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At least 379 records · Page 21

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DOE OSTI2020

The role of collective elasticity on activated structural relaxation, yielding, and steady state flow in hard sphere fluids and colloidal suspensions under strong deformation

In this work, we theoretically study the effect of external deformation on activated structural relaxation and aspects of the nonlinear mechanical response of glassy hard sphere fluids in the context of elastically collective nonlinear Langevin equation theory. This microscopic force-based approach describes activated relaxation as a coupled local–nonlocal event involving caging and longer range collective elasticity, with the latter becoming more important and ultimately dominant with increasing packing fraction under equilibrium conditions. The central new question we address is how this physical picture of activated relaxation, and the relative importance of local caging vs collective elasticity physics, depends on external deformation. Theoretical predictions are presented for deformation-induced enhancement of mobility, the onset of relaxation speed up at remarkably low values of stress, strain, or shear rate, apparent power law thinning of the steady state structural relaxation time and viscosity, a non-vanishing activation barrier in the shear thinning regime, an apparent Herschel–Bulkley form of the rate dependence of the steady state shear stress, exponential growth of different measures of a dynamic yield or flow stress with the packing fraction, and reduced fragility and dynamic heterogeneity under deformation. The results are contrasted with experiments and simulations, and qualitative or better agreement is found. An overarching conclusion is that deformation strongly reduces the importance of longer range collective elastic effects relative to the local caging aspect for most, but not all, physical questions, with deformation-dependent fragility and dynamic heterogeneity phenomena being qualitatively sensitive to collective elasticity. Overall, nonlinear rheology is predicted to be a more local problem than quiescent structural relaxation, albeit with deformation-modified activated processes still important.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Coherent heteroepitaxial growth of I-III-VI 2 Ag(In,Ga)S 2 colloidal nanocrystals with near-unity quantum yield for use in luminescent solar concentrators

Colloidal Ag(In,Ga)S 2 nanocrystals (AIGS NCs) with the band gap tunability by their size and composition within visible range have garnered surging interest. High absorption cross-section and narrow emission linewidth of AIGS NCs make them ideally suited to address the challenges of Cd-free NCs in wide-ranging photonic applications. However, AIGS NCs have shown relatively underwhelming photoluminescence quantum yield (PL QY) to date, primarily because coherent heteroepitaxy has not been realized. Here, we report the heteroepitaxy for AIGS-AgGaS 2 (AIGS-AGS) core-shell NCs bearing near-unity PL QYs in almost full visible range (460 to 620 nm) and enhanced photochemical stability. Key to the successful growth of AIGS-AGS NCs is the use of the Ag-S-Ga(OA) 2 complex, which complements the reactivities among cations for both homogeneous AIGS cores in various compositions and uniform AGS shell growth. The heteroepitaxy between AIGS and AGS results in the Type I heterojunction that effectively confines charge carriers within the emissive core without optically active interfacial defects. AIGS-AGS NCs show higher extinction coefficient and narrower spectral linewidth compared to state-of-the-art heavy metal-free NCs, prompting their immediate use in practicable applications including displays and luminescent solar concentrators (LSCs).

42 ENGINEERING↗

DOE OSTI2023

Unraveling capacity fading in lithium-ion batteries using advanced cyclic tests: A real-world approach

Battery lifespan estimation is essential for effective battery management systems, aiding users and manufacturers in strategic planning. However, accurately estimating battery capacity is complex, owing to diverse capacity fading phenomena tied to factors such as temperature, charge-discharge rate, and rest period duration. In this work, we present an innovative approach that integrates real-world driving behaviors into cyclic testing. Unlike conventional methods that lack rest periods and involve fixed charge-discharge rates, our approach involves 1000 unique test cycles tailored to specific objectives and applications, capturing the nuanced effects of temperature, charge-discharge rate, and rest duration on capacity fading. This yields comprehensive insights into cell-level battery degradation, unveiling growth patterns of the solid electrolyte interface (SEI) layer and lithium plating, influenced by cyclic test parameters. Here, the results yield critical empirical relations for evaluating capacity fading under specific testing conditions.

25 ENERGY STORAGE↗

NASA NTRS1974

An investigation of the plastic fracture of AISI 4340 and 18 nickel - 200 grade maraging steels

The mechanisms of plastic fracture (dimpled rupture) in high-purity and commercial 18 Ni, 200 grade maraging steels and quenched and tempered AISI 4340 steels have been studied. Plastic fracture takes place in the maraging alloys through void initiation by fracture of titanium carbo-nitride inclusions and the growth of these voids until impingement results in coalescence and final fracture. The fracture of AISI 4340 steel at a yield strength of 200 ksi occurs by nucleation and subsequent growth of voids formed by fracture of the interface between manganese sulfide inclusions and the matrix. The growth of these inclusion-nucleated voids is interrupted long before coalescence by impingement, by the formation of void sheets which connect neighboring sulfide-nucleated voids.

Cox, T. B.↗

DOE OSTI2020

Engineering of Lead Selenide Quantum Dot Based Devices and Core/Shell Heterostructures

Near infrared (NIR) emitting colloidal quantum dots (QDs) such as PbSe are interesting materials for implementation in various optoelectronic devices such as solar cells, photodetectors, and radiation detectors. Material properties like size tunable emission wavelengths, facile solution processability, the possibility of carrier multiplication and Auger assisted up-conversion, and high Z number provide PbSe QDs with unique advantages over many currently available commercial materials used in these devices. In this dissertation, after an introduction to QDs in general, we first focus on synthesis of PbSe-based heterostructured QDs for study via optical spectroscopy. PbSe/CdSe QDs synthesized via cation exchange reaction were used as seeds to study the proper conditions for further CdSe or CdS shell growth. Optical spectroscopy studies show that growth of thicker CdSe shells leads to tunable visible emission, while growth of thick CdS shells can greatly increase the photoluminescence quantum yield (PLQY) observed from the intermediate CdSe shell. NIR PL lifetimes can be greatly enhanced by the growth of CdS shells, due to strong delocalization of the hole wavefunction within the PbSe core, while the electron is delocalized throughout the QD including in the CdS shell, resulting in radiative lifetimes in the tens of microseconds. Two pulse delay measurements show that Auger assisted up conversion is also taking place in these engineered QD dot heterostructures. In the sections that follow, we look at QD devices, first with a focus on novel devices fabricated from PbSe QDs, using an amine synthesis method that allows for facile in-solution ligand exchange. QD film mobilities are measured for PbSe QDs capped with various short ionic ligands. Carrier densities in PbSe QD films are calculated from C-V measurements, showing for the first time that carrier densities can be modulated by simply changing the capping ligand. vii Radiation detectors utilizing PbSe QDs capped with KI and NH4I ligands show tangible response to incident alpha radiation. Current output response to alpha radiation is dependent on strength of radiation source and amount of bias voltage applied. In the final section a critical review of hybrid layered 2D-QD photodetectors is presented. In a typical example, PbSe and PbS QDs act as the absorbing layer in phototransistor devices which utilize layered 2D materials such as graphene and transition metal dichalcogenides as transport layers. Resulting devices display high gains and improved directivities compared to QD only and 2D only devices.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Valorization of CO 2 through lithoautotrophic production of sustainable chemicals in Cupriavidus necator

Coupling recent advancements in genetic engineering of diverse microbes and gas-driven fermentation provides a path toward sustainable commodity chemical production. Cupriavidus necator H16 is a suitable species for this task because it effectively utilizes H 2 and CO 2 and is genetically tractable. Here, we demonstrate the versatility of C. necator for chemical production by engineering it to produce three products from CO 2 under lithotrophic conditions: sucrose, polyhydroxyalkanoates (PHAs), and lipochitooligosaccharides (LCOs). We engineered sucrose production in a co-culture system with heterotrophic growth 30 times that of WT C. necator. We engineered PHA production (20-60% DCW) and selectively altered product composition by combining different thioesterases and phaCs to produce copolymers directly from CO 2 . And, we engineered C. necator to convert CO 2 into the LCO, a plant growth enhancer, with titers of ~1.4 mg/L—equivalent to yields in its native source, Bradyrhizobium. Here, we applied the LCOs to germinating seeds as well as corn plants and observed increases in a variety of growth parameters. Taken together, these results expand our understanding of how a gas-utilizing bacteria can promote sustainable production.

09 BIOMASS FUELS↗

NASA NTRS1975

Precision compliance techniques for slow crack growth measurements

A method is presented for using simple electronic components to obtain the high sensitivity needed to measure very slow crack growth rates. The technique presented can reduce the experimental time considerably and also yield a greater amount of data more accurately than optical techniques for measuring crack growth rates.

Noronha, P. J.↗

NASA NTRS1975

Silicon ribbon study program

The feasibility is studied of growing wide, thin silicon dendritic web for solar cell fabrication and conceptual designs are developed for the apparatus required. An analysis of the mechanisms of dendritic web growth indicated that there were no apparent fundamental limitations to the process. The analysis yielded quantitative guidelines for the thermal conditions required for this mode of crystal growth. Crucible designs were then investigated: the usual quartz crucible configurations and configurations in which silicon itself is used for the crucible. The quartz crucible design is feasible and is incorporated into a conceptual design for a laboratory scale crystal growth facility capable of semi-automated quasi-continuous operation.

Seidensticker, R. G.↗

NASA NTRS2017

Classifying Multi-Model Wheat Yield Impact Response Surfaces Showing Sensitivity to Temperature and Precipitation Change

Crop growth simulation models can differ greatly in their treatment of key processes and hence in their response to environmental conditions. Here, we used an ensemble of 26 process-based wheat models applied at sites across a European transect to compare their sensitivity to changes in temperature (minus 2 to plus 9 degrees Centigrade) and precipitation (minus 50 to plus 50 percent). Model results were analysed by plotting them as impact response surfaces (IRSs), classifying the IRS patterns of individual model simulations, describing these classes and analysing factors that may explain the major differences in model responses. The model ensemble was used to simulate yields of winter and spring wheat at four sites in Finland, Germany and Spain. Results were plotted as IRSs that show changes in yields relative to the baseline with respect to temperature and precipitation. IRSs of 30-year means and selected extreme years were classified using two approaches describing their pattern. The expert diagnostic approach (EDA) combines two aspects of IRS patterns: location of the maximum yield (nine classes) and strength of the yield response with respect to climate (four classes), resulting in a total of 36 combined classes defined using criteria pre-specified by experts. The statistical diagnostic approach (SDA) groups IRSs by comparing their pattern and magnitude, without attempting to interpret these features. It applies a hierarchical clustering method, grouping response patterns using a distance metric that combines the spatial correlation and Euclidian distance between IRS pairs. The two approaches were used to investigate whether different patterns of yield response could be related to different properties of the crop models, specifically their genealogy, calibration and process description. Although no single model property across a large model ensemble was found to explain the integrated yield response to temperature and precipitation perturbations, the application of the EDA and SDA approaches revealed their capability to distinguish: (i) stronger yield responses to precipitation for winter wheat than spring wheat; (ii) differing strengths of response to climate changes for years with anomalous weather conditions compared to period-average conditions; (iii) the influence of site conditions on yield patterns; (iv) similarities in IRS patterns among models with related genealogy; (v) similarities in IRS patterns for models with simpler process descriptions of root growth and water uptake compared to those with more complex descriptions; and (vi) a closer correspondence of IRS patterns in models using partitioning schemes to represent yield formation than in those using a harvest index. Such results can inform future crop modelling studies that seek to exploit the diversity of multi-model ensembles, by distinguishing ensemble members that span a wide range of responses as well as those that display implausible behaviour or strong mutual similarities.

Classification; Climate change; Crop model; Ensemb↗

DOE OSTI2024

Microbe of the month: Methanococcus maripaludis

Methanococcus maripaludis was first isolated in 1983 from the anoxic sediment of a salt marsh in South Carolina, USA. M. maripaludis grows by using H 2 or formate to reduce CO 2 to CH 4 and is an autotroph that assimilates CO 2 via the archaeal version of the Wood–Ljungdahl pathway. In some strains, supplementation of growth medium with acetate or propionate can increase biomass yield. Furthermore, this microorganism is strictly anaerobic, has a pleomorphic coccoid shape, and forms translucent, pale yellow, smooth colonies within 3 days on agar plates. The optimum temperature for growth is 38°C with optimal pH between 6.8 and 7.2.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Non-Equilibrium in a Dust-Forming Low-Temperature Plasma: A CARS Study

Dust-forming low-temperature plasmas are versatile systems for the production of nanoparticles with tunable functionalities. While attractive from a materials processing point of view, these systems are inherently complex, with several plasma-induced phenomena determining the properties of the produced materials. Here, we characterize a carbon nanoparticle-forming plasma using coherent anti-Stokes Raman spectroscopy (CARS), with the primary goal of measuring gas temperature. While gas temperature is typically assumed to be at or slightly above room temperature in these reactors, we measure gas temperatures exceeding 1000 K under typical process conditions. We find a correlation between the gas temperature and the nanoparticle yield, suggesting that the particle nucleation and growth process releases energy within the reaction volume, leading to significant gas heating. In addition, we find that the relaxation of vibrationally excited species at the particle surfaces is a major contributor to their heating. In conclusion, these results underscore the complexity of these systems and the need for their more in-depth characterization using advanced techniques such as CARS.

Basic Plasma Phenomena and Gas Discharges↗

DOE OSTI2025

Sequential Infiltration Synthesis of Multinary Metal Oxides: The Role of Precursor Diffusion and Reactivity

Understanding volatile metal–organic precursor transport in polymer matrices during sequential infiltration synthesis (SIS) is critical to the design of hybrid materials of tailored composition and uniform structure. Here, we investigate the diffusion and reaction behavior of diethylzinc (DEZ) in poly(methyl methacrylate) (PMMA) matrices with variable indium and zinc incorporation. Unlike conventional SIS where precursors adduct or react directly with the polymer backbone, DEZ shows minimal interaction with PMMA. However, DEZ may interact strongly with In–OH or Zn–OH moieties that are previously incorporated into a PMMA thick film. Using spectroscopic ellipsometry, X-ray photoelectron spectroscopy depth profiling, and EDX line scans, we quantify Zn incorporation as a function of exposure time, polymer thickness, and previous infiltration steps. The Zn distribution evolves from surface-localized to deep within the ∼1 μm thick film with increasing DEZ exposures up to 30 min. A reaction-diffusion model incorporating a hindering factor to capture diffusivity decay due to product accumulation reproduces the Zn depth profile and yields physically meaningful parameters to guide future growth. Furthermore, this study provides a framework for interpreting metal–organic precursor infiltration behavior and highlights the utility of model-guided SIS process design.

diethylzinc↗

DOE OSTI2024

Genetic modification of the shikimate pathway to reduce lignin content in switchgrass ( Panicum virgatum L.) significantly impacts plant microbiomes

Switchgrass (Panicum virgatum L.) is considered a sustainable biofuel feedstock, given its fast-impact growth, low input requirements, and high biomass yields. Improvements in bioenergy conversion efficiency of switchgrass could be made by reducing its lignin content. Engineered switchgrass that expresses a bacterial 3-dehydroshikimate dehydratase (QsuB) has reduced lignin content and improved biomass saccharification due to the rerouting of the shikimate pathway towards the simple aromatic protocatechuate at the expense of lignin biosynthesis. However, the impacts of this QsuB trait on switchgrass microbiome structure and function remain unclear. To address this, wild-type and QsuB-engineered switchgrass were grown in switchgrass field soils, and samples were collected from inflorescences, leaves, roots, rhizospheres, and bulk soils for microbiome analysis. We investigated how QsuB expression influenced switchgrass-associated fungal and bacterial communities using high-throughput Illumina MiSeq amplicon sequencing of ITS and 16S rDNA. Compared to wild-type, QsuB-engineered switchgrass hosted different microbial communities in roots, rhizosphere, and leaves. Specifically, QsuB-engineered plants had a lower relative abundance of arbuscular mycorrhizal fungi (AMF). Additionally, QsuB-engineered plants had fewer Actinobacteriota in root and rhizosphere samples. These findings may indicate that changes in the plant metabolism impact both AMF and Actinobacteriota similarly or potential interactions between AMF and the bacterial community. This study enhances understanding of plant-microbiome interactions by providing baseline microbial data for developing beneficial bioengineering strategies and by assessing nontarget impacts of engineered plant traits on the plant microbiome.

09 BIOMASS FUELS↗

DOE OSTI2021

CRISPR/Cas9-Induced fad2 and rod1 Mutations Stacked With f ae1 Confer High Oleic Acid Seed Oil in Pennycress (Thlaspi arvense L.)

Pennycress (Thlaspi arvense L.) is being domesticated as an oilseed cash cover crop to be grown in the off-season throughout temperate regions of the world. With its diploid genome and ease of directed mutagenesis using molecular approaches, pennycress seed oil composition can be rapidly tailored for a plethora of food, feed, oleochemical and fuel uses. Here, we utilized Clustered Regularly Interspaced Short Palindromic Repeats (CRISPR)/Cas9 technology to produce knockout mutations in the FATTY ACID DESATURASE2 (FAD2) and REDUCED OLEATE DESATURATION1 (ROD1) genes to increase oleic acid content. High oleic acid (18:1) oil is valued for its oxidative stability that is superior to the polyunsaturated fatty acids (PUFAs) linoleic (18:2) and linolenic (18:3), and better cold flow properties than the very long chain fatty acid (VLCFA) erucic (22:1). When combined with a FATTY ACID ELONGATION1 (fae1) knockout mutation, fad2 fae1 and rod1 fae1 double mutants produced ~90% and ~60% oleic acid in seed oil, respectively, with PUFAs in fad2 fae1 as well as fad2 single mutants reduced to less than 5%. MALDI-MS spatial imaging analyses of phosphatidylcholine (PC) and triacylglycerol (TAG) molecular species in wild-type pennycress embryo sections from mature seeds revealed that erucic acid is highly enriched in cotyledons which serve as storage organs, suggestive of a role in providing energy for the germinating seedling. In contrast, PUFA-containing TAGs are enriched in the embryonic axis, which may be utilized for cellular membrane expansion during seed germination and seedling emergence. Under standard growth chamber conditions, rod1 fae1 plants grew like wild type whereas fad2 single and fad2 fae1 double mutant plants exhibited delayed growth and overall reduced heights and seed yields, suggesting that reducing PUFAs below a threshold in pennycress had negative physiological effects. Taken together, our results suggest that combinatorial knockout of ROD1 and FAE1 may be a viable route to commercially increase oleic acid content in pennycress seed oil whereas mutations in FAD2 will likely require at least partial function to avoid fitness trade-offs.

09 BIOMASS FUELS↗

NASA NTRS1981

Improved liquid phase epitaxial GaAs for low series resistance Schottky barrier mixer diodes

Millimeter wave Schottky barrier mixer diodes are extremely important devices for radio astronomy. The performance of the Schottky diodes depends largely on the characteristics and quality of the GaAs epitaxial materials used. Systematic manipulation of the liquid phase epitaxial growth conditions and substrate surface treatments has yielded significantly improved surface morphology. Initial problems of high resistivity interfacial layers have been reduced without the use of an in situ etchback. Two-micron diameter Schottky diodes fabricated from epitaxial layers grown at 725 C exhibit a 9-ohm series resistance very near the theoretical minimum.

Binari, S. C.↗

NASA NTRS1988

Application of the V(R) resistance curve method to fracture of various crack configurations

The fracture resistance curve method of Newman (1985), based on the crack-tip-opening displacement, V(R), for a 'stationary' crack, was applied to various crack configurations in 2024-T351 and 7075-T651 aluminum alloys tested at room temperature. Using a stationary crack solution, the crack-tip-displacement was calculated at the current crack length for the crack configurations which included compact, middle-crack, single-edge-crack, and three-hole-crack tension specimens. The results showed that the V(R) resistance curves are insensitive to crack length, specimen width, and specimen type up to maximum load. After the maximum load is reached, the V(R) remains nearly constant; this constant depends only on specimen type, specimen width, and crack length. The V(R) resistance curve method can be used with the strip-yield analyses to accurately predict stable crack growth and instability of cracked metallic materials.

Newman, J. C., Jr.↗

NASA NTRS1989

Stability of compressible boundary layers over a smooth backward-facing step

An investigation is conducted into the determination of the credibility of interacting boundary layers in predicting compressible subsonic flows over smooth surface imperfections. The case of smooth backward-facing steps is considered. The predicted mean flows are compared with those obtained using a Navier-Stokes solver. Moreover, the linear 2-D compressible stability characteristics of both mean flows are compared. The results show that the interacting boundary-layer formulation produces accurate mean flows that yield accurate linear stability characteristics, such as growth rates and amplification factors.

Ragab, S. A.↗

NASA NTRS1990

Stability of compressible boundary layers over a smooth backward-facing step

Ragab, S. A.↗