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DOE OSTI2012

Experimental tests of stereological estimates of grain boundary populations

We present experimental validation of a method for estimating three-dimensional (3-D) relative numerical populations of grain boundaries from measurements of individual two-dimensional (2-D) cross-sections. Such numerical populations are relevant to network topology and the modeling of intergranular failure modes in grain boundary engineered materials, and are distinct from geometrical population measures such as area per volume. We examine 3-D reconstructions of stainless steel and copper, with varying populations of twin-related boundaries, generated by serial-section electron backscatter diffraction and high-energy X-ray diffraction microscopy. We show that 2-D length fractions, 2-D number fractions and 3-D number fractions are all distinct quantities when grain boundary type is correlated with grain boundary size. We also demonstrate that the last quantity may be reliably inferred from the first two, provided the experimental spatial resolution is much finer than the grain size, eliminating the need to use 3-D experimental methods to access at least some information about 3-D network properties. Many of the {Sigma}3 boundaries are extremely complex, with highly re-entrant shapes that can intersect a sample plane many times, giving a false impression of multiple separate boundaries.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Direct observation of distinct bulk and edge nonequilibrium spin accumulation in ultrathin MoTe 2

Low-symmetry two-dimensional (2D) topological materials such as MoTe 2 host efficient charge-to-spin conversion (CSC) mechanisms that can be harnessed for novel electronic and spintronic devices. However, the nature of the various CSC mechanisms and their correlation with underlying crystal symmetries remain unsettled. In this work, we use local spin-sensitive electrochemical potential measurements to directly probe the spatially dependent nonequilibrium spin accumulation in MoTe 2 flakes down to four atomic layers. We are able to clearly disentangle contributions originating from the spin Hall and Rashba-Edelstein effects and uncover an abundance of unconventional spin polarizations that develop uniquely in the sample bulk and edges with decreasing thickness. Using ab-initio calculations, we construct a unified understanding of all the observed CSC components in relation to the material dimensionality and stacking arrangement. Our findings not only illuminate previous CSC results on MoTe 2 but also have important ramifications for future devices that can exploit the local and layer-dependent spin properties of this 2D topological material.

Science & Technology - Other Topics↗

DOE OSTI2020

$t_1$-Noise eliminated dipolar heteronuclear multiple-quantum coherence solid-state NMR spectroscopy

Heteronuclear correlation (HETCOR) spectroscopy is one of the key tools in the arsenal of the solid-state NMR spectroscopist to probe chemical and spatial proximities between two different nuclei and enhance spectral resolution. Dipolar heteronuclear multiple-quantum coherence (D-HMQC) is a powerful technique that can be potentially utilized to obtain 1 H detected 2D HETCOR solid-state NMR spectra of any NMR active nucleus. A long-standing problem in 1 H detected D-HMQC solid-state NMR experiments is the presence of t 1 -noise which reduces sensitivity and impedes spectral interpretation. In this contribution, we describe novel pulse sequences, termed t 1 -noise eliminated (TONE) D-HMQC, that minimize t 1 -noise and can provide higher sensitivity and resolution than conventional D-HMQC. Monte-Carlo and numerical simulations confirm that t 1 -noise in conventional D-HMQC primarily occurs because random MAS frequency fluctuations cause variations in the NMR signal amplitude from scan to scan, leading to imperfect cancellation of uncorrelated signals by phase cycling. The TONE D-HMQC sequence uses 1 H π-pulses to refocus the evolution of 1 H CSA across each SR4 2 1 recoupling block, improving the stability of the pulse sequence to random MAS frequency fluctuations. The 1 H refocusing pulses also restore the orthogonality of in-phase and anti-phase magnetization for all crystallite orientations at the end of each recoupling block, enabling the use of 90° flip-back or LG spin-lock trim pulses to reduce the intensity of uncorrelated signals. We demonstrate the application of these methods to acquire 1 H detected 2D 1 H{ 35 Cl} and 1 H{ 13 C} HETCOR spectra of histidine·HCl·H 2 O with reduced t 1 -noise. To show generality, we also apply these methods to obtain 2D 1 H{ 17 O} spectra of 20%- 17 O fmoc-alanine and for the first time at natural abundance, 2D 1 H{ 25 Mg} HETCOR spectra of magnesium hydroxide. The TONE D-HMQC sequences are also used to probe 1 H– 25 Mg and 1 H– 27 Al proximities in Mg–Al layered double hydroxides and confirm the even mixing of Mg and Al in these materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Fast reconstruction of a bounded ultrasonic beam using acoustically induced piezo-luminescence

We report on the conversion of ultrasound into light by the process of piezo-luminescence in epoxy with embedded BaSi{sub 2}O{sub 2}N{sub 2}:Eu as active component. We exploit this acoustically induced piezo-luminescence to visualize several cross-sectional slices of the radiation field of an ultrasonic piston transducer (f = 3.3 MHz) in both the near-field and the far-field. Simply combining multiple slices then leads to a fast representation of the 3D spatial radiation field. We have confronted the luminescent results with both scanning hydrophone experiments and digital acoustic holography results, and obtained a good correlation between the different approaches.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Effect of insulator surface conditioning on the pinch dynamics and x-ray production of a Ne-filled dense plasma focus

The dense plasma focus (DPF) can be an intense source of x rays, wherein the insulator sleeve strongly dictates the electrical breakdown, which subsequently affects the formation of a plasma sheath and a collapse phase. Experiments on a 25 kJ DPF (operated at 4.4 kJ) are carried out to demonstrate the influence of insulator surface morphology on the pinch structure, dynamics, and x-ray yield using a Ne fill. Two borosilicate insulators are directly compared, one with a smooth finish and the other machined with four circumferential grooves traversing the perimeter of the exterior insulator surface. Comparisons are made through same-shot imaging diagnostics of the evolving plasma sheath during breakdown, rundown, and at the pinch in addition to the time-resolved measurements of emitted x rays via filtered photodiodes. The presence of structures on the insulator sleeve reduces x-ray production across all fill pressures by a factor of 2.8 ± 2.4 on average and reduces the highest x ray producing shots by a factor of 5. ± 1.8. Observations of sheath asymmetry and inhomogeneity at lift-off are observed and correlated with subsequent observations of off-axis radial collapse. Taken together, this suggests that local variations in the insulator surface decrease the spatial uniformity of the sheath, leading to an azimuthally asymmetric focus, reduced electron densities, and, ultimately, degraded x-ray production.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2012

THE BARYON CENSUS IN A MULTIPHASE INTERGALACTIC MEDIUM: 30% OF THE BARYONS MAY STILL BE MISSING

Although galaxies, groups, and clusters contain {approx}10% of the baryons, many more reside in the photoionized and shocked-heated intergalactic medium (IGM) and in the circumgalactic medium (CGM). We update the baryon census in the (H I) Ly{alpha} forest and warm-hot IGM (WHIM) at 10{sup 5-6} K traced by O VI {lambda}1032, 1038 absorption. From Enzo cosmological simulations of heating, cooling, and metal transport, we improve the H I and O VI baryon surveys using spatially averaged corrections for metallicity (Z/Z {sub Sun }) and ionization fractions (f {sub HI}, f {sub OVI}). Statistically, the O VI correction product correlates with column density, (Z/Z {sub Sun })f {sub OVI} Almost-Equal-To (0.015)(N {sub OVI}/10{sup 14} cm{sup -2}){sup 0.70}, with an N {sub OVI}-weighted mean of 0.01, which doubles previous estimates of WHIM baryon content. We also update the Ly{alpha} forest contribution to baryon density out to z = 0.4, correcting for the (1 + z){sup 3} increase in absorber density, the (1 + z){sup 4.4} rise in photoionizing background, and cosmological proper length dl/dz. We find substantial baryon fractions in the photoionized Ly{alpha} forest (28% {+-} 11%) and WHIM traced by O VI and broad-Ly{alpha} absorbers (25% {+-} 8%). The collapsed phase (galaxies, groups, clusters, CGM) contains 18% {+-} 4%, leaving an apparent baryon shortfall of 29% {+-} 13%. Our simulations suggest that {approx}15% reside in hotter WHIM (T {>=} 10{sup 6} K). Additional baryons could be detected in weaker Ly{alpha} and O VI absorbers. Further progress requires higher-precision baryon surveys of weak absorbers, down to minimum column densities N {sub HI} {>=} 10{sup 12.0} cm{sup -2}, N {sub OVI} {>=} 10{sup 12.5} cm{sup -2}, N {sub OVII} {>=} 10{sup 14.5} cm{sup -2}, using high signal-to-noise data from high-resolution UV and X-ray spectrographs.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Isospin 0 and 2 two-pion scattering at physical pion mass using all-to-all propagators with periodic boundary conditions in lattice QCD

A study of two-pion scattering for the isospin channels, 𝐼 = 0 and 𝐼 = 2, using lattice QCD is presented. Möbius domain-wall fermions, on top of the Iwasaki-DSDR gauge action for gluons with periodic boundary conditions, are used for the lattice computations, which are carried out on two ensembles of gauge field configurations generated by the RBC and UKQCD Collaborations with physical masses, inverse lattice spacings of 1.023 and 1.378 GeV, and spatial extents of 𝐿 = 4.63 and 4.58 fm, respectively. The all-to-all propagator method is employed to compute a matrix of correlation functions of two-pion operators. The generalized eigenvalue problem (GEVP) is solved for a matrix of correlation functions to extract phase shifts with multiple states—two pions with a nonzero relative momentum, as well as two pions at rest. Our results for phase shifts for both the 𝐼 = 0 and 𝐼 = 2 channels are consistent with the Roy equation and chiral perturbation theory, though at this preliminary stage our errors for 𝐼 = 0 are large. An important outcome of this work is that we are successful in extracting two-pion excited states, which are useful for studying 𝐾 → 𝜋⁢𝜋 decay, on physical-mass ensembles using the GEVP.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2013

Multiple transient memories in sheared suspensions: Robustness, structure, and routes to plasticity

Multiple transient memories, first discovered in charge-density-wave conductors, are a remarkable and initially counterintuitive example of how a system can store information about its driving. In this class of memories, a system can learn multiple driving inputs, nearly all of which are eventually forgotten despite their continual input. If sufficient noise is present, the system regains plasticity so that it can continue to learn new memories indefinitely. Recently, Keim and Nagel [Phys. Rev. Lett. 107, 010603 (2011)] showed how multiple transient memories could be generalized to a generic driven disordered system with noise, giving as an example simulations of a simple model of a sheared non-Brownian suspension. Here, we further explore simulation models of suspensions under cyclic shear, focusing on three main themes: robustness, structure, and overdriving. We show that multiple transient memories are a robust feature independent of many details of the model. The steady-state spatial distribution of the particles is sensitive to the driving algorithm; nonetheless, the memory formation is independent of such a change in particle correlations. Finally, we demonstrate that overdriving provides another means for controlling memory formation and retention.

42 ENGINEERING↗

DOE OSTI2026

Linking Domain Structure Evolution at a Grain Boundary to Piezoelectric Response via Nano‐Diffraction

Electric-field-induced domain structure switching in a 1 𝜇⁢m -thick Pb 0.99 (Zr 0.45 Ti 0.55 ) 0.98 Nb 0.02 O 3 (Nb-doped PZT) bicrystal film was characterized in situ via nano-focused synchrotron diffraction. The epitaxial film was deposited on a (100) SrTiO 3 bicrystal substrate. The changes in domain structure were mapped within a 5 𝜇⁢m × 5 𝜇⁢m area at and around an in-plane tilt-type (23.6°) grain boundary with 50 nm spatial resolution. Rocking curves collected at each point of the mapped area provided the ability to reconstruct spatially-varying three-dimensional (3D) reciprocal space maps around the grain boundary. The 3D reciprocal space maps reveal how different tilted 𝑎 -type domain variants interact with the grain boundary as a function of increasing electric field. Initially, a subset of 𝑎 -type domain variants with their polarization vectors largely orthogonal to the grain boundary were found in greater abundance within 570 nm of the grain boundary, possibly due to X-ray beam-induced local increases in the electrical conductivity, but after the coercive field was exceeded, reconfiguration of the ferroelastic domains was observed. The spatially-varying reciprocal space maps also facilitated evaluation of the strain field across the mapped area, along with 𝑑 33,𝑓 . Significant spatial heterogeneity of strain and 𝑑 33,𝑓 are observed, especially at the coercive field, which was attributed to maintaining deformation compatibility and correlated ferroelastic switching.

36 MATERIALS SCIENCE↗

DOE OSTI2016

SU-G-JeP1-13: Innovative Tracking Detector for Dose Monitoring in Hadron Therapy: Realization and Monte Carlo Simulations

Purpose: Development of strategies to monitor range uncertainties is necessary to improve treatment planning in Charged Particle Therapy (CPT) and fully exploit the advantages of ion beams. Our group developed (within the framework of the INSIDE project funded by the Italian research ministry) and is currently building a compact detector Dose Profiler (DP) able to backtrack charged secondary particles produced in the patient during the irradiation. Furthermore we are studying monitoring strategy exploiting charged secondary emission profiles to control the range of the ion beam. Methods: This contribution reports on the DP detector design and construction status. The detector consists of a charged secondary tracker composed of scintillating fiber layers and a LYSO calorimeter for particles energy measurement.The detector layout has been optimized using the FLUKA Monte Carlo (MC) simulation software. The simulation of a 220 MeV Carbon beam impinging on a PMMA target has been performed to study the detector response, exploiting previous secondary radiation measurements performed by our group. The emission profile of charged secondary particles was reconstructed backtracking the particles to their generation point to benchmark the DP performances. Results: The DP construction status, including the technological details will be presented. The feasibility of range monitoring with DP will be demonstrated by means of MC studies. The correlation of the charged secondary particles emission shape with the position of the Bragg peak (BP) will be shown, as well as the spatial resolution achievable on the BP position estimation (less than 3 mm) in the clinical like conditions. Conclusion: The simulation studies supported the feasibility of an accurate range monitoring technique exploiting the use of charged secondary fragments emitted during the particle therapy treatment. The DP experimental tests are foreseen in 2016, at CNAO particle therapy center in Pavia.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2014

Drifty shifty deluxe.m

Performs a cross-correlation calculation to align images. This is particularly useful for aligning frames of a movie so that an object of interest does not spatially drift. For in situ microscopy experiments. Movies are collected where an object changes with time. At the same time, the object usually drifts too. This shifts the movie frames so that the object is aligned from frame to frame. Then it is easy to see the object changes without the added complication of it moving too.

Josh Sugar, DaveRobinson↗

DOE OSTI2026

Quantum correlation imaging via X-ray parametric down-conversion

Quantum imaging leverages correlations between pairs of photons and has the potential to obtain image information beyond what classical sources provide. Extending this approach to the X-ray regime has been limited by low photon-pair generation rates and the lack of suitable detectors. Here, we demonstrate X-ray coincidence imaging using spontaneous parametric down-conversion (SPDC) and a pixelated area detector with time- and energy-resolved capabilities. This configuration enables simultaneous detection of correlated X-ray photon pairs and coincidence-based imaging of test objects, including a biological specimen. The increased coincidence rate and spatially resolved detection establish a basis for future quantum-enhanced and low-dose X-ray imaging.

Goodrich, Justin C. [Brookhaven National Laborator↗

DOE OSTI2023

Entrainment and aerosol effects on marine boundary-layer clouds: An investigation using ACE-ENA data from HOLODEC, G1, Pico and ACTOS (Final Report on Project Activities)

Marine boundary-layer clouds cover large regions of the globe and are known to strongly influence radiative balances. The microphysical properties and persistence of these clouds are tightly coupled with cloud-top entrainment and aerosol properties within both the boundary layer and the overlying free troposphere. This work addressed the microphysical response to entrainment and aerosol properties in marine stratocumulus clouds, using data from the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) project. Specifically, emphasis was placed on 1. extensive in situ measurements taken with the Atmospheric Radiation Measurement (ARM) G1 aircraft using the Holographic Detector for Clouds (Holodec) instrument; 2. airborne measurements obtained with the helicopter-borne Airborne Cloud Turbulence Observation System (ACTOS) operated by the Leibniz Institute for Tropospheric Research (TROPOS) during the first phase of ACE-ENA; and 3. above-boundary-layer, mountain-top measurements taken at the Pico Mountain Observatory (OMP) by the research group of the co-investigator and scientists from TROPOS during the first phase of ACE-ENA. The work is aligned with the topic “Warm Boundary-Layer Atmospheric Processes.” Key results include the following. Data from the Holographic Detector for Clouds (Holodec) were reprocessed, refined, and validated through a careful instrument intercomparison, resulting in a high-quality dataset available on the ARM archive for ACE-ENA. High-resolution ACTOS measurements of thermodynamics, microphysical, and turbulence properties were analyzed to explore the behavior of the entrainment velocity at cloud top. Analysis of the vertical variability of cloud droplet size distribution shape suggests that mixing is more inhomogeneous near cloud top, and more homogeneous deeper into the cloud. Analysis of aerosol measurements from OMP explored the mixing state and cloud condensation nucleus properties, as well as the implications for radiative forcing. Finally, a machine learning algorithm was developed for identifying characteristic cloud droplet size distributions, and was employed to explore microphysical regimes in stratocumulus clouds observed during ACE-ENA. The characteristic size distributions are narrow, and only when spatially averaged do they produce the broad “gamma” distributions typically assumed in models. This implies that precipitation development should account for variability and correlations in the distribution shape as well as the number concentration of cloud droplets.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Multidimensional Coherent Spectroscopy of van der Waals materials and heterostructures (Final Technical Report)

This project advanced multidimensional coherent spectroscopy (MDCS) and related spectroscopic-imaging methods as quantitative probes of many-body optical excitations in two-dimensional (2D) van der Waals (vdW) semiconductors and their heterostructures. Monolayer transition-metal dichalcogenides (TMDs) such as MoSe 2 and WSe 2 provide a uniquely strong platform for excitonic physics due to reduced dielectric screening, which enhances Coulomb interactions and makes higher-order correlated states (e.g., biexcitons and exciton–trion correlations) more prominent than in conventional bulk semiconductors. At the same time, the same sensitivity that enables strong interactions also increases susceptibility to spatial inhomogeneity—e.g., strain gradients, wrinkles, nanoscale disorder potentials, and charge puddling—which can broaden resonances, obscure interaction signatures, and complicate device-to-device reproducibility. The work reported here addressed this dual opportunity and challenge by: (i) developing and deploying coherent multidimensional methods (including double-quantum MDCS) capable of isolating interaction signals with reduced background, (ii) integrating electrostatic control to tune carrier populations and interaction strengths in situ, and (iii) introducing complementary spatially resolved photoluminescence (PL) techniques—hyperspectral PL imaging and polarization-/field-dependent PL lineshape analysis—to directly quantify disorder, strain, and localization that govern the coherent response.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Fifty ways to build a deuteron: a variational calculation of two-nucleon systems

A variational study of two-nucleon systems with lattice quantum chromodynamics is performed using a wide range of interpolating operators: dibaryon operators built from products of momentum-projected nucleons, hexaquark operators built from six spatially localized quarks, and quasi-local operators inspired by two-nucleon bound-state wavefunctions in nuclear effective field theories. Correlation-function matrices involving products of these operators are constructed by computing timeslice-to-all quark propagators with sparsening techniques. Comparisons between results obtained using the same gauge-field ensemble but different interpolating-operator sets demonstrate that interpolating-operator dependence can lead to significant effects on the two-nucleon energy spectra obtained using both variational and non-variational methods.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2025

Topological phase transition to a hidden charge density wave liquid

Charge density waves (CDWs), electronic crystals that form within a host solid, have long been speculated to melt into a spatially textured electronic liquid. Though they have not been previously detected, liquid CDWs may nonetheless be fundamental to the phase diagrams of many correlated electron systems, including high temperature superconductors and quantum Hall states. In one of the most promising candidate materials capable of hosting a liquid CDW, 1T-TaS2, a structural phase transition impedes its observation. Here, by irradiating the material with a femtosecond light pulse, we circumvent the structural phase transition to reveal how topological defect dynamics govern the otherwise invisible CDW correlations. Upon photoexcitation, the CDW diffraction peaks broaden azimuthally, initially revealing a hexatic state. At higher temperatures, photoexcitation completely destroys translational and orientational order and only a ring of diffuse scattering is observed, a key signature of a liquid CDW. Our work provides compelling evidence for a defect-unbinding transition to a CDW liquid and presents a protocol for uncovering states that are hidden by other transitions in thermal equilibrium.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

Drifty shifty deluxe.m

Josh Sugar, Dave Robinson↗

DOE OSTI2025

Integrating Contaminant Source Indicators, Water Quality Measures, and Ecotoxicity to Characterize Contaminant Mixtures and Per- and Polyfluoroalkyl Substance (PFAS) Variability in an Urban Watershed

Thousands of chemical contaminants threaten watersheds but are time and cost prohibitive to monitor. Identifying their sources, transport, and ecological risk is limited in heterogeneous urban watersheds. We present an integrative watershed approach using source-specific indicator compounds, common water quality measures, and ecotoxicity assays to examine the distribution of contaminant mixtures in an urbanized watershed. Indicator compound concentrations were temporally and spatially distributed for treated/untreated sewage (sucralose, artificial sweetener), road runoff (diphenyl-guanidine [DPG] and 6PPD-quinone [6PPD-Q], automobile tire additives), and lawncare runoff (aminomethanephosphonic acid (AMPA), major degradant of the herbicide glyphosate). Sucralose was predominately sourced from treated wastewater; measurable concentrations in tributaries indicated raw sewage inputs. DPG and 6PPD-Q concentrations correlated to road density during base flow and were elevated during stormflow. AMPA was measurable spring through fall, especially where lawns were dense. When specific sources dominated flow, water quality measures correlated with wastewater (sulfate, potassium, chloride, and sodium) and road runoff (chromium and lead) indicators. The limited behavioral toxicity observed in exposed zebrafish (Danio rerio) (18%) was not well explained by source-indicators. PFAS concentrations were highly variable spatially but not well explained by our source-specific indicator compounds. Here, more costly compound-specific monitoring may be necessary when multiple sources exist or when unexpected toxicity trends occur.

computer simulations↗