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DOE OSTI2023

Effects of rejuvenation modes on the microstructures and mechanical properties of metallic glasses

This study systematically investigates the effects of three rejuvenation modes, namely biaxial loading, thermal pressure loading, and cryogenic thermal cycling, on the microstructures and mechanical properties of Cu 64 Zr 36 metallic glasses (MGs) using molecular dynamics (MD) simulations. The simulation results demonstrate that biaxial tension application during loading results in a rejuvenated glassy state with high strength. Specifically, we find that the yield stress, Young's modulus, and shear modulus of the rejuvenated glass obtained by biaxial tensile loading decreased by 2.8%, 2.1%, and 2.7%, respectively, compared to an as-cast MG reference. We also find that MGs achieve the greatest degree of rejuvenation, at the expense of strength, with the use of thermal pressure loading. Interestingly, the application of cryogenic thermal cycling results in a rejuvenated state with a lower strength drop compared to thermal pressure loading. Furthermore, analysis of the potential energy and medium-range-order (MRO) size indicates that the microstructures of MGs achieves a high-energy ordered glass state after thermal pressure loading, but a high-energy disordered glass state after biaxial tensile loading and cryogenic thermal cycling. Furthermore, these findings provide meaningful insights into the effect of rejuvenation modes on the microstructures and mechanical properties of MGs, as well as useful guidelines for designing MGs with high strength and superior plasticity for prospective applications in industry.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Doppler Lidar Measurements of Wind Variability and LLJ Properties in Central Oklahoma during the August 2017 Land–Atmosphere Feedback Experiment

Abstract Low-level jets (LLJs) are an important nocturnal source of wind energy in the U.S. Great Plains. An August 2017 lidar-based field-measurement campaign [the Land–Atmosphere Feedback Experiment (LAFE)] studied LLJs over the central SGP site in Oklahoma and found nearly equal occurrences of the usual southerly jets and postfrontal northeasterly jets—typically rare during this season—for an opportunity to compare the two types of LLJs during this month. Southerly winds were stronger than the northeasterlies by more than 4 m s −1 on average, reflecting a significantly higher frequency of winds stronger than 12 m s −1 . The analysis of this dataset has been expanded to other SGP Doppler-lidar sites to quantify the variability of winds and LLJ properties between sites of different land use. Geographic variations of winds over the study area were noted: on southerly wind nights, the winds blew stronger at the highest, westernmost sites by 2 m s −1 , whereas on the northeasterly flow nights, the easternmost sites had the strongest wind speeds. Lidar measurements at 5 sites during August 2017, contrasted to the 2016–21 summertime data, revealed unusual wind and LLJ conditions. Temporal hodographs using hourly averaged winds at multiple heights revealed unorganized behavior in the turbulent stable boundary layer (SBL) below the jet nose. Above the nose, some nights showed veering qualitatively similar to inertial oscillation (IO) behavior, but at amplitudes much smaller than expected for an IO, whereas other nights showed little veering. Vertical hodographs had a linear shape in the SBL, indicating little directional shear there, and veering above, resulting in a hook-shaped hodograph with height. Significance Statement Doppler-lidar measurements at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) were used to quantify the variability of winds and low-level jet (LLJ) properties between five sites of different land use and wind regimes across this area. Knowledge of wind and LLJ structure and dynamics is important for many applications, and strong southerly LLJ winds at night are an important resource for wind energy. The analysis of multiyear (2016–21) summertime LLJ parameters provided insight into the LLJ climatology in this part of the Great Plains.

Meteorology & Atmospheric Sciences↗

DOE OSTI2025

Electroplated Polymer‐Modified Carbon Fiber for Performance‐Enhancing Composite Interfaces

Carbon fiber composite performance relies on the fiber-matrix interface for effective load transfer. To enhance interfacial properties between the fiber and matrix, often carbon fiber surfaces are oxidatively and covalently modified to incorporate chemical functional groups. By contrast, here, noncovalent electrodeposition of functional polyelectrolyte is applied onto conducting carbon fibers from aqueous solutions. A natural polymer, chitosan (CS), is electro-deposited onto the fiber surface, which undergoes multi-scale physical interactions. The bound CS layer with abundant amine functionalities reacts with epoxy moieties within the matrix to improve the interfacial properties. The scalable and energy-efficient electrodeposition eliminates traditional functionalization and sizing requirements of carbon fiber while delivering significantly higher mechanical performance with enhanced consistency. For continuous fiber reinforced composites, compared to conventional fibers, apparent interlaminar shear strength increases by 27%, reaching ≈86 MPa. The short fiber composites with only 2–11 wt.% fibers exhibit ≈20% increase in tensile strength with a peak performance of 120 MPa. Unlike traditionally treated and sized carbon fiber, this approach delivers coated fibers with long shelf-life and allows recovery of both CS in electrolyte form and carbon fiber by continuous electrochemical processing of the modified fibers with inverse polarity; thus, it promotes overall fiber recyclability.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Self-Assembly of a Triblock Copolymer in the Presence of a Rigid Conjugated Polyelectrolyte

The properties of conducting polymers are strongly influenced by structural changes induced by long-range order, which can be achieved by using block copolymers that self-assemble into crystalline structures. These blends result in unique mesophases distinct from the pure components with self-assembly behavior modulated by solution conditions and polymer architectures. High-throughput small-angle X-ray scattering data of aqueous Pluronic P123 (PEO 20 –PPO 70 –PEO 20 ) and conjugated polyelectrolyte poly[3-(potassium-4-butanoate) thiophene-2,5-diyl] (PPBT) blends at various concentrations and temperatures were automatically classified into phase maps by autophasemap, an unsupervised statistical analysis algorithm. The outlined phase boundaries revealed that adding PPBT to high P123 concentrations induced a transition from cubicly ordered spherical micelles to hexagonally packed cylindrical micelles. Shear alignment via rheological small-angle neutron scattering of the blends produced monolithic oriented cubic and hexagonal crystal gels. Furthermore, these insights into the self-assembly of conductive polymer blends will aid in the design of soft materials with tunable structural and electronic properties.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Measurement of flow properties coupled to experimental and numerical analyses of dense, granular flows for solar thermal energy storage

Granular flows of sintered bauxite proppants were researched along an inclined plane for solar thermal energy storage applications. Granular flow properties needed to drive numeric granular models were measured for improved numerical model predictions for Carbobead CP 50/140, 40/100, and 30/60 particles. Particle shape and size distributions were determined by coupling optical microscopy to an in-house image processing algorithm. The impulse excitation technique was used to measure elastic and shear moduli, and compute Poisson’s ratio. The coefficient of static sliding friction was measured using the slip-stick method, and the static rolling friction was determined from measured shear on particles positioned between two hot-pressed plates. The coefficient of restitution was measured by dropping particles on a surface and determining the kinetic energy before and after impact with the surface using high resolution particle tracking velocimetry. Particle size did not significantly impact the coefficients of restitution and static rolling friction, however, particle shape distribution resulted in a large variation in measurements. An inclined flow experiment was performed to characterize granular flows of Carbobead CP 30/60 particles using particle image velocimetry. Numerical models of the experiment using discrete element method were generated with the measured mechanical properties as inputs for comparison with experimental results. A constant directional torque rolling friction model best predicted bulk granular flow behavior. Furthermore, good agreement between the model and experiment was achieved at ambient, steady state conditions, with average velocity differences <10%.

14 SOLAR ENERGY↗

DOE OSTI2020

Internal short circuit and failure mechanisms of lithium-ion pouch cells under mechanical indentation abuse conditions: An experimental study

Electromechanical structural integrity and thermal stability dictate the safety performance of lithium-ion batteries. Progressive deformation and failure across microscopic and macroscopic lengths scales that are responsible for internal short circuit (ISC) in lithium-ion cells under mechanical abuse conditions remains elusive. In this study, a series of indentation tests were conducted on lithium-ion cells with different capacities up to the occurrence of ISC. The external response and internal configuration of these cells were investigated. It is discovered that cells with different capacities and state of charges exhibited different behaviors. Maximum temperature, which is often regarded as the most important parameter related to thermal runaway (TR), varied considerably due to the complicated contact configurations. X-ray computed tomography (XCT) showed that ISC was a collective result of shear band or other strain-localization modes in the electrode assembly, shear offsets in the granular coatings of electrodes, and the accompanying ductile fracture in the metal foils. We believe that the irregular strain-localization modes (kinks, cusps, and buckles), radical mismatches in mechanical properties of different layers, and geometric features of the indenter eventually lead to the tearing/puncture of cell separator at various locations. Furthermore, the results could provide useful guidance for the micromechanical modeling of lithium-ion cells.

25 ENERGY STORAGE↗

DOE OSTI2022

Dark Energy Survey Year 3 results: galaxy clustering and systematics treatment for lens galaxy samples

ABSTRACT In this work, we present the galaxy clustering measurements of the two DES lens galaxy samples: a magnitude-limited sample optimized for the measurement of cosmological parameters, maglim, and a sample of luminous red galaxies selected with the redmagic algorithm. maglim/redmagic sample contains over 10 million/2.5 million galaxies and is divided into six/five photometric redshift bins spanning the range z ∈ [0.20, 1.05]/z ∈ [0.15, 0.90]. Both samples cover 4143 $\deg ^2$ over which we perform our analysis blind, measuring the angular correlation function with an S/N ∼ 63 for both samples. In a companion paper, these measurements of galaxy clustering are combined with the correlation functions of cosmic shear and galaxy–galaxy lensing of each sample to place cosmological constraints with a 3 × 2pt analysis. We conduct a thorough study of the mitigation of systematic effects caused by the spatially varying survey properties and we correct the measurements to remove artificial clustering signals. We employ several decontamination methods with different configurations to ensure the robustness of our corrections and to determine the systematic uncertainty that needs to be considered for the final cosmology analyses. We validate our fiducial methodology using lognormal mocks, showing that our decontamination procedure induces biases no greater than 0.5σ in the (Ωm, b) plane, where b is the galaxy bias.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Prediction of Aluminum to Steel RSW Joint Failure (CRADA 405)

General Motors, LLC has developed a resistance spot welding process to join aluminum sheet to steel for body-in-white manufacturing. Efforts to develop the process for any one joint configuration (combination of alloy and thicknesses) is intensive. To aid in process understanding and eventual reduction in process development efforts, an initiative was created to develop an finite element model of the various destructive test configurations (lap shear, cross-tension, and coach peel) to help predict the failure mode and load displacement curves under tensile testing. This report describes the finite element modeling approach, the means by which local material properties were determined, as well as model validation and refinement efforts.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Dynamic Bottlebrush Polymer Networks: Self-Healing in Super-Soft Materials

Here, we introduce a design strategy to expand the range of accessible mechanical properties in covalent adaptable networks (CANs) using bottlebrush polymer building blocks. Well-defined bottlebrush polymers with rubbery poly(4-methylcaprolactone) side-chains were crosslinked in formulations that include a bislactone and strong Lewis acid (tin ethylhexanoate). The resulting materials exhibit tunable stress relaxation rates at elevated temperatures (160–180 °C) due to dynamic ester crosslinks that undergo transesterification with residual hydroxy groups. Varying the crosslinker loading or bottlebrush backbone degree of polymerization yields predictable low-frequency shear moduli ca. 10–100 kPa, well below values typical of linear polymer CANs (1 MPa). These extensible networks can be stretched to strains as large as 350% before failure and undergo efficient self-healing to recover >85% of their original toughness upon repeated fracture and melt processing. In summary, molecular architecture creates new opportunities to tailor the mechanical properties of CANs in ways that are otherwise difficult to achieve.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Microstructure and mechanical properties of nanoscale Cu/(Ta50Nb25Mo25) multilayers

Nanoscale Cu/(Ta50Nb25Mo25) multilayers comprised of medium entropy alloy Ta50Nb25Mo25 and pure Cu are found to exhibit similar length-scale-dependent deformation mechanisms as metallic multilayers with elemental individual layers, i.e., confined layer slip at layer thickness of tens of nanometers and shear localization at several nanometers. The hardness of the nanoscale Cu/(Ta50Nb25Mo25) multilayers is higher as compared to the pure element FCC/BCC multilayers due to the extra solid solution strengthening contribution in the BCC layer. The synergy between the size effect and solid solution strengthening mechanism is discussed. In conclusion, this is an early report of the multi-component multilayers, which serves to provide directions for developing novel multilayer materials.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Bond clusters control rupture force limit in shear loaded histidine-Ni 2+ metal-coordinated proteins

Dynamic noncovalent interactions are pivotal to the structure and function of biological proteins and have been used in bioinspired materials for similar roles. Metal-coordination bonds, in particular, are especially tunable and enable control over static and dynamic properties when incorporated into synthetic materials. Despite growing efforts to engineer metal-coordination bonds to produce strong, tough, and self-healing materials, the systematic characterization of the exact contribution of these bonds towards mechanical strength and the effect of geometric arrangements is missing, limiting the full design potential of these bonds. In this work, we engineer the cooperative rupture of metal-coordination bonds to increase the rupture strength of metal-coordinated peptide dimers. Utilizing all-atom steered molecular dynamics simulations on idealized bidentate histidine-Ni 2+ coordinated peptides, we show that histidine-Ni 2+ bonds can rupture cooperatively in groups of two to three bonds. We find that there is a strength limit, where adding additional coordination bonds does not contribute to the additional increase in the protein rupture strength, likely due to the highly heterogeneous rupture behavior exhibited by the coordination bonds. Further, we show that this coordination bond limit is also found natural metal-coordinated biological proteins. Using these insights, we quantitatively suggest how other proteins can be rationally designed with dynamic noncovalent interactions to exhibit cooperative bond breaking behavior. Altogether, this work provides a quantitative analysis of the cooperativity and intrinsic strength limit for metal-coordination bonds with the aim of advancing clear guiding molecular principles for the mechanical design of metal-coordinated materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Ion Transport and Mechanical Properties of Non-Crystallizable Molecular Ionic Composite Electrolytes

Polymer electrolytes show promise as alternatives to conventional electrolytes in energy storage and conversion devices but have been limited due to their inverse correlation between ionic conductivity and modulus. In this study, we examine surface morphology, linear viscoelastic, dielectric and diffusive properties of molecular ionic composites (MICs), materials produced through the combination of a rigid and charged double helical polymer, known as poly(2,2’)-disulfonyl-4,4’benzidine terepthalamide (PBDT), with ionic liquids (ILs). To probe temperature extremes, we incorporate a non-crystallizable IL to allow measurements from to -90 to 200°C. As we increase PBDT weight percentage (wt%), shear moduli increase and do not decay up to 200°C while maintaining room temperature ionic conductivity within a factor of two of the neat IL. We connect diffusion coefficients of IL ions with ionic conductivity through the Haven ratio across a wide temperature range and analyze trends in ion transport based on a relatively high and composition-dependent static dielectric constant. This behavior may result from collective rearrangement of IL ions in these networks. We propose that these properties are driven by a two-phase system in MICs corresponding to IL-rich “puddles” and PBDT-IL associated “bundles” where IL ions form alternating sheaths of cations and anions around each PBDT rod. Furthermore, these polymer-based MIC electrolytes show great promise for use in electrochemical devices that require fast ion transport, high modulus, and a broad thermal window.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Dark Energy Survey Year 3 results: Exploiting small-scale information with lensing shear ratios

Using the first three years of data from the Dark Energy Survey (DES), we use ratios of small-scale galaxy-galaxy lensing measurements around the same lens sample to constrain source redshift uncertainties, intrinsic alignments and other systematics or nuisance parameters of our model. Instead of using a simple geometric approach for the ratios as has been done in the past, we use the full modeling of the galaxy-galaxy lensing measurements, including the corresponding integration over the power spectrum and the contributions from intrinsic alignments and lens magnification. We perform extensive testing of the small-scale shear-ratio (SR) modeling by studying the impact of different effects such as the inclusion of baryonic physics, nonlinear biasing, halo occupation distribution descriptions and lens magnification, among others, and using realistic N -body simulations of the DES data. We validate the robustness of our constraints in the data by using two independent lens samples with different galaxy properties, and by deriving constraints using the corresponding large-scale ratios for which the modeling is simpler. The results applied to the DES Y3 data demonstrate how the ratios provide significant improvements in constraining power for several nuisance parameters in our model, especially on source redshift calibration and intrinsic alignments. For source redshifts, SR improves the constraints from the prior by up to 38% in some redshift bins. Such improvements, and especially the constraints it provides on intrinsic alignments, translate to tighter cosmological constraints when shear ratios are combined with cosmic shear and other 2pt functions. In particular, for the DES Y3 data, SR improves S 8 constraints from cosmic shear by up to 31%, and for the full combination of probes ( 3 × 2 pt ) by up to 10%. The shear ratios presented in this work are used as an additional likelihood for cosmic shear, 2 × 2 pt and the full 3 × 2 pt in the fiducial DES Y3 cosmological analysis.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Compatibility of mesophase pitch and linear low-density polyethylene for low-cost carbon fiber

Mesophase pitch and linear low-density polyethylene (LLDPE) were blended by shear mixing and extruded producing precursor fibers which were then converted to carbon fibers (CFs). LLDPE additives agglomerate within the isotropic spheres rather than uniformly dispersing throughout the entire matrix. The blends possess different thermal properties and precursor tensile properties evident by two-phase tensile stress nature not present in precursor fibers produced from pure pitch. The resultant CFs were oxidized at 280 °C for 4 h and carbonized at 1000 °C for 15 min. This process created pitch CFs with a tensile strength of 1.23 GPa and a Young’s modulus of 99 GPa. All CFs produced from blends of pitch and LLDPE possessed a tensile strength of 0.63 GPa and less. These CFs showed a microstructure slightly different from the pure pitch CFs with fractured CF cross sections revealing voids present in all blended CFs due to burnt off LLDPE stemming from carbonization. Further study into compatibilizers and new conversion processes is required to successfully blend LLDPE with mesophase pitch for the purpose of producing a new low-cost CF.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Pressure dependence of Poisson’s ratio of glassy Baltic amber studied by Brillouin scattering spectroscopy

Amber is a typical natural glass with very long aging time. Elastic properties of amber at high pressures have been studied using Brillouin scattering and a diamond anvil cell. Both longitudinal and transverse acoustic modes have been observed up to 12 GPa. The pressure dependences of longitudinal, shear, Young’s, and bulk moduli, compressibility, and Poisson’s ratio were determined. The longitudinal, shear, Young’s, bulk moduli show the remarkable increase, and compressibility shows a marked decrease with increasing pressure. However, it is found that the pressure dependence of Poisson’s ratio is very small. The mechanism of this small pressure dependence was discussed. Finally, the Cauchy type relation between longitudinal and shear moduli was examined. Its coefficients show the deviation from the Cauchy relation owing to the coexistence of different intermolecular interactions in amber.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2023

Spin–phonon interactions and magnetoelectric coupling in Co 4 B 2 O 9 ( B = Nb, Ta)

In order to explore the consequences of spin–orbit coupling on spin–phonon interactions in a set of chemically similar mixed metal oxides, we measured the infrared vibrational properties of Co 4 B 2 O 9 (B = Nb, Ta) as a function of temperature and compared our findings with lattice dynamics calculations and several different models of spin–phonon coupling. Frequency vs temperature trends for the Co 2+ shearing mode near 150 cm –1 reveal significant shifts across the magnetic ordering temperature that are especially large in relative terms. Bringing these results together and accounting for noncollinearity, we obtain spin–phonon coupling constants of –3.4 and –4.3 cm –1 for Co 4 Nb 2 O 9 and the Ta analog, respectively. Analysis reveals that these coupling constants are derived from interlayer (rather than intralayer) exchange interactions and that the interlayer interactions contain competing antiferromagnetic and ferromagnetic contributions. At the same time, beyond-Heisenberg terms are minimized due to fortuitous symmetry considerations, different from most other 4d- and 5d-containing oxides. Comparison with other contemporary oxides shows that spin–phonon coupling in this family of materials is among the strongest ever reported, suggesting an origin for magnetoelectric coupling.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Graph-component approach to defect identification in large atomistic simulations

In this work, the graph-theoretical concept of connected components is employed to extract the evolution of defect configurations in a polycrystalline aluminum structure containing ~8.3 million atoms. This graph-component approach is applied to reveal details of defect formation, transport, and transformation in the polycrystalline Al under large shear deformation. Building upon standard nearest neighbor analysis, graph theory and associated tools are used to reduce the multi-million-atom system into discrete component subgraphs that represent distinct structural defects. This method allows the automated identification, characterization, and tracking of defective regions within large volumes of data representing atomic-scale processes. Such analysis elucidates relationships between external stimuli, such as strain, and defect distributions, which have a large influence on material properties. The Graph Analytics for Large Atomistic Simulations (GALAS) codebase that implements this analysis, together with user guidance, is openly available at https://github.com/pnnl/galas.

36 MATERIALS SCIENCE↗

DOE OSTI2023

The effects of Fe and Al on the phase transformations and mechanical behavior of β-Ti alloy Ti-11at.%Cr

Alloy composition is important for developing desired microstructures in beta-titanium (β-Ti) alloys during thermomechanical processing. In this work, the relatively low-cost alloying elements iron (Fe) and aluminum (Al) were added to a base Ti-11at%chromium (Cr) alloy and in-situ and ex-situ examination of the microstructural evolution and mechanical properties during tension, hardness, elevated temperature X-ray diffraction (XRD) and resonance ultrasound spectroscopy (RUS) were performed. The 400 °C XRD revealed that Ti-11at%Cr underwent β-to-ω and β-to-α transformations. Adding 0.85at% Fe reduced the volume fraction of the ω- and α-phases, and adding 5.3at% Al inhibited the β-to-ω transformation. The 400 °C RUS showed that the alloys containing the ω phase exhibited an increase in shear modulus (G) of ~140%, while the ω-free alloys exhibited an increase of only ~102%. The hardness and strength values of the ω-containing Ti-11Cr and Ti-11Cr-0.85Fe increased with increased ω-phase volume fraction when the ω/α ratio was greater than 0.25. The relationship between ω/α volume ratios and mechanical properties is discussed.

36 MATERIALS SCIENCE↗