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At least 919 records · Page 51

MISSE 2 PEACE Polymers Experiment Atomic Oxygen Erosion Yield Error Analysis

Atomic oxygen erosion of polymers in low Earth orbit (LEO) poses a serious threat to spacecraft performance and durability. To address this, 40 different polymer samples and a sample of pyrolytic graphite, collectively called the PEACE (Polymer Erosion and Contamination Experiment) Polymers, were exposed to the LEO space environment on the exterior of the International Space Station (ISS) for nearly 4 years as part of the Materials International Space Station Experiment 1 & 2 (MISSE 1 & 2). The purpose of the PEACE Polymers experiment was to obtain accurate mass loss measurements in space to combine with ground measurements in order to accurately calculate the atomic oxygen erosion yields of a wide variety of polymeric materials exposed to the LEO space environment for a long period of time. Error calculations were performed in order to determine the accuracy of the mass measurements and therefore of the erosion yield values. The standard deviation, or error, of each factor was incorporated into the fractional uncertainty of the erosion yield for each of three different situations, depending on the post-flight weighing procedure. The resulting error calculations showed the erosion yield values to be very accurate, with an average error of 3.30 percent.

McCarthy, Catherine E.↗

Enforcing detailed balance in the Borgnakke–Larsen redistribution method with temperature dependent relaxation models

For decades, it has been observed that the commonly used Borgnakke–Larsen method for energy redistribution in Direct Simulation Monte Carlo codes fails to satisfy the principle of detailed balance when coupled to a wide variety of temperature dependent relaxation models, while seemingly satisfying detailed balance when coupled to others. Many attempts have been made to remedy the issue, yet much ambiguity remains, and no consensus appears in the literature regarding the root cause of the intermittent compatibility of the Borgnakke–Larsen method with temperature dependent relaxation models. This paper alleviates that ambiguity by presenting a rigorous theoretical derivation of the Borgnakke–Larsen method's requirement for satisfying detailed balance. Specifically, it is shown that the Borgnakke–Larsen method maintains detailed balance if and only if the probability of internal-energy exchange during a collision depends only on collision invariants (e.g., total energy). Here, the consequences of this result are explored in the context of several published definitions of relaxation temperature, including translational, total, and cell-averaged temperatures. Of particular note, it is shown that cell-averaged temperatures, which have been widely discussed in the literature as a way to ensure equilibrium is reached, also fail in a similar, although less dramatic, fashion when the aforementioned relationship is not enforced. The developed theory can be used when implementing existing or new relaxation models and will ensure that detailed balance is satisfied.

74 ATOMIC AND MOLECULAR PHYSICS↗

Superconductivity in a strange metal

In a gas of charged particles with the density n, mass m, and charge e, the electrical conductivity σ is given by the Drude formula: σ = ne 2 /mΓ, where Γ is the scattering rate. Standard metals are well described by Landau's Fermi Liquid (FL) theory, in which the electric current is carried by quasi-particles, low-energy excitations of the FL that resemble electrons with some effective mass m*. The scattering rate Γ= 1/τ= v F /l, where t is the (momentum) relaxation) time, l is the mean-free path, and v F is the Fermi velocity, can be expressed ("Matthiessen's Rule") as a sum of contributions from various scattering channels: Γ = Γ 0 + Γ el-el + Γ el-ph + …, where Γ 0 describes scattering on lattice imperfections, Γ el-el the electron-electron scattering, Γ el-ph the electron-phonon scattering, etc. Of these, Γ 0 = v F /l 0 , where l 0 is the average distance between the defects, is temperature-independent. Γ el-el should scale as T 2 because of Fermi statistics; for two electrons to scatter on one another, both must come from the "Debye shell" of the width k B T/E F , where k B is the Boltzmann constant and E F is the Fermi energy. Γ el-ph typically grows as T 5 , so we expect this to overwhelm the other channels at a high enough T. However, since l cannot be shorter than the distance between the atoms, the total Γ saturates at Mott-Ioffe-Regel (MIR) limit, roughly v F /a 0 , where v F is the Fermi velocity and a 0 is the lattice constant. The resistivity should also saturate at low T, at ρ 0 = m*v F /ne 2 l 0 T. FL theory also describes other electronic properties; e.g., it predicts that in the magnetic field B, the resistivity of the metal should increase with B 2 , because σ(B) = σ(B=0)/(1 + (ω c /Γ) 2 ), where ω c = eB/m*.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

First experimental determination of the ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar reaction cross section and ³⁹Ar production in Earth’s atmosphere

The cosmogenic ³⁹Ar(t1∕2 = 268 years) isotope of argon is used for geophysical dating and tracing of underground and ocean water, as well as ice owing to its appropriate half-life and chemical inertness as a noble gas; ³⁹Ar serves also in nuclear weapon test monitoring. We measured for the first time the total cross section of the main ³⁹Ar cosmogenic production reaction in the atmosphere, namely ⁴⁰Ar(𝑛, 2𝑛)39 Ar, using 14.8 ± 0.3 MeV neutrons. The neutrons, produced by a deuterium-tritium generator, impinged on a stainless steel sphere filled with Ar gas highly enriched in the ⁴⁰Ar isotope and were monitored by a stack of fast-neutron activation foils. The reaction yield was measured by atom counting of long-lived ³⁹Ar with noble gas accelerator mass spectrometry and, independently, by decay counting relative to atmospheric argon (³⁹Ar/Ar= 8.12 × 10−16 ). A total ⁴⁰Ar(𝑛, 2𝑛)39 Ar cross section of 610 ± 100 mb was determined at 14.8 ± 0.3 MeV incident neutron energy. This result serves as a benchmark for recent theoretical calculations and evaluations, found to reproduce well the experimental total cross section. We use these energy-dependent theoretical cross sections together with experimental spectra of cosmogenic neutrons at different altitudes to calculate the global average rate of neutron-induced ³⁹Ar atmospheric production, resulting in 770 ± 240 39 Ar atoms/cm²/day. The secular equilibrium between the ³⁹Ar calculated production rate and radioactive decay rate leads to a partial isotopic abundance ³⁹Ar/Ar = (5.9 ± 1.8) × 10−16 , showing that ≈73% of atmospheric ³⁹Ar is produced by cosmogenic neutrons, the remaining part believed to be induced by muons and high-energy 𝛾 rays. The ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar cross section at 14 MeV is also a key parameter for quantifying the anthropogenic contribution to atmospheric 39 Ar produced during the thermonuclear tests of the 1960s. We estimate that anthropogenic ³⁹Ar accounts for roughly 20% of the present atmospheric inventory.

39 Ar atmospheric production↗

Detailed investigation of a vaporising fuel spray. Part 1: Experimental investigation of time averaged spray

A laser tomographic light scattering technique provides rapid and accurate high resolution measurements of droplet sizes, concentrations, and vaporization. Measurements using a computer interfaced thermocouple are presented and it is found that the potential exists for separating gas and liquid temperature measurements and diagnosing local spray density by in situ analysis of the response characteristics of the thermocouple. The thermocouple technique provides a convenient means for measuring mean gas velocity in both hot and cold two phase flows. The experimental spray is axisymmetric and has carefully controlled initial and boundary conditions. The flow is designed to give relatively insignificant transfer of momentum and mass from spray to air flow. The effects of (1) size-dependent droplet dispersion by the turbulence, (2) the initial spatial segregation of droplet sizes during atomization, and (3) the interaction between droplets and coherent large eddies are diagnosed.

Yule, A. J.↗

Reduced thermal resistance of Al-rich AlGaN HEMTs via top-side diamond integration

We report back-end-of-line growth of nanocrystalline diamond (NCD) on ultrawide bandgap (UWBG) high Al content aluminum gallium nitride (AlGaN) channel high electron mobility transistors for thermal management. A thin (∼15 nm) silicon nitride (SiN x ) interlayer was deposited to protect the device surface before performing a low temperature (500 °C) NCD growth process in an attempt to protect the gates on these fully fabricated devices. Notably, atomic force microscopy showed that the maximum lateral grain size exceeded 300 nm even though the film thickness was ∼250 nm. Comparing electrical (DC) performance before and after NCD growth, the gate leakage increased by ∼10 2 after NCD growth. Despite the lower NCD growth temperature, intermixing of the Ni and Au was observed in the Schottky gate metal stack; however, we believe there is another mechanism, possibly hydrogen-related, that is responsible for the measured increase in gate leakage. Regarding thermal management, the device-level thermal resistance (quantified using the average gate temperature rise measured by thermoreflectance imaging) was reduced by 29% through the incorporation of the top-side diamond film. Using time-domain thermoreflectance, the thermal conductivity of the ≈250 nm thick NCD film was measured to be 45 ± 25 W m −1 K −1 . This is expected to be at least 5× greater than the thermal conductivity of the thin disordered AlGaN alloy. There could also be a coupled electrothermal component contributing to the reduced temperature rise from electric field spreading and consequent heat spreading. This study demonstrates a promising first step toward device-level thermal management of high power UWBG Al-rich AlGaN devices.

Lundh, James Spencer [U.S. Naval Research Laborato↗

Electronic structure of α - RuCl 3 by fixed-node and fixed-phase diffusion Monte Carlo methods

Layered material α-RuCl 3 has caught wide attention due to its possible realization of Kitaev's spin liquid and its electronic structure that involves the interplay of electron-electron correlations and spin-orbit effects. Several DFT+U studies have suggested that both electron-electron correlations and spin-orbit effects are crucial for accurately describing the band gap. This work studies the importance of these two effects using fixed-node and fixed-phase diffusion Monte Carlo calculations both in spin-averaged and explicit spin-orbit formalisms. In the latter, the Slater-Jastrow trial function is constructed from two-component spin orbitals using our recent quantum Monte Carlo (QMC) developments and thoroughly tested effective core potentials. Our results show that the gap in the ideal crystal is already accurately described by the spin-averaged case, with the dominant role being played by the magnetic ground state with significant exchange and electron correlation effects. We find qualitative agreement between hybrid DFT, DFT+U, and QMC. In addition, QMC results agree very well with available experiments, and we identify the values of exact Fock exchange mixing that provide comparable gaps. Explicit spin-orbit QMC calculations reveal that the effect of spin-orbit coupling on the gap is minor, of the order of 0.2 eV, which corresponds to the strength of the spin orbit of the Ru atom.

36 MATERIALS SCIENCE↗

Insights into radiation resistance of titanium alloys from displacement cascade simulations

Radiation damage in beam window materials limits the use of high power proton beams in high energy physics research. The alloy Ti-6Al-4V is presently used as a beam window material but a prospective alternative, Ti-15V-3Cr-3Sn-3Al has been proposed. Since both these alloys contain dual phases at room temperature, we compare the radiation damage in the α and ß-phases of these two materials via primary knock-on atom (PKA) cascade simulations in the 10-40keV energy range. At PKA energies 30 and 40keV, the number of Frenkel pairs in the ballistic stage is higher in the ß-phase of Ti-6Al-4V than that in the ß-phase of Ti-15V-3Cr-3Sn-3Al almost by a factor of 2. The α-phase, of both these alloys, by far outperforms the ß-phases of the two alloys, both in terms of damage during the ballistic stage and in terms of the surviving defects. The average displacement threshold energy (E d ) in the α-phase of both alloys was found to be 66eV while that in the ß-phase of Ti-15-3 was 55 eV and in the ß-phase of Ti-6-4 was 46. Further, while the number of surviving defects is almost equal in both alloys, the vacancy and interstitial clustering mechanisms differ notably, which can impact the degree of radiation hardening and loss of ductility. Our simulations show larger vacancy and interstitial clusters form in Ti-6Al-4V as compared to that in Ti-15-3-3-3 alloy. These results indicate that Ti-15-3-3-3 alloys may be a promising candidate for next generation beam window material with a higher radiation tolerance than the existing Ti-6-4 alloy.

36 MATERIALS SCIENCE↗

Machine learning enabled quantification of the hydrogen bonds inside the polyelectrolyte brush layer probed using all-atom molecular dynamics simulations

The configuration of densely grafted charged polyelectrolyte (PE) brushes is strongly dictated by the properties and behavior of the counterions that screen the PE brush charges and the solvent molecules (typically water) that solvate the brush molecules and these screening counterions. Only recently, efforts have been made to study the PE brushes atomistically, thereby shedding light on the properties of brush-supported ions and water molecules. However, even for such efforts, there are limitations associated with using a generic definition to estimate certain properties of water and ions inside the brush layer. For example, water–water hydrogen bonds (HBs) will behave differently for locations outside and inside the brush layer, given the fact that the densely closely grafted PE brush molecules create a soft nanoconfinement where the water connectivity becomes highly disrupted: therefore, using the same definition to quantify the HBs inside and outside the brush layer will be unwise. In this paper, we address this limitation by employing an unsupervised machine learning (ML) approach to predict the water–water hydrogen bonding inside a cationic PE brush layer modeled using all-atom molecular dynamics (MD) simulations. Here, the ML method, which relies on a clustering approach and uses the equilibrium coordinates of the water molecules (obtained from the all-atom MD simulations) as the input, is capable of identifying the structural modification of water–water HBs (revealed through appropriate clustering of the data) inside the PE brush layer induced soft nanoconfinement. Such capabilities would not have been possible by using a generic definition of the HBs. Our calculations lead to four key findings: (1) the clusters formed inside and outside the brush layer are structurally similar; (2) the margin of the cluster is shorter inside the PE brush layer confirming the possible disruption of the HBs inside the PE brush layer; (3) the average “hydrogen–acceptor-oxygen–donor-oxygen” angle that defines the HB is reduced for the HBs formed inside the brush layer; (4) the use of the generic definition (definition usable for characterizing the HBs in brush-free bulk) leads to an overprediction of the number of HBs formed inside the PE brush layer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Airborne Measurements of BrO and the Sum of HOBr and Br2 over the Tropical West Pacific from 1 to 15 Km During the CONvective TRansport of Active Species in the Tropics (CONTRAST) Experiment

A chemical ionization mass spectrometer was used to measure BrO and HOBr + Br2 over the Tropical West Pacific Ocean within the altitude range of 1 to 15 km, during the CONvective TRansport of Active Species in the Tropics (CONTRAST) campaign in 2014. Isolated episodes of elevated BrO (up to 6.6 pptv) and/or HOBr + Br2 (up to 7.3 pptv) were observed in the tropical free troposphere (TFT) and were associated with biomass burning. However, most of the time we did not observe significant BrO or HOBr + Br2 in the TFT and the tropical tropopause layer (TTL) above our limits of detection (LOD). The 1 min average LOD for BrO ranged from 0.6 to 1.6 pptv and for HOBr + Br2 ranged from 1.3 to 3.5 pptv. During one flight, BrO observations from the TTL to the extratropical lowermost stratosphere were used to infer a profile of inorganic bromine (Br(sub y)). Based on this profile, we estimated the product gas injection of bromine species into the stratosphere to be 2 pptv. Analysis of Br(sub y) partitioning further indicates that BrO levels are likely very low in the TFT environment and that future studies should target the measurement of HBr or atomic Br.

Isolated episodes of elevated BrO↗

Performance and stability of a booster class LOX/hydrogen swirl coaxial-element injector

Initial tests were conducted with an axisymmetric subscale version of the Advanced Launch System (ALS) prototype injector, with a pattern of pressure-atomizing LOX-swirled injector elements flowing about 50 percent more propellant per element than the Space Shuttle Main Engine injector element. The swirl coax combustion was statistically stable and quiet with and without combustion stability aids. Artificial perturbations to assess dynamic stability generated overpressures from 2 to 15 percent of chamber pressure, and all combustion oscillations were damped within 3 millisec. Chug-free throttle was demonstrated to 65 percent of the nominal operating chamber pressure. Combustion performance in an ablative-lined chamber was calculated with both specific impulse and characteristic exhaust velocity, and averaged about 97 percent. Combustion performance of the injector element depended upon the momentum angle of the injected propellants rather than the shearing rate of the fuel on the oxidizer.

Hulka, J.↗

Hydrocarbon photochemistry in the upper atmosphere of Jupiter

The hydrocarbon photochemistry in the upper atmosphere of Jupiter is investigated using a one-dimensional, photochemical-diffusive, and diurnally averaged model. The important chemical cycles and pathways among the major species are outlined and a standard model for the North Equatorial Belt region is examined in detail. It is found that several traditionally dominant chemical pathways among the C and C2 species are replaced in importance by cycles involving C-C4 species. The pressure and altitude profiles of mixing ratios for several observable hydrocarbon species are compared with available ultraviolet- and infrared-derived abundances. The results of sensitivity studies on the standard model with respect to variations in eddy diffusion profile, solar flux, atomic hydrogen influx, latitude, temperature, and important chemical reaction rates are presented. Measured and calculated airglow emissions of He at 584 angstroms and H at 1216 angstroms are also used to provide some constraints on the range of model parameters. The relevance of the model results to the upcoming Galileo mission is briefly discussed. The model is subject to considerable improvement; there is a great need for laboratory measurements of basic reaction rates and photodissociation quantum yields, even for such simple species as methylacetylene and allene. Until such laboratory measurements exist there will be considerable uncertainty in the understanding of the C3 and higher hydrocarbons in the atmospheres of the jovian planets.

NASA Discipline Number 52-20↗

First-principles study of the structures and redox mechanisms of Ni-rich lithium nickel manganese cobalt oxides

To reduce the cobalt (Co) content in lithium-ion batteries, Ni-rich (high-Ni) lithium nickel manganese cobalt oxides (NMC) are pursued as one of the next-generation cathode materials. However, there is still debate on the crystal and electronic structures of the baseline, LiNiO 2 . Density Functional Theory (DFT) calculations were performed to provide a theoretical understanding of Ni-rich NMC. First, it was found that the commonly used $R\bar{3}m$ structure for LiNiO 2 is metallic, contrary to the experimentally reported mix-conducting behavior. Among the four different space groups, $R\bar{3}m$, C2/m, P2 1 /c, and P2/c, P2/c with charge disproportionation of Ni 2+ and Ni 4+ is the most energetically stable and semiconducting structure of LiNiO 2 . Therefore, the atomic structures of representative Ni-rich NMC were built by partially replacing Ni with Co or Mn in the P2/c LiNiO 2 to form Li x Ni y Mn z Co 1-y-z O 2 . In the fully lithiated (x=1.0) high Ni content NMC (y>0.5), the oxidation state of all Mn ions becomes 4+, while Co ions still maintain 3+, and part of the Ni ions become 3+ to compensate for the charge. Upon delithiation, the local environment shows more variation of the charge states on the transition metal (TM) ions. The average oxidation on each TM follows a sequence of losing electrons that starts from Ni 2+ to Ni 3+ , then oxidizing Ni 3+ and Co 3+ , while Mn 4+ remains electrochemically inactive till x=0. Finally, a general relationship for the oxidation state change in each TM as a function of x is derived and shows agreement with both modeling and experimental data.

25 ENERGY STORAGE↗

Optimizing the Internal Cell Structure of the Radon Monitor Based on Electrostatic Collection Method

Abstract As Rn-222 decays, an alpha particle is emitted and the residual polonium nucleus recoils in the opposite direction. At the end of the recoil path, 88% of the polonium atoms have a positive charge and 12% are neutral. The electric potential distribution in the 60 ml hemispherical internal cell of the radon monitor based on electrostatic collection is studied for reducing the combined probability of the positively charged Po-218 and the OH− produced by the ionization of water vapour in the air. The COMSOL software is used to simulate the electric potential distribution in the internal cell of the radon monitor based on the electrostatic collection method at 27°C, a pressure of 0.1 Mpa. For improving the collection efficiency of Po-218 ions, the average collection time along vertical and oblique lines is calculated when the upper surface of the internal cell is plastic, uncharged metal and charged metal, respectively. Assuming that the gas in the internal cell is uniformly distributed, the results show that if the upper surface of the hemispherical internal cell is plastic or uncharged metal, the electric potential formed in the internal cell is more uniform, and it is beneficial to reduce the total collection time of the positively charged Po-218 ions, thereby improving collection efficiency. The simulation results can be used as an effective reference for optimizing the design of the internal cell structure of the radon monitor based on electrostatic collection method.

Fan, Zhongkai (ORCID:0000000181247459)↗

A Numerical Model for the Dynamics of Pickup Ions Outside the Heliopause and IBEX “Ribbon” Observation

The leading mechanism for the origin of the Interstellar Boundary Explorer (IBEX) “ribbon” of enhanced energetic neutral atoms (ENAs) from the outer heliosphere is the so-called secondary ENA process. In this mechanism, neutralized ions escape the heliosphere, and after several times of charge exchange collision,s some propagate back toward Earth in directions nearly perpendicular to the local interstellar magnetic field. However, the physical processes governing the distribution of the pickup ions (PUIs) outside the heliopause are still unclear. In this study, we build a new global model of the IBEX ribbon, where a key component is to calculate the dynamics of the PUIs outside the heliopause by solving the gyrophase-averaged focused transport equations on top of the background magnetohydrodynamic-kinetic model for the heliosphere-interstellar medium interaction. We discuss how the properties of the simulated ribbon change with different scattering parameters and show simulation results of the ENA sky maps, ribbon centers, ribbon profiles at several azimuthal slices, the ribbon ENA source region, and the velocity distribution of PUIs in the ENA source region for different scattering frequencies. Our results show that the model can provide reasonable ribbon sky maps comparable to the observed ribbon when the PUI mean free path is on the order of several thousand astronomical units.

79 ASTRONOMY AND ASTROPHYSICS↗

Detecting rare neutral atomic-carbon absorbers with a deep neural network

ABSTRACT C i absorbers play an important role as indicators for exploring the presence of cold gas in the interstellar medium of galaxies. However, the current data base of C i absorbers is very limited due to their weak absorption feature and rarity. Here, we report results from a search of C i λλ1560, 1656 absorption lines using Mg ii absorbers as signposts with modified deep learning algorithms, which provides a very quick way to search for weak C i absorber candidates. A total of 107 C i absorbers were detected, which nearly doubles the size of previously known samples. In addition, we found 17 C i absorbers to be associated with 2175 Å dust absorbers (2DAs), i.e. about 16 per cent C i absorbers are associated with 2DAs. Comparing the average dust depletion patterns of C i absorbers with those of damped Lyman α absorbers (DLAs), Mg ii absorbers, Ca ii absorbers, and 2175 Å dust absorbers (2DAs) shows that C i absorbers generally have environments with more dust than DLAs, Mg ii, and Ca ii absorbers, but similar to dust in 2DAs. Similarity between the dust depletion pattern of C i absorbers to that of the warm disc in the Milky Way indicates that C i absorption clouds are possibly associated with disc components in distant galaxies. Therefore, C i absorbers are confirmed to be excellent probes to trace cold gas and dust in the Universe.

Ge, Jian↗

Importance of imposing gauge invariance in time-dependent density functional theory calculations with meta-generalized gradient approximations

It has been known for more than a decade that the gauge variance of the kinetic energy density τ leads to additional terms in the magnetic orbital rotation Hessian used in linear-response time-dependent density functional theory (TDDFT), affecting excitation energies obtained with τ-dependent exchange–correlation functionals. While previous investigations found that a correction scheme based on the paramagnetic current density has a small effect on benchmark results, we report more pronounced effects here, in particular, for the popular M06-2X functional and for some other meta-generalized gradient approximations (mGGAs). In the first part of this communication, this is shown by a reassessment of a set of five Ni(II) complexes for which a previous benchmark study that did not impose gauge invariance has found surprisingly large errors for excitation energies obtained with M06-2X. These errors are more than halved by restoring gauge invariance. The variable importance of imposing gauge invariance for different mGGA-based functionals can be rationalized by the derivative of the mGGA exchange energy integrand with respect to τ. In the second part, a large set of valence excitations in small main-group molecules is analyzed. For M06-2X, several selected n → π* and π→π$^{*}_{⊥}$ excitations are heavily gauge-dependent with average changes of –0.17 and –0.28 eV, respectively, while π→π$^{*}_{∥}$ excitations are marginally affected (–0.04 eV). Similar patterns, but of the opposite signs, are found for SCAN0. Here, the results suggest that reevaluation of previous gauge variant TDDFT results based on M06-2X and other mGGA functionals is warranted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗