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DOE OSTI2019

Effect of Ion (Ar{sup +}) Irradiation on Cluster Magnetism and Magnetic Interactions in Fe{sub 67}Cr{sub 18}B{sub 15} Amorphous Alloy

The comparison of the resonance magnetic absorption spectra with the data on structure and magnetic properties of Fe{sub 67}Cr{sub 18}B{sub 15} amorphous samples has shown that a randomly inhomogeneous medium of amorphous alloy is multiphase. Two types of samples with the same chemical composition, but with a different clusterized structure, and the use of (Ar{sup +}) ion irradiation in the experiment made it possible to separate four basic phases with different magnetic properties. The basic phase α-(Fe,Cr) contains large clusters of D < 400 Å in size with a tendency to phase separation of iron (α-Fe) and chromium (α-Cr), which under irradiation, enhances the competing FM and AFM magnetic interactions and increases the intensity of the resonance magnetic absorption lines associated with α-Fe and α-Cr. The phase Fe{sub 3}B (D < 100 Å) is detected by independent line in the resonance absorption spectra only when its groupings are isolated from the α-(Fe,Cr) metal phase clusters. The fourth phase contains precluster groupings and disappears when the sample is irradiated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Effects of Non-Electrostatic Intermolecular Interactions on the Phase Behavior of pH-Sensitive Polyelectrolyte Complexes

Polyelectrolyte complexes (PECs) offer enormous material tunability and desirable functionalities, and consequently have found broad utility in biomedical and material industries. While poly(acrylic acid) (PAA) and poly( allylamine hydrochloride) (PAH) are a commonly used pairing, various aspects of the phase behavior of PAA-PAH complexes have not been sufficiently quantified. In this work, we present a comprehensive experimental study depicting the binodal phase boundaries for the PAA-PAH complexes prepared under acidic, neutral, and basic conditions using thermogravimetric analysis, turbidimetry, and optical microscopy. Under neutral and basic conditions, phase behaviors of the complexes were largely similar to one another and followed general expectations of PEC phase behavior, except for unusually high resistance to disruption of the complex with added salt. Stable complexes are observed up to 4 M NaCl concentrations. Under acidic conditions, strikingly different phase behaviors of the PAA-PAH complexes were observed. The polymer content in the complex phase increased initially, followed by an expected decrease as salt was added to the complexes. This behavior may result from a combination of associative phase separation of PAA and PAH chains, influenced by electrostatic interactions, and segregative phase separation, which can be ascribed to the influence of a combination of the hydrophobic interactions of the aliphatic polymer backbone and the interpolymer hydrogen bonding of unionized acrylic monomer units. Our systematic investigations over a range of pH detailing these discrepancies in the PAA-PAH phase behavior are expected to clarify the inconsistencies among the reports in the literature and provide the material design strategies for practical use of the PAA-PAH complexes and multilayer assemblies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

Phase diagrams of mixtures of a polymer and a cholesteric liquid crystal under an external field

We present a mean field theory to describe phase behaviors in mixtures of a polymer and a cholesteric liquid crystal under an external magnetic or electric field. Taking into account a chiral coupling between a polymer and a liquid crystal under the external field, we examine twist-untwist phase transitions and phase separations in the mixtures. It is found that a cholesteric-nematic phase transition can be induced by not only the external field but also concentration and temperature. Depending on the strength of the external field, we predict cholesteric-paranematic (Ch+pN), nematic-paranematic (N+pN), cholesteric-nematic (Ch+N) phase separations, etc., on the temperature-concentration plane. We also discuss mixtures of a non-chiral nematic liquid crystal and a chiral dopant.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Out of the Dark and Into the Light: A New View of Phytochrome Photobodies

Light is a critical environmental stimulus for plants, serving as an energy source via photosynthesis and a signal for developmental programming. Plants perceive light through various light-responsive proteins, termed photoreceptors. Phytochromes are red-light photoreceptors that are highly conserved across kingdoms. In the model plant Arabidopsis thaliana , phytochrome B serves as a light and thermal sensor, mediating physiological processes such as seedling germination and establishment, hypocotyl growth, chlorophyll biogenesis, and flowering. In response to red light, phytochromes convert to a biologically active form, translocating from the cytoplasm into the nucleus and further compartmentalizes into subnuclear compartments termed photobodies. PhyB photobodies regulate phytochrome-mediated signaling and physiological outputs. However, photobody function, composition, and biogenesis remain undefined since their discovery. Based on photobody cellular dynamics and the properties of internal components, photobodies have been suggested to undergo liquid-liquid phase separation, a process by which some membraneless compartments form. Here, we explore photobodies as environmental sensors, examine the role of their protein constituents, and outline the biophysical perspective that photobodies may be undergoing liquid-liquid phase separation. Understanding the molecular, cellular, and biophysical processes that shape how plants perceive light will help in engineering improved sunlight capture and fitness of important crops.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

In-Situ Study of Microstructure Evolution of Spinodal Decomposition in an Al-Rich High-Entropy Alloy

High-entropy alloys (HEAs) are materials which leverage the entropy of mixing to motivate the formation of single-phase solid solutions, even of immiscible elements. While these materials are well-recognized for their application to structural engineering, there is increasing interest in the use of HEAs for functional applications such as memory storage and energy devices. The current work investigates the HEA Al 1.3 CoCrCuFeNi, which has been previously shown to be single-phase at high temperatures, but undergoes phase separation at lower temperatures, transforming the structural and the functional properties. This phase separation is investigated at high temperatures with in-situ small angle neutron scattering (SANS) and scanning transmission electron microscopy (EDS). These techniques show that increasing the temperature up to 800°C, the microstructure of the HEA adiabatically disorders and abruptly homogenizes near 700°C, which is consistent with spinodal decomposition. Overall, the microstructural evolution proceeds mainly by the atomistic redistribution of the constituent elements within simple crystal lattices, producing coherent phase mixtures.

36 MATERIALS SCIENCE↗

DOE OSTI2021

When SLIPS meets TIPS: An endogenous lubricant-infused surface by taking the diluent as the lubricant

Slippery lubricant-infused porous surfaces (SLIPSs) hold great promise in fields requiring adhesion resistance such as self-cleaning, anti-fouling, anti-icing, and anti-scaling. However, their road to practical application is still blocked by the complicated fabrication process and the restricted coating area. To address these challenges, we propose a new concept of endogenous SLIPS in which the porous structure grows from the solution coating of polypropylene/caprylyl methicone undergoing a thermally induced phase separation (TIPS) process. Caprylyl methicone serves as the diluent during TIPS as well as the lubricant in the SLIPS so that the coating can be fabricated in one step and unrestrictedly. Furthermore, the dissolution and phase separation mechanisms have been revealed by molecular dynamic simulation and in situ microscopic observation. Such SLIPSs exhibits impressive sliding property even for sticky and viscous liquids and exhibit extremely low ice adhesion in anti-icing tests.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Assessment of thermal embrittlement in duplex stainless steels 2003 and 2205 for nuclear power applications

Here, duplex stainless steels are desirable for use in power generation systems because of their attractive combination of strength, corrosion resistance and cost. However, thermal embrittlement at intermediate homologous temperatures of ~475 °C and below, limits upper service temperatures for many applications. New lean grade duplex alloys have improved thermal stability over standard grades and potentially increase the upper service temperature or the lifetime at a given temperature for this class of material. The present work compares the thermal stability of lean grade, alloy 2003, to standard grade, alloy 2205, through a series of isothermal agings between 260 °C and 482 °C for times between 1 and 10,000 h. Aged samples were characterized by changes in microhardness and impact toughness. Additionally, atom probe tomography was performed to illustrate the evolution of the alpha-alpha' phase separation in both alloys at select conditions. Atom probe tomography confirmed that phase separation occurs via spinodal decomposition for both alloys, and identified the presence of Ni-Cu-Si-Mn-P clusters in alloy 2205, which may contribute to the embrittlement of this alloy. The impact toughness model predictions for the upper service temperature show that alloy 2003 may be viable for use in 288 degrees C applications for 80-year service lifetimes based on a Charpy V-notch criteria of 47 J at room temperature. In comparison, alloy 2205 should be limited to 260 °C applications for the same room temperature toughness of 47 J.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Local electric field direct writing – Electron-beam lithography and mechanism

Local electric field induced by a focused electron probe in silicate glass thin films is evaluated in this paper by the migration of cations. Extremely strong local electric fields can be obtained by the focused electron probe from a scanning transmission electron microscope. As a result, collective atomic displacements occur. This newly revised mechanism provides an efficient tool to write patterned nanostructures directly, and thus overcome the low efficiency of the conventional electron-beam lithography. Applying this technique to silicate glass thin films, as an example, a grid of rods of nanometer dimension can be efficiently produced by rapidly scanning a focused electron probe. This nanopatterning is achieved through swift phase separation in the sample, without any post-development processes. The controlled phase separation is induced by massive displacements of cations (glass modifiers) within the glass-former network, driven by the strong local electric fields. The electric field is induced by accumulated charge within the electron probed region, which is generated by the excitation of atomic electrons by the incident electron. Throughput is much improved compared to other scanning probe techniques. Finally, the half-pitch spatial resolution of nanostructure in this particular specimen is 2.5 nm.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Crowding-induced mixing behavior of lipid bilayers: Examination of mixing energy, phase, packing geometry, and reversibility

In an effort to develop a general thermodynamic model from first-principles to describe the mixing behavior of lipid membranes, we examined lipid mixing induced by targeted binding of small (Green Fluorescent Protein (GFP)) and large (nanolipoprotein particles (NLPs)) structures to specific phases of phase-separated lipid bilayers. Phases were targeted by incorporation of phase-partitioning iminodiacetic acid (IDA)-functionalized lipids into ternary lipid mixtures consisting of DPPC, DOPC, and cholesterol. GFP and NLPs, containing histidine tags, bound the IDA portion of these lipids via a metal, Cu 2+ , chelating mechanism. In giant unilamellar vesicles (GUVs), GFP and NLPs bound to the Lo domains of bilayers containing DPIDA, and bound to the Ld region of bilayers containing DOIDA. At sufficiently large concentrations of DPIDA or DOIDA, lipid mixing was induced by bound GFP and NLPs. The validity of the thermodynamic model was confirmed when it was found that the statistical mixing distribution as a function of crowding energy for smaller GFP and larger NLPs collapsed to the same trend line for each GUV composition. Moreover, results of this analysis show that the free energy of mixing for a ternary lipid bilayer consisting of DOPC, DPPC, and cholesterol varied from 7.9 × 10 –22 to 1.5 × 10 –20 J/lipid at the compositions observed, decreasing as the relative cholesterol concentration was increased. It was discovered that there appears to be a maximum packing density, and associated maximum crowding pressure, of the NLPs, suggestive of circular packing. A similarity in mixing induced by NLP1 and NLP3 despite large difference in projected areas was analytically consistent with monovalent (one histidine tag) versus divalent (two histidine tags) surface interactions, respectively. In addition to GUVs, binding and induced mixing behavior of NLPs was also observed on planar, supported lipid multibilayers. Furthermore, the mixing process was reversible, with Lo domains reappearing after addition of EDTA for NLP removal.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2014

Electric-field-controlled interface strain coupling and non-volatile resistance switching of La{sub 1-x}Ba{sub x}MnO₃ thin films epitaxially grown on relaxor-based ferroelectric single crystals

We have fabricated magnetoelectric heterostructures by growing ferromagnetic La{sub 1-x}Ba{sub x}MnO₃ (x=0.2, 0.4) thin films on (001)-, (110)-, and (111)-oriented 0.31Pb(In{sub 1/2}Nb{sub 1/2})O₃-0.35Pb(Mg{sub 1/3}Nb{sub 1/2})O₃-0.34PbTiO₃ (PINT) ferroelectric single-crystal substrates. Upon poling along the [001], [110], or [111] crystal direction, the electric-field-induced non-180° domain switching gives rise to a decrease in the resistance and an enhancement of the metal-to-insulator transition temperature T C of the films. By taking advantage of the 180° ferroelectric domain switching, we identify that such changes in the resistance and T C are caused by domain switching-induced strain but not domain switching-induced accumulation or depletion of charge carriers at the interface. Further, we found that the domain switching-induced strain effects can be efficiently controlled by a magnetic field, mediated by the electronic phase separation. Moreover, we determined the evolution of the strength of the electronic phase separation against temperature and magnetic field by recording the strain-tunability of the resistance [(ΔR/R){sub strain}] under magnetic fields. Additionally, opposing effects of domain switching-induced strain on ferromagnetism above and below 197 K for the La₀.₈Ba₀.₂MnO₃ film and 150 K for the La₀.₆Ba₀.₄MnO₃ film, respectively, were observed and explained by the magnetoelastic effect through adjusting the magnetic anisotropy. Finally, using the reversible ferroelastic domain switching of the PINT, we realized non-volatile resistance switching of the films at room temperature, implying potential applications of the magnetoelectric heterostructure in non-volatile memory devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Ferromagnetism in Laves-phase WFe{sub 2} nanoparticles

While rare-earth based Laves phases are known to exhibit large magnetostriction, the magnetic properties of some binary Laves phases containing transition metals alone are not well known. This is because many of these compounds contain refractory elements that complicate melt processing due to high melting temperatures and extensive phase separation. Here, phase-pure WFe{sub 2} nanoclusters, with the hexagonal C14 Laves structure, were deposited via inert gas condensation, allowing for the first known measurement of ferromagnetism in this phase, with M{sub S} of 26.4 emu/g (346 emu/cm{sup 3}) and a K{sub U} of 286 kerg/cm{sup 3}, at 10 K, and a T{sub C} of 550 K.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Quantum Ising model on (2+1)-dimensional anti–de Sitter space using tensor networks

We study the quantum Ising model on (2+1)-dimensional anti-de Sitter space using matrix product states (MPS) and matrix product operators (MPOs). We explore the bulk phase diagram of the theory on regular tessellations of hyperbolic space with coordination number seven and find disordered and ordered phases separated by a phase transition. We find that the boundary-boundary spin correlation function exhibits power law scaling deep in the disordered phase of the Ising model consistent with holography. At the critical point, we find the boundary entanglement entropy scales logarithmically with subsystem size but away from this, we see a linear scaling. In comparison, the full system exhibits a volume law scaling, which is expected in chaotic and/or highly connected systems. We also measure out of time ordered correlators (OTOCs) to explore the scrambling behavior of the theory.

Quantum spin models↗

NASA NTRS2002

PCS: The First Fluid Physics Payload on ISS

The Physics of Colloids in Space (PCS) experiment was accommodated within International Space Station (ISS) EXpedite the PRocessing of Experiments to Space Station (EXPRESS) Rack 2 and was remotely operated from early June 2001 until February 2002 from NASA Glenn Research Center's Telescience Support Center in Cleveland, Ohio and from a remote site at Harvard University in Cambridge, Massachusetts. PCS is an experiment conceived by Professor David A. Weitz of Harvard University (the Principal Investigator), focusing on the behavior of three different classes of colloid mixtures. The sophisticated light scattering instrumentation comprising PCS is capable of color imaging, and dynamic and static light scattering from 11 to 169 degrees, Bragg scattering over the range from 10 to 60 degrees, and laser light scattering at low angles from 0.3 to 6.0 degrees. The PCS instrumentation performed remarkably well, demonstrating a flexibility that enabled experiments to be performed that had not been envisioned prior to launch. While on-orbit, PCS accomplished 2400 hours of science operations, and was declared a resounding success. Each of the eight sample cells worked well and produced interesting and important results. Crystal nucleation and growth and the resulting structures of two binary colloidal crystal alloys were studied, with the long duration microgravity environment of the ISS facilitating extended studies on the growth and coarsening characteristics of the crystals. In another experiment run, the de-mixing of the colloid-polymer critical-point sample was studied as it phase-separates into two phases, one that resembles a gas and one that resembles a liquid. This process was studied over four decades of length scale, from 1 micron to 1 centimeter, behavior that cannot be observed in this sample on Earth because sedimentation would cause the colloids to fall to the bottom of the cell faster than the de-mixing process could occur. Similarly, the study of gelation and aging of another colloid-polymer sample, the colloid-polymer gel, also provided valuable information on gelation mechanisms, as did investigations on the extremely the low concentration silica and polystyrene fractal gel samples.

Doherty, M.↗

NASA NTRS2002

Results From the Physics of Colloids Experiment on ISS

Weitz, David↗

DOE OSTI2021

Controlling the Morphology of Dynamic Thia-Michael Networks to Target Pressure-Sensitive and Hot Melt Adhesives

A series of multistage (pressure-sensitive/hot melt) adhesives utilizing dynamic thia-Michael bonding motifs are reported. The benzalcyanoacetate Michael acceptors used in this work undergo bond exchange under ambient conditions without external catalysis, facilitating pressure-sensitive adhesion. A key feature of this system is the dynamic reaction-induced phase separation that lends reinforcement to the otherwise weakly bonded materials, enabling weak, repeatable pressure-sensitive adhesion under ambient conditions and strong adhesion when processed as a hot melt adhesive. Furthermore, by using different pairs of benzalcyanoacetate cross-linking units, the phase separation characteristics of the adhesives can be directly manipulated, allowing for a tailored adhesive response.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2013

Advanced Colloids Experiment (ACE) Science Overview

The Advanced Colloids Experiment is being conducted on the International Space Station (ISS) using the Light Microscopy Module (LMM) in the Fluids Integrated Rack (FIR). Work to date will be discussed and future plans and opportunities will be highlighted. The LMM is a microscope facility designed to allow scientists to process, manipulate, and characterize colloidal samples in micro-gravity where the absence of gravitational settling and particle jamming enables scientists to study such things as:a.The role that disordered and ordered-packing of spheres play in the phase diagram and equation of state of hard sphere systems,b.crystal nucleation and growth, growth instabilities, and the glass transition, c.gelation and phase separation of colloid polymer mixtures,d.crystallization of colloidal binary alloys,e.competition between crystallization and phase separation,f.effects of anisotropy and specific interactions on packing, aggregation, frustration and crystallization,g.effects of specific reversible and irreversible interactions mediated in the first case by hybridization of complementary DNA strands attached to separate colloidal particles,h.Lock and key interactions between colloids with dimples and spheres which match the size and shape of the dimples,i.finding the phase diagrams of isotropic and interacting particles,j.new techniques for complex self-assembly including scenarios for self-replication, k.critical Casimir forces,l.biology (real and model systems) in microgravity,m.etc. By adding additional microscopy capabilities to the existing LMM, NASA will increase the tools available for scientists that fly experiments on the ISS enabling scientists to observe directly what is happening at the particle level. Presently, theories are needed to bridge the gap between what is being observed (at a macroscopic level when photographing samples) with what is happening at a particle (or microscopic) level. What is happening at a microscopic level will be directly accessible with the availability of the Light Microscopy Module (LMM) on ISS. To meet these goals, the ACE experiment is being built-up in stages, with the availability of confocal microscopy being the ultimate objective. Supported by NASAs Physical Sciences Research Program, ESAESTEC, and the authors respective governments.

Microgravity Biology Research↗

DOE OSTI2023

Microphysics of liquid water in sub-10 nm ultrafine aerosol particles

Abstract. Ultrafine aerosol particles with sizes smaller than 50 nm have been shown in recent studies to serve as a large source of cloud condensation nuclei that can promote additional cloud droplet formation under supersaturation conditions. Knowledge of the microphysics of liquid water in these droplets remains limited, particularly in the sub-10 nm particle size range, due to experimental and theoretical challenges associated with the complexity of aerosol components and the small length scales of interest (e.g., difficulty of precisely sampling the liquid–air interface, questionable validity of mean-field theoretical representations). Here, we carried out molecular dynamics (MD) simulations of aerosol particles with diameters between 1 and 10 nm and characterized atomistic-level structure and water dynamics in well-mixed and phase-separated systems with different particle sizes, NaCl salinities, and pimelic acid (PML) organic surface loadings as a function of distance from the time-averaged Gibbs dividing interface or instantaneous water–air interface. We define a sphericity factor (ϕ) that can shed light on the phase-mixing state of nanodroplets, and we reveal an unexpected dependence of mixing state on droplet size. Our results also evidence an ion concentration enhancement in ultrafine aerosols, which should modulate salt nucleation kinetics in sub-10 nm droplets, and provide detailed characterization of the influence of droplet size on surface tension and on water self-diffusivity near the interface. Analysis of water evaporation free energy and water activity demonstrates the validity of the Kelvin equation and Köhler theory at droplet sizes larger than 4 nm under moderate salinities and organic loadings and the need for further extension to account for ion concentration enhancement in sub-10 nm aerosols, droplet-size-dependent phase separation effects, and a sharp decrease in the cohesiveness of liquid water in sub-4 nm droplets. Finally, we show that an idealized fractional surface coating factor (fs) can be used to categorize and reconcile water accommodation coefficients (α*) observed in MD simulations and experimental results in the presence of organic coatings, and we resolve the droplet size dependence of α*.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1992

A novel membrane device for the removal of water vapor and water droplets from air

One of the key challenges facing NASA engineers is the development of systems for separating liquids and gases in microgravity environments. In this paper, a novel membrane-based phase separator is described. This device, known as a water recovery heat exchanger (WRHEX), overcomes the inherent deficiencies of current phase-separation technology. Specifically, the WRHEX cools and removes water vapor or water droplets from feed-air streams without the use of a vacuum or centrifugal force. As is shown in this paper, only a low-power air blower and a small stream of recirculated cool water is required for WRHEX operation. This paper presents the results of tests using this novel membrane device over a wide range of operating conditions. The data show that the WRHEX produces a dry air stream containing no entrained or liquid water - even when the feed air contains water droplets or mist. An analysis of the operation of the WRHEX is presented.

Ray, Rod↗