Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “point defect”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 1,315 records · Page 73
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

A computational study of yttria-stabilized zirconia: I. Using crystal chemistry to search for the ground state on a glassy energy landscape

Yttria-stabilized zirconia (YSZ), a ZrO 2 -Y 2 O 3 solid solution that contains a large population of oxygen vacancies, is widely used in energy and industrial applications. Past computational studies correctly predicted the anion diffusivity but not the cation diffusivity, which is important for material processing and stability. One of the challenges lies in identifying a plausible configuration akin to the ground state in a glassy landscape. This is unlikely to come from random sampling of even a very large sample space, but the odds are much improved by incorporating packing preferences revealed by a modest sized configurational library established from empirical potential calculations. Ab initio calculations corroborated these preferences, which prove remarkably robust extending to the fifth cation-oxygen shell about 8 Å away. Yet because of frustration there are still rampant violations of packing preferences and charge neutrality in the ground state, and the approach toward it bears a close analogy to glass relaxations. Fast relaxations proceed by fast oxygen movement around cations, while slow relaxations require slow cation diffusion. The latter is necessarily cooperative because of strong coupling imposed by the long-range packing preferences.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Effects of transition metals on the evolution of polymer-derived SiOC ceramics

This work focuses on catalytic graphitization from different metals, iron (Fe), cobalt (Co), and nickel (Ni), for inducing carbon growth in silicon oxycarbides (SiOCs) during the pyrolysis. Fe, Co, and Ni-modified SiOCs were synthesized by pyrolysis to 900, 1100, and 1300 °C respectively in Ar. The transition metals induced the formation of the corresponding metal silicides, β-SiC, and graphitic carbon with the catalytic activity in the order of Fe > Co > Ni, in agreement with the activation energy calculation based on the carbon types and amounts. Lateral growth of turbostratic carbon followed a 2D grain growth process and its point-like defect density decreased based on the catalytic order of the transition metals, with SiOC/Fe having the lowest defect density. Quantitative analysis of the XPS results with Rietveld refinement illustrated that the phase separation of SiOC is more dominant than local carbothermal reduction between SiO 2 and C in the SiOC/M (M = Ni, Co, or Fe) systems. Understanding the catalytic graphitization effect of Ni, Co, and Fe on polymer derived ceramics offers new strategies in increasing high-temperature phase amounts and thus creating novel materials for heterogeneous catalysis, magnetic, and other applications.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Effects of proton irradiation on flux-pinning properties of underdoped Ba(Fe 0.96 Co 0.04 ) 2 As 2 pnictide superconductor

We study the effect of proton irradiation on Ba(Fe 0.96 Co 0.04 ) 2 As 2 superconducting single crystals from combined magnetisation and magnetoresistivity measurements. The study allows the extraction of the values of the apparent pinning energy U 0 of the samples prior to and after irradiation, as well as comparison of the values of U 0 obtained from the flux-flow reversible region with those from the flux-creep irreversible region. Irradiation reduces T c modestly, but significantly reduces U 0 in both regimes: the critical current density J c is modified, most strikingly by the disappearance of the second magnetisation peak after irradiation. Analysis of the functional form of the pinning force and of the temperature dependence of J c for zero field, indicates that proton irradiation in this case has not changed the pinning regime, but has introduced a high density of shallow point-like defects. Lastly, by considering a model that takes into account the effect of disorder on the irreversibility line, the data suggests that irradiation produced a considerable reduction in the average effective disorder overall, consistent with the changes observed in U 0 and J c .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Microstructural evolution of compositionally complex solid-solution alloys under in-situ dual-beam irradiation

Here, this work attempts to link the microstructural evolution of single-phase compositionally complex alloy (CCA) compositions under dual-beam irradiation to their Mn-content via the stacking-fault energy (SFE) and vacancy migration energies. Two alloys, Cr 18 Fe 27 Mn 27 Ni 28 and Cr 15 Fe 35 Mn 15 Ni 35 , along with less compositionally complex pure Ni and Fe 56 Ni 44 binary were irradiated at 500 and 600 °C under dual-beam 1 MeV Kr 2+ and 16 keV He + heavy-ions up to 7 displacements per atom (dpa) with a He/dpa ratio of 0.75 %/dpa using in situ transmission electron microscopy (TEM). Due to the bubble-stabilizing effect of implanted He, bubbles were observed in all irradiations, and populations of faulted interstitial loops were characterized in Cr 18 Fe 27 Mn 27 Ni 28 and Cr 15 Fe 35 Mn 15 Ni 35 . A reduction in swelling was observed in the two CCAs compared to pure Ni and Fe 56 Ni 44 . Although swelling increased from 500 to 600 °C in Fe 56 Ni 44 , Cr 15 Fe 35 Mn 15 Ni 35 and Cr 18 Fe 27 Mn 27 Ni 28 both swelled slightly more at 500 °C. This was attributed to the difference in vacancy mobility, stronger pinning effect of vacancies on He, and the sink strength of faulted dislocation loops. Faulted interstitial loops nucleated with a higher number density and dislocation line density in Cr 15 Fe 35 Mn 15 Ni 35 at both temperatures, and at 600 °C in both materials. The differences in faulted loop population and temperature effect on swelling are correlated to the Mn-content and the measured SFE (20.2 ± 6.7 mJ/m 2 for Cr 18 Fe 27 Mn 27 Ni 28 and 9.2 ± 3.4 mJ/m 2 for Cr 15 Fe 35 Mn 15 Ni 35 ).

36 MATERIALS SCIENCE↗
DOE OSTI2025

p-Type BiVO 4 for Solar O 2 Reduction to H 2 O 2

Photoelectrochemical cells (PECs) can directly utilize solar energy to drive chemical reactions to produce fuels and chemicals. Oxide-based photoelectrodes in general exhibit enhanced stability against photocorrosion, which is a critical advantage for building a sustainable PEC. However, most oxide-based semiconductors are n-type, and p-type oxides that can be used as photocathodes are limited. In this study, we report the synthesis, characterization, and application of p-type BiVO 4 with a monoclinic scheelite (ms) structure. ms-BiVO 4 is inherently n-type, and it has been investigated only as a photoanode to date. In this study, we prepared p-type ms-BiVO 4 (bandgap of 2.4 eV) via atomic doping of Ca 2+ at the Bi 3+ site under an O 2 -rich environment and examined its performance as a photocathode. We then demonstrated that the Ca-doped ms-BiVO 4 photocathode can be used for solar O 2 reduction to H 2 O 2 when coupled with appropriate catalysts. Our computational investigation using hybrid density functional theory revealed that holes are stable as polarons in ms-BiVO 4 and have a low self-trapping energy, that may lead to free carriers in the valence band at finite temperature. Our calculations also show that Ca is an effective shallow acceptor dopant with low formation energy and thermal ionization energy leading to p-type conductivity. In conclusion, our joint experimental and computational results provide critical insights into the design of p-type ms-BiVO 4 , enabling its use as a polaronic oxide photocathode.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Site selective substitution Pt for Ti in KTiOPO{sub 4}:Ga crystals revealed by electron paramagnetic resonance

Electron Paramagnetic Resonance at low temperatures has been used to characterize potassium titanyl phosphate (KTiOPO{sub 4}) single crystals grown by different techniques. Irradiation with 20 MeV electrons performed at room temperature and liquid nitrogen temperature caused an appearance of electrons and holes. Platinum impurities act as electron traps in KTiOPO{sub 4} creating Pt{sup 3+} centers. Two different Pt{sup 3+} centers were observed, Pt(A) and Pt(D). The Pt(A) centers are dominant in undoped samples, whereas Pt(D)—in Ga-doped KTP crystals. Superhyperfine structure registered for Pt(D) centers was attributed to interactions of platinum electrons with {sup 39}K and two {sup 31}P nuclei in their surroundings. In both Pt(A) and Pt(D) centers, Pt{sup 3+} ions substitute for Ti{sup 4+} ions, but with a preference to one of two electrically distinct crystallographic positions. The site selective substitution can be controlled by the Ga-doping.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Negative terahertz conductivity in disordered graphene bilayers with population inversion

The gapless energy band spectra make the structures based on graphene and graphene bilayer with the population inversion to be promising media for the interband terahertz (THz) lasing. However, a strong intraband absorption at THz frequencies still poses a challenge for efficient THz lasing. In this paper, we show that in the pumped graphene bilayer, the indirect interband radiative transitions accompanied by scattering of carriers by disorder can provide a substantial negative contribution to the THz conductivity (together with the direct interband transitions). In the graphene bilayer on high-κ substrates with point charged defects, these transitions substantially compensate the losses due to the intraband (Drude) absorption. We also demonstrate that the indirect interband contribution to the THz conductivity in a graphene bilayer with the extended defects (such as the charged impurity clusters) can surpass by several times the fundamental limit associated with the direct interband transitions, and the Drude conductivity as well. These predictions can affect the strategy of the graphene-based THz laser implementation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Multimode resistive switching in nanoscale hafnium oxide stack as studied by atomic force microscopy

The nanoscale resistive switching in hafnium oxide stack is investigated by the conductive atomic force microscopy (C-AFM). The initial oxide stack is insulating and electrical stress from the C-AFM tip induces nanometric conductive filaments. Multimode resistive switching can be observed in consecutive operation cycles at one spot. The different modes are interpreted in the framework of a low defect quantum point contact theory. The model implies that the optimization of the conductive filament active region is crucial for the future application of nanoscale resistive switching devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Machine learning for impurity charge-state transition levels in semiconductors from elemental properties using multi-fidelity datasets

Quantifying charge-state transition energy levels of impurities in semiconductors is critical to understanding and engineering their optoelectronic properties for applications ranging from solar photovoltaics to infrared lasers. While these transition levels can be measured and calculated accurately, such efforts are time-consuming and more rapid prediction methods would be beneficial. Here, we significantly reduce the time typically required to predict impurity transition levels using multi-fidelity datasets and a machine learning approach employing features based on elemental properties and impurity positions. We use transition levels obtained from low-fidelity (i.e., local-density approximation or generalized gradient approximation) density functional theory (DFT) calculations, corrected using a recently proposed modified band alignment scheme, which well-approximates transition levels from high-fidelity DFT (i.e., hybrid HSE06). Further, the model fit to the large multi-fidelity database shows improved accuracy compared to the models trained on the more limited high-fidelity values. Crucially, in our approach, when using the multi-fidelity data, high-fidelity values are not required for model training, significantly reducing the computational cost required for training the model. Our machine learning model of transition levels has a root mean squared (mean absolute) error of 0.36 (0.27) eV vs high-fidelity hybrid functional values when averaged over 14 semiconductor systems from the II–VI and III–V families. As a guide for use on other systems, we assessed the model on simulated data to show the expected accuracy level as a function of bandgap for new materials of interest. Finally, we use the model to predict a complete space of impurity charge-state transition levels in all zinc blende III–V and II–VI systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Recombination radius of a Frenkel pair and capture radius of a self-interstitial atom by vacancy clusters in bcc Fe

The recombination radius of a Frenkel pair is a fundamental parameter for the object kinetic Monte Carlo (OKMC) and mean field rate theory (RT) methods that are used to investigate irradiation damage accumulation in neutron irradiated nuclear materials. The recombination radius in bcc Fe has been studied both experimentally and numerically, however there is no general consensus about its value. The detailed atomistic processes of recombination also remain uncertain. Values from 1:0a₀ to 3:3a₀ have been employed as a recombination radius in previous studies using OKMC and RT. The recombination process of a Frenkel pair is investigated at the atomic level using the self-evolved atomistic kinetic Monte Carlo (SEAKMC) method in this paper. SEAKMC calculations reveal that a self-interstitial atom recombines with a vacancy in a spontaneous reaction from several nearby sites following characteristic pathways. The recombination radius of a Frenkel pair is estimated to be 2.26a₀ by taking the average of the recombination distances from 80 simulation cases. This value agrees well with the experimental estimate. In addition, we apply these procedures to the capture radius of a self-interstitial atom by a vacancy cluster. The capture radius is found to gradually increase with the size of the vacancy cluster. The fitting curve for the capture radius is obtained as a function of the number of vacancies in the cluster.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Development of next generation tempered and ODS reduced activation ferritic/martensitic steels for fusion energy applications

Reduced activation ferritic/martensitic steels are currently the most technologically mature option for the structural material of proposed fusion energy reactors. Advanced next-generation higher performance steels offer the opportunity for improvements in fusion reactor operational lifetime and reliability, superior neutron radiation damage resistance, higher thermodynamic efficiency, and reduced construction costs. The two main strategies for developing improved steels for fusion energy applications are based on (1) an evolutionary pathway using computational thermodynamics modelling and modified thermomechanical treatments (TMT) to produce higher performance reduced activation ferritic/martensitic (RAFM) steels and (2) a higher risk, potentially higher payoff approach based on powder metallurgy techniques to produce very high strength oxide dispersion strengthened (ODS) steels capable of operation to very high temperatures and with potentially very high resistance to fusion neutron-induced property degradation. The current development status of these next-generation high performance steels is summarized, and research and development challenges for the successful development of these materials are outlined. In conclusion, material properties including temperature-dependent uniaxial yield strengths, tensile elongations, high-temperature thermal creep, Charpy impact ductile to brittle transient temperature (DBTT) and fracture toughness behaviour, and neutron irradiation-induced low-temperature hardening and embrittlement and intermediate-temperature volumetric void swelling (including effects associated with fusion-relevant helium and hydrogen generation) are described for research heats of the new steels.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2016

Flux line relaxation kinetics following current quenches in disordered type-II superconductors

We investigate the relaxation dynamics of magnetic vortex lines in type-II superconductors following rapid changes of the external driving current by means of an elastic line model simulated with Langevin molecular dynamics. A system of flux vortices in a sample with randomly distributed point-like defects is subjected to an external current of appropriate strength for a sufficient period of time so as to be in a moving non-equilibrium steady state. Here, the current is then instantaneously lowered to a value that pertains to either the moving or pinned regime. The ensuing relaxation of the flux lines is studied via one-time observables such as their mean velocity and radius of gyration. We have in addition measured the two-time flux line height autocorrelation function to investigate dynamical scaling and aging behavior in the system, which in particular emerge after quenches into the glassy pinned state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Equilibrium field theory of magnetic monopoles in degenerate square spin ice: Correlations, entropic interactions, and charge screening regimes

In this work, we describe degenerate square spin as an ensemble of magnetic monopoles coupled via an emergent entropic field that subsumes the effect of the underlying spin vacuum. We compute their effective free energy, entropic interaction, correlations, screening, and structure factor, and find that they coincide with the experimental ones. Unlike in pyrochlore ices, a dimensional mismatch between real and entropic interactions leads to weak singularities at the pinch points and algebraic correlations at long distances. This algebraic screening can be, however, camouflaged by a pseudoscreening regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Role of carbon and hydrogen in limiting n -type doping of monoclinic ( Al x Ga 1 – x ) 2 O 3

In this study, we use hybrid density functional calculations to assess n -type doping in monoclinic ( Al x Ga 1 – x ) 2 O 3 alloys. We focus on silicon, the most promising donor dopant, and study the structural properties, formation energies, and charge-state transition levels of its various configurations. We also explore the impact of carbon and hydrogen, which are common impurities in metal-organic chemical vapor deposition (MOCVD). In Ga 2 O 3 , Si Ga is an effective shallow donor, but in Al 2 O 3 Si Al acts as a DX center with a ( + / – ) transition level in the band gap. Interstitial hydrogen acts as a shallow donor in Ga 2 O 3 but behaves as a compensating acceptor in n -type Al 2 O 3 . Interpolation indicates that Si is an effective donor in ( Al x Ga 1 – x ) 2 O 3 up to 70% Al, but it can be compensated by hydrogen already at 1% Al. We also assess the diffusivity of hydrogen and study complex formation. Si cation – H complexes have relatively low binding energies. Substitutional carbon on a cation site acts as a shallow donor in Ga 2 O 3 , but can be stable in a negative charge state in ( Al x Ga 1 – x ) 2 O 3 when x > 5 % . Substitutional carbon on an oxygen site ( C O ) always acts as an acceptor in n -type ( Al x Ga 1 – x ) 2 O 3 , but will incorporate only under relatively oxygen-poor conditions. C O – H complexes can actually incorporate more easily, explaining observations of carbon-related compensation in Ga 2 O 3 grown by MOCVD. We also investigate C cation – H complexes, finding they have high binding energies and act as compensating acceptors when x > 56 % ; otherwise the hydrogen just passivates the unintentional carbon donors. C-H complex formation explains why MOCVD-grown Ga 2 O 3 can exhibit record-low free-carrier concentrations, in spite of the unavoidable incorporation of carbon. Our study highlights that, while Si is in principle a suitable shallow donor in ( Al x Ga 1 – x ) 2 O 3 alloys up to high Al compositions, control of unintentional impurities is essential to avoid compensation.

36 MATERIALS SCIENCE↗