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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 865 records · Page 48
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Nanoscale Particle Motion Reveals Polymer Mobility Gradient in Nanocomposites

Polymer mobility near nanoparticle surfaces has been extensively discussed; however, direct experimental observation in the nanocomposite melts has been a difficult task. Here, by taking advantage of large dynamical asymmetry between the miscible matrix and surface-bound polymers, we highlighted their interphases and studied the resulting effect on the nanoparticle relaxation using X-ray photon correlation spectroscopy. Here, the local mobility gradient is signified by an unprecedented increase in the relaxation time at length scales on the order of polymer radius of gyration. The effect is accompanied by a transition from simple diffusive to subdiffusive behavior in accord with viscous and entangled dynamics of polymers in the matrix and in the interphase, respectively. Our results demonstrate that the nanoparticle-induced polymer mobility changes in the interphases of nanocomposite melts can be extracted from the length-scale-dependent slow particle motion.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2015

Dynamics of water around the complex structures formed between the KH domains of far upstream element binding protein and single-stranded DNA molecules

Single-stranded DNA (ss-DNA) binding proteins specifically bind to the single-stranded regions of the DNA and protect it from premature annealing, thereby stabilizing the DNA structure. We have carried out atomistic molecular dynamics simulations of the aqueous solutions of two DNA binding K homology (KH) domains (KH3 and KH4) of the far upstream element binding protein complexed with two short ss-DNA segments. Attempts have been made to explore the influence of the formation of such complex structures on the microscopic dynamics and hydrogen bond properties of the interfacial water molecules. It is found that the water molecules involved in bridging the ss-DNA segments and the protein domains form a highly constrained thin layer with extremely retarded mobility. These water molecules play important roles in freezing the conformational oscillations of the ss-DNA oligomers and thereby forming rigid complex structures. Further, it is demonstrated that the effect of complexation on the slow long-time relaxations of hydrogen bonds at the interface is correlated with hindered motions of the surrounding water molecules. Importantly, it is observed that the highly restricted motions of the water molecules bridging the protein and the DNA components in the complexed forms originate from more frequent hydrogen bond reformations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Epitaxial TiO x Surface in Ferroelectric BaTiO 3 : Native Structure and Dynamic Patterning at the Atomic Scale

Surfaces and interfaces of ferroelectric oxides exhibit enhanced functionality, and therefore serve as a platform for novel nano and quantum technologies. Experimental and theoretical challenges associated with examining the subtle electro-chemo-mechanical balance at metal-oxide surfaces have hindered the understanding and control of their structure and behavior. Here, we combine advanced electron-microscopy and first-principles thermodynamics methods to reveal the atomic-scale chemical and crystallographic structure of the surface of the seminal ferroelectric BaTiO 3 . Here, we show that the surface is composed of a native < 2-nm thick TiOx rock-salt layer in epitaxial registry with the BaTiO 3 . Using electron-beam irradiation, we successfully patterned artificially TiO x sites with sub-nanometer resolution, by inducing Ba escape. Therefore, our work offers electro-chemo-mechanical insights into ferroelectric surface behavior in addition to a method for scalable high-resolution beam-induced chemical lithography for selectively driving surface phase transitions, and thereby functionalizing metal-oxide surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Ultrafast Formation of Charge Transfer Trions at Molecular‐Functionalized 2D MoS 2 Interfaces

Abstract In this work, we investigate trion dynamics occurring at the heterojunction between organometallic molecules and a monolayer transition metal dichalcogenide (TMD) with transient electronic sum frequency generation (tr‐ESFG) spectroscopy. By pumping at 2.4 eV with laser pulses, we have observed an ultrafast hole transfer, succeeded by the emergence of charge‐transfer trions. This observation is facilitated by the cancellation of ground state bleach and stimulated emission signals due to their opposite phases, making tr‐ESFG especially sensitive to the trion formation dynamics. The presence of charge‐transfer trion at molecular functionalized TMD monolayers suggests the potential for engineering the local electronic structures and dynamics of specific locations on TMDs and offers a potential for transferring unique electronic attributes of TMD to the molecular layers.

Jing, Yuancheng↗
DOE OSTI2022

Evaluation of erosion potential of bio-based multicomponent blendstocks using experimentally-validated computational fluid dynamics

The optimization of the fuel-engine interface and associated performance is a significant goal for CoOptima and the industry. The strategic driver for fuel-engine optimization is clear: diesel optimization can significantly reduce emissions including NOx, particulate matter, and CO2 emissions. Previous evaluations of ethanol and diesel blends raised significant concerns with fuel injector erosion using ethanol blends. While Sylvatex’s technology can use ethanol, it also utilizes a surfactant and water to compatibilize and modify ethanol blends, thereby controlling its impact in diesel engines. The results from the project will (1) provide important insights into complex fuels and erosion, which will be used to design additional, improved formulations; and (2) expand capabilities of Argonne’s cavitation-induced erosion risk assessment (CIERA) tool to model multi-component systems, furthering Co-Optima objectives.

09 BIOMASS FUELS↗
DOE OSTI2019

Estimates of Decadal Climate Predictability From an Interactive Ensemble Model

Decadal climate predictability has received considerable scientific interest in recent years, yet the limits and mechanisms for decadal predictability are currently not well known. It is widely accepted that noise due to internal atmospheric dynamics at the air-sea interface influences predictability. The purpose of this paper is to use the interactive ensemble (IE) coupling strategy to quantify how internal atmospheric noise at the air-sea interface impacts decadal predictability. The IE technique can significantly reduce internal atmospheric noise and has proven useful in assessing seasonal-to-interannual variability and predictability. Here we focus on decadal timescales and apply the nonlinear local Lyapunov exponent method to the Community Climate System Model comparing control simulations with IE simulations. This is the first time the nonlinear local Lyapunov exponent has been applied to the state-of-the-art coupled models. The global patterns of decadal predictability are discussed from the perspective of internal atmospheric noise and ocean dynamics.

58 GEOSCIENCES↗
DOE OSTI2014

In-operando hard X-ray photoelectron spectroscopy study on the impact of current compliance and switching cycles on oxygen and carbon defects in resistive switching Ti/HfO{sub 2}/TiN cells

In this study, direct experimental materials science evidence of the important theoretical prediction for resistive random access memory (RRAM) technologies that a critical amount of oxygen vacancies is needed to establish stable resistive switching in metal-oxide-metal samples is presented. In detail, a novel in-operando hard X-ray photoelectron spectroscopy technique is applied to non-destructively investigates the influence of the current compliance and direct current voltage sweep cycles on the Ti/HfO{sub 2} interface chemistry and physics of resistive switching Ti/HfO{sub 2}/TiN cells. These studies indeed confirm that current compliance is a critical parameter to control the amount of oxygen vacancies in the conducting filaments in the oxide layer during the RRAM cell operation to achieve stable switching. Furthermore, clear carbon segregation towards the Ti/HfO{sub 2} interface under electrical stress is visible. Since carbon impurities impact the oxygen vacancy defect population under resistive switching, this dynamic carbon segregation to the Ti/HfO{sub 2} interface is suspected to negatively influence RRAM device endurance. Therefore, these results indicate that the RRAM materials engineering needs to include all impurities in the dielectric layer in order to achieve reliable device performance.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Probing multiscale dissolution dynamics in natural rocks through microfluidics and compositional analysis

Mineral dissolution significantly impacts many geological systems. Carbon released by diagenesis, carbon sequestration, and acid injection are examples where geochemical reactions, fluid flow, and solute transport are strongly coupled. The complexity in these systems involves interplay between various mechanisms that operate at timescales ranging from microseconds to years. Current experimental techniques characterize dissolution processes using static images that are acquired with long measurement times and/or low spatial resolution. These limitations prevent direct observation of how dissolution reactions progress within an intact rock with spatially heterogeneous mineralogy and morphology. We utilize microfluidic cells embedded with thin rock samples to visualize dissolution with significant temporal resolution (100 ms) in a large observation window (3 × 3 mm). Here we injected acidic fluid into eight shale samples ranging from 8 to 86 wt % carbonate. The pre- and postreaction microstructures are characterized at the scale of pores (0.1 to 1 µm) and fractures (1 to 1,000 µm). We observe that nonreactive particle exposure, fracture morphology, and loss of rock strength are strongly dependent on both the relative volume of reactive grains and their distribution. Time-resolved images of the rock unveil the spatiotemporal dynamics of dissolution, including two-phase flow effects in real time and illustrate the changes in the fracture interface across the range of compositions. Moreover, the dynamical data provide an approach for characterizing reactivity parameters of natural heterogeneous samples when porous media effects are not negligible. The platform and workflow provide real-time characterization of geochemical reactions and inform various subsurface engineering processes.

58 GEOSCIENCES↗
DOE OSTI2026

Controlling Deformation in Al/Ti: How Interface Roughness and Orientation Drive Bimetal Mechanics

The microstructural characteristics and morphology of interfaces in metals can be crucial in governing the initiation of plasticity and early deformation mechanisms under extreme conditions. During high-strain-rate deformation, these interfaces significantly affect dislocation nucleation, twinning, and other mechanisms that directly impact material strength and failure. Despite their importance, a substantial knowledge gap remains between the observed macroscopic material behavior and the underlying role of bimetal interfaces in plasticity initiation. Here, to address this gap, large-scale molecular dynamics simulations are performed on Al/Ti bimetal structures to examine the effect of interface characteristics on the onset of plasticity under uniaxial compression. Specifically, this study investigates how interface roughness (flat vs waveform interfaces) modifies the initiation of plastic events in the microstructure. Atomistic simulations indicate that interface roughness (a microscopic behavior) reduces the stress required for dislocation nucleation, thereby reducing the peak stress relative to a flat interface. For the square interface, the step height strongly influences plasticity initiation by setting the separation of locally flat regions. Varying the interface rotation relative to the loading direction (macroscopic behavior) reveals that the peak stress for both flat and waveform interfaces initially decreases and then increases with rotation, accompanied by a shift in dominant mechanisms—from Al twinning (flat) to interface sliding and Ti-dominated phase transformation and twinning at lower angles. The change in the stress-strain slope during initial compression reflects how rotation alters the resolved shear stress and activates different slip systems. Overall, the study provides valuable insights into the role of bimetal interfaces in controlling plasticity initiation and early deformation pathways for Al/Ti under extreme loading conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Structure and dynamics of POPC bilayers in water solutions of room temperature ionic liquids

Molecular dynamics simulations in the NPT ensemble have been carried out to investigate the effect of two room temperature ionic liquids (RTILs), on stacks of phospholipid bilayers in water. We consider RTIL compounds consisting of chloride ([bmim][Cl]) and hexafluorophosphate ([bmim][PF{sub 6}]) salts of the 1-buthyl-3-methylimidazolium ([bmim]{sup +}) cation, while the phospholipid bilayer is made of 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine (POPC). Our investigations focus on structural and dynamical properties of phospholipid and water molecules that could be probed by inelastic and quasi-elastic neutron scattering measurements. The results confirm the fast incorporation of [bmim]{sup +} into the lipid phase already observed in previous simulations, driven by the Coulomb attraction of the cation for the most electronegative oxygens in the POPC head group and by sizeable dispersion forces binding the neutral hydrocarbon tails of [bmim]{sup +} and of POPC. The [bmim]{sup +} absorption into the bilayer favours the penetration of water into POPC, causes a slight but systematic thinning of the bilayer, and further stabilises hydrogen bonds at the lipid/water interface that already in pure samples (no RTIL) display a lifetime much longer than in bulk water. On the other hand, the effect of RTILs on the diffusion constant of POPC (D{sub POPC}) does not reveal a clearly identifiable trend, since D{sub POPC} increases upon addition of [bmim][Cl] and decreases in the [bmim][PF{sub 6}] case. Moreover, because of screening, the electrostatic signature of each bilayer is only moderately affected by the addition of RTIL ions in solution. The analysis of long wavelength fluctuations of the bilayers shows that RTIL sorption causes a general decrease of the lipid/water interfacial tension and bending rigidity, pointing to the destabilizing effect of RTILs on lipid bilayers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Structure and Dynamics of the Liver Receptor Homolog 1–PGC1 α Complex

Peroxisome proliferator-activated gamma coactivator 1-α (PGC1α) regulates energy metabolism by directly interacting with transcription factors to modulate gene expression. Among the PGC1α binding partners is liver receptor homolog 1 (LRH-1; NR5A2), an orphan nuclear hormone receptor that controls lipid and glucose homeostasis. Although PGC1α is known to bind and activate LRH-1, mechanisms through which PGC1α changes LRH-1 conformation to drive transcription are unknown. Here, we used biochemical and structural methods to interrogate the LRH-1–PGC1α complex. Purified, full-length LRH-1, as well as isolated ligand binding domain, bound to PGC1α with higher affinity than to the coactivator, nuclear receptor coactivator-2 (Tif2), in coregulator peptide recruitment assays. We present the first crystal structure of the LRH-1–PGC1α complex, which depicts several hydrophobic contacts and a strong charge clamp at the interface between these partners. In molecular dynamics simulations, PGC1α induced correlated atomic motion throughout the entire LRH-1 activation function surface, which was dependent on charge-clamp formation. In contrast, Tif2 induced weaker signaling at the activation function surface than PGC1α but promoted allosteric signaling from the helix 6/β-sheet region of LRH-1 to the activation function surface. These studies are the first to probe mechanisms underlying the LRH-1–PGC1α interaction and may illuminate strategies for selective therapeutic targeting of PGC1α-dependent LRH-1 signaling pathways.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2020

Characterizing the diverse hydrogeology underlying rivers and estuaries using new floating transient electromagnetic methodology

We report the hydrogeology below large surface water features such as rivers and estuaries is universally under-informed at the long reach to basin scales (tens of km+). This challenge inhibits the accurate modeling of fresh/saline groundwater interfaces and groundwater/surface water exchange patterns at management-relevant spatial extents. Here we introduce a towed, floating transient electromagnetic (TEM) system (i.e. FloaTEM) for rapid (up to 15 km/h) high resolution electrical mapping of the subsurface below large water bodies to depths often a factor of 10 greater than other towed instruments. The novel FloaTEM system is demonstrated at a range of diverse 4th through 6th-order riverine settings across the United States including 1) the Farmington River, near Hartford, Connecticut; 2) the Upper Delaware River near Barryville, New York; 3) the Tallahatchie River near Shellmound, Mississippi; and, 4) the Eel River estuary, on Cape Cod, near Falmouth, Massachusetts. Airborne frequency-domain electromagnetic and land-based towed TEM data are also compared at the Tallahatchie River site, and streambed geologic scenarios are explored with forward modeling. A range of geologic structures and pore water salinity interfaces were identified. Process-based interpretation of the case study data indicated FloaTEM can resolve varied sediment-water interface materials, such as the accumulation of fines at the bottom of a reservoir and permeable sand/gravel riverbed sediments that focus groundwater discharge. Bedrock layers were mapped at several sites, and aquifer confining units were defined at comparable resolution to airborne methods. Terrestrial fresh groundwater discharge with flowpaths extending hundreds of meters from shore was also imaged below the Eel River estuary, improving on previous hydrogeological characterizations of that nutrient-rich coastal exchange zone. In summary, the novel FloaTEM system fills a critical gap in our ability to characterize the hydrogeology below surface water features and will support more accurate prediction of groundwater/surface water exchange dynamics and fresh-saline groundwater interfaces.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Nonequilibrium statistical thermodynamics of multicomponent interfaces

Nonequilibrium interfacial thermodynamics has important implications for crucial biological, physical, and industrial-scale transport processes. Here, we discuss a theory of local equilibrium for multiphase multicomponent interfaces that builds upon the “sharp” interface concept first introduced by Gibbs, allowing for a description of nonequilibrium interfacial processes such as those arising in evaporation, condensation, adsorption, etc. By requiring that the thermodynamics be insensitive to the precise location of the dividing surface, one can identify conditions for local equilibrium and develop methods for measuring the values of intensive variables at the interface. We then use extensive, high-precision nonequilibrium molecular dynamics (NEMD) simulations to verify the theory and establish the validity of the local equilibrium hypothesis. In particular, we demonstrate that equilibrium equations of state are also valid out of equilibrium, and can be used to determine interfacial temperature and chemical potential(s) that are consistent with nonequilibrium generalizations of the Clapeyron and Gibbs adsorption equations. We also show, for example, that, far from equilibrium, temperature or chemical potential differences need not be uniform across an interface and may instead exhibit pronounced discontinuities. However, even in these circumstances, we demonstrate that the local equilibrium hypothesis and its implications remain valid. These results provide a thermodynamic foundation and computational tools for studying or revisiting a wide variety of interfacial transport phenomena.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Facet-dependent structure and dissociation of water at pristine IrO 2 /water interfaces

Understanding the microscopic structure of water at metal oxide interfaces is crucial for advancing electrocatalysis. IrO 2 , specifically, has shown exceptional activity for electrochemical water oxidation, but we currently lack a fundamental understanding of how the surface structure of IrO 2 impacts water reactivity. In this work, we developed a machine learning potential trained to first-principles accuracy for modeling IrO 2 /water interfaces across different facets: (110), (100), (101), and (001). Using extensive machine learning molecular dynamics simulations, we investigated the spontaneous dissociation of water molecules at these interfaces. Our results reveal a distinct dissociation probability trend: (110) > (100) ≈ (101) > (001), which we attribute primarily to the reaction thermodynamics of surface water dissociation. A strong correlation is observed between the surface Ir–O bond distances and the dissociation probabilities, highlighting the role of surface geometry in modulating reactivity. As a consequence, the interfacial solvation structures and hydrogen bonding environments are dynamically tuned by the varying water dissociation capabilities across facets. This work elucidates how water dissociation energetics depend on surface orientation and interfacial structure, offering atomistic insights into manipulating reaction chemistry at electrocatalytic interfaces.

organic↗
DOE OSTI2014

Near-surface density profiling of Fe ion irradiated Si (100) using extremely asymmetric x-ray diffraction by variation of the wavelength

In this work, we report on correlations between surface density variations and ion parameters during ion beam-induced surface patterning process. The near-surface density variations of irradiated Si(100) surfaces were investigated after off-normal irradiation with 5 keV Fe ions at different fluences. In order to reduce the x-ray probing depth to a thickness below 5 nm, the extremely asymmetrical x-ray diffraction by variation of wavelength was applied, exploiting x-ray refraction at the air-sample interface. Depth profiling was achieved by measuring x-ray rocking curves as function of varying wavelengths providing incidence angles down to 0°. The density variation was extracted from the deviations from kinematical Bragg angle at grazing incidence angles due to refraction of the x-ray beam at the air-sample interface. The simulations based on the dynamical theory of x-ray diffraction revealed that while a net near-surface density decreases with increasing ion fluence which is accompanied by surface patterning, there is a certain threshold of ion fluence to surface density modulation. Our finding suggests that the surface density variation can be relevant with the mechanism of pattern formation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Spiers Memorial Lecture: Water at interfaces

In this article we discuss current issues in the context of the four chosen subtopics for the meeting: dynamics and nano-rheology of interfacial water, electrified/charged aqueous interfaces, ice interfaces, and soft matter/water interfaces.

Devlin, Shane W.↗
DOE OSTI2021

Anomalous interfacial dynamics of single proton charges in binary aqueous solutions

Our understanding of the dynamics of charge transfer between solid surfaces and liquid electrolytes has been hampered by the difficulties in obtaining interface, charge, and solvent-specific information at both high spatial and temporal resolution. Here, we measure at the single charge scale the dynamics of protons at the interface between an hBN crystal and binary mixtures of water and organic amphiphilic solvents (alcohols and acetone), evidencing a marked influence of solvation on interfacial dynamics. Applying single-molecule localization microscopy to emissive crystal defects, we observe correlated activation between adjacent ionizable surface defects, mediated by the transport of single excess protons along the solid/liquid interface. Solvent content has a nontrivial effect on interfacial dynamics, leading at intermediate water fraction to an increased surface diffusivity, as well as an increased affinity of the proton charges to the solid surface. Our measurements evidence the notable role of solvation on interfacial proton charge transport.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Thermal unfolding of barstar and the properties of interfacial water around the unfolded forms

Identification of the intermediates along the folding-unfolding pathways and probing their interactions with surrounding solvent are two important but relatively unexplored issues in protein folding. In this work, we have carried out atomistic molecular dynamics simulations to study the thermal unfolding of barstar in aqueous solution from its folded native form at two different temperatures (400 K and 450 K). The calculations at 400 K reveal partial unfolding of two α-helices (helix-1 and helix-2) and their interconnecting loop. At 450 K, on the other hand, the entire protein attains an expanded flexible conformation due to disruption of a large fraction of tertiary contacts and breaking of almost all the secondary structures. These two disordered structures obtained at such high temperatures are then studied around room temperature to probe their influence on the properties of surrounding solvent. It is found that though the unfolding of the protein in general leads to increasingly hydrated interface, but new structural motifs with locally dehydrated interface may also form during the structural transition. Additionally, independent of the conformational state of the protein, its influence on surrounding solvent has been found to be restricted to the first hydration layer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗