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At least 1,135 records · Page 63
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Untangling the threads of cellulose mercerization

Naturally occurring plant cellulose, our most abundant renewable resource, consists of fibers of long polymer chains that are tightly packed in parallel arrays in either of two crystal phases collectively referred to as cellulose I. During mercerization, a process that involves treatment with sodium hydroxide, cellulose goes through a conversion to another crystal form called cellulose II, within which every other chain has remarkably changed direction. We designed a neutron diffraction experiment with deuterium labelling in order to understand how this change of cellulose chain direction is possible. Here we show that during mercerization of bacterial cellulose, chains fold back on themselves in a zigzag pattern to form crystalline anti-parallel domains. This result provides a molecular level understanding of one of the most widely used industrial processes for improving cellulosic materials.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Estimating the randomness of quantum circuit ensembles up to 50 qubits

Random quantum circuits have been utilized in the contexts of quantum supremacy demonstrations, variational quantum algorithms for chemistry and machine learning, and blackhole information. The ability of random circuits to approximate any random unitaries has consequences on their complexity, expressibility, and trainability. To study this property of random circuits, we develop numerical protocols for estimating the frame potential, the distance between a given ensemble and the exact randomness. Our tensor-network-based algorithm has polynomial complexity for shallow circuits and is high-performing using CPU and GPU parallelism. We study 1. local and parallel random circuits to verify the linear growth in complexity as stated by the Brown–Susskind conjecture, and; 2. hardware-efficient ansätze to shed light on its expressibility and the barren plateau problem in the context of variational algorithms. Our work shows that large-scale tensor network simulations could provide important hints toward open problems in quantum information science.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2020

Intra- and Intermolecular Self-Assembly of a 20-nm-Wide Supramolecular Hexagonal Grid.

For the past three decades, the coordination-driven self-assembly of three-dimensional structures has undergone rapid progress; however, parallel efforts to create large discrete two-dimensional architectures-as opposed to polymers-have met with limited success. The synthesis of metallo-supramolecular systems with well-defined shapes and sizes in the range of 10-100 nm remains challenging. Here we report the construction of a series of giant supramolecular hexagonal grids, with diameters on the order of 20 nm and molecular weights greater than 65 kDa, through a combination of intra- and intermolecular metal-mediated self-assembly steps. The hexagonal intermediates and the resulting self-assembled grid architectures were imaged at submolecular resolution by scanning tunnelling microscopy. Characterization (including by scanning tunnelling spectroscopy) enabled the unambiguous atomic-scale determination of fourteen hexagonal grid isomers.

Zhang, Zhe↗
DOE OSTI2023

Massively scalable Kerr comb-driven silicon photonic link

Abstract The growth of computing needs for artificial intelligence and machine learning is critically challenging data communications in today’s data-centre systems. Data movement, dominated by energy costs and limited ‘chip-escape’ bandwidth densities, is perhaps the singular factor determining the scalability of future systems. Using light to send information between compute nodes in such systems can dramatically increase the available bandwidth while simultaneously decreasing energy consumption. Through wavelength-division multiplexing with chip-based microresonator Kerr frequency combs, independent information channels can be encoded onto many distinct colours of light in the same optical fibre for massively parallel data transmission with low energy. Although previous high-bandwidth demonstrations have relied on benchtop equipment for filtering and modulating Kerr comb wavelength channels, data-centre interconnects require a compact on-chip form factor for these operations. Here we demonstrate a massively scalable chip-based silicon photonic data link using a Kerr comb source enabled by a new link architecture and experimentally show aggregate single-fibre data transmission of 512 Gb s −1 across 32 independent wavelength channels. The demonstrated architecture is fundamentally scalable to hundreds of wavelength channels, enabling massively parallel terabit-scale optical interconnects for future green hyperscale data centres.

Rizzo, Anthony (ORCID:000000034752797X)↗
DOE OSTI2023

Non-thermal electron acceleration from magnetically driven reconnection in a laboratory plasma

Magnetic reconnection rapidly converts magnetic energy into some combination of plasma flow energy, thermal energy and non-thermal energetic particles. Various reconnection acceleration mechanisms have been theoretically proposed and numerically studied in different collisionless and low-β environments, where β refers to the plasma-to-magnetic pressure ratio. These mechanisms include Fermi acceleration, betatron acceleration, parallel electric field acceleration along magnetic fields and direct acceleration by the reconnection electric field. However, none of them have been experimentally confirmed, as the direct observation of non-thermal particle acceleration in laboratory experiments has been difficult due to short Debye lengths for in situ measurements and short mean free paths for ex situ measurements. Here we report the direct measurement of accelerated non-thermal electrons from magnetically driven reconnection at low β in experiments using a laser-powered capacitor coil platform. We use kilojoule lasers to drive parallel currents to reconnect megagauss-level magnetic fields in a quasi-axisymmetric geometry. The angular dependence of the measured electron energy spectrum and the resulting accelerated energies, supported by particle-in-cell simulations, indicate that the mechanism of direct electric field acceleration by the out-of-plane reconnection electric field is at work. Scaled energies using this mechanism show direct relevance to astrophysical observations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Resonance from antiferromagnetic spin fluctuations for superconductivity in UTe 2

We report superconductivity originates from the formation of bound (Cooper) pairs of electrons that can move through the lattice without resistance below the superconducting transition temperature $T_c$. Electron Cooper pairs in most superconductors form anti-parallel spin singlets with total spin S = 0, although they can also form parallel spin-triplet Cooper pairs with S = 1 and an odd parity wavefunction. Spin-triplet pairing is important because it can host topological states and Majorana fermions relevant for quantum computation. Because spin-triplet pairing is usually mediated by ferromagnetic (FM) spin fluctuations3, uranium-based materials near an FM instability are considered to be ideal candidates for realizing spin-triplet superconductivity. Indeed, UTe 2 , which has a $T_c$ ≈ 1.6 K, has been identified as a candidate for a chiral spin-triplet topological superconductor near an FM instability, although it also has antiferromagnetic (AF) spin fluctuations. Here we use inelastic neutron scattering (INS) to show that superconductivity in UTe 2 is coupled to a sharp magnetic excitation, termed resonance, at the Brillouin zone boundary near AF order. Because the resonance has only been found in spin-singlet unconventional superconductors near an AF instability, its observation in UTe 2 suggests that AF spin fluctuations may also induce spin-triplet pairing or that electron pairing in UTe 2 has a spin-singlet component.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

A quantum processor based on coherent transport of entangled atom arrays

The ability to engineer parallel, programmable operations between desired qubits within a quantum processor is key for building scalable quantum information systems. In most state-of-the-art approaches, qubits interact locally, constrained by the connectivity associated with their fixed spatial layout. Here we demonstrate a quantum processor with dynamic, non-local connectivity, in which entangled qubits are coherently transported in a highly parallel manner across two spatial dimensions, between layers of single- and two-qubit operations. Our approach makes use of neutral atom arrays trapped and transported by optical tweezers; hyperfine states are used for robust quantum information storage, and excitation into Rydberg states is used for entanglement generation. We use this architecture to realize programmable generation of entangled graph states, such as cluster states and a seven-qubit Steane code state. Furthermore, we shuttle entangled ancilla arrays to realize a surface code state with thirteen data and six ancillary qubits and a toric code state on a torus with sixteen data and eight ancillary qubits. Finally, we use this architecture to realize a hybrid analogue–digital evolution and use it for measuring entanglement entropy in quantum simulations, experimentally observing non-monotonic entanglement dynamics associated with quantum many-body scars. Realizing a long-standing goal, these results provide a route towards scalable quantum processing and enable applications ranging from simulation to metrology.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Scalable and accurate multi-GPU-based image reconstruction of large-scale ptychography data

Abstract While the advances in synchrotron light sources, together with the development of focusing optics and detectors, allow nanoscale ptychographic imaging of materials and biological specimens, the corresponding experiments can yield terabyte-scale volumes of data that can impose a heavy burden on the computing platform. Although graphics processing units (GPUs) provide high performance for such large-scale ptychography datasets, a single GPU is typically insufficient for analysis and reconstruction. Several works have considered leveraging multiple GPUs to accelerate the ptychographic reconstruction. However, most of these works utilize only the Message Passing Interface to handle the communications between GPUs. This approach poses inefficiency for a hardware configuration that has multiple GPUs in a single node, especially while reconstructing a single large projection, since it provides no optimizations to handle the heterogeneous GPU interconnections containing both low-speed (e.g., PCIe) and high-speed links (e.g., NVLink). In this paper, we provide an optimized intranode multi-GPU implementation that can efficiently solve large-scale ptychographic reconstruction problems. We focus on the maximum likelihood reconstruction problem using a conjugate gradient (CG) method for the solution and propose a novel hybrid parallelization model to address the performance bottlenecks in the CG solver. Accordingly, we have developed a tool, called PtyGer ( Pty chographic G PU(multipl e )-based r econstruction), implementing our hybrid parallelization model design. A comprehensive evaluation verifies that PtyGer can fully preserve the original algorithm’s accuracy while achieving outstanding intranode GPU scalability.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2022

Multi-beam X-ray ptychography using coded probes for rapid non-destructive high resolution imaging of extended samples

Imaging large areas of a sample non-destructively and with high resolution is of great interest for both science and industry. For scanning coherent X-ray diffraction microscopy, i. e., ptychography, the achievable scan area at a given spatial resolution is limited by the coherent photon flux of modern X-ray sources. Multibeam X-ray ptychography can improve the scanning speed by scanning the sample with several parallel mutually incoherent beams, e. g., generated by illuminating multiple focusing optics in parallel by a partially coherent beam. The main difficulty with this scheme is the robust separation of the superimposed signals from the different beams, especially when the beams and the illuminated sample areas are quite similar. We overcome this difficulty by encoding each of the probing beams with its own X-ray phase plate. This helps the algorithm to robustly reconstruct the multibeam data. We compare the coded multibeam scans to uncoded multibeam and single beam scans, demonstrating the enhanced performance on a microchip sample with regular and repeating structures.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Collisionless cooling of perpendicular electron temperature in the thermal quench of a magnetized plasma

Thermal quench of a nearly collisionless plasma against an isolated cooling boundary or region is an undesirable off-normal event in magnetic fusion experiments, but an ubiquitous process of cosmological importance in astrophysical plasmas. Parallel transport theory of ambipolar-constrained tail electron loss is known to predict rapid cooling of the parallel electron temperature $T_{e\Vert}$ although $T_{e\Vert}$ is difficult to diagnose in actual experiments. Instead direct experimental measurements can readily track the perpendicular electron temperature $T_{e\bot}$ via electron cyclotron emission. The physics underlying the observed fast drop in $T_{e\bot}$ requires a resolution. Here two collisionless mechanisms, dilutional cooling by infalling cold electrons and wave-particle interaction by two families of whistler instabilities, are shown to enable fast $T_{e\bot}$ cooling that closely tracks the mostly collisionless crash of $T_{e\Vert}$. These findings motivate both experimental validation and reexamination of a broad class of plasma cooling problems in laboratory, space, and astrophysical settings.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Steerable terahertz beams using surface waves on an active metasurface

The development of dynamic components for controlling wave fronts in the sub-terahertz region of the electromagnetic spectrum has emerged as a frontier research topic for many applications in sensing and communications. One approach which has attracted much attention involves the use of active metasurfaces, tiled arrays of sub-wavelength elements with properties that can be reconfigured via external actuation. In nearly all cases, these metasurfaces are employed as either transmissive or reflective elements, taking advantage of their strong and tunable interaction with free-space electromagnetic waves. These interactions can be significantly enhanced through the use of surface waves propagating parallel to the metasurface array, although very few studies have exploited this option. Here, we integrate a metasurface into the interior of a parallel-plate waveguide in a configuration explicitly designed to exploit this surface-wave geometry. We show that varying the electrical properties of the active metasurface changes the wave vector of the guided mode, and thereby alters the emission angle of radiation out-coupled through a leaky-wave slot aperture. These results, which are consistent with numerical simulations, represent a new approach to broadband beam steering suitable for the sub-terahertz spectral range.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Global tuning of hadronic interaction models with accelerator-based and astroparticle data

In high-energy and astroparticle physics, event generators play an essential role, even in the simplest data analyses. As analysis techniques become more sophisticated, e.g. based on deep neural networks, their correct description of the observed event characteristics becomes even more important. Physical processes occurring in hadronic collisions are simulated within a Monte Carlo framework. A major challenge is the modeling of hadron dynamics at low momentum transfer, which includes the initial and final phases of every hadronic collision. QCD-inspired phenomenological models used for these phases cannot guarantee completeness or correctness over the full phase space. These models usually include parameters which must be tuned to suitable experimental data. Until now, event generators have been developed and tuned mainly on the basis of data from high-energy physics experiments at accelerators. The wealth of data available from the latest generation of astroparticle experiments has not yet been fully exploited, and in many cases is not satisfactorily described. Both kinds of data sets are complementary as astroparticle experiments provide sensitivity especially to hadrons produced nearly parallel to the collision axis and cover center-of-mass energies up to several hundred TeV, well beyond those reached at colliders so far. In this report, we provide an overview of state-of-the-art event generators and their tuning, including the most relevant inputs from high-energy accelerator and astroparticle experiments. We present a road map that shows, for the first time, how the unified tuning of event generators with accelerator-based and astroparticle data can be performed.

Albrecht, J. [Ruhr U., Bochum, RAPP Ctr.; Ruhr U.,↗
DOE OSTI2020

Understanding resistances in capacitive deionization devices

The desalination characteristics of capacitive deionization (CDI) are significantly impacted by the cell resistance. Here we apply electrochemical impedance spectroscopy (EIS) to analyze the resistive properties of a CDI device, which include EIS measurements on a complete assembled cell (in two wire mode) and EIS measurements with additional contacts to decouple electrode/electrolyte and contact impedances (four wire mode). These measurements shed light on the interface between current collector and electrode as well as the internal capacitive and resistive elements of the cell. With two-wire and four-wire EIS measurements, we find that the often observed high-frequency arc(s) in the impedance spectra can be due to contact effects and/or an internal ionic-transfer resistance that is locally in parallel with macropore wall capacitance. In some cases, the two associated arcs in the Nyquist plot are overlapping and present simultaneously, making their identification in the EIS spectra difficult unless both two-wire and four-wire measurements are made. Despite causing a large high-frequency arc in the Nyquist plot, we find that the apparent internal ionic-transfer resistance is negligible compared to the resistances of the electrode, separator, and external electronic components. Here, an investigation of the contact impedance between the electrode and current collector reveals a parallel RC arc that can grow over time if an improper material is used (e.g., titanium). In our system, the electrode ionic resistance dominates the total Ohmic power dissipation, which has implications for scale-up of CDI systems and future improvements of cell design.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Tailorable Cellulose II Nanocrystals (CNC II) Prepared in Mildly Acidic Lithium Bromide Trihydrate (MALBTH)

Preparing cellulose II nanocrystals (CNC II) requires a polymorph transformation of natural cellulose I feedstocks. The transformation is usually achieved via a process such as mercerization or dissolution–regeneration. This study demonstrated a new method to prepare CNC II directly from bleached kraft pulp (BKP, a commercially available cellulose I feedstock) in a mildly acidic lithium bromide trihydrate (MALBTH) system, a concentrated (~61 wt%) solution of LiBr in water with a very low concentration (2.5 mM) of sulfuric acid. First, the BKP was treated in the MALBTH system to generate a cellulose II hydrolysis solid residue (CHR) with a yield of 64–86%, during which the selective hydrolysis of disordered cellulose and the polymorph transformation were completed simultaneously. Then, subsequent oxidation of the CHR by ammonium persulfate (APS, 0.1–0.6 M) resulted in the CNC II with high yield (up to 62%), high crystallinity (over 90%), rich surface carboxyl group (0.3–1.2 mmol g-1 cellulose), excellent colloidal stability (up to -59 mV zeta potential), and high thermal stability. The CNC II had a tunable length (26–57 nm), determined by the conditions of the MALBTH hydrolysis and the APS oxidation, but similar lateral dimension (8–10 nm). The characterization of the CHR by wide-angle X-ray diffraction and Fourier transform infrared spectroscopy verified the polymorphic transformation from cellulose I to II during the MALBTH treatment. The swelling of the BKP in the MALBTH enabled cellulose crystallites to slide and reassemble, which completed the rearrangement of cellulose chains from parallel to anti-parallel conformation (polymorph transformation from cellulose I to II). This study provided an efficient and green method to produce cellulose II nanocrystals with controllable aspect ratios via the simultaneous hydrolysis and polymorph transformation of cellulose I feedstocks.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2022

Controlled hydrogenation of a biomass-derived platform chemical formed by aldol-condensation of 5-hydroxymethyl furfural (HMF) and acetone over Ru, Pd, and Cu catalysts

Her we report that we studied the hydrogenation at temperatures from 313–393 K of a biomass-derived platform molecule, 5-hydroxymethyl furfural (HMF)-acetone-HMF (HAH) over Pd, Ru, and Cu based catalysts. HAH was selectively hydrogenated to produce partially-hydrogenated monomers (PHAH) over Cu and Ru catalysts and to fully-hydrogenated HAH monomers (FHAH) over the Ru catalyst. Pd based catalysts yielded a mixture of partially and fully hydrogenated monomers. Lumped reaction kinetics models were employed to quantify the kinetic behavior for hydrogenation over Ru, Cu, and Pd catalysts. The 5-step pathway exhibited over Pd and Ru catalysts consists of both series and parallel reaction steps, where HAH is both converted to fully hydrogenated products sequentially via series reactions of partially hydrogenated intermediates, as well as converted directly in parallel reactions to form the fully hydrogenated products. In contrast, the 3-step pathway over the Cu catalyst consists only of the consecutive reaction steps, where the final product was formed via series reactions of intermediate products. Additionally, reaction over the Cu catalyst did not hydrogenate the furan rings of the HAH molecule and yielded a different final product than those hydrogenation over Pd and Ru catalysts. Batch conditions are determined for each hydrogenated product that give the highest yields in both batch and plug flow reactors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Magnetism and interlayer bonding in pores of Bernal-stacked hexagonal boron nitride

When single-layer h-BN is subjected to a high-energy electron beam, triangular pores with nitrogen edges are formed. Because of the broken sp 2 bonds, these pores are known to possess magnetic states. Here, we report on the magnetism and electronic structure of triangular pores as a function of their size. Moreover, in the Bernal-stacked h-BN (AB-h-BN), multilayer pores with parallel edges can be created, which is not possible in the commonly fabricated multilayer AA'-h-BN. Given that these pores can be manufactured in a well-controlled fashion using an electron beam, it is important to understand the interactions of pores in neighboring layers. We find that in certain configurations, the edges of the neighboring pores remain open and retain their magnetism, and in others, they form interlayer bonds. We present a comprehensive report on these configurations for small nanopores. We find that at low temperatures, these pores have near degenerate magnetic configurations, and may be utilized in magnetoresistance and spintronics applications. In the process of forming larger multilayer nanopores, interlayer bonds can form, reducing the magnetization. Yet, unbonded parallel multilayer edges remain available at all sizes. Understanding these pores is also helpful in a multitude of applications such as DNA sequencing and quantum emission.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Field tunable magnetic transitions of CsCo 2 (MoO 4 ) 2 (OH): a triangular chain structure with a frustrated geometry

The sawtooth chain compound CsCo 2 (MoO 4 ) 2 (OH) is a complex magnetic system and here, we present a comprehensive series of magnetic and neutron scattering measurements to determine its magnetic phase diagram. The magnetic properties of CsCo 2 (MoO 4 ) 2 (OH) exhibit a strong coupling to the crystal lattice and its magnetic ground state can be easily manipulated by applied magnetic fields. There are two unique Co 2+ ions, base and vertex, with J bb and J bv magnetic exchange. The magnetism is highly anisotropic with the b-axis (chain) along the easy axis and the material orders antiferromagnetically at T N = 5 K. There are two successive metamagnetic transitions, the first at H c 1 = 0.2 kOe into a ferrimagnetic structure, and the other at H c 2 = 20 kOe to a ferromagnetic phase. Heat capacity measurements in various fields support the metamagnetic phase transformations, and the magnetic entropy value is intermediate between S = 3/2 and 1/2 states. The zero field antiferromagnetic phase contains vertex magnetic vectors (Co(1)) aligned parallel to the b-axis, while the base vectors (Co(2)) are canted by 34° and aligned in an opposite direction to the vertex vectors. The spins in parallel adjacent chains align in opposite directions, creating an overall antiferromagnetic structure. Further, at a 3 kOe applied magnetic field, adjacent chains flip by 180° to generate a ferrimagnetic phase. An increase in field gradually induces the Co(1) moment to rotate along the b-axis and align in the same direction with Co(2) generating a ferromagnetic structure. The antiferromagnetic exchange parameters are calculated to be J bb = 0.028 meV and J bv = 0.13 meV, while the interchain exchange parameter is considerably weaker at J ch = (0.0047/N ch ) meV. Our results demonstrate that the CsCo 2 (MoO 4 ) 2 (OH) is a promising candidate to study new physics associated with sawtooth chain magnetism and it encourages further theoretical studies as well as the synthesis of other sawtooth chain structures with different magnetic ions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Radial structure and formation of the Milky Way disc

The formation of the Galactic disc is an enthusiastically debated issue. Numerous studies and models seek to identify the dominant physical process(es) that shaped its observed properties; for example, satellite accretion, starburst, quenching, gas infall, and stellar radial migration. Taking advantage of the improved coverage of the inner Milky Way provided by the SDSS DR16 APOGEE catalogue and of the ages published in the APOGEE-AstroNN Value Added Catalogue (VAC), we examined the radial evolution of the chemical and age properties of the Galactic stellar disc with the aim of better constraining its formation. Using a sample of 199 307 giant stars with precise APOGEE abundances and APOGEE-AstroNN ages, selected in a ±2 kpc layer around the galactic plane, we assessed the dependency as a function of guiding radius of (i) the median metallicity, (ii) the ridge lines of the [Fe/H] – [Mg/Fe] and age–[Mg/Fe] distributions, and (iii) the age distribution function (ADF). The giant star sample allows us to probe the radial behaviour of the Galactic disc from R g = 0 to 14–16 kpc. The thick disc [Fe/H] – [Mg/Fe] ridge lines follow closely grouped parallel paths, supporting the idea that the thick disc did form from a well-mixed medium. However, the ridge lines present a small drift in [Mg/Fe], which decreases with increasing guiding radius. At sub-solar metallicity, the intermediate and outer thin disc [Fe/H] – [Mg/Fe] ridge lines follow parallel sequences shifted to lower metallicity as the guiding radius increases. We interpret this pattern as the signature of a dilution of the interstellar medium from R g ~ 6 kpc to the outskirts of the disc, which occurred before the onset of the thin disc formation. The APOGEE-AstroNN VAC provides stellar ages for statistically significant samples of thin disc stars from the Galactic centre up to R g ~ 14 kpc. An important result provided by this dataset is that the thin disc presents evidence of an inside-out formation up to R g ~ 10 – 12 kpc. Moreover, about ~7 Gyr ago, the [Mg/Fe] ratio in the outer thin disc (R g > 10 kpc) was higher by about ~0.03–0.05 dex than in the more internal regions of the thin disc. This could be the fossil record of a pollution of the outer disc gas reservoir by the thick disc during its starburst phase.

79 ASTRONOMY AND ASTROPHYSICS↗