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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Effect of Block Length and Side Chain Length Ratios on Determining a Multicompartment Micelle Structure

Previous work has identified the importance of the lipophilic-fluorophilic block length ratio R l in predicting the morphology of linear lipophilic-hydrophilic-fluorophilic (hereafter referred to as BAC) micelle systems. Here, a generalized form R of this structural parameter is developed that makes no assumption of BAC triblock copolymer linearity, while still providing accurate predictions of micelle morphology. Here, the morphologies of BAC micelles formed by triblock copolymers with R <<1 or R >>1 have similar features, with the only notable difference being an inversion of the lipophilic and fluorophilic regions. A destabilization of the single-core micelle structure occurs as R approaches unity from either direction. Finally, the extent to which micelle morphology depends on polymer architecture instead of composition alone is examined, with decreased patchiness observed in BAC systems with very long block lengths. Through modification of both the R-value and the polymer architecture, the micelle morphology can be effectively tuned for use in immobilized catalysis and nanoreactor applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Experimental determination of electron attenuation lengths in complex materials by means of epitaxial film growth: advantages and challenges

Accurate electron attenuation lengths are of critical importance in using electron spectroscopic methods to quantitatively characterize complex materials. Here we show that analysis of core-level and valence-band x-ray photoelectron spectra excited with monochromatic AlK? x-rays from the substrate and measured as a function of film thickness can be used to determine electron attenuation lengths in epitaxial SrTiO3 films on Ge(001). Closely lattice-matched epitaxial heterojunctions are ideal systems for determining attenuation lengths provided the films grow in a layer-by-layer fashion, leading to atomically flat surfaces, and the buried interfaces are atomically abrupt. In principle, either the rate of attenuation of substrate peak intensities or the rate of increase of film peak intensities can be used for this purpose. However, we find that structural nonuniformities in the films reduce the accuracy of electron attenuation lengths determined from photoelectrons that originate within the films. A more reliable source of information is found in photoelectrons from the substrate which traverse the film. By using the energy dependence of calculated electron attenuation lengths from the NIST database in combination with Ge 3d core and Ge-derived valence band intensities, we determine electron attenuation length as a function of kinetic energy for SrTiO3.

Chambers, Scott A.↗
DOE OSTI2020

Data-driven predictive probability density function control of fiber length stochastic distribution shaping in refining process

Pulp is the most important raw material in paper in paper industries, whose Fiber Length Stochastic Distribution (FLSD) shaping directly determines the energy consumption and paper quality of the subsequent papermaking processes. However, the mean and variance are insufficient to describe the output FLSD shaping, which display non-Gaussian distribution properties. Therefore, the traditional control, method based on the mean and variance of fiber length is difficult to control the FLSD shaping effectively. In this paper, a novel data-driven predictive probability density function (PDF) control method is proposed for output FLSD shaping in refining process. Primarily, in order to improve the approximation accuracy of the PDF employing RBF neural network, the parameters (center value and width) of each RBF basis functions are tuned via utilizing iterative learning control (ILC) law, and the corresponding estimations of weights law can be obtained. Secondly, considering that the conventional linear model of weights vector has drawbacks of low accuracy and weak generalization ability, random vector functional link networks (RVFLNs) based data driven nonlinear modelling method is employed to characterize the prediction model between the input variables and weights vector. Finally, in order to reduce the randomness of the output FLSD, a minimum entropy control method under mean constraint is employed to design the predictive PDF controller for the output FLSD shaping with the help of the established nonlinear stochastic distribution model. Both simulations and experiments are given to illustrate the effectiveness and practicability of the proposed method.

Probability debsity function, Fiber length distrib↗
DOE OSTI2022

Interferometric bunch length measurements of 3 MeV picocoulomb electron beams

We report picosecond bunch length measurements using an interferometric method for a 3 MeV electron beam having bunch charge ranging from 1 to 14 pC. The method senses the single-cycle sub-terahertz (THz) pulse emitted by each electron bunch as coherent transition radiation which, in turn, is analyzed using a Michelson-type interferometer, forming an interferogram that is then processed to yield the nominal electron bunch length. This sub-THz coherent radiation intensity was measured using a quasi-optical detector (QOD) operated at room temperature. This experiment was quite challenging since the divergence angle of the sub-THz pulse emitted by the low-energy electron bunch exceeds ±10°, and its pulse energy at the entrance to the detector was as low as 100 pJ. When compared to a conventional helium-cooled silicon composite bolometer designed for frequencies above 0.5 THz, the QOD provided much better signal-to-noise ratio in the ~80 GHz frequency range, which was critical for the successful measurement of the bunch length.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Evolution of Chain Dynamics and Oxidation States with Increasing Chain Length for a Donor–Acceptor-Conjugated Oligomer Series

While it is known that the chain length strongly affects the properties of π-conjugated polymers, the effects of chain length on the molecular structure, chain conformation, and oxidation state properties in donor–acceptor-type conjugated structures remain unclear. This limits our understanding of how the polymer molecular weight impacts material properties. Here, a discrete and monodisperse oligomer series (n = 3, 5, 7, 9, 15, and 21) and polymers (nPB), composed of the donor 3,4-propylenedioxythiophene (ProDOT), the acceptor benzothiadiazole (BTD), and methylthio end-capping groups, are synthesized by C–H-activated cross-coupling. The molecular structure, molecular weight, and dispersity of each oligomer/polymer are thoroughly characterized by nuclear magnetic resonance spectroscopy, mass spectrometry, and gel permeation chromatography. This series reveals a rod-to-coil transition at n = 15 and coil formation at polymer length scales of ~28 units via solution small-angle neutron scattering characterization. The oxidation states are deciphered via cyclic voltammetry, differential pulse voltammetry, spectroelectrochemistry, and density functional theory calculations. Oligomers 3–9 undergo successive one-electron oxidation steps, while 15 and higher undergo multielectron oxidations per step in CH 2 Cl 2 –TBAPF6 at a Pt ultramicroelectrode. The electronic transition of each oxidation state (1+, 2+, 3+, etc.) is tracked by absorption spectroscopy, revealing a “bipolaron to di-polaron” transition at n = 7 at which shorter oligomers prefer bipolaron formation and longer oligomers prefer di-polaron formation in their dication states. Furthermore, oxidized 15 has a lower electronic transition energy compared to its polymer homologue, as shown by spectroelectrochemistry, revealing a synergy between the chain length and the oxidation state properties. This study proves that the convergence limit between small molecule and polymer behavior occurs at approximately 15 units and highlights the property transitions that occur as a function of chain length for a donor–acceptor class of conjugated organic materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Cumulene Wires Display Increasing Conductance with Increasing Length

One-dimensional sp-hybridized carbon wires, including cumulenes and polyynes, can be regarded as finite versions of carbynes. They are likely to be good candidates for molecular-scale conducting wires as they are predicted to have a high-conductance. In this study, we first characterize the single-molecule conductance of a series of cumulenes and polyynes with a backbone ranging in length from 4 to 8 carbon atoms, including [7]cumulene, the longest cumulenic carbon wire studied to date for molecular electronics. We observe different length dependence of conductance when comparing these two forms of carbon wires. Polyynes exhibit conductance decays with increasing molecular length, while cumulenes show a conductance increase with increasing molecular length. Their distinct conducting behaviors are attributed to their different bond length alternation, which is supported by theoretical calculations. Furthermore, this study confirms the long-standing theoretical predictions on sp-hybridized carbon wires and demonstrates that cumulenes can form highly conducting molecular wires.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Geometric Analysis Based Double Closed-loop Iterative Learning Control of Output PDF Shaping of Fiber Length Distribution in Refining Process

In order to improve the pulp quality and to reduce the energy consumption, the fiber length distribution (FLD) is generally employed as one of the important technological indexes in the refining process. Considering that the traditional mean and variance of fiber length are unable to adequately characterize the non-Gaussian distribution properties, this paper proposes a novel geometric analysis based double closed-loop iterative learning control (ILC) method for probability density function (PDF) shaping of output FLD in the refining process. Primarily, a RBF neural network (NN) with Gaussian-type is utilized to approximate the square root PDF in the inner loop, where the RBF basis function parameters (center and width) are tuned between any two adjacent batches by using an ILC law, and the subspace identification method can be applied to establish the state-space model of weight vector. Then, for the sake of accelerating the convergence rate of the closed-loop sysyem, a geometric analysis based ILC method is adopted in the outer loop. Lastly, both simulation and experiments demonstrate the effectiveness and practicability of the proposed approach.

42 ENGINEERING↗
DOE OSTI2024

Efficacy of using a dynamic length representation vs. a fixed-length for neuroarchitecture search

Deep learning neuroarchitecture and hyperparameter search are important in finding the best configuration that maximizes learned model accuracy. However, the number of types of layers, their associated hyperparameters, and the myriad of ways to connect layers poses a significant computational challenge in discovering ideal model configurations. Here, we assess two different approaches for neuroarchitecture search for a LeNet style neural network, one that uses a fixed-length approach where there is a preset number of possible layers that can be toggled on or off via mutation, and a variable-length approach where layers can be freely added or removed via special mutation operators. We found that the variable-length implementation trained better models while discovering unusual layer configurations worth further exploration.

Coletti, Mark↗
DOE OSTI2021

Effect of Polymer Chain Length on the Superlattice Assembly of Functionalized Gold Nanoparticles

We report on the assembly of gold nanoparticle (AuNPs) superlattices at the liquid/vapor interface and in the bulk of their suspensions. Interparticle distances in the assemblies are achieved on multiple length scales by varying chain lengths of surface grafted AuNPs by polyethylene glycol (PEG) with molecular weights in the range 2000–40,000 Da. Crystal structures and lattice constants in both 2D and 3D assemblies are determined by synchrotron-based surface-sensitive and small-angle X-ray scattering. Here, assuming knowledge of grafting density, we show that experimentally determined interparticle distances are adequately modeled by spherical brushes close to the θ point (Flory–Huggins parameter, x ≈ 1/2) for 2D superlattices at a liquid interface and a nonsolvent (χ = ∞) for the 3D dry superlattices.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Structural Tunability of Multicompartment Micelles as a Function of Lipophilic–Fluorophilic Block Length Ratio

Structural variation in multicompartment micelles consisting of lipophilic–hydrophilic–fluorophilic (hereafter referred to as BAC) triblock copolymers is investigated using the dissipative particle dynamics simulation method. It is demonstrated from our results that the structure of BAC multicompartment micelles is effectively tuned as a function of the lipophilic–fluorophilic ratio parameter, here termed $R_1$, of the constituent linear triblock copolymers. In particular, a morphological deviation from onion-like ABC micelles arises in BAC micelle systems as $R_1$ increases. The morphologies of BAC micelles with $R_1\ll$1 or $R_1\gg$1 display striking similarities, with the only notable difference being an inversion of the lipophilic and fluorophilic regions. When $R\approx$ 1, segmented worm-like structures with multiple cores are favored in BAC micelle systems. Through this study, it is confirmed that the block length ratio is an effective control parameter to tune the structure of multicompartment micelles.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Two Diverging Length Scales in the Structure of Jammed Packings

Here, at densities higher than the jamming transition for athermal, frictionless repulsive spheres we find two distinct length scales, both of which diverge as a power law as the transition is approached. The first, ξ Z , is associated with the two-point correlation function for the number of contacts on two particles as a function of the particle separation. Additionally, the second, ξ f , is associated with contact-number fluctuations in subsystems of different sizes. On scales below ξ f , the fluctuations are highly suppressed, similar to the phenomenon of hyperuniformity usually associated with density fluctuations. The exponents for the divergence of ξ Z and ξ f are different and appear to be different in two and three dimensions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Site-Specific Structure at Multiple Length Scales in Kagome Quantum Spin Liquid Candidates

Realizing a quantum spin liquid (QSL) ground state in a real material is a leading issue in condensed matter physics research. In this pursuit, it is crucial to fully characterize the structure and influence of defects, as these can significantly affect the fragile QSL physics. In this work, we perform a variety of cutting-edge synchrotron x-ray scattering and spectroscopy techniques, and we advance new methodologies for site-specific diffraction and L-edge Zn absorption spectroscopy. The experimental results along with our first-principles calculations address outstanding questions about the local and long-range structures of the two leading kagome QSL candidates, Zn-substituted barlowite Cu 3 Zn x Cu 1-x (OH) 6 FBr and herbertsmithite Cu 3 Zn(OH) 6 Cl 2 . On all length scales probed, there is no evidence that Zn substitutes onto the kagome layers, thereby preserving the QSL physics of the kagome lattice. Our calculations show that antisite disorder is not energetically favorable and is even less favorable in Zn-barlowite compared to herbertsmithite. Site-specific x-ray diffraction measurements of Zn-barlowite reveal that Cu 2+ and Zn 2+ selectively occupy distinct interlayer sites, in contrast to herbertsmithite. Using the first measured Zn L-edge inelastic x-ray absorption spectra combined with calculations, we discover a systematic correlation between the loss of inversion symmetry from pseudo-octahedral (herbertsmithite) to trigonal prismatic coordination (Zn-barlowite) with the emergence of a new peak. Overall, our measurements suggest that Zn-barlowite has structural advantages over herbertsmithite that make its magnetic properties closer to an ideal QSL candidate: its kagome layers are highly resistant to nonmagnetic defects while the interlayers can accommodate a higher amount of Zn substitution.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Vertical Magnetic Measurements of the First Full-Length Prototype MQXFAP2 Quadrupole for the LHC Hi-Lumi Accelerator Upgrade Project

This paper reports the commissioning of the vertical magnetic measurement system and the room temperature (warm) and cryogenic (cold) magnetic field measurements of the first full-length (4.2 m) quadrupole built by the U.S. Accelerator Upgrade Project (AUP) (formerly the LARP collaboration) for the high luminosity upgrade of the Large Hadron Collider at CERN. The magnet, designated MQXFAP2, is a prototype preceding production for the AUP which will provide ten sets of 8.4-m superconducting insertion region quadrupoles for the Hi-Lumi Upgrade. The quadrupoles will be built by assembling two 4.2-m magnets in a single cryostat. Agreement between Brookhaven National Laboratory's (BNL's) and Lawrence Berkeley National Laboratory's (LBNL's) warm measurement data has indicated that the upgraded vertical magnetic measurement system at Brookhaven National Laboratory is ready for MQXFA magnet production testing. Lastly, the cold magnetic measurement has been performed and preliminary data analysis has been conducted.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗