Modeling the influence of interaction layer formation on thermal conductivity of U–Mo dispersion fuel
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Burkes, Douglas E.↗
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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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Efficient Isoprene Secondary Organic Aerosol Formation from a Non-IEPOX Pathway
With a large global emission rate and high reactivity, isoprene has a profound effect upon atmospheric chemistry and composition. The atmospheric pathways by which isoprene converts to secondary organic aerosol (SOA) and how anthropogenic pollutants such as nitrogen oxides and sulfur affect this process are subjects of intense research because particles affect Earth’s climate and local air quality. Thus, in the absence of both nitrogen oxides and reactive aqueous seed particles, we measure SOA mass yields from isoprene photochemical oxidation of up to 15%, which are factors of 2 or more higher than those typically used in coupled chemistry climate models. SOA yield is initially constant with the addition of increasing amounts of nitric oxide (NO) but then sharply decreases for input concentrations above 50 ppbv. Online measurements of aerosol molecular composition show that the fate of second-generation RO 2 radicals is key to understanding the efficient SOA formation and the NO x -dependent yields described here and in the literature. Our insights allow for improved quantitative estimates of SOA formation in the preindustrial atmosphere and in biogenic-rich regions with limited anthropogenic impacts and suggest that a more-complex representation of NO x -dependent SOA yields may be important in models
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
In Situ TEM Observations of Sn-Containing Silicon Nanowires Undergoing Reversible Pore Formation Due to Fast Lithiation/Delithiation Kinetics
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Lu, Xiaotang↗
Investigation of Solid Electrolyte Interphase Layer Formation and Electrochemical Reversibility of Magnetite, Fe 3 O 4 , Electrodes: A Combined X-ray Absorption Spectroscopy and X-ray Photoelectron Spectroscopy Study
Magnetite (Fe 3 O 4 ) is a promising electrode material for the next generation of Li-ion batteries with multiple electron transfers per metal center and a theoretical capacity of 924 mAh/g. However, multiple phase conversions during (de)lithiation of Fe 3 O 4 and formation of a surface electrolyte interphase (SEI) contribute to capacity fade. In this study, X-ray Absorption Spectroscopy (XAS), and X-ray Photoelectron Spectroscopy (XPS) were used to determine the surface chemistry, redox chemistry, and the impact on the electrochemical reversibility in the presence and absence of fluoroethylene carbonate (FEC) solvent. With FEC improved capacity retention and enhanced reversibility are observed. In contrast, electrodes cycled with no FEC exhibit decreased reversibility where the active material remains as reduced Fe 0 . XPS results reveal LiF and lower quantities of oxygen containing species, especially carbonates at the electrode surface tested in FEC. The improvement in electrochemical reversibility with FEC is attributed to the formation of a solid electrolyte interphase which forms prior to initiation of the conversion reaction limiting SEI growth on the reduced products, Fe0 and Li 2 O. In contrast, EC-based carbonate electrolyte forms SEI at a potential where formation of Fe0 and Li 2 O has already initiated resulting in SEI formation on Fe 0 nanograins.
25 ENERGY STORAGE↗
Probing the Formation of Cathode-Electrolyte Interphase on Lithium Iron Phosphate Cathodes via Operando Mechanical Measurements
Interfacial instabilities in electrodes control the performance and lifetime of Li-ion batteries. While the formation of solid-electrolyte interface (SEI) on anodes has received much attention, there is still lack of understanding about the formation of cathode-electrolyte interface (CEI) on the cathodes. To fill this gap, we report on dynamic deformations on lithium iron phosphate, LiFePO 4 cathodes during charge / discharge by utilizing in-operando digital image correlation, impedance spectroscopy and Cryo X-ray photoelectron spectroscopy. LiFePO4 cathodes were cycled in either LiPF 6 , LiClO 4 or LiTFSI- containing organic liquid electrolytes. Beyond the first cycle, Li-ion intercalation results in a nearly linear correlation between electrochemical strains and the state of (dis)-charge, regardless of the electrolyte chemistry. However, during the first charge in LiPF 6 - containing electrolyte, there is a distinct irreversible positive strain evolution at the onset of anodic current rise as well as current decay at around 4.0V. Impedance studies show the increase in surface resistance in the same potential window, suggesting the formation of CEI layers on the cathode. The chemistry of the CEI layer was characterized by X-ray photoelectron spectroscopy. LiF is detected in CEI layer starting as early as 3.4 V and Li $x$ PO $y$ F $z$ appeared at voltages higher than 4.0 V during the first charge. In conclusion, our approach offers new insights into the formation mechanism of CEI layers on the cathode electrodes, which is crucial for the development of robust cathode and electrolyte chemistries for higher performance batteries.
25 ENERGY STORAGE↗
Investigation of Isobaric Mixing as a Mechanism for Boundary‐Layer Cloud Formation
This study investigates the potential role of isobaric mixing in the formation of marine boundary layer clouds. Cloud formation theory emphasizes uplift and adiabatic cooling, but recent observations support the existence of small clouds forming at various altitudes, even below the lifting condensation level. Isobaric mixing of air with different thermodynamic properties can generate localized supersaturation. A Gaussian mixing model is employed to simulate this process, considering the correlation between temperature and water vapor. Cloud droplet size distributions from aircraft measurements show a persistent and prominent mode of small droplets at 9 m, and the size of this mode compares favorably with predictions from the model. The results suggests that isobaric mixing plausibly contributes to the formation of clouds, particularly those observed at multiple altitudes with narrow droplet size distributions. This finding highlights the importance of considering isobaric mixing processes in understanding and modeling cloud formation.
54 ENVIRONMENTAL SCIENCES↗
Gel phase formation in dilute triblock copolyelectrolyte complexes
Assembly of oppositely charged triblock copolyelectrolytes into phase-separated gels at low polymer concentrations (<1% by mass) has been observed in scattering experiments and molecular dynamics simulations. Here we show that in contrast to uncharged, amphiphilic block copolymers that form discrete micelles at low concentrations and enter a phase of strongly interacting micelles in a gradual manner with increasing concentration, the formation of a dilute phase of individual micelles is prevented in polyelectrolyte complexation-driven assembly of triblock copolyelectrolytes. Gel phases form and phase separate almost instantaneously on solvation of the copolymers. Furthermore, molecular models of self-assembly demonstrate the presence of oligo-chain aggregates in early stages of copolyelectrolyte assembly, at experimentally unobservable polymer concentrations. Our discoveries contribute to the fundamental understanding of the structure and pathways of complexation-driven assemblies, and raise intriguing prospects for gel formation at extraordinarily low concentrations, with applications in tissue engineering, agriculture, water purification and theranostics.
36 MATERIALS SCIENCE↗
Anionic redox reaction in layered NaCr2/3Ti1/3S2 through electron holes formation and dimerization of S-S
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99 GENERAL AND MISCELLANEOUS↗
Large polaron formation and its effect on electron transport in hybrid perovskites
Many experiments have indicated that a large polaron may be formed in hybrid perovskites, and its existence is proposed to screen the carrier-carrier and carrier-defect scattering, thus contributing to the long lifetime of the carriers. However, a detailed theoretical study of the large polaron and its effect on carrier transport at the atomic level is still lacking. In particular, how strong is the large polaron binding energy? How does its effect compare with the effect of dynamic disorder caused by the A-site molecular rotation? And how does the inorganic sublattice vibration impact the motion of the large polaron? All of these questions are largely unanswered. In this work, using CH3NH3PbI3 as an example, we implement a tight-binding model fitted from density-functional theory to describe the electron large polaron ground state and to understand the large polaron formation and transport at its strong-coupling limit. We find that the formation energy of the large polaron is around -12 meV for the case without dynamic disorder, and -55 meV by including dynamic disorder. By performing the explicit time-dependent wavefunction evolution of the polaron state, together with the rotations of CH 3 NH 3 + and vibrations of the PbI3- sublattice, we studied the diffusion constant and mobility of the large polaron state driven by the dynamic disorder and the sublattice vibration. Two effects of the inorganic sublattice vibrations are found: on one hand, the vibration of the sublattice provides an additional driving force for carrier mobility; on the other hand, the large polaron polarization further localizes the electron, reducing its mobility. Overall, the effect of the large polaron is to slow down the electron mobility by roughly a factor of two. We believe that both dynamic disorder due to rotation of the organic molecule, and large polaron effects induced by the polarization and vibration of the inorganic sublattice, play important roles for the electronic structure and carrier dynamics of the system.
36 MATERIALS SCIENCE↗
Nanodot formation induced by femtosecond laser irradiation
The femtosecond laser generation of ZnSe nanoscale features on ZnSe surfaces was studied. Irradiation with multiple exposures produces 10–100 nm agglomerations of nanocrystalline ZnSe while retaining the original single crystal structure of the underlying material. The structure of these nanodots was verified using a combination of scanning transmission electron microscopy, scanning electron microscopy, and atomic force microscopy. The nanodots continue to grow hours after irradiation through a combination of bulk and surface diffusion. We suggest that in nanodot formation the result of ultrafast laser induced point defect formation is more than an order of magnitude below the ZnSe ultrafast melt threshold fluence. This unique mechanism of point defect injection will be discussed.
36 MATERIALS SCIENCE↗
Phase formation and texture of thin nickel germanides on Ge(001) and Ge(111)
We studied the solid-phase reaction between a thin Ni film and a single crystal Ge(001) or Ge(111) substrate during a ramp anneal. The phase formation sequence was determined using in situ X-ray diffraction and in situ Rutherford backscattering spectrometry (RBS), while the nature and the texture of the phases were studied using X-ray pole figures and transmission electron microscopy. The phase sequence is characterized by the formation of a single transient phase before NiGe forms as the final and stable phase. X-ray pole figures were used to unambiguously identify the transient phase as the ϵ-phase, a non-stoichiometric Ni-rich germanide with a hexagonal crystal structure that can exist for Ge concentrations between 34% and 48% and which forms with a different epitaxial texture on both substrate orientations. The complementary information gained from both RBS and X-ray pole figure measurements revealed a simultaneous growth of both the ϵ-phase and NiGe over a small temperature window on both substrate orientations.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Gas cluster ion beam assisted NiPt germano-silicide formation on SiGe
We report the formation of very uniform and smooth Ni(Pt)Si on epitaxially grown SiGe using Si gas cluster ion beam treatment after metal-rich silicide formation. The gas cluster ion implantation process was optimized to infuse Si into the metal-rich silicide layer and lowered the NiSi nucleation temperature significantly according to in situ X-ray diffraction measurements. This novel method which leads to more uniform films can also be used to control silicide depth in ultra-shallow junctions, especially for high Ge containing devices, where silicidation is problematic as it leads to much rougher interfaces.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Theory of multiple quantum dot formation in strained-layer heteroepitaxy
We develop a theory for the experimentally observed formation of multiple quantum dots (QDs) in strained-layer heteroepitaxy based on surface morphological stability analysis of a coherently strained epitaxial thin film on a crystalline substrate. Using a fully nonlinear model of surface morphological evolution that accounts for a wetting potential contribution to the epitaxial film's free energy as well as surface diffusional anisotropy, we demonstrate the formation of multiple QD patterns in self-consistent dynamical simulations of the evolution of the epitaxial film surface perturbed from its planar state. The simulation predictions are supported by weakly nonlinear analysis of the epitaxial film surface morphological stability. We find that, in addition to the Stranski-Krastanow instability, long-wavelength perturbations from the planar film surface morphology can trigger a nonlinear instability, resulting in the splitting of a single QD into multiple QDs of smaller sizes, and predict the critical wavelength of the film surface perturbation for the onset of the nonlinear tip-splitting instability. The theory provides a fundamental interpretation for the observations of “QD pairs” or “double QDs” and other multiple QDs reported in experimental studies of epitaxial growth of semiconductor strained layers and sets the stage for precise engineering of tunable-size nanoscale surface features in strained-layer heteroepitaxy by exploiting film surface nonlinear, pattern forming phenomena.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
The interstellar medium and star formation in local galaxies: Variations of the star formation law in simulations
We use the adaptive mesh refinement code Enzo to model the interstellar medium (ISM) in isolated local disk galaxies. The simulation includes a treatment for star formation and stellar feedback. We get a highly supersonic turbulent disk, which is fragmented at multiple scales and characterized by a multi-phase ISM. We show that a Kennicutt-Schmidt relation only holds when averaging over large scales. However, values of star formation rates and gas surface densities lie close in the plot for any averaging size. This suggests an intrinsic relation between stars and gas at cell-size scales, which dominates over the global dynamical evolution. To investigate this effect, we develop a method to simulate the creation of stars based on the density field from the snapshots, without running the code again. We also investigate how the star formation law is affected by the characteristic star formation timescale, the density threshold, and the efficiency considered in the recipe. We find that the slope of the law varies from ∼1.4 for a free-fall timescale, to ∼1.0 for a constant depletion timescale. We further demonstrate that a power law is recovered just by assuming that the mass of the new stars is a fraction of the mass of the cell m {sub *} = ερ{sub gas}Δx {sup 3}, with no other physical criteria required. We show that both efficiency and density threshold do not affect the slope, but the right combination of them can adjust the normalization of the relation, which in turn could explain a possible bi-modality in the law.
79 ASTRONOMY AND ASTROPHYSICS↗
SPT-CL J2040–4451: An SZ-selected galaxy cluster at z = 1.478 with significant ongoing star formation
SPT-CL J2040–4451—spectroscopically confirmed at z = 1.478—is the highest-redshift galaxy cluster yet discovered via the Sunyaev-Zel'dovich effect. SPT-CL J2040–4451 was a candidate galaxy cluster identified in the first 720 deg{sup 2} of the South Pole Telescope Sunyaev-Zel'dovich (SPT-SZ) survey, and has been confirmed in follow-up imaging and spectroscopy. From multi-object spectroscopy with Magellan-I/Baade+IMACS we measure spectroscopic redshifts for 15 cluster member galaxies, all of which have strong [O II] λλ3727 emission. SPT-CL J2040–4451 has an SZ-measured mass of M {sub 500,} {sub SZ} = 3.2 ± 0.8 × 10{sup 14} M {sub ☉} h {sub 70}{sup −1}, corresponding to M {sub 200,} {sub SZ} = 5.8 ± 1.4 × 10{sup 14} M {sub ☉} h {sub 70}{sup −1}. The velocity dispersion measured entirely from blue star-forming members is σ {sub v} = 1500 ± 520 km s{sup –1}. The prevalence of star-forming cluster members (galaxies with >1.5 M {sub ☉} yr{sup –1}) implies that this massive, high-redshift cluster is experiencing a phase of active star formation, and supports recent results showing a marked increase in star formation occurring in galaxy clusters at z ≳ 1.4. We also compute the probability of finding a cluster as rare as this in the SPT-SZ survey to be >99%, indicating that its discovery is not in tension with the concordance ΛCDM cosmological model.
79 ASTRONOMY AND ASTROPHYSICS↗
GAS PHASE SYNTHESIS OF (ISO)QUINOLINE AND ITS ROLE IN THE FORMATION OF NUCLEOBASES IN THE INTERSTELLAR MEDIUM
Nitrogen-substituted polycyclic aromatic hydrocarbons (NPAHs) have been proposed to play a key role in the astrochemical evolution of the interstellar medium, yet the formation mechanisms of even their simplest prototypes—quinoline and isoquinoline—remain elusive. Here, we reveal a novel concept that under high temperature conditions representing circumstellar envelopes of carbon stars, (iso)quinoline can be synthesized via the reaction of pyridyl radicals with two acetylene molecules. The facile gas phase formation of (iso)quinoline in circumstellar envelopes defines a hitherto elusive reaction class synthesizing aromatic structures with embedded nitrogen atoms that are essential building blocks in contemporary biological-structural motifs. Once ejected from circumstellar shells and incorporated into icy interstellar grains in cold molecular clouds, these NPAHs can be functionalized by photo processing forming nucleobase-type structures as sampled in the Murchison meteorite.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DEEP CHANDRA, HST-COS, AND MEGACAM OBSERVATIONS OF THE PHOENIX CLUSTER: EXTREME STAR FORMATION AND AGN FEEDBACK ON HUNDRED KILOPARSEC SCALES
We present new ultraviolet, optical, and X-ray data on the Phoenix galaxy cluster (SPT-CLJ2344-4243). Deep optical imaging reveals previously undetected filaments of star formation, extending to radii of ∼50–100 kpc in multiple directions. Combined UV-optical spectroscopy of the central galaxy reveals a massive (2 × 10{sup 9} M{sub ⊙}), young (∼4.5 Myr) population of stars, consistent with a time-averaged star formation rate of 610 ± 50 M{sub ⊙} yr{sup −1}. We report a strong detection of O vi λλ1032,1038, which appears to originate primarily in shock-heated gas, but may contain a substantial contribution (>1000 M{sub ⊙} yr{sup −1}) from the cooling intracluster medium (ICM). We confirm the presence of deep X-ray cavities in the inner ∼10 kpc, which are among the most extreme examples of radio-mode feedback detected to date, implying jet powers of 2–7 × 10{sup 45} erg s{sup −1}. We provide evidence that the active galactic nucleus inflating these cavities may have only recently transitioned from “quasar-mode” to “radio-mode,” and may currently be insufficient to completely offset cooling. A model-subtracted residual X-ray image reveals evidence for prior episodes of strong radio-mode feedback at radii of ∼100 kpc, with extended “ghost” cavities indicating a prior epoch of feedback roughly 100 Myr ago. This residual image also exhibits significant asymmetry in the inner ∼200 kpc (0.15R{sub 500}), reminiscent of infalling cool clouds, either due to minor mergers or fragmentation of the cooling ICM. Taken together, these data reveal a rapidly evolving cool core which is rich with structure (both spatially and in temperature), is subject to a variety of highly energetic processes, and yet is cooling rapidly and forming stars along thin, narrow filaments.
79 ASTRONOMY AND ASTROPHYSICS↗
The formation of IRIS diagnostics. V. A quintessential model atom of C ii and general formation properties of the C ii lines at 133.5 nm
The C ii 133.5 nm lines are important observables for the NASA/SMEX mission Interface Region Imaging Spectrograph. To make three-dimensional (3D) non-LTE radiative transfer computationally feasible, it is crucial to have a model atom with as few levels as possible while retaining the main physical processes. We here develop such a model atom and we study the general formation properties of the C ii lines. We find that a nine-level model atom of C i–C iii with the transitions treated assuming complete frequency redistribution (CRD) suffices to describe the C ii 133.5 nm lines. 3D scattering effects are important for the intensity in the core of the line. The lines are formed in the optically thick regime. The core intensity is formed in layers where the temperature is about 10 kK at the base of the transition region. The lines are 1.2–4 times wider than the atomic absorption profile due to the formation in the optically thick regime. The smaller opacity broadening happens for single peak intensity profiles where the chromospheric temperature is low with a steep source function increase into the transition region, the larger broadening happens when there is a temperature increase from the photosphere to the low chromosphere leading to a local source function maximum and a double peak intensity profile with a central reversal. Assuming optically thin formation with the standard coronal approximation leads to several errors: neglecting photoionization severly underestimates the amount of C ii at temperatures below 16 kK, erroneously shifts the formation from 10 kK to 25 kK, and leads to too low intensities.
79 ASTRONOMY AND ASTROPHYSICS↗