However, the multilayer geometry and three-dimensional (3D) edge effects are relatively unexplored. In this work, a new diffusion-limited reaction model for Co/Al multilayers was implemented in large, novel 3D finite element analysis (FEA) simulations, in order to study the origins of these spinlike flames. This reaction model builds upon previous work by introducing three new phase-dependent property models for: (1) the diffusion coefficient, (2) anisotropic thermal conductivity tensor, and (3) bulk heat capacity, as well as one additional model for the bilayer-dependent heat of reaction. These novel 3D simulations are the first to predict both steady and unsteady flames in Co/Al multilayers. Moreover, two unsteady modes of flame propagation are identified, which depend on the enhanced conduction losses with slower flames, as well as flame propagation around notched edges. Future work will consider the generality of the current modeling approach and also seek to define a more generalized set of stability criteria for additional multilayer systems.

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Germanium Telluride Chalcogenide Switches for RF Applications

Hummel, Gwendolyn H.; Patrizi, G.A.; Young, Andrew I.; Schroeder, Katlin S.; Ruyack, Alexander R.; Schiess, Adrian R.; Finnegan, Patrick S.; Adams, David P.; Nordquist, Christopher N.

This project developed prototype germanium telluride switches, which can be used in RF applications to improve SWAP (size, weight, and power) and signal quality in RF systems. These switches can allow for highly reconfigurable systems, including antennas, communications, optical systems, phased arrays, and synthetic aperture radar, which all have high impact on current National Security goals for improved communication systems and communication technology supremacy. The final result of the project was the demonstration of germanium telluride RF switches, which could act as critical elements necessary for a single chip RF communication system that will demonstrate low SWAP and high reconfigurability

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Basic Research of Intrinsic, Tamper Indication Markings and Patterns Defined by Pulsed Laser Irradiation: 2015 Annual Report IACRO 13-5897I (DTRA Project Year End Report)

Adams, David P.

Information from 2015 annual report highlighting several tasks, including: Task 7: Research of microspectrophotometry for inspection and validation of laser color markings. Task 8: Investigate new laser fabrication techniques that produce color markings with improved corrosion resistance. Task 9: Research new methods for laser marking curved surfaces (and large areas). Task 10: Complete model simulations of laser-induced ripple formation-involves an ElectroMagnetic field solver.

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Simultaneous thickness and thermal conductivity measurements of thinned silicon from 100 nm to 17 μ m

Applied Physics Letters

Scott, Ethan A.; Perez, Christopher P.; Saltonstall, Christopher B.; Adams, David P.; Carter Hodges, V.; Asheghi, Mehdi; Goodson, Kenneth E.; Hopkins, Patrick E.; Leonhardt, Darin L.; Ziade, Elbara Z.

Studies of size effects on thermal conductivity typically necessitate the fabrication of a comprehensive film thickness series. In this Letter, we demonstrate how material fabricated in a wedged geometry can enable similar, yet higher-throughput measurements to accelerate experimental analysis. Frequency domain thermoreflectance (FDTR) is used to simultaneously determine the thermal conductivity and thickness of a wedged silicon film for thicknesses between 100 nm and 17 μm by considering these features as fitting parameters in a thermal model. FDTR-deduced thicknesses are compared to values obtained from cross-sectional scanning electron microscopy, and corresponding thermal conductivity measurements are compared against several thickness-dependent analytical models based upon solutions to the Boltzmann transport equation. Our results demonstrate how the insight gained from a series of thin films can be obtained via fabrication of a single sample.

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Variable Laser Ignition Pathways in Al/Pt Reactive Multilayers across 10 Decades of Pulse Duration

Journal of Physical Chemistry C

Abere, Michael J.; Yarrington, Cole D.; Kotula, Paul G.; McDonald, Joel P.; Adams, David P.

Pulsed laser irradiation is used to investigate the local initiation of rapid, self-propagating formation reactions in Al/Pt multilayers. The single pulse direct laser ignition of these 1.6 μm thick freestanding foils was characterized over 10 decades of pulse duration (10 ms to 150 fs). Finite element, reactive heat transport modeling of the near-threshold conditions has identified three distinct ignition pathways. For milli- to microsecond pulses, ignition occurs following sufficient absorption of laser energy to enable diffusion of Al and Pt between layers such that the heat released from the corresponding exothermic reaction overcomes conductive losses outside the laser-irradiated zone. When pulse duration is decreased into the nanosecond regime, heat is concentrated near the surface such that the Al locally melts, and a portion of the top-most bilayers react initially. The favorable kinetics and additional heat enable ignition. Further reducing pulse duration to hundreds of femtoseconds leads to a third ignition pathway. While much of the energy from these pulses is lost to ablation, the remaining heat beneath the crater can be sufficiently concentrated to drive a transverse self-propagating reaction, wherein the heat released from mixing at each interface occurs under kinetic conditions capable of igniting the subsequent layer.

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The role of grain boundary character in solute segregation and thermal stability of nanocrystalline Pt-Au

Nanoscale

Barr, Christopher M.; Foiles, Stephen M.; Alkayyali, Malek; Mahmood, Yasir; Price, Patrick M.; Adams, David P.; Boyce, Brad B.; Abdeljawad, Fadi; Hattar, Khalid M.

Nanocrystalline (NC) metals suffer from an intrinsic thermal instability; their crystalline grains undergo rapid coarsening during processing treatments or under service conditions. Grain boundary (GB) solute segregation has been proposed to mitigate grain growth and thermally stabilize the grain structures of NC metals. However, the role of GB character in solute segregation and thermal stability of NC metals remains poorly understood. Herein, we employ high resolution microscopy techniques, atomistic simulations, and theoretical analysis to investigate and characterize the impact of GB character on segregation behavior and thermal stability in a model NC Pt-Au alloy. High resolution electron microscopy along with X-ray energy dispersive spectroscopy and automated crystallographic orientation mapping is used to obtain spatially correlated Pt crystal orientation, GB misorientation, and Au solute concentration data. Atomistic simulations of polycrystalline Pt-Au systems are used to reveal the plethora of GB segregation profiles as a function of GB misorientation and the corresponding impact on grain growth processes. With the aid of theoretical models of interface segregation, the experimental data for GB concentration profiles are used to extract GB segregation energies, which are then used to elucidate the impact of GB character on solute drag effects. Our results highlight the paramount role of GB character in solute segregation behavior. In broad terms, our approach provides future avenues to employ GB segregation as a microstructure design strategy to develop NC metallic alloys with tailored microstructures. This journal is

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Thin film graded density impactors for high rate off-Hugoniot loading: Application to Ta strength

2019 15th Hypervelocity Impact Symposium, HVIS 2019

Brown, Justin L.; Adams, David P.; Alexander, Charles S.; Wise, Jack L.; Reinhart, William D.

Graded density impactors (GDIs) have long been of interest to provide off-Hugoniot loading capabilities for impact systems. We describe a new technique which utilizes sputter deposition to produce an approximately 40 µm-thick film containing alternating layers of Al and Cu. The thicknesses of the respective layers are adjusted to give an effective density gradient through the film. The GDIs were launched into samples of interest with a 2-stage light gas gun, and the resulting shock-ramp-release velocity profiles were measured over timescales of ~10 ns with a new velocimetry probe. Results are shown for the direct impact of the film onto a LiF window, which allows for the dynamic characterization of the GDI, as well as from impact onto a thin (~40 µm) sputtered Ta sample backed by a LiF window. These measurements were coupled into mesoscale numerical simulations to infer the strength of Ta at the high rate (107 s-1), and high pressure (1 MBar) conditions this unique capability provides. Initial results suggest this is a viable strength platform which fills a critical gap and aids in cross-platform comparisons with other high-pressure strength platforms.

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Thermal conductivity of (Ge2Sb2Te5)1–xCx phase change films

Journal of Applied Physics

Scott, Ethan A.; Ziade, Elbara Z.; Saltonstall, Christopher B.; McDonald, Anthony E.; Rodriguez, Mark A.; Hopkins, Patrick E.; Beechem, Thomas E.; Adams, David P.

Germanium–antimony–telluride has emerged as a nonvolatile phase change memory material due to the large resistivity contrast between amorphous and crystalline states, rapid crystallization, and cyclic endurance. Improving thermal phase stability, however, has necessitated further alloying with optional addition of a quaternary species (e.g., C). In this work, the thermal transport implications of this additional species are investigated using frequency-domain thermoreflectance in combination with structural characterization derived from x-ray diffraction and Raman spectroscopy. Specifically, the room temperature thermal conductivity and heat capacity of (Ge2Sb2Te5)1–xCx are reported as a function of carbon concentration (x ≤ 0:12) and anneal temperature (T ≤ 350 °C) with results assessed in reference to the measured phase, structure, and electronic resistivity. Phase stability imparted by the carbon comes with comparatively low thermal penalty as materials exhibiting similar levels of crystallinity have comparable thermal conductivity despite the addition of carbon. The additional thermal stability provided by the carbon does, however, necessitate higher anneal temperatures to achieve similar levels of structural order.

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Complexion dictated thermal resistance with interface density in reactive metal multilayers

Physical Review B

Saltonstall, Christopher B.; McClure, Zachary D.; Abere, Michael J.; Guzman, David; Reeve, Samuel T.; Strachan, Alejandro; Kotula, Paul G.; Adams, David P.; Beechem, Thomas E.

Multilayers composed of aluminum (Al) and platinum (Pt) exhibit a nonmonotonic trend in thermal resistance with bilayer thickness as measured by time domain thermoreflectance. The thermal resistance initially increases with reduced bilayer thickness only to reach a maximum and then decrease with further shrinking of the multilayer period. These observations are attributed to the evolving impact of an intermixed amorphous complexion approximately 10 nm in thickness, which forms at each boundary between Al- and Pt-rich layers. Scanning transmission electron microscopy combined with energy dispersive x-ray spectroscopy find that the elemental composition of the complexion varies based on bilayer periodicity as does the fraction of the multilayer composed of this interlayer. These variations in complexion mitigate boundary scattering within the multilayers as shown by electronic transport calculations employing density-functional theory and nonequilibrium Green's functions on amorphous structures obtained via finite temperature molecular dynamics. The lessening of boundary scattering reduces the total resistance to thermal transport leading to the observed nonmonotonic trend thereby highlighting the central role of complexion on thermal transport within reactive metal multilayers.

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Results 1–25 of 215
Results 1–25 of 215