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At least 1,387 records · Page 77
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

A gedankenexperiment for anomalous diffusion in a charge-fluctuating dusty plasma

Brownian motion with Gaussian-distributed step-sizes is the prototype of diffusive processes with the typical scaling of the mean-square displacement linear with time. There are, however, processes scaling slower or faster in time due to differently (e.g., power-law) distributed step-sizes, commonly referred to as sub- and superdiffusion, respectively. We address the question whether there is actually a physical reason for a discrimination between normal and anomalous diffusion or whether such processes can be regarded as a special case of normal diffusion with a complicated space- and time-dependent diffusion coefficient. In order to get to the bottom of this question, we construct a numerical gedankenexperiment, which is designed to be as simple as possible and consists of dust particles embedded as test particles into a homogeneous magnetic field that randomly changes their charge. The only parameter governing the system is the ratio of the time-scales for gyration and for recharging. By performing full-orbit simulations of such particles, we are for the first time able to (i) describe a system exhibiting sub-, normal, or superdiffusion as an asymptotic behavior, i.e., not merely as an intermediate state during the evolution of the system. We (ii) observe superdiffusion for low values of the controlling parameter, normal diffusion over a wide plateau of intermediate values, and subdiffusion for high values, i.e., we found (iii) a simple system with one single and illustrative parameter controlling whether the system exhibits super-, normal, or subdiffusion. The crucial point is (iv) a competition between ballistic (particles uncharged, extreme superdiffusion) and confined (charged, extreme subdiffusion) motions. Our system is homogeneous in space and time, so that its (v) behavior cannot be described by normal diffusion with a special diffusion coefficient, and the competition is (vi) fundamentally different from a Gaussian random walk and may be regarded as one possible prototype of anomalous diffusion. We discuss briefly possible implications to space and astrophysical dusty plasma. In particular, we show that in a plasma with polydisperse dust particles, a superposition of the three regimes of the anomalous diffusion can simultaneously come into play.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Automated High-Pressure Titration System with In Situ Infrared Spectroscopic Detection

A fully automated titration system with infrared detection was developed for investigating interfacial chemistry at high pressures. The apparatus consists of a high-pressure fluid generation and delivery system coupled to a high-pressure cell with infrared optics. A manifold of electronically actuated valves is used to direct pressurized fluids into the cell. Precise reagent additions to the pressurized cell are made with calibrated tubing loops that are filled with reagent and placed in-line with the cell and a syringe pump. The cell’s infrared optics facilitate both transmission and attenuated total reflection (ATR) measurements to monitor bulk-fluid composition and solid-surface phenomena such as adsorption, desorption, complexation, dissolution, and precipitation. Switching between the two measurement modes is accomplished with moveable mirrors that direct radiation from a Fourier transform infrared spectrometer into the cell along transmission or ATR light paths. The versatility of the high-pressure IR titration system is demonstrated with three case studies. First, we titrated water into supercritical CO2 (scCO2) to generate an infrared calibration curve and determine the solubility of water in CO2 at 50 °C and 90 bar. Next, we characterized the partitioning of water between a montmorillonite clay and scCO2 at 50 °C and 90 bar. Transmission-mode spectra were used to quantify changes in the clay’s sorbed water concentration as a function of scCO2 hydration, and ATR measurements provided insights into competitive residency of water and CO2 on the clay surface and in the interlayer. Finally, we demonstrated how time-dependent studies can be conducted with the system by monitoring the carbonation reaction of forsterite (Mg2SiO4) in water-bearing scCO2 at 50 °C and 90 bar. Immediately after water dissolved in the scCO2, a thin film of adsorbed water formed on the mineral surface, and the film thickness increased with time as the forsterite began to dissolve. However, after approximately 2.5 hours, the trend reversed, and a carbonate precipitate began to form on the forsterite surface, exposing dramatic chemical changes in the thin-water film. Collectively, these applications illustrate how the high-pressure IR titration system can provide molecular-level information about the interactions between variably wet scCO2 and minerals relevant to underground storage of CO2 (geologic carbon sequestration). The apparatus could also be utilized to study high-pressure interfacial chemistry in other areas such as catalysis, polymerization, food processing, and oil and gas recovery.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2014

van der Waals density functionals built upon the electron-gas tradition: Facing the challenge of competing interactions

The theoretical description of sparse matter attracts much interest, in particular for those ground-state properties that can be described by density functional theory. One proposed approach, the van der Waals density functional (vdW-DF) method, rests on strong physical foundations and offers simple yet accurate and robust functionals. A very recent functional within this method called vdW-DF-cx [K. Berland and P. Hyldgaard, Phys. Rev. B 89, 035412 (2014)] stands out in its attempt to use an exchange energy derived from the same plasmon-based theory from which the nonlocal correlation energy was derived. Encouraged by its good performance for solids, layered materials, and aromatic molecules, we apply it to several systems that are characterized by competing interactions. These include the ferroelectric response in PbTiO{sub 3}, the adsorption of small molecules within metal-organic frameworks, the graphite/diamond phase transition, and the adsorption of an aromatic-molecule on the Ag(111) surface. Our results indicate that vdW-DF-cx is overall well suited to tackle these challenging systems. In addition to being a competitive density functional for sparse matter, the vdW-DF-cx construction presents a more robust general-purpose functional that could be applied to a range of materials problems with a variety of competing interactions.

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

Impact of the uncertainty in α-captures on {sup 22}Ne on the weak s-process in massive stars

Massive stars at solar metallicity contribute to the production of heavy elements with atomic masses between A = 60 and A = 90 via the so-called weak s-process (which takes place during core He and shell C burning phases). Furthermore, recent studies have shown that rotation boosts the s-process production in massive stars at low metallicities, with a production that may reach the barium neutron-magic peak. These results are very sensitive to neutron source and neutron poison reaction rates. For the weak s-process, the main neutron source is the reaction {sup 22}Ne(α,n){sup 25}Mg, which is in competition with {sup 22}Ne(α,γ){sup 26}Mg. The uncertainty of both rates strongly affects the nucleosynthesis predictions from stellar model calculations. In this study, we investigate the impact of the uncertainty in α-captures on {sup 22}Ne on the s-process nucleosynthesis in massive stars both at solar and at very low metallicity. For this purpose, we post-process, with the Nugrid mppnp code, non-rotating and rotating evolutionary models 25M{sub ⊙} stars at two different metallicities: Z = Z{sub ⊙} and Z = 10{sup −5}Z{sub ⊙}, respectively. Our results show that uncertainty of {sup 22}Ne(α,n){sup 25}Mg and {sup 22}Ne(α,γ){sup 26}Mg rates have a significant impact on the final elemental production especially for metal poor rotating models. Beside uncertainties in the neutron source reactions, for fast rotating massive stars at low metallicity we revisit the impact of the neutron poisoning effect by the reaction chain {sup 16}O(n,γ){sup 17}O(α,γ){sup 21}Ne, in competition with the {sup 17}O(α,n){sup 20}Ne, recycling the neutrons captured by {sup 16}O.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2014

Photoluminescence properties and exciton dynamics in monolayer WSe{sub 2}

In this work, comprehensive temperature and excitation power dependent photoluminescence and time-resolved photoluminescence studies are carried out on monolayer WSe{sub 2} to reveal its properties of exciton emissions and related excitonic dynamics. Competitions between the localized and delocalized exciton emissions, as well as the exciton and trion emissions are observed, respectively. These competitions are suggested to be responsible for the abnormal temperature and excitation intensity dependent photoluminescence properties. The radiative lifetimes of both excitons and trions exhibit linear dependence on temperature within the temperature regime below 260 K, providing further evidence for two-dimensional nature of monolayer material.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Role of structural factors in formation of chiral magnetic soliton lattice in Cr{sub 1/3}NbS₂

The sign and strength of magnetic interactions not only between nearest neighbors, but also for longer-range neighbors in the Cr{sub 1/3}NbS₂ intercalation compound have been calculated on the basis of structural data. It has been found that left-handed spin helices in Cr{sub 1/3}NbS₂ are formed from strength-dominant at low temperatures antiferromagnetic (AFM) interactions between triangular planes of Cr³⁺ ions through the plane of just one of two crystallographically equivalent diagonals of side faces of embedded into each other trigonal prisms building up the crystal lattice of magnetic Cr³⁺ ions. These helices are oriented along the c axis and packed into two-dimensional triangular lattices in planes perpendicular to these helices directions and lay one upon each other with a displacement. The competition of the above AFM helices with weaker inter-helix AFM interactions could promote the emergence of a long-period helical spin structure. One can assume that in this case, the role of Dzyaloshinskii-Moriya interaction consists of final ordering and stabilization of chiral spin helices into a chiral magnetic soliton lattice. The possibility of emergence of solitons in M{sub 1/3}NbX{sub 2} and M{sub 1/3}TaX₂ (M = Cr, V, Ti, Rh, Ni, Co, Fe, and Mn; X = S and Se) intercalate compounds has been examined. Two important factors caused by the crystal structure (predominant chiral magnetic helices and their competition with weaker inter-helix interactions not destructing the system quasi-one-dimensional character) can be used for the crystal chemistry search of solitons.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Co-non-solvency: Mean-field polymer theory does not describe polymer collapse transition in a mixture of two competing good solvents

Smart polymers are a modern class of polymeric materials that often exhibit unpredictable behavior in mixtures of solvents. One such phenomenon is co-non-solvency. Co-non-solvency occurs when two (perfectly) miscible and competing good solvents, for a given polymer, are mixed together. As a result, the same polymer collapses into a compact globule within intermediate mixing ratios. More interestingly, polymer collapses when the solvent quality remains good and even gets increasingly better by the addition of the better cosolvent. This is a puzzling phenomenon that is driven by strong local concentration fluctuations. Because of the discrete particle based nature of the interactions, Flory-Huggins type mean field arguments become unsuitable. In this work, we extend the analysis of the co-non-solvency effect presented earlier [D. Mukherji et al., Nat. Commun. 5, 4882 (2014)]. We explain why co-non-solvency is a generic phenomenon, which can only be understood by the thermodynamic treatment of the competitive displacement of (co)solvent components. This competition can result in a polymer collapse upon improvement of the solvent quality. Specific chemical details are not required to understand these complex conformational transitions. Therefore, a broad range of polymers are expected to exhibit similar reentrant coil-globule-coil transitions in competing good solvents.

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

CUORE-0 results and prospects for the CUORE experiment

With 741 kg of TeO{sub 2} crystals and an excellent energy resolution of 5 keV (0.2%) at the region of interest, the CUORE (Cryogenic Underground Observatory for Rare Events) experiment aims at searching for neutrinoless double beta decay of {sup 130}Te with unprecedented sensitivity. Expected to start data taking in 2015, CUORE is currently in an advanced construction phase at LNGS. CUORE projected neutrinoless double beta decay half-life sensitivity is 1.6 × 10{sup 26} y at 1σ (9.5 × 10{sup 25} y at the 90 % confidence level), in five years of live time, corresponding to an upper limit on the effective Majorana mass in the range 40–100 meV (50–130 meV). Further background rejection with auxiliary bolometric detectors could improve CUORE sensitivity and competitiveness of bolometric detectors towards a full analysis of the inverted neutrino mass hierarchy. CUORE-0 was built to test and demonstrate the performance of the upcoming CUORE experiment. It consists of a single CUORE tower (52 TeO{sub 2} bolometers of 750 g each, arranged in a 13 floor structure) constructed strictly following CUORE recipes both for materials and assembly procedures. An experiment its own, CUORE-0 is expected to reach a sensitivity to the ββ(0ν) half-life of {sup 130}Te around 3×10{sup 24} y in one year of live time. We present an update of the data, corresponding to an exposure of 18.1 kg y. An analysis of the background indicates that the CUORE performance goal is satisfied while the sensitivity goal is within reach.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2015

Ferroelectricity in high-density H{sub 2}O ice

The origin of longstanding anomalies in experimental studies of the dense solid phases of H{sub 2}O ices VII, VIII, and X is examined using a combination of first-principles theoretical methods. We find that a ferroelectric variant of ice VIII is energetically competitive with the established antiferroelectric form under pressure. The existence of domains of the ferroelectric form within anti-ferroelectric ice can explain previously observed splittings in x-ray diffraction data. The ferroelectric form is stabilized by density and is accompanied by the onset of spontaneous polarization. The presence of local electric fields triggers the preferential parallel orientation of the water molecules in the structure, which could be stabilized in bulk using new high-pressure techniques.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Probing the deep nonlinear stage of the ablative Rayleigh-Taylor instability in indirect drive experiments on the National Ignition Facility

Academic tests in physical regimes not encountered in Inertial Confinement Fusion will help to build a better understanding of hydrodynamic instabilities and constitute the scientifically grounded validation complementary to fully integrated experiments. Under the National Ignition Facility (NIF) Discovery Science program, recent indirect drive experiments have been carried out to study the ablative Rayleigh-Taylor Instability (RTI) in transition from weakly nonlinear to highly nonlinear regime [A. Casner et al., Phys. Plasmas 19, 082708 (2012)]. In these experiments, a modulated package is accelerated by a 175 eV radiative temperature plateau created by a room temperature gas-filled platform irradiated by 60 NIF laser beams. The unique capabilities of the NIF are harnessed to accelerate this planar sample over much larger distances (≃1.4 mm) and longer time periods (≃12 ns) than previously achieved. This extended acceleration could eventually allow entering into a turbulent-like regime not precluded by the theory for the RTI at the ablation front. Simultaneous measurements of the foil trajectory and the subsequent RTI growth are performed and compared with radiative hydrodynamics simulations. We present RTI growth measurements for two-dimensional single-mode and broadband multimode modulations. The dependence of RTI growth on initial conditions and ablative stabilization is emphasized, and we demonstrate for the first time in indirect-drive a bubble-competition, bubble-merger regime for the RTI at ablation front.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

CALDER: Cryogenic light detectors for background-free searches

The development of background-free detectors is essential for experiments searching for rare events. Bolometers, that are among the most competitive devices for the study of neutrino-less double beta decay (0νDBD) and Dark Matter interactions, suffer from the absence of techniques that allow to identify the nature of the interacting particles. This limit can be overcome by coupling the bolometer to an independent device for the measurement of the light emitted by interactions, as the combined read-out of the bolometric and light signals allows to identify and reject particles different from those of interest. CUORE, the most advanced bolometric experiment for 0νDBD searches, could disentangle the electrons produced by 0νDBD from the dangerous background due to α particles, by measuring the (tiny) Cherenkov light emitted by electrons and not by α’s. LUCIFER, a project based on ZnSe scintillating bolometers for the study of {sup 82}Se 0νDBD, would be competitive also in the search of Dark Matter interactions if equipped with light detectors that allow to distinguish and reject the background due to electrons and γ’s. These advances require cryogenic detectors characterized by noise lower than 20 eV, large active area, wide temperature range of operation, high radio-purity and ease in fabricating hundreds of channels. The CALDER collaboration aims to develop such detectors by exploiting the superb energy resolution and natural multiplexed read-out provided by Kinetic Inductance Detectors.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

Hot-carrier-induced linear drain current and threshold voltage degradation for thin layer silicon-on-insulator field P-channel lateral double-diffused metal-oxide-semiconductor

Hot-carrier-induced linear drain current (I{sub dlin}) and threshold voltage (V{sub th}) degradations for the thin layer SOI field p-channel lateral double-diffused MOS (pLDMOS) are investigated. Two competition degradation mechanisms are revealed and the hot-carrier conductance modulation model is proposed. In the channel, hot-hole injection induced positive oxide trapped charge and interface trap gives rise to the V{sub th} increasing and the channel conductance (G{sub ch}) decreasing, then reduces I{sub dlin}. In the p-drift region, hot-electron injection induced negative oxide trapped charge enhances the conductance of drift doping resistance (G{sub d}), and then increases I{sub dlin}. Consequently, the eventual I{sub dlin} degradation is controlled by the competition of the two mechanisms due to conductance modulation in the both regions. Based on the model, it is explained that the measured I{sub dlin} anomalously increases while the V{sub th} is increasing with power law. The thin layer field pLDMOS exhibits more severe V{sub th} instability compared with thick SOI layer structure; as a result, it should be seriously evaluated in actual application in switching circuit.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Local structure, composition, and crystallization mechanism of a model two-phase “composite nanoglass”

We report a detailed study of the local composition and structure of a model, bi-phasic nanoglass with nominal stoichiometry Cu{sub 55}Nb{sub 45}. Three dimensional atom probe data suggest a nanoscale-phase-separated glassy structure having well defined Cu-rich and Nb-rich regions with a characteristic length scale of ≈3 nm. However, extended x-ray absorption fine structure analysis indicates subtle differences in the local environments of Cu and Nb. While the Cu atoms displayed a strong tendency to cluster and negligible structural order beyond the first coordination shell, the Nb atoms had a larger fraction of unlike neighbors (higher chemical order) and a distinctly better-ordered structural environment (higher topological order). This provides the first experimental indication that metallic glass formation may occur due to frustration arising from the competition between chemical ordering and clustering. These observations are complemented by classical as well as ab initio molecular dynamics simulations. Our study indicates that these nanoscale phase-separated glasses are quite distinct from the single phase nanoglasses (studied by Gleiter and others) in the following three respects: (i) they contain at least two structurally and compositionally distinct, nanodispersed, glassy phases, (ii) these phases are separated by comparatively sharp inter-phase boundaries, and (iii) thermally induced crystallization occurs via a complex, multi-step mechanism. Such materials, therefore, appear to constitute a new class of disordered systems that may be called a composite nanoglass.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Is organic photovoltaics promising for indoor applications?

This work utilizes organic photovoltaics (OPV) for indoor applications, such as powering small electronic devices or wireless connected Internet of Things. Three representative polymer-based OPV systems, namely, poly(3-hexylthiophene-2,5-diyl), poly[N-9′-heptadecanyl-2,7-carbazole-alt-5,5-(4′,7′-di-2-thienyl-2′, 1′,3′-benzothiadiazole)], and poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b′]dithiophene-2,6-diyl] [3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b]thiophenediyl]], were selected as the donor materials in blend with fullerene derivatives for comparison under low light level condition using fluorescent lamps. PCDTBT based devices are found to be the best performing system, generating 13.9 μW/cm{sup 2} corresponding to 16.6% power conversion efficiency at 300 lx, although PTB7 based devices show the highest efficiency under one sun conditions. This high performance suggests that OPV is competitive to the other PV technologies under low light condition despite much lower performance under one sun condition. Different properties of these devices are studied to explain the competitive performance at low light level. A low energy consuming method for maximum power point tracking is introduced for the operation of the OPV devices. Finally, a 14 cm × 14 cm OPV module with 100 cm{sup 2} active area is demonstrated for real applications. These findings suggest that OPV, in particular, PCDTBT based devices, could be a promising candidate for indoor applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

The near-infrared spectrum of ethynyl radical

Transient diode laser absorption spectroscopy has been used to measure three strong vibronic bands in the near infrared spectrum of the C{sub 2}H, ethynyl, radical not previously observed in the gas phase. The radical was produced by ultraviolet excimer laser photolysis of either acetylene or (1,1,1)-trifluoropropyne in a slowly flowing sample of the precursor diluted in inert gas, and the spectral resolution was Doppler-limited. The character of the upper states was determined from the rotational and fine structure in the observed spectra and assigned by measurement of ground state rotational combination differences. The upper states include a {sup 2}Σ{sup +} state at 6696 cm{sup −1}, a second {sup 2}Σ{sup +} state at 7088 cm{sup −1}, and a {sup 2}Π state at 7110 cm{sup −1}. By comparison with published calculations [R. Tarroni and S. Carter, J. Chem. Phys 119, 12878 (2003); Mol. Phys. 102, 2167 (2004)], the vibronic character of these levels was also assigned. The observed states contain both X{sup 2}Σ{sup +} and A{sup 2}Π electronic characters. Several local rotational level perturbations were observed in the excited states. Kinetic measurements of the time-evolution of the ground state populations following collisional relaxation and reactive loss of the radicals formed in a hot, non-thermal, population distribution were made using some of the strong rotational lines observed. The case of C{sub 2}H may be a good place to investigate the behavior at intermediate pressures of inert colliders, where the competition between relaxation and reaction can be tuned and observed to compare with master equation models, rather than deliberately suppressed to measure thermal rate constants.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Pressure effects on the vibrational and rotational relaxation of vibrationally excited OH (ν, J ) in an argon bath

Quasi-classical molecular dynamics simulations were used to study the energy relaxation of an initially non-rotating, vibrationally excited ( v = 4) hydroxyl radical (OH) in an Ar bath at 300 K and at high pressures from 50 atm to 400 atm. A Morse oscillator potential represented the OH, and two sets of interaction potentials were used based on whether the Ar-H potential was a Buckingham (Exp6) or a Lennard-Jones (LJ) potential. The vibrational and rotational energies were monitored for 25 000-90 000 ps for Exp6 trajectories and 5000 ps for LJ trajectories. Comparisons to measured vibrational relaxation rates show that Exp6 rates are superior. Simulated initial vibrational relaxation rates are linearly proportional to pressure, implying no effect of high-pressure breakdown in the isolated binary collision approximation. The vibrational decay curves upward from single-exponential decay. A model based on transition rates that exponentially depend on the anharmonic energy gap between vibrational levels fits the vibrational decay well at all pressures, suggesting that anharmonicity is a major cause of the curvature. Due to the competition of vibration-to-rotation energy transfer and bath gas relaxation, the rotational energy overshoots and then relaxes to its thermal value. Approximate models with adjustable rates for this competition successfully reproduced the rotational results. These models show that a large fraction of the vibrational energy loss is initially converted to rotational energy but that fraction decreases rapidly as the vibrational energy content of OH decreases. Finally, while simulated rates change dramatically between Exp6 and LJ potentials, the mechanisms remain the same.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Competing phases in epitaxial vanadium dioxide at nanoscale

Phase competition in correlated oxides offers tantalizing opportunities as many intriguing physical phenomena occur near the phase transitions. Owing to a sharp metal-insulator transition (MIT) near room temperature, the correlated vanadium dioxide (VO 2 ) exhibits a strong competition between insulating and metallic phases, which is important for practical applications. However, the phase boundary undergoes a strong modification when strain is involved, yielding complex phase transitions. Here, we report the emergence of nanoscale M2 phase domains in VO 2 epitaxial films under anisotropic strain relaxation. The competing phases of the films are imaged by multilength-scale probes, detecting the structural and electrical properties in individual local domains. Competing evolution of the M1 and M2 phases indicates the critical role of lattice-strain on both the stability of the M2 Mott phase and the energetics of the MIT in VO 2 films. This study demonstrates how strain engineering can be utilized to design phase states, which allow deliberate control of MIT behavior at the nanoscale in epitaxial VO 2 films.

36 MATERIALS SCIENCE↗