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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Coherent Acoustic Interferometry during the Photodriven Oxygen Evolution Reaction Associates Strain Fields with the Reactive Oxygen Intermediate (Ti–OH*)

The oxygen evolution reaction (OER) from water requires the formation of metastable, reactive oxygen intermediates to enable oxygen–oxygen bond formation. Conversely, such reactive intermediates could also structurally modify the catalyst. Here, a descriptor for the overall catalytic activity, the first electron and proton transfer OER intermediate from water, (M–OH*), has been associated with significant distortions of the metal–oxygen bonds upon charge-trapping. Time-resolved spectroscopy of in situ, photodriven OER on transition metal oxide surfaces has characterized M–OH* for the charge trapping and the symmetry of the lattice distortions by optical and vibrational transitions, respectively, but had yet to detect an interfacial strain field arising from a surface coverage M–OH*. Here, we utilize picosecond, coherent acoustic interferometry to detect the uniaxial strain normal to the SrTiO 3 /aqueous interface directly caused by Ti–OH*. The spectral analysis applies a fairly general methodology for detecting a combination of the spatial extent, magnitude, and generation time of the interfacial strain through the coherent oscillations’ phase. For lightly n-doped SrTiO 3 , we identify the strain generation time (1.31 ps), which occurs simultaneously with Ti–OH* formation, and a tensile strain of 0.06% (upper limit 0.6%). In addition to fully characterizing this intermediate across visible, mid-infrared, and now GHz-THz probes on SrTiO 3 , we show that strain fields occur with the creation of some M–OH*, which modifies design strategies for tuning catalytic activity and provides insight into photo-induced degradation so prevalent for OER. To that end, the work put forth here provides a unique methodology to characterize intermediate-induced interfacial strain across OER catalysts.

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

Pseudoelastic deformation in Mo-based refractory multi-principal element alloys

Phase diagrams supported by density functional theory methods can be crucial for designing high-entropy alloys that are subset of multi-principal-element alloys. We present phase and property analysis of quinary (MoW) x Zr y (TaTi) 1-x-y refractory high-entropy alloys from combined Calculation of Phase Diagram (CALPHAD) and density-functional theory results, supplemented by molecular dynamics simulations. Both CALPHAD and density-functional theory analysis of phase stability indicates a Mo-W-rich region of this quinary has a stable single-phase body-centered-cubic structure. We report first quinary composition from Mo-W-Ta-Ti-Zr family of alloy with pseudo-elastic behavior, i.e., hysteresis in stress-strain. Our analysis shows that only Mo-W-rich compositions of Mo-W-Ta-Ti-Zr, i.e., Mo+W, show reproducible hysteresis in stress-strain responsible for pseudo-elastic behavior. The (MoW) 85 Zr 7.5 (TaTi) 7.5 was down-selected based on temperature-dependent phase diagram analysis and molecular dynamics simulations predicted elastic behavior that reveals twinning-assisted pseudoelastic behavior. While mostly unexplored in body-centered-cubic crystals, twinning is a fundamental deformation mechanism that competes against dislocation slip in crystalline solids. Furthermore, this alloy shows identical cyclic deformation characteristics during uniaxial < 100 > loading, i.e., the pseudoelasticity is isotropic in loading direction. Additionally, a temperature increase from 77 to 1,500 K enhances the elastic strain recovery in load-unload cycles, offering possibly control to tune the pseudoelastic behavior.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Self-Assembled Periodic Nanostructures Using Martensitic Phase Transformations

We describe a novel approach for the rational design and synthesis of self-assembled periodic nanostructures using martensitic phase transformations. We demonstrate this approach in a thin film of perovskite SrSnO 3 with reconfigurable periodic nanostructures consisting of regularly spaced regions of sharply contrasted dielectric properties. The films can be designed to have different periodicities and relative phase fractions via chemical doping or strain engineering. The dielectric contrast within a single film can be tuned using temperature and laser wavelength, effectively creating a variable photonic crystal. Our results show the realistic possibility of designing large-area self-assembled periodic structures using martensitic phase transformations with the potential of implementing "built-to-order" nanostructures for tailored optoelectronic functionalities.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Structural chirality and related properties in periodic inorganic solids: review and perspectives

Abstract Chirality refers to the asymmetry of objects that cannot be superimposed on their mirror image. It is a concept that exists in various scientific fields and has profound consequences. Although these are perhaps most widely recognized within biology, chemistry, and pharmacology, recent advances in chiral phonons, topological systems, crystal enantiomorphic materials, and magneto-chiral materials have brought this topic to the forefront of condensed matter physics research. Our review discusses the symmetry requirements and the features associated with structural chirality in inorganic materials. This allows us to explore the nature of phase transitions in these systems, the coupling between order parameters, and their impact on the material’s physical properties. We highlight essential contributions to the field, particularly recent progress in the study of chiral phonons, altermagnetism, magnetochirality between others. Despite the rarity of naturally occurring inorganic chiral crystals, this review also highlights a significant knowledge gap, presenting challenges and opportunities for structural chirality mostly at the fundamental level, e.g. chiral displacive phase transitions, possibilities of tuning and switching structural chirality by external means (electric, magnetic, or strain fields), whether chirality could be an independent order parameter, and whether structural chirality could be quantified, etc. Beyond simply summarizing this field of research, this review aims to inspire further research in materials science by addressing future challenges, encouraging the exploration of chirality beyond traditional boundaries, and seeking the development of innovative materials with superior or new properties.

Bousquet, Eric (ORCID:0000000292903463)↗
DOE OSTI2026

Harnessing the Spin-Flip Radiative Lifetimes of Optically Addressable Molecular Qubits

Optically addressable molecular qubits based on spin-flip (SF) emissive transitions are promising candidates for quantum technologies due to their sharp luminescence lines and tunable optical-spin interfaces. Yet, the microscopic mechanisms controlling the spin-flip radiative lifetime of SF emitters, a key property for efficient spin readout, remain largely unexplored. Here, we present a computational study of several Cr 4+ and Mo 4+ pseudotetrahedral molecular qubits, and we identify chemical and structural features that influence the transition dipole moment associated with the SF emission, which, in turn, governs the SF radiative lifetime. We find that the magnitude of the dipole moment is governed by the multireference character of the spin-flip excited-state wave function, which can be modulated by tuning the energy separation between the d orbitals of the metal and the spin-pairing energy. Both parameters are sensitive to molecular symmetry, metal–ligand bond covalency, and bond anisotropy and leave room for modulation via ligand and metal design, as well as applied strain, which is relevant for sensing applications. Our findings provide a mechanistic framework for understanding and tuning the spin-flip radiative behavior of molecular qubits and SF emitters that may guide future advances in quantum information science.

molecular qubits↗
DOE OSTI2020

Operando Tailoring of Defects and Strains in Corrugated β-Ni(OH) 2 Nanosheets for Stable and High-Rate Energy Storage

Nickel hydroxide represents a technologically important material for energy storage, such as hybrid supercapacitors. It has two different crystallographic polymorphs, α- and β-Ni(OH) 2 , showing advantages in either theoretical capacity or cycling/rate performance, manifesting a trade-off trend that needs to be optimized for practical applications. In this work, the synergistic superiorities in both activity and stability of corrugated β-Ni(OH) 2 nanosheets are demonstrated through an electrochemical abuse approach. With ≈91% capacity retention after 10 000 cycles, the corrugated β-Ni(OH) 2 nanosheets can deliver a gravimetric capacity of 457 C g -1 at a high current density of 30 A g -1 , which is nearly two and four times that of the regular α- and β-Ni(OH) 2 , respectively. Operando spectroscopy and finite element analysis reveal that greatly enhanced chemical activity and structural robustness can be attributed to the in situ tailored lattice defects and the strain-induced highly curved micromorphology. This work demonstrates a multi-scale defect-and-strain co-design strategy, which is helpful for rational design and tuned fabrication of next-generation electrode materials for stable and high-rate energy storage.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Pseudomonas aeruginosa Adhesion and Biofilm Formation on Poly(l-lysine)-Tethered Hydrogels: Synergistic Effect of Substrate Stiffness and Positive Charge Density

Infections associated with antibacterial-resistant Pseudomonas aeruginosa (P. aeruginosa) are the major cause of morbidity and mortality of patients, presenting one of the greatest therapeutic challenges for treatment of community-acquired and nosocomial infections. To develop antimicrobial hydrogel coatings to control the adhesion and subsequent biofilm formation of P. aeruginosa, we have used photo-cross-linked poly(ethylene glycol) diacrylate (PEGDA) hydrogels with varied cross-linking densities and covalently grafted poly(l-lysine) (PLL) at different weight compositions (ϕ PLL ). Both surface stiffness and positive charge density of the hydrogels were efficiently tuned over a broad range to investigate their effects on two main strains of P. aeruginosa, PA01 and PA14. We found that both number and viability of attached cells were positively correlated with the hydrogel stiffness, leading to thicker and larger coverage of cell colonies at 72 h postseeding on the stiffer substrates. The dependence of both PA01 and PA14 strains on ϕ PLL , however, was nonmonotonic. Positive charges from dissociated amine groups in the grafted PLL chains significantly promoted initial adhesion and proliferation of both strains at low ϕ PLL and developed into the thickest biofilms on the stiffest hydrogels grafted with ϕ PLL of 1–2%. Nevertheless, on the softest hydrogels grafted with PLL at high ϕ PLL of 7–10%, the bacteria no longer attached or survived. These results not only improved our fundamental understanding of bacteria-material interactions but also provided a series of PLL-grafted PEGDA hydrogels with controlled stiffness and positive charge density as ideal surface coating materials to prevent bacterial infections.

bacteria↗
DOE OSTI2021

Sonic Lift-off of GaAs-based Solar Cells with Reduced Surface Facets

Spalling has been proposed as a promising kerfless technique for slicing thin wafers and devices, enhancing the wafer yield from an ingot by reducing kerf-losses and enabling substrate reuse for the case of costly devices. The main challenge of spalling is to control the roughness and thickness variation of the spalled wafers that can be as high as 100% of the wafer thickness. Here, we have shown previously that the thickness variations are largely influenced by the interaction of the crack front with its own reflected waves. Herein we show that through Sonic Lift-off we can offer a modification to standard spalling technologies that minimizes the interaction of reflected waves with the crack front during lift-off of GaAs(100)-based solar cells. We show that the average surface facets amplitude can be reduced by 96% while obtaining a high quality bulk with no discernible residual strain as measured by PL. The resulting spalling depth can easily be tuned from 100 µm to less than 15µm. The electrical characterization of the Sonic lift-off cell shows no degradation of the VOC and a power conversion within 99% relative of a non-spalled baseline.

42 ENGINEERING↗
DOE OSTI2020

Extreme tensile strain states in La 0.7 Ca 0.3 MnO 3 membranes

A defining feature of emergent phenomena in complex oxides is the competition and cooperation between ground states. In manganites, the balance between metallic and insulating phases can be tuned by the lattice; extending the range of lattice control would enhance the ability to access other phases. We stabilized uniform extreme tensile strain in nanoscale La 0.7 Ca 0.3 MnO 3 membranes, exceeding 8% uniaxially and 5% biaxially. Uniaxial and biaxial strain suppresses the ferromagnetic metal at distinctly different strain values, inducing an insulator that can be extinguished by a magnetic field. Electronic structure calculations indicate that the insulator consists of charge-ordered Mn 4+ and Mn 3+ with staggered strain-enhanced Jahn-Teller distortions within the plane. This highly tunable strained membrane approach provides a broad opportunity to design and manipulate correlated electron states.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Limits to the strain engineering of layered square-planar nickelate thin films

The layered square-planar nickelates, Nd n+1 Ni n O 2n+2 , are an appealing system to tune the electronic properties of square-planar nickelates via dimensionality; indeed, superconductivity was recently observed in Nd 6 Ni 5 O 12 thin films. Here, we investigate the role of epitaxial strain in the competing requirements for the synthesis of the n = 3 Ruddlesden-Popper compound, Nd 4 Ni 3 O 10 , and subsequent reduction to the square-planar phase, Nd 4 Ni 3 O 8 . We synthesize our highest quality Nd 4 Ni 3 O 10 films under compressive strain on LaAlO 3 (001), while Nd 4 Ni 3 O 10 on NdGaO 3 (110) exhibits tensile strain-induced rock salt faults but retains bulk-like transport properties. A high density of extended defects forms in Nd 4 Ni 3 O 10 on SrTiO 3 (001). Films reduced on LaAlO 3 become insulating and form compressive strain-induced c-axis canting defects, while Nd 4 Ni 3 O 8 films on NdGaO 3 are metallic. This work provides a pathway to the synthesis of Nd n+1 Ni n O 2n+2 thin films and sets limits on the ability to strain engineer these compounds via epitaxy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Toughening Brittle Bio‐P3HB with Synthetic P3HB of Engineered Stereomicrostructures

Abstract Poly(3‐hydroxybutyrate) (P3HB), a biologically produced, biodegradable natural polyester, exhibits excellent thermal and barrier properties but suffers from mechanical brittleness, largely limiting its applications. Here we report a mono‐material product design strategy to toughen stereoperfect, brittle bio or synthetic P3HB by blending it with stereomicrostructurally engineered P3HB. Through tacticity ([ mm ] from 0 to 100 %) and molecular weight ( M n to 788 kDa) tuning, high‐performance synthetic P3HB materials with tensile strength to ≈30 MPa, fracture strain to ≈800 %, and toughness to 126 MJ m −3 (>110× tougher than bio‐P3HB) have been produced. Physical blending of the brittle P3HB with such P3HB in 10 to 90 wt % dramatically enhances its ductility from ≈5 % to 95–450 % and optical clarity from 19 % to 85 % visible light transmittance while maintaining desirably high elastic modulus (>1 GPa), tensile strength (>35 MPa), and melting temperature (160–170 °C). This P3HB‐toughening‐P3HB methodology departs from the traditional approach of incorporating chemically distinct components to toughen P3HB, which hinders chemical or mechanical recycling, highlighting the potential of the mono‐material product design solely based on biodegradable P3HB to deliver P3HB materials with diverse performance properties.

Zhang, Zhen↗
DOE OSTI2023

Toughening Brittle Bio‐P3HB with Synthetic P3HB of Engineered Stereomicrostructures

Abstract Poly(3‐hydroxybutyrate) (P3HB), a biologically produced, biodegradable natural polyester, exhibits excellent thermal and barrier properties but suffers from mechanical brittleness, largely limiting its applications. Here we report a mono‐material product design strategy to toughen stereoperfect, brittle bio or synthetic P3HB by blending it with stereomicrostructurally engineered P3HB. Through tacticity ([ mm ] from 0 to 100 %) and molecular weight ( M n to 788 kDa) tuning, high‐performance synthetic P3HB materials with tensile strength to ≈30 MPa, fracture strain to ≈800 %, and toughness to 126 MJ m −3 (>110× tougher than bio‐P3HB) have been produced. Physical blending of the brittle P3HB with such P3HB in 10 to 90 wt % dramatically enhances its ductility from ≈5 % to 95–450 % and optical clarity from 19 % to 85 % visible light transmittance while maintaining desirably high elastic modulus (>1 GPa), tensile strength (>35 MPa), and melting temperature (160–170 °C). This P3HB‐toughening‐P3HB methodology departs from the traditional approach of incorporating chemically distinct components to toughen P3HB, which hinders chemical or mechanical recycling, highlighting the potential of the mono‐material product design solely based on biodegradable P3HB to deliver P3HB materials with diverse performance properties.

Chemistry↗
DOE OSTI2024

Soft matter approach for creating novel protein hydrogels using fractal whey protein assemblies as building blocks

In this study, mesoscopic sized fractal assembly (FA) particles were prepared using whey protein isolate; the coldset gelation properties of FA particles were investigated in-depth. Two types of FA particles (FA -62 and FA -90) with different mean sizes were synthesized through controlled thermal treatment of whey protein solutions at two concentrations (62 g/L and 90 g/L). Particle characteristics e.g. hydrodynamic radius, ζ-potential and surface hydrophobicity were dependent on pH and structure of FA. Transmission electron microscopy (TEM) observation confirmed the fractal morphology and small-angle X-ray scattering (SAXS) analysis suggested an internal fractal structure for the obtained FA particles. Eight cold-set FA protein gels (2 % w/v) were manufactured by controlling two gelling factors at two levels: pH (5.8 and 7.0) and Ca 2+ content (5 mM and 10 mM). Rheological characteristics in the large amplitude oscillatory shear regime revealed that pH 7.0 gels were softer and elastic while pH 5.8 gels were harder and brittle. Rheology Pipkin diagrams demonstrated that the strain softening/stiffening and the shear-thinning/thickening behaviors may be fine-tuned by manipulating the key gelation factors: e.g. FA structure, pH, and Ca 2+ . The entrainment speed-dependent friction coefficient curves showed that at an intermediate velocity regime (6-250 mm s -1 ), FA -90 particles induced hydrogels had superior lubrication effect compared to FA -62 gels. Further, this work demonstrated a food structure design approach regarding tuning texture and lubrication properties of protein gels without changing protein content and protein composition. The optimized protein hydrogels may be used as texturizer for "cleaner label" food formulas and/or as delivery system for carrying micronutrients.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2023

Defining the Minimal Set of Microbial Genes Required for Valorization of Lignin Biomass (Final Report)

Project Goals: Lignin is the second most abundant biopolymer on earth and represents a critically underutilized biomass resource for hydrocarbon feedstocks. Despite substantial effort, there is still no efficient process to convert lignin to useable carbon-based platform chemicals and materials. The goal of this project is identify a minimal set of microbial enzymes necessary for lignin breakdown and sufficient for the synthesis of valuable chemical intermediates from lignin isolated as a byproduct of lignocellulosic ethanol production. These genes will be then used to engineer functional whole cell biocatalysts for tunable lignin metabolism. To date, although a number of enzymes have been associated with lignin degradation, most have been tested in isolation (as individual enzymes) and on drastically different substrates -- often dyes that are not related to lignin. In contrast, lignin utilization in nature likely occurs by microbial consortia with multiple enzymes acting synergistically. We propose to examine two separate stages of lignin breakdown carried out by the microbes that do it best: (1) early breakdown of native polymeric lignin into soluble fragments by a set of sequenced wood-rotting fungal species, and (2) downstream metabolism of these soluble lignin fragments to useful chemical intermediates by a panel of sequenced soil saprophytes. Our approach involves testing sets of genes that will be assayed combinatorially in the context of a heterologous expression host. The resulting engineered strains will be systematically assayed using soluble lignin fragments, synthetic defined polymeric lignin, and finally lignin directly sourced from lignocellulosic processing streams. In addition to resulting in a functional whole cell biocatalyst for lignin utilization, we anticipate that this approach will allow us to address key unanswered questions about lignin metabolism in nature, including: (1) Why does the Trametes versicolor genome contain 25 different class II peroxidases? (2) What is the role of laccases in lignin metabolism? Why do some aggressive lignin degraders have many laccases (e.g. >7 in T. versicolor) while others have none (e.g. P. chrysosporium)? (3) How is peroxide provided in a controlled manner to drive peroxidase activity without causing the enzyme inhibition that is so often observed in vitro? (4) What strategies do microbial lignin degraders use to avoid the problem of repolymerization during active lignin degradation? and (5) Can microbial lignin metabolism be diverted for high level production of defined aromatics? A final critical question is whether combining key minimal sets of enzymes from a wide range of organisms will result in engineered strains capable of highly efficient, streamlined pathways for lignin utilization that can be tuned for a specific carbon output. This effort will leverage DOE investments in microbial genome sequencing, and secure a critical channel for lignin biomass utilization that will also help to render lignocellulosic a viable feedstock for the production of renewable liquid biofuels.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Orientation dependence of the effect of short-range ordering on the plastic deformation of a medium entropy alloy

Multi-principal-element alloys (also known as medium and high entropy alloys) offer a much larger and richer design space than conventional alloys, providing opportunities for discovering new functionalities and their governing physics. Some of these alloys exhibit an outstanding combination of high strength and ductility, linked to the activation of various deformation modes triggered by low-energy stacking faults. However, a pressing question remains: Is the plasticity of medium- and high-entropy alloys governed only by stacking fault energy, or does atomic short-range order (SRO) play a role? Here, to answer this, we investigated how SRO affects the deformation in single-crystalline NiCoCr, with previous contradictory findings. First, we established unique experimental evidence for SRO formation in bulk single crystals using high-energy synchrotron transmission X-Ray Diffraction. By tuning the degree of SRO by aging at high temperatures, twinning density and strain-induced martensitic phase transformation can be significantly increased in the [110] and [111] orientations under tension, increasing the tensile ductility; yet, no increase was observed along the [001] orientation due to lack of TWinning-Induced Plasticity (TWIP) or TRansformation-Induced Plasticity (TRIP), indicating a strong crystallographic orientation dependence. Our first-principles thermodynamic calculations unequivocally show SRO exists and governs the observed microstructural evolution and deformation hardening behavior. Here we find direct proof that SRO triggers a simultaneous TWIP and TRIP in NiCoCr, a rare microstructural evolution path. Our findings establish that the interplay of SRO and plasticity could be exploited to alter deformation modes and yield unprecedented mechanical response in medium- and high-entropy alloys.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Optomechanical Tuning of Second Harmonic Generation Anisotropy in Janus MoSSe/MoS 2 Heterostructures

Symmetry breaking in van der Waals materials enables the realization of quantum states and advanced device functionalities. Janus transition-metal dichalcogenides (TMDs) exhibit distinctive nonlinear optical properties due to their broken out-of-plane mirror symmetry. However, the dynamic control of second harmonic generation (SHG) anisotropy and resonance behavior via optical excitation remains elusive. Here, in this work, we investigate the SHG response of Janus MoSSe/MoS 2 heterostructures with 2H and 3R stackings. We can tune the SHG response by varying the incident photon wavelength from 800 to 1000 nm, which shows a resonance-dependent enhancement in intensity and a deviation from 6-fold symmetry, indicating wavelength-dependent anisotropy. The ratio between maximum and minimum intensity in the armchair directions, associated with the SHG anisotropy, reaches a value of 1.73 at the excitation wavelength of 1000 nm. Group theory analysis and first-principles calculations reveal that the observed anisotropy arises from optically induced strain. Our findings highlight the role of symmetry breaking and optical resonance contributing to the optomechanical tuning of SHG anisotropy, offering opportunities for developing Janus TMD-based photonic devices for frequency conversion, light generation, and optical switching.

Janus transition metal dichalcogenides↗
DOE OSTI2025

Subsurface hydrogen, curvature, and strain: lessons from electro-reduction of benzaldehyde on nano-structured Pd catalysts

The unique ability of palladium (Pd) to absorb hydrogen and form a bulk hydride is vital for chemical transformations that involve hydrogenation reactions. Nano-structured Pd catalysts offer a promise of tuning these reaction rates by exploiting variations of reactant binding energies depending on the surface structure and morphological constraints that result in inhomogeneous strain. However, the interplay between the nano-structure of Pd and the ability of Pd to adsorb (and absorb) hydrogen as well as other reactive species needs to be better understood for a rational understanding of competitive chemical transformations at Pd surfaces. We consider the effects of the surface corrugation, strain, and subsurface Pd hydride on the reduction of benzaldehyde to benzyl alcohol in two qualitatively different samples – Pd nanoparticles and Pd gels formed by quasi-one-dimensional chains of these nanoparticles. Our electrochemical measurements and computational modelling suggest that surface concave sites, inherent to Pd gels, facilitate hydrogen transfer to the Pd subsurface region, thus weakening benzaldehyde binding to the surface. This effect is further modulated by the strain, depending on the local coordination environment on the corrugated surface. Furthermore, these findings demonstrate how structurally complex samples in the form of gels provide degrees of freedom for controlling the behavior of metal catalysts that are not available in isolated nanoparticles, which paves the way for new approaches in the design of catalytic materials and synthesis of metal hydrides.

Padavala, Sri Krishna Murthy [University of Minnes↗