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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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At least 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Engineering Gram Selectivity of Mixed‐Charge Gold Nanoparticles by Tuning the Balance of Surface Charges

Abstract Nanoparticles covered with ligand shells comprising both positively and negatively charged ligands exhibit Gram‐selective antibacterial action controlled by a single experimental parameter, namely the proportion of [+] and [−] ligands tethered onto these particles. Gram selectivity is attributed to the interplay between polyvalent electrostatic and non‐covalent interactions that work in unison to disrupt the bacterial cell wall. The [+/−] nanoparticles are effective in low doses, are non‐toxic to mammalian cells, and are tolerated well in mice. These results constitute the first example of rational engineering of Gram selectivity at the (macro)molecular level.

Pillai, Pramod P.↗
DOE OSTI2017

Evolutionary Description of Giant Molecular Cloud Mass Functions on Galactic Disks

Recent radio observations show that giant molecular cloud (GMC) mass functions noticeably vary across galactic disks. High-resolution magnetohydrodynamics simulations show that multiple episodes of compression are required for creating a molecular cloud in the magnetized interstellar medium. In this article, we formulate the evolution equation for the GMC mass function to reproduce the observed profiles, for which multiple compressions are driven by a network of expanding shells due to H ii regions and supernova remnants. We introduce the cloud–cloud collision (CCC) terms in the evolution equation in contrast to previous work (Inutsuka et al.). The computed time evolution suggests that the GMC mass function slope is governed by the ratio of GMC formation timescale to its dispersal timescale, and that the CCC effect is limited only in the massive end of the mass function. In addition, we identify a gas resurrection channel that allows the gas dispersed by massive stars to regenerate GMC populations or to accrete onto pre-existing GMCs. Our results show that almost all of the dispersed gas contributes to the mass growth of pre-existing GMCs in arm regions whereas less than 60% contributes in inter-arm regions. Our results also predict that GMC mass functions have a single power-law exponent in the mass range <10{sup 5.5} M{sub ⊙} (where M{sub ⊙} represents the solar mass), which is well characterized by GMC self-growth and dispersal timescales. Measurement of the GMC mass function slope provides a powerful method to constrain those GMC timescales and the gas resurrecting factor in various environments across galactic disks.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

Visible Photoelectrochemical Water Splitting Based on a Ru(II) Polypyridyl Chromophore and Iridium Oxide Nanoparticle Catalyst

Preparation of Ru(II) polypyridyl-iridium oxide nanoparticle (IrO X NP) chromophore-catalyst assemblies on an FTO$|nano$ITO$|$TiO2 core/shell by a layer-bylayer procedure is described for application in dye-sensitized photoelectrosynthesis cells (DSPEC). Significantly enhanced, bias-dependent photocurrents with Lumencor 455 nm 14.5 mW/cm 2 irradiation are observed for core/shell structures compared to TiO 2 after derivatization with [Ru(4,4$'$-PO 3 H 2 bpy) 2 (bpy)] 2+ (RuP 2 ) and uncapped IrO X NPs at pH 5.8 in NaSiF6 buffer with a Pt cathode. Photocurrents arising from photolysis of the resulting photoanodes, FTO$|nano$ITO$|$TiO 2 |-RuP 2 ,IrO 2 , are dependent on TiO2 shell thickness and applied bias, reaching 0.2 mA/cm2 at 0.5 V vs AgCl/Ag with a shell thickness of 6.6 nm. Long-term photolysis in the NaSiF6 buffer results in a marked decrease in photocurrent over time due to surface hydrolysis and loss of the chromophore from the surface. Long-term stability, with sustained photocurrents, has been obtained by atomic layer deposition (ALD) of overlayers of TiO 2 to stabilize surface binding of -RuP 2 prior to the addition of the IrO X NPs.

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

Use of Encapsulated Zinc Particles in a Eutectic Chloride Salt to Enhance Thermal Energy Storage Capacity for Concentrated Solar Power

Concentrated Solar Power (CSP) is considered as a viable large-scale renewable energy source to produce electricity. However, current costs to produce electricity from CSP are not cost competitive as compared to the traditional energy generation technologies based on fossil fuels and nuclear. It is envisioned that development of high efficiency and high heat capacity thermal storage fluids will increase system efficiency, reduce structural storage volume, and hence, contribute to reducing costs. Particularly, with respect to CSP, current high temperature energy storage fluids, such as molten salts, are relatively limited in terms of their thermal energy storage capacity and thermal conductivity. The current work explores possibility of boosting the thermal storage capacity of molten salts through latent heat of added phase change materials. We studied the advantage Of adding coated Zn micron-sized particles to alkali chloride salt eutectic for enhanced thermal energy storage. Zinc particles (0.6 mu m and 5 mu m) obtained from commercial source were coated with an organo-phosphorus shell to improve chemical stability and to prevent individual particles from coalescing with one another during melt/freeze cycles. Thermal cycling tests (200 melt/freeze cycles) showed that coated Zn particles have good thermal stability and are chemically inert to alkali chloride salt eutectic in both N-2 and in air atmospheres. Elemental mapping of the cross-sectional view of coated Zn particles from the composite after thermal cycles showed no signs of oxidation, agglomeration or other type of particle degradation. The measured enhancement in volumetric thermal storage capacity of the composite with just similar to 10 vol% of coated Zn particles over the base chloride salt eutectic varies from 15% to 34% depending on cycling temperature range (Delta T = 50 degrees C -100 degrees C. (C) 2015 Elsevier Ltd. All rights reserved.

encapsulation↗
DOE OSTI2013

REPRODUCING THE OBSERVED ABUNDANCES IN RCB AND HdC STARS WITH POST-DOUBLE-DEGENERATE MERGER MODELS-CONSTRAINTS ON MERGER AND POST-MERGER SIMULATIONS AND PHYSICS PROCESSES

The R Coronae Borealis (RCB) stars are hydrogen-deficient, variable stars that are most likely the result of He-CO WD mergers. They display extremely low oxygen isotopic ratios, {sup 16}O/{sup 18}O {approx_equal} 1-10, {sup 12}C/{sup 13}C {>=} 100, and enhancements up to 2.6 dex in F and in s-process elements from Zn to La, compared to solar. These abundances provide stringent constraints on the physical processes during and after the double-degenerate merger. As shown previously, O-isotopic ratios observed in RCB stars cannot result from the dynamic double-degenerate merger phase, and we now investigate the role of the long-term one-dimensional spherical post-merger evolution and nucleosynthesis based on realistic hydrodynamic merger progenitor models. We adopt a model for extra envelope mixing to represent processes driven by rotation originating in the dynamical merger. Comprehensive nucleosynthesis post-processing simulations for these stellar evolution models reproduce, for the first time, the full range of the observed abundances for almost all the elements measured in RCB stars: {sup 16}O/{sup 18}O ratios between 9 and 15, C-isotopic ratios above 100, and {approx}1.4-2.35 dex F enhancements, along with enrichments in s-process elements. The nucleosynthesis processes in our models constrain the length and temperature in the dynamic merger shell-of-fire feature as well as the envelope mixing in the post-merger phase. s-process elements originate either in the shell-of-fire merger feature or during the post-merger evolution, but the contribution from the asymptotic giant branch progenitors is negligible. The post-merger envelope mixing must eventually cease {approx}10{sup 6} yr after the dynamic merger phase before the star enters the RCB phase.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2017

Reversible Modulation of the Electrostatic Potential of a Colloidal Quantum Dot through the Protonation Equilibrium of Its Ligands

This Letter describes the reversible modulation of the electrostatic potential at the interface between a colloidal PbS quantum dot (QD) and solvent, through the protonation equilibrium of the QD’s histamine-derivatized dihydrolipoic acid (DHLA) ligand shell. The electrostatic potential is sensitively monitored by the yield of photoinduced electron transfer from the QD to a charged electron acceptor, 9,10-anthraquinone-2-sulfonate (AQ). The permeability of the DHLA coating to the AQ progressively increases as the average degree of protonation of the ligand shell increases from 0 to 92%, as quantified by 1H NMR, upon successive additions of p-toluenesulfonic acid; this increase results in a decrease in the photoluminescence (PL) intensity of the QDs by a factor of 6.7. The increase in permeability is attributable to favorable electrostatic interactions between the ligands and AQ. This work suggests the potential of the combination of near-IR-emitting QDs and molecular quenchers as robust local H+ sensors.

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

A MULTI-WAVELENGTH 3D MODEL OF BD+30°3639

We present a 3D multi-wavelength reconstruction of BD+30°3639, one of the best-studied planetary nebulae in the solar neighborhood. BD+30°3639, which hosts a [WR]-type central star, has been imaged at wavelength regimes that span the electromagnetic spectrum, from radio to X-rays. We have used the astrophysical modeling software SHAPE to construct a 3D morpho-kinematic model of BD+30°3639. This reconstruction represents the most complete 3D model of a PN to date from the standpoint of the incorporation of multi-wavelength data. Based on previously published kinematic data in optical emission lines and in lines of CO (radio) and H{sub 2} (near-IR), we were able to reconstruct BD+30's basic velocity components assuming a set of homologous velocity expansion laws combined with collimated flows along the major axis of the nebula. We confirm that the CO “bullets” in the PN lie along an axis that is slightly misaligned with respect to the major axis of the optical nebula, and that these bullets are likely responsible for the disrupted structures of the ionized and H{sub 2}-emitting shells within BD+30. Given the relative geometries and thus dynamical ages of BD+30's main structural components, it is furthermore possible that the same jets that ejected the CO bullets are responsible for the generation of the X-ray-emitting hot bubble within the PN. Comparison of alternative viewing geometries for our 3D reconstruction of BD+30°3639 with imagery of NGC 40 and NGC 6720 suggests a common evolutionary path for these nebulae.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2016

Continuous injection synthesis of indium arsenide quantum dots emissive in the short-wavelength infrared

With the emergence of applications based on short-wavelength infrared light, indium arsenide quantum dots are promising candidates to address existing shortcomings of other infrared-emissive nanomaterials. However, III–V quantum dots have historically struggled to match the high-quality optical properties of II–VI quantum dots. Here we present an extensive investigation of the kinetics that govern indium arsenide nanocrystal growth. Based on these insights, we design a synthesis of large indium arsenide quantum dots with narrow emission linewidths. We further synthesize indium arsenide-based core-shell-shell nanocrystals with quantum yields up to 82% and improved photo- and long-term storage stability. We then demonstrate non-invasive through-skull fluorescence imaging of the brain vasculature of murine models, and show that our probes exhibit 2–3 orders of magnitude higher quantum yields than commonly employed infrared emitters across the entire infrared camera sensitivity range. Finally, we anticipate that these probes will not only enable new biomedical imaging applications, but also improved infrared nanocrystal-LEDs and photon-upconversion technology.

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

Evolution of the Single-Nanocrystal Photoluminescence Linewidth with Size and Shell: Implications for Exciton–Phonon Coupling and the Optimization of Spectral Linewidths

The optimization of photoluminescence spectral linewidths in semiconductor nanocrystal preparations involves minimizing both the homogeneous and inhomogeneous contributions to the ensemble spectrum. Although the inhomogeneous contribution can be controlled by eliminating interparticle inhomogeneities, far less is known about how to synthetically control the homogeneous, or single-nanocrystal, spectral linewidth. Here, we use solution photon-correlation Fourier spectroscopy (S-PCFS) to measure how the sample-averaged single-nanocrystal emission linewidth of CdSe core and core/shell nanocrystals change with systematic changes in the size of the cores and the thickness and composition of the shells. We find that the single-nanocrystal linewidth at room temperature is heavily influenced by the nature of the CdSe surface and the epitaxial shell, which have a profound impact on the internal electric fields that affect exciton–phonon coupling. Our results explain the wide variations, both experimental and theoretical, in the magnitude and size dependence in previous reports on exciton–phonon coupling in CdSe nanocrystals. Furthermore, our findings offer a general pathway for achieving the narrow spectral linewidths required for many applications of nanocrystals.

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

Using excitation-energy dependent fission yields to identify key fissioning nuclei in r -process nucleosynthesis

The possibility that nucleosynthesis in neutron star mergers may reach fissioning nuclei introduces significant uncertainties in predicting the relative abundances of $r$-process material from such events. We evaluate the impact of using sets of fission yields given by the 2016 GEF code for spontaneous (sf), neutron-induced $((n, f))$, and $β$-delayed (βdf) fission processes which take into account the approximate initial excitation energy of the fissioning compound nucleus. We further explore energy-dependent fission dynamics in the $r$ process by considering the sensitivity of our results to the treatment of the energy sharing and de-excitation of the fission fragments using the FREYA code. We show that the asymmetric-to-symmetric yield trends predicted by GEF 2016 can reproduce the high-mass edge of the second $r$-process peak seen in solar data and examine the sensitivity of this result to the mass model and astrophysical conditions applied. We consider the effect of fission yields and barrier heights on the nuclear heating rates used to predict kilonova light curves. We find that fission barriers influence the contribution of 254 Cf spontaneous fission to the heating at ~100 d, such that a light curve observation consistent with such late-time heating would both confirm that actinides were produced in the event and imply the fission barriers are relatively high along the 254 Cf β-feeding path. We lastly determine the key nuclei responsible for setting the r-process abundance pattern by averaging over thirty trajectories from a 1.2–1.4 M ⊙ neutron star merger simulation. Finally, we show it is largely the odd-N nuclei undergoing $(Z, N)(n, f)$ and $(Z, N)β$df that control the relative abundances near the second peak. We find the 'hot spots' for β-delayed and neutron-induced fission given all mass models considered and show most of these nuclei lie between the predicted $N$ = 184 shell closure and the location of currently available experimental decay data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2018

Convective boundary mixing in a post-He core burning massive star model

Convective boundary mixing (CBM) in the advanced evolutionary stages of massive stars is not well understood. Structural changes caused by convection have an impact on the evolution as well as the subsequent supernova, or lack thereof. The effects of convectively driven mixing across convective boundaries during the post He core burn- ing evolution of 25M ⊙ , solar-metallicity, non-rotating stellar models is studied using the MESA stellar evolution code. CBM is modelled using the exponentially decaying dif- fusion coeffcient equation, the free parameter of which, fCBM, is varied systematically throughout the course of the stellar model's evolution with values of (0.002, 0.012, 0.022, 0.032). The effect of varying this parameter produces mass ranges at collapse in the ONe, Si, Fe cores of (1.82M ⊙ , 4.36M ⊙ ), (1.67M ⊙ , 1.99M ⊙ ) and (1.46M ⊙ , 1.70M ⊙ ) respectively, with percent differences from the model with minimal CBM as large as 86.3%. At the presupernova stage, the compactness of the stellar cores from O'Connor & Ott (2011), ξ M , exhibit a range of (0.120, 0.354), suggesting that the extent of CBM in the advanced burning stages of massive stars is an important consideration for the explodability and type of compact remnant. The nucleosynthetic yields from the models, most notably C, O, Ne, Mg and Si are also signi cantly affected by the CBM assumptions, showing non-linear trends with increased mixing. The simulations show that interactions between convective C, Ne and O shells produce signi cant non- linear changes in the evolution, whereas from the end of Si burning, the structural changes attributed to the CBM are dominated by the growth of the convective C shell.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2014

Effect of spatial density variation and O+ concentration on the growth and evolution of electromagnetic ion cyclotron waves

We simulate electromagnetic ion cyclotron (EMIC) wave growth and evolution within three regions, the plasmasphere (or plasmaspheric plume), the plasmapause, and the low-density plasmatrough outside the plasmapause. First, we use a ring current simulation with a plasmasphere model to model the particle populations that give rise to the instability for conditions observed on 9 June 2001. Then, using two different models for the cold ion composition, we do a full scale hybrid code simulation in dipole coordinates of the EMIC waves on a meridional plane at MLT = 18 and at 1900 UT within a range of L shell from L = 4.9 to 6.7. EMIC waves were observed during June 9, 2001 by Geostationary Operational Environmental Satellite (GOES) spacecraft. While an exact comparison between observed and simulated spectra is not possible here, we do find significant similarities between the two, at least at one location within the region of largest wave growth. We find that the plasmapause is not a preferred region for EMIC wave growth, though waves can grow in that region. The density gradient within the plasmapause does, however, affect the orientation of wave fronts and wave vector both within the plasmapause and in adjacent regions. There is a preference for EMIC waves to be driven in the He+ band (frequencies between the O+ and He+ gyrofrequencies) within the plasmasphere, although they can also grow in the plasmatrough. If present, H+ band waves are more likely to grow in the plasmatrough. This fact, plus L dependence of the frequency and possible time evolution toward lower frequency waves, can be explained by a simple model. Large O+ concentration limits the frequency range of or even totally quenches EMIC waves. This is more likely to occur in the plasmatrough at solar maximum. Such large O+ concentration significantly affects the H+ cutoff frequency and hence the width in frequency of the stop band above the He+ gyrofrequency. EMIC wave surfaces predicted by cold plasma theory are altered by the finite temperature of the ring current H+.

58 GEOSCIENCES↗
DOE OSTI2016

Time Resolved Optical Studies on The Plasmonic Field Enhancement of Bacteriorhodopsin Proton Photo-current: Final Technical Report Covering Aug 31, 2015–Aug 31, 2016

Our research continues to focus on the effects of plasmonic nanoparticles on organic and inorganic light-harvesting materials. Recent work has focused on the synthesis of stabilized gold nanoparticles to enhance the efficiency of dye-sensitized solar cells (DSSCs). Two major concerns in dye sensitized solar cells (DSSCs) are efficient light absorption and charge collection. Charge collection typically suffers because transport of electrons through the mesoporous TiO 2 substrate is slow. Thus, one obvious way to improve charge collection is to reduce the thickness of the TiO 2 . Alternatively, a form of TiO 2 with fewer grain boundaries, such as nanotubes, could be used in place of sintered nanospheres. Unfortunately, both of these solutions end up reducing the amount of surface area available to adsorb dye molecules. This directly reduces the percentage of photons absorbed. This problem could be avoided if dye molecules with larger absorption were designed; although synthetic chemists seem to be pushing the limits of what is achievable. Plasmonic nanoparticles offer an alternative way to boost light absorption. It is well known that plasmonic nanoparticles can enhance the local electric field of resonant frequencies of light. If this were in the same spectral region as the dye’s absorption band it would increase the percentage of absorbed photons. One concern is that if the nanoparticles are too close to the dye molecules they can quench the excited state. To avoid this problem, we prepared gold nanoparticles with a silica shell. This limited the amount of quenching while still permitting some enhancement of absorption. Unfortunately, we ran into some serious issues. The iodide based electrolyte etched the gold nanoparticles, completely dissolving them within a few hours. The silica shell should have provided protection but there were pinholes through which iodide could diffuse. Increasing the thickness of the silica to over 10 nm prevented etching but also limited any photon absorption enhancement.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Elucidating the sole contribution from electromagnetic near-fields in plasmon-enhanced Cu 2 O photocathodes

Despite many promising reports of plasmon-enhanced photocatalysis, the inability to identify the individual contributions from multiple enhancement mechanisms has delayed the development of general design rules for engineering efficient plasmonic photocatalysts. Herein, we construct a plasmonic photocathode comprised of Au@SiO 2 (core@shell) nanoparticles embedded within a Cu 2 O nanowire network to exclusively examine the contribution from one such mechanism: electromagnetic near-field enhancement. The influence of the local electromagnetic field intensity is correlated with the overall light-harvesting efficiency of the device through variation of the SiO 2 shell thickness (5—22 nm) to systematically tailor the distance between the plasmonic Au nanoparticles and the Cu 2 O nanowires. A three-fold increase in device photocurrent is achieved upon integrating the Au@SiO 2 nanoparticles into the Cu 2 O nanowire network, further enabling a ~40% reduction in semiconductor film thickness while maintaining photocathode performance. Photoelectrochemical results are further correlated with photoluminescence studies and optical simulations to confirm that the near-field enhancement is the sole mechanism responsible for increased light absorption in the plasmonic photocathode.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2016

Hexadecapolar Colloids

Outermost occupied electron shells of chemical elements can have symmetries resembling that of monopoles, dipoles, quadrupoles and octupoles corresponding to filled s-, p-, d- and forbitals. Theoretically, elements with hexadecapolar outer shells could also exist, but none of the known elements have filled g-orbitals. On the other hand, the research paradigm of ‘colloidal atoms’ displays complexity of particle behaviour exceeding that of atomic counterparts, which is driven by DNA functionalization, geometric shape and topology and weak external stimuli. We describe elastic hexadecapoles formed by polymer microspheres dispersed in a liquid crystal, a nematic fluid of orientationally ordered molecular rods. Because of conically degenerate boundary conditions, the solid microspheres locally perturb the alignment of the nematic host, inducing hexadecapolar distortions that drive anisotropic colloidal interactions. We uncover physical underpinnings of formation of colloidal elastic hexadecapoles and report the ensuing bonding inaccessible to elastic dipoles, quadrupoles and other nematic colloids studied previously.

14 SOLAR ENERGY↗
DOE OSTI2016

RELATIVE CONTRIBUTIONS OF THE WEAK, MAIN, AND FISSION-RECYCLING r-PROCESS

There has been a persistent conundrum in attempts to model the nucleosynthesis of heavy elements by rapid neutron capture (the r-process). Although the locations of the abundance peaks near nuclear mass numbers 130 and 195 identify an environment of rapid neutron capture near closed nuclear shells, the abundances of elements just above and below those peaks are often underproduced by more than an order of magnitude in model calculations. At the same time, there is a debate in the literature as to what degree the r-process elements are produced in supernovae or the mergers of binary neutron stars. In this paper we propose a novel solution to both problems. We demonstrate that the underproduction of nuclides above and below the r-process peaks in main or weak r-process models (like magnetohydrodynamic jets or neutrino-driven winds in core-collapse supernovae) can be supplemented via fission fragment distributions from the recycling of material in a neutron-rich environment such as that encountered in neutron star mergers (NSMs). In this paradigm, the abundance peaks themselves are well reproduced by a moderately neutron-rich, main r-process environment such as that encountered in the magnetohydrodynamical jets in supernovae supplemented with a high-entropy, weakly neutron-rich environment such as that encountered in the neutrino-driven-wind model to produce the lighter r-process isotopes. Moreover, we show that the relative contributions to the r-process abundances in both the solar system and metal-poor stars from the weak, main, and fission-recycling environments required by this proposal are consistent with estimates of the relative Galactic event rates of core-collapse supernovae for the weak and main r-process and NSMs for the fission-recycling r-process.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2018

Engineering a Full Gamut of Structural Colors in All-Dielectric Mesoporous Network Metamaterials

Structural colors are a result of the scattering of certain frequencies of the incident light on micro- or nanoscale features in a material. This is a quite different phenomenon from that of colors produced by absorption of different frequencies of the visible spectrum by pigments or dyes, which is the most common way of coloring used in our daily life. However, structural colors are more robust and can be engineered to span most of the visible spectrum without changing the base material, only its internal structure. They are abundant in nature, with examples as colorful as beetle shells and butterfly wings, but there are few ways of preparing them for large-scale commercial applications for real-world uses. In this work, we present a technique to create a full gamut of structural colors based on a low-cost, robust, and scalable fabrication of periodic network structures in porous alumina as well as the strategy to theoretically predict and engineer different colors on demand. We experimentally demonstrate mesoporous network metamaterial structures with engineered colors spanning the whole optical spectrum and discuss their applications in sensing, environmental monitoring, biomimetic tissues engineering, etc.

36 MATERIALS SCIENCE↗