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All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Solvents Polarity Governs Ion Interactions and Transport in a Solvated Room Temperature Ionic Liquid

We explore the influence of the solvent dipole moment on cation anion interactions and transport in 1-butyl-3-methyl-imidazolium bis-(trifluoromethylsulfonyl), [BMIM+][Tf2N ]. Free energy profiles derived from atomistic molecular dynamics (MD) simulations show a correlation of the cation anion separation and the equilibrium depth of the potential of mean force with the dipole moment of the solvent. Correlations of the ion diffusivity with the dipole moment and the concentration of the solvent were further demonstrated by classical MD simulations. Quasi-elastic neutron scattering experiments with deuterated solvents reveal a complex picture of nanophase separation into the ionic liquid-rich and solvent-rich phases. The experiment corroborates the trend of concentration- and dipole moment-dependent enhancement of ion mobility by the solvent, as suggested by the simulations. Despite the considerable structural complexity of ionic liquid solvent mixtures, we can rationalize and generalize the trends governing ionic transport in these complex electrolytes.

Osti, Naresh C↗
DOE OSTI2020

Leveraging Sequential Doping of Semiconducting Polymers to Enable Functionally Graded Materials for Organic Thermoelectrics

With the ability to modulate electronic properties through molecular doping coupled with ease in processability, semiconducting polymers are at the forefront in enabling organic thermoelectric devices for thermal energy management. In contrast to uniform thermoelectric material properties, an alternative route focuses on functionally graded materials (FGMs) where one spatially controls and optimizes transport properties across the length of a thermoelectric material. While primarily studied in the context of inorganic materials, the concept of FGMs for organic thermoelectrics has not been explored. Herein, we introduce how molecular doping of semiconducting polymers enables spatial compositional control of thin-film FGMs. Specifically, we utilize sequential vapor doping of poly[2,5-bis(3-tetradecylthiophen-2-yl) thieno [3,2-b]thiophene] (PBTTT) with the small molecule acceptor 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ) to fabricate the simplest form of FGMs – double- segmented thin films. The two thin-film segments are of equal length (7.5 mm), but each set to different doping levels. Our study focuses on understanding the thermoelectric properties (Seebeck coefficient, α, and electronic conductivity, σ) and structural properties (through X-ray scattering, UV-vis-NIR spectroscopy, and Raman spectroscopy) within and across the two segments. We observe the presence of a small diffuse interfacial region of 0.5 – 1 mm between the two segments where the doping level and transport properties vary continuously. Despite the diffuse interface, the measured effective Seebeck coefficient (αeff) across the two segments is simply the average of α within each segment. Importantly, this experimental result is consistent with reported mathematical models describing αeff in graded thermoelectric materials. Finally, our results demonstrate the facile fabrication and characterization of functionally graded organic thermoelectric materials, providing guidelines for further development on more complex FGMs.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Ultra-luminous X-ray sources in Haro 11 and the role of X-ray binaries in feedback in Lyα emitting galaxies

Lyman Break Analogs (LBAs) are local proxies of high-redshift Lyman Break Galaxies. Spatially resolved studies of nearby starbursts have shown that Lyman continuum and line emission are absorbed by dust and that the Lyα is resonantly scattered by neutral hydrogen. In order to observe Lyα emission from star-forming regions, some source of feedback is required to blow the neutral gas away from the starburst to prevent scattering and allow the Lyα emission to escape. We show that there are two X-ray point sources embedded in the diffuse emission of the LBA galaxy Haro 11. CXOU J003652.4-333316 (abbreviated to Haro 11 X-1) is an extremely luminous (L{sub X}∼10{sup 41} erg s{sup −1}), spatially compact source with a hard-X-ray spectrum. We suggest that the X-ray emission from Haro 11 X-1 is dominated by a single accretion source. This might be an active galactic nucleus or a source similar to the extreme black hole binary (BHB) M82 X-1. The hard X-ray spectrum indicates that Haro 11 X-1 may be a BHB in a low accretion state. In this case, the very high X-ray luminosity suggests an intermediate mass black hole that could be the seed for formation of a supermassive black hole. Source CXOU J003652.7-33331619.5 (abbreviated Haro 11 X-2) has an X-ray luminosity of L{sub X}∼5×10{sup 40} erg s{sup −1} and a soft X-ray spectrum (power-law photon index Γ ∼ 2.2). This strongly suggests that Haro 11 X-2 is an X-ray binary in the ultra luminous state (i.e., an Ultra Luminous X-ray source, ULX). Haro 11 X-2 is coincident with the star-forming knot that is the source of the Lyα emission. The association of a ULX with Lyα emission raises the possibility that strong winds from X-ray binaries play an important role in injecting mechanical power into the interstellar medium, thus blowing away neutral material from the starburst region and allowing the Lyα to escape. We suggest that feedback from X-ray binaries may play a significant role in allowing Lyα emission to escape from galaxies in the early universe.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2013

ENERGETIC PARTICLE ANISOTROPIES AT THE HELIOSPHERIC BOUNDARY

In 2012 August the Voyager 1 space probe entered a distinctly new region of space characterized by a virtual absence of heliospheric energetic ions and magnetic fluctuations, now interpreted as a part of the local interstellar cloud. Prior to their disappearance, the ion distributions strongly peaked at a 90° pitch angle, implying rapid escape of streaming particles along the magnetic field lines. Here we investigate the process of particle crossing from the heliosheath into the interstellar space, using a kinetic approach that resolves scales of the particle's cyclotron radius and smaller. It is demonstrated that a 'pancake' pitch-angle distribution naturally arises at a tangential discontinuity separating a weakly turbulent plasma from a laminar region with a very low pitch-angle scattering rate. The relatively long persistence of gyrating ions is interpreted in terms of field line meandering facilitating their cross-field diffusion within the depletion region.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2017

Quantitative 3D evolution of colloidal nanoparticle oxidation in solution

Watching nanomaterials transform in time Real-time analysis of chemical transformations of nanoparticles is usually done with electron microscopy of a few particles. One limitation is interference by the electron beam. Sun et al. monitored the oxidation of iron nanoparticles in solution by using small- and wide-angle x-ray scattering and molecular dynamics simulations (see the Perspective by Cadavid and Cabot). These methods revealed the formation of voids within the nanoparticles, diffusion of material into and out of the nanoparticles, and ultimately the coalescence of the voids. Science , this issue p. 303 ; see also p. 245

36 MATERIALS SCIENCE↗
DOE OSTI2017

Rosseland and Flux Mean Opacities for Compton Scattering

Rosseland mean opacity plays an important role in theories of stellar evolution and X-ray burst models. In the high-temperature regime, when most of the gas is completely ionized, the opacity is dominated by Compton scattering. Our aim here is to critically evaluate previous works on this subject and to compute the exact Rosseland mean opacity for Compton scattering over a broad range of temperature and electron degeneracy parameter. We use relativistic kinetic equations for Compton scattering and compute the photon mean free path as a function of photon energy by solving the corresponding integral equation in the diffusion limit. As a byproduct we also demonstrate the way to compute photon redistribution functions in the case of degenerate electrons. We then compute the Rosseland mean opacity as a function of temperature and electron degeneracy and present useful approximate expressions. We compare our results to previous calculations and find a significant difference in the low-temperature regime and strong degeneracy. We then proceed to compute the flux mean opacity in both free-streaming and diffusion approximations, and show that the latter is nearly identical to the Rosseland mean opacity. We also provide a simple way to account for the true absorption in evaluating the Rosseland and flux mean opacities.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS1974

Atlas of lunar radar maps at 70-cm wavelength

The intensity distribution of lunar radar echoes has been mapped for two-thirds of the earth-visible lunar surface at a wavelength of 70 cm. The depolarizing effects of the lunar surface were observed by simultaneously receiving the radar echoes in opposite polarizations. These echoes were mapped with areal resolutions of 25-100 sq km. Mapping with this resolution confirmed that the young craters have enhanced returns. A few craters were found to have enhanced echoes only from their rims. Backscattering differences were also observed between various areas within a mare, between different highland areas, and between maria and adjacent highlands. These scattering differences were interpreted with a simple model, which assumed that the surface backscattered with varying amounts of quasi-specular and diffuse power. Only an increase in the diffuse power was needed to give the numerical values of the enhancements.

Thompson, T. W.↗
NASA NTRS1983

How do cosmic rays change their energy in the solar wind?

The diffusion-convection (modulation) equation is derived directly from the Boltzmann equation on the basis of a minimum number of assumptions concerning the scattering process, among which are: (1) that the scattered particles undergo no energy change, and (2) that isotropy is an equilibrium state. It is noted that, in the event that the background plasma contains a magnetic field and the flow speeds of the plasma and scattering centers are different, additional terms arise that will modify the equations. If, moreover, the scatterers have individual motions relative to their average flow, the second-order Fermi acceleration term will appear.

Jones, F. C.↗
NASA NTRS1987

A new interpretation of plasma-line overshoot phenomena

The temporal evolution of Langmuir waves excited by high-power, high-frequency (HF) radio waves in the ionosphere is studied theoretically. This study is motivated by past observations made with the 450 MHz radar at Arecibo Observatory in Puerto Rico. Two kinds of nonlinear damping to the parametric decay instability are considered in the derivation of the rate equation for the spectral intensity of enhanced Langmuir waves. They are Langmuir wave cascading caused by nonlinear Landau damping and cross-field electron diffusion. The first damping process leads to the saturation of individual unstable Langmuir wave. The second process, which results from the incoherent scattering of electron orbits by the total excited Langmuir waves, yields anomalous damping that applies to each Langmuir wave. Consequently, Langmuir waves with smaller growth rates will be suppressed by those with larger growth rates. Such a mode competition process may cause the overshoot of the HF-enhanced plasma line observed with the Arecibo 430 MHz radar. Favorable agreement is obtained between theory and the Arecibo observations.

Kuo, S. P.↗
NASA NTRS1996

Hard Gamma Ray Emission from the Starburst Galaxy NGC 253

We have completed the study to search for hard gamma ray emission from the starburst galaxy NGC 253. Since supernovae are thought to provide the hard gamma ray emission from the Milky Way, starburst galaxies, with their extraordinarily high supernova rates, are prime targets to search for hard gamma ray emission. We conducted a careful search for hard gamma ray emission from NGC 253 using the archival data from the EGRET experiment aboard the CGRO. Because this starburst galaxy happens to lie near the South Galactic Pole, the Galactic gamma ray background is minimal. We found no significant hard gamma ray signal toward NGC 253, although a marginal signal of about 1.5 sigma was found. Because of the low Galactic background, we obtained a very sensitive upper limit to the emission of greater than 100 MeV gamma-rays of 8 x 10(exp -8) photons/sq cm s. Since we expected to detect hard gamma ray emission, we investigated the theory of gamma ray production in a dense molecular medium. We used a leaky-box model to simulate diffusive transport in a starburst region. Since starburst galaxies have high infrared radiation fields, we included the effects of self-Compton scattering, which are usually ignored. By modelling the expected gamma-ray and synchrotron spectra from NGC 253, we find that roughly 5 - 15% of the energy from supernovae is transferred to cosmic rays in the starburst. This result is consistent with supernova acceleration models, and is somewhat larger than the value derived for the Galaxy (3 - 10%). Our calculations match the EGRET and radio data very well with a supernova rate of 0.08/ yr, a magnetic field B approx. greater than 5 x 10(exp -5) G, a density n approx. less than 100/sq cm, a photon density U(sub ph) approx. 200 eV/sq cm, and an escape time scale tau(sub 0) approx. less than 10 Myr. The models also suggest that NGC 253 should be detectable with only a factor of 2 - 3 improvement in sensitivity. Our results are consistent with the standard picture of gamma-ray acceleration by supernovae.

Jackson, James M.↗
NASA NTRS2017

Products of the SNPP VIIRS SD Screen Transmittance and the SD BRDFs From Both Yaw Maneuver and Regular On-Orbit Data

To ensure data quality, the Earth-observing Visible Infrared Imaging Radiometer Suite (VIIRS) on the Suomi National Polar-orbiting Partnership satellite regularly performs on-orbit radiometric calibration of its 22 spectral bands. The primary radiance source for the calibration of the VIIRS reflective solar bands (RSBs) is a sunlit onboard solar diffuser (SD).During the calibration process, sunlight goes through a perforated plate (the SD screen) and then strikes the SD. The sunlight, scattered off the SD of near-Lambertian property, is used for the calibration. Consequently, the spectral radiance of the scattered sunlight is proportional to the product of the SD screen transmittance and the SD bidirectional reflectance distribution function (BRDF) value at the observation direction. The BRDF value is decomposed to the product of its initial value at launch and a numerical degradation factor that quantifies the decrease from the initial value. The degradation factor is determined by an onboard SD stability monitor (SDSM). During the BRDF degradation factor determination process, the SDSM receives the SD scattered sunlight and the sunlight that goes through another perforated plate at almost the same time. The ratio of the signal strengths from the two observations is used to determine the BRDF degradation factor. Consequently, the RSB radiometric calibration requires the accurate knowledge of the product of the SD screen transmittance and the initial BRDF value as sensed by the RSB and the SDSM detectors. We use both yaw maneuver and a small portion of regular on-orbit data to determine the products.

Lei, Ning↗
DOE OSTI2015

Magnetotransport in p-type Ge quantum well narrow wire arrays

We report magnetotransport measurements of a SiGe heterostructure containing a 20 nm p-Ge quantum well with a mobility of 800 000 cm{sup 2} V{sup −1} s{sup −1}. By dry etching arrays of wires with widths between 1.0 μm and 3.0 μm, we were able to measure the lateral depletion thickness, built-in potential, and the phase coherence length of the quantum well. Fourier analysis does not show any Rashba related spin-splitting despite clearly defined Shubnikov-de Haas oscillations being observed up to a filling factor of ν = 22. Exchange-enhanced spin-splitting is observed for filling factors below ν = 9. An analysis of boundary scattering effects indicates lateral depletion of the hole gas by 0.5 ± 0.1 μm from the etched germanium surface. The built-in potential is found to be 0.25 ± 0.04 V, presenting an energy barrier for lateral transport greater than the hole confinement energy. A large phase coherence length of 3.5 ± 0.5 μm is obtained in these wires at 1.7 K.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

A cell-local finite difference discretization of the low-order quasidiffusion equations for neutral particle transport on unstructured quadrilateral meshes

We present a quasidiffusion (QD) method for solving neutral particle transport problems in Cartesian XY geometry on unstructured quadrilateral meshes, including local refinement capability. Neutral particle transport problems are central to many applications including nuclear reactor design, radiation safety, astrophysics, medical imaging, radiotherapy, nuclear fuel transport/storage, shielding design, and oil well-logging. The primary development is a new discretization of the low-order QD (LOQD) equations based on cell-local finite differences. The accuracy of the LOQD equations depends on proper calculation of special non-linear QD (Eddington) factors from a transport solution. In order to completely define the new QD method, a proper discretization of the transport problem is also presented. The transport equation is discretized by a conservative method of short characteristics with a novel linear approximation of the scattering source term and monotonic, parabolic representation of the angular flux on incoming faces. Analytic and numerical tests are used to test the accuracy and spatial convergence of the non-linear method. All tests exhibit O(h{sup 2}) convergence of the scalar flux on orthogonal, random, and multi-level meshes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Morphology and CO Oxidation Activity of Pd Nanoparticles on SrTiO 3 Nanopolyhedra

Single crystal SrTiO 3 nanocuboids having primarily TiO 2 -(001) surfaces and nanododecahedra having primarily (110) surfaces were created by two separate hydrothermal synthesis processes. Pd nanoparticles grown on the two sets of STO nanopolyhedra by atomic layer deposition show different morphologies and CO oxidation performance. Transmission electron microscopy and small-angle X-ray scattering show that 2-3 nm Pd nanoparticles with 3-5 nm interparticle distances decorate the STO surfaces. When the number of ALD cycles increases, the growth of the Pd nanoparticles is more significant in size on TiO 2 -(001)-STO surfaces, while that on (110)-STO surfaces is more predominant in number. High resolution electron microscopy images show that single crystal and multiply twinned Pd nanoparticles coexist on both types of the STO nanopolyhedra and exhibit different degrees of adhesion. The CO oxidation reaction, which was employed to determine the dependence of catalytic activity, demonstrated that the Pd catalytic performance was dominated by the coverage of CO, which is more directly related to Pd nanoparticle size than to shape. CO turnover frequency analysis and diffuse reflectance infrared Fourier transform spectroscopy show that regardless of the shape or degrees of wetting, larger Pd nanoparticles (~ 3 nm) have lower catalytic activity due to high CO coverage on nanoparticle facets. Smaller nanoparticles (~ 2 nm) have more edge and corner sites and present 2-3 times higher TOF at 80 and 100 degrees C.

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

Simultaneous Thermal Stability and Ultrahigh Sensitivity of Heterojunction SERS Substrates

This paper reports the design of Ag-Al 2 O 3 -Ag heterojunctions based on Ag nanorods (AgNRs) and their applications as thermally stable and ultrasensitive substrates of surface-enhanced Raman scattering (SERS). Specifically, an ultrathin Al 2 O 3 capping layer of 10 nm on top of AgNRs serves to slow down the surface diffusion of Ag at high temperatures. Then, an additional Ag layer on top of the capping layer creates AgNRs-Al 2 O 3 -Ag heterojunctions, which lead to giant enhancement of electromagnetic fields within the Al 2 O 3 gap regions that could boost the SERS enhancement. As a result of this design, the SERS substrates are thermally stable up to 200 °C, which has been increased by more than 100 °C compared with bare AgNRs, and their sensitivity is about 400% that of pure AgNRs. This easy yet effective capping approach offers a pathway to fabricate ultrasensitive, thermally stable and easily prepared SERS sensors, and to extend SERS applications for high-temperature detections, such as monitoring in situ the molecule reorientation process upon annealing. Such simultaneous achievement of thermal stability and SERS sensitivity represents a great advance in the design of SERS sensors and will inspire the fabrication of novel hetero-nanostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2017

CMB spectral distortions as solutions to the Boltzmann equations

We propose to re-interpret the cosmic microwave background spectral distortions as solutions to the Boltzmann equation. This approach makes it possible to solve the second order Boltzmann equation explicitly, with the spectral y distortion and the momentum independent second order temperature perturbation, while generation of μ distortion cannot be explained even at second order in this framework. We also extend our method to higher order Boltzmann equations systematically and find new type spectral distortions, assuming that the collision term is linear in the photon distribution functions, namely, in the Thomson scattering limit. As an example, we concretely construct solutions to the cubic order Boltzmann equation and show that the equations are closed with additional three parameters composed of a cubic order temperature perturbation and two cubic order spectral distortions. The linear Sunyaev-Zel'dovich effect whose momentum dependence is different from the usual y distortion is also discussed in the presence of the next leading order Kompaneets terms, and we show that higher order spectral distortions are also generated as a result of the diffusion process in a framework of higher order Boltzmann equations. The method may be applicable to a wider class of problems and has potential to give a general prescription to non-equilibrium physics.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Adapting confocal Raman microscopy for in situ studies of redox transformations at electrode-electrolyte interfaces

Confocal Raman microscopy was applied to quantify redox species present within the diffusion layer adjacent to an electrode surface under potentiostatic control. A glass microscope coverslip with a thin indium tin oxide (ITO) coating served as both the working electrode and optical window for a microscope-stage mountable spectroelectrochemical cell. A high numerical aperture objective mounted in an inverted microscope frame just below the stage brought excitation radiation through the coverslip window and to a tight focus a few micrometers above the ITO film surface. Species diffusing into the confocal probe volume defined by the excitation beam focus and the collected light region were detected, identified and quantified based on their Raman scattering frequencies and intensities. Here, in measurements that interrogated the interconversion of ferrocyanide and ferricyanide ions as a function of applied voltage, least-squares regression analysis of spectral datasets predicted the formal potential and relative surface concentrations of the ions in good agreement with the expected Nernstian response. Preliminary studies of methyl viologen reduction at an ITO film/Nafion membrane interface were conducted and show the possibility for estimation of mass transport coefficients of redox species within ionic polymer materials.

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

Effects of configurational changes on molecular dynamics in polyvinylidene fluoride and poly(vinylidene fluoride-trifluoroethylene) ferroelectric polymers

Here, we present a comparative study of proton dynamics in unpoled non-ferroelectric polymer polyvinylidene fluoride (PVDF) and in its trifluoroethylene containing ferroelectric copolymer (with 70/30 molar proportion), using quasi-elastic neutron scattering. The neutron data reveal the existence of two distinct types of molecular motions in the temperature range investigated. Moreover, the slower motion, which is characterized in details here, is ascribed to protons jump diffusion along the polymeric carbon chains, while the faster motion could be attributed to localized rotational motion of methylene groups. At temperatures below the Curie point (T-c similar to 385 K) of the composite polymer, the slower diffusive mode experiences longer relaxation times in the ferroelectric blend than in the bare PVDF, although the net corresponding diffusion coefficient remains comparatively the same in both polymers with characteristic activation energy of E-A approximate to 27-33 kJ/mol. This arises because of a temperature dependent jump length r(0), which we observe to be effectively longer in the copolymer, possibly due to the formation of ordered ferroelectric domains below Tc. Above Tc, there is no appreciable difference in r(0) between the two systems. Our observation directly relates the known dependence of Tc on molar ratio to changes in r(0), providing fundamental insight into the ferroelectric properties of PVDF-based copolymers.

36 MATERIALS SCIENCE↗