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DOE OSTI2019

Perfection in Nucleation and Growth of Blue-Phase Single Crystals: Small Free-Energy Required to Self-Assemble at Specific Lattice Orientation

Chemically patterned surfaces can be used to selectively stabilize blue phases as macroscopic single crystals with a prescribed lattice orientation. By tailoring the interfacial free energy through the pattern characteristics, it is possible to set, with nanoscale precision, the optimal conditions to induce spontaneously blue-phase crystal nucleation on the patterned substrate where a uniform, defect-free, blue-phase single crystal is finally formed in a matter of seconds. The chemical patterns taken into consideration in this work are made up of alternated stripelike regions of homeotropic and planar anchoring. By varying the stripe pattern dimension, including the period and ratio of the planar/homeotropic anchoring width, it is possible to generate blue-phase I single crystals with (110) lattice orientation and blue-phase II single crystals with either the (100), (110), or (111) lattice orientation. Continuum mean-field calculations of the studied systems serve to explain, in terms of the free energy of the systems, how the pattern dimensions favor certain crystallographic orientations while penalizing the others. We found that a small free-energy difference is sufficient to drive the nucleation and growth of blue phases into a certain lattice orientation. Furthermore, a processing window for obtaining arbitrary large blue-phase single crystals with predesigned lattice orientation, highly aligned reflective peaks, and significantly short forming time is provided here, which is essential for manufacturing and modulating optical devices and photonics.

36 MATERIALS SCIENCE↗

NASA NTRS2019

Simultaenous Retrieval of Surface Roughness Parameters from Combined Active-Passive SMAP Observations

Soil roughness strongly influences processes like erosion, infiltration, moisture and evaporation of soils as well as growth of agricultural plants. An approach to soil roughness based on active-passive microwave covariation is proposed in order to simultaneously retrieve the vertical RMS height (s) and horizontal correlation length (l) of soil surfaces from simultaneously measured radar and radiometer microwave signatures. The approach is based on a retrieval algorithm for active-passive covariation including the improved Integral Equation Method (I2EM). The algorithm is tested with the global active-passive microwave observations of the SMAP mission. The developed roughness retrieval algorithm shows independence of permittivity for > 10 [-] due to the covariation formalism. Results reveal that s and l can be estimated simultaneously by the proposed approach since surface patterns of non-vegetated areas become evident on global scale. In regions with sandy deserts, like the Sahara or the outback in Australia, determined and confirm rather smooth to semi-rough surface roughness patterns with small vertical RMS heights and corresponding higher horizontal correlation lengths.

correlation length↗

DOE OSTI2017

Shape-Specific Patterning of Polymer-Functionalized Nanoparticles

Chemically and topographically patterned nanoparticles (NPs) with dimensions on the order of tens of nanometers have a diverse range of applications and are a valuable system for fundamental research. Recently, thermodynamically controlled segregation of a smooth layer of polymer ligands into pinned micelles (patches) offered an approach to nanopatterning of polymer-functionalized NPs. Control of the patch number, size, and spatial distribution on the surface of spherical NPs has been achieved, however, the role of NP shape remained elusive. Here, we report the role of NP shape, namely, the effect of the local surface curvature, on polymer segregation into surface patches. For polymer-functionalized metal nanocubes, we show experimentally and theoretically that the patches form preferentially on the high-curvature regions such as vertices and edges. An in situ transformation of the nanocubes into nanospheres leads to the change in the number and distribution of patches; a process that is dominated by the balance between the surface energy and the stretching energy of the polymer ligands. The experimental and theoretical results presented in this work are applicable to surface patterning of polymer-capped NPs with different shapes, which then enables the exploration of patch-directed self-assembly, as colloidal surfactants, and as templates for the synthesis of hybrid nanomaterials.

36 MATERIALS SCIENCE↗

DOE OSTI2024

3D Temperature-Controlled Interchangeable Pattern for Size-Selective Nanoparticle Capture

Patterned surfaces with distinct regularity and structured arrangements have attracted great interest due to their extensive promising applications. Although colloidal patterning has conventionally been used to create such surfaces, herein, we introduce a novel 3D patterned poly(N-isopropylacrylamide) (PNIPAM) surface, synthesized by using a combination of colloidal templating and surface-initiated photoinduced electron transfer-reversible addition–fragmentation chain transfer (SI-PET-RAFT) polymerization. In order to investigate the temperature-driven 3D morphological variations at a lower critical solution temperature (LCST) of ~32 °C, multifaceted characterization techniques were employed. Atomic force microscopy confirmed the morphological transformations at 20 and 40 °C, while water contact angle measurements, upon heating, revealed distinct trends, offering insights into the correlation between surface wettability and topography adaptations. Moreover, quartz crystal microbalance with dissipation monitoring and electrochemical measurements were employed to detect the topographical adjustments of the unique hollow capsule structure within the LCST. Tests using different sizes of PSNPs shed light on the size-selective capture–release potential of the patterned PNIPAM, accentuating its biomimetic open–close behavior. Notably, our approach negates the necessity for expensive proteins, harnessing temperature adjustments to facilitate the noninvasive and efficient reversible capture and release of nanostructures. Finally, this advancement hopes to pave the way for future innovative cellular analysis platforms.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Guided Lithium Deposition by Surface Micro-Patterning of Lithium-Metal Electrodes

Uncontrolled lithium (Li) deposition has hampered the evolution of Li metal electrode-based Li batteries. In this work, we report the differences of a guided Li deposition with a size change of the square hole micro-patterns carved on the Li metal surface with two different dimensions using a simple stamping method. Li deposition is preferentially initiated on the top edge for the smaller pattern and on the bottom for the larger pattern. Although the two patterns lead to a more uniform utilization of the Li, the larger pattern shows a higher cycling stability with a LiFePO4/Li cell than that of the smaller one indicating that initiating the Li deposition from the bottom of the hole is more efficient in confining the deposited Li. Based on the impedance analysis of the compressed Li electrodes, we suggest that the guided Li deposition on the bottom of the hole is attributed to a large contrast in the resistance of native surface passivation layer between the top and hole surfaces. This improved understanding can further advance guided Li deposition induced by surface patterns for high performance Li metal batteries.

Kim, Yun-Jung↗

DOE OSTI2017

Improved block copolymer domain dispersity on chemical patterns via homopolymer-blending and molecular transfer printing

Herein we have investigated the domain width distributions of block copolymers and their ternary blends after directed assembly on chemically patterned surfaces with and without density multiplication. On chemical patterns with density multiplication, the width of the interpolated block copolymer domains was bimodal. Once blended with the corresponding homopolymers, the block copolymers exhibited unimodal distributions of domain width due to the redistribution of homopolymers in the block copolymer domains. When the block copolymers were blended with hydroxyl-terminated homopolymers, the homopolymers with functional end-groups healed the chemical patterns and facilitated the formation of nanostructures with further improved domain width distributions. Lastly, it is demonstrated that the block copolymers achieved the most improved domain width distributions when directed to assemble without density multiplication on one-to-one chemical patterns generated by molecular transfer printing.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Liquid Crystals-Enabled AC Electrokinetics

Phenomena of electrically driven fluid flows, known as electro-osmosis, and particle transport in a liquid electrolyte, known as electrophoresis, collectively form a subject of electrokinetics. Electrokinetics shows a great potential in microscopic manipulation of matter for various scientific and technological applications. Electrokinetics is usually studied for isotropic electrolytes. Recently it has been demonstrated that replacement of an isotropic electrolyte with an anisotropic, or liquid crystal (LC), electrolyte, brings about entirely new mechanisms of spatial charge formation and electrokinetic effects. This review presents the main features of liquid crystal-enabled electrokinetics (LCEK) rooted in the field-assisted separation of electric charges at deformations of the director that describes local molecular orientation of the LC. Since the electric field separates the charges and then drives the charges, the resulting electro-osmotic and electrophoretic velocities grow as the square of the applied electric field. We describe a number of related phenomena, such as alternating current (AC) LC-enabled electrophoresis of colloidal solid particles and fluid droplets in uniform and spatially-patterned LCs, swarming of colloids guided by photoactivated surface patterns, control of LCEK polarity through the material properties of the LC electrolyte, LCEK-assisted mixing at microscale, separation and sorting of small particles. LC-enabled electrokinetics brings a new dimension to our ability to manipulate dynamics of matter at small scales and holds a major promise for future technologies of microfluidics, pumping, mixing, sensing, and diagnostics.

47 OTHER INSTRUMENTATION↗

NASA NTRS1986

Analysis of rotordynamic coefficients of helically-grooved turbulent annular seals

An analysis for helically-grooved turbulent annular seals is developed to predict leakage and dynamic coefficients, as related to rotordynamics. The grooved surface pattern is formulated as an inhomogeneous directivity in surface shear stress. The zeroth-order equations define the steady-state leakage and the circumferential velocity development due to wall shear for a centered rotor position. The first-order equations define perturbations in the pressure and axial and circumferential velocity fields due to small motion of the rotor about the centered position. Numerical results are presented for proposed grooved seals in the High Pressure Oxygen Turbopump (HPTOP) of the Space Shuttle Main Engine (SSME) and for a water-pump application. The results show that an optimum helix angle exists from a rotordynamic stability viewpoint. Further, a properly designed helically-grooved stator is predicted to have pronounced stability advantages over other currently used seals.

Kim, C.-H.↗

NASA NTRS1980

Spaceborne imaging radar - Geologic and oceanographic applications

Synoptic, large-area radar images of the earth's land and ocean surface, obtained from the Seasat orbiting spacecraft, show the potential for geologic mapping and for monitoring of ocean surface patterns. Structural and topographic features such as lineaments, anticlines, folds and domes, drainage patterns, stratification, and roughness units can be mapped. Ocean surface waves, internal waves, current boundaries, and large-scale eddies have been observed in numerous images taken by the Seasat imaging radar. This article gives an illustrated overview of these applications.

Elachi, C.↗

DOE OSTI2023

Correcting Hohlraum Drive Asymmetry with Glow Discharge Polymerization Coated Capsule Shims

In inertial confinement fusion target design, the shape discrepancy between the cylindrical hohlraum and the spherical capsule creates a low mode asymmetry in the implosion. One way to correct such asymmetry is to shim the target capsule surface with extra mass in specific locations following a 3D P4 Legendre mode. Previously, the desired surface pattern was precision machined out of the capsule. The resulting 2DConA experiments that investigated the implosion’s shape demonstrated the shimming method’s success. However, machining leaves large defects on the capsule surface which will degrade neutron yield in a DT implosion. An alternative shimming approach is to grow the pattern on the capsule surface using a glow discharge polymerization coating process in a stencil lithography application. In this study, we discuss the fabrication, characterization and challenges of making shimmed target capsules with this new method.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

On the role of α-alumina in the origin of life: Surface-driven assembly of amino acids

We investigate the hypothesis that mineral/water interfaces played a crucial catalytic role in peptide formation by promoting the self-assembly of amino acids. Using classical molecular dynamics simulations, we demonstrate that the α-alumina(0001) surface exhibits an affinity of 4k B Tfor individual glycine or GG dipeptide molecules due to hydrogen bonds. In simulations with multiple glycine molecules, surface-bound glycine enhances further adsorption, leading to the formation of long chains connected by hydrogen bonds between the carboxyl and amine groups of glycine molecules. We find that the likelihood of observing chains longer than 10 glycine units increases by at least five orders of magnitude at the surface compared to the bulk. This surface-driven assembly is primarily due to local high density and alignment with the alumina surface pattern. Together, these results propose a model for how mineral surfaces can induce configuration-specific assembly of amino acids, thereby promoting condensation reactions.

Science & Technology - Other Topics↗

NASA NTRS2013

The Face that Launched a Thousand Slips

Helene, (approximately 17.6 kilometers mean radius) is an L4 Trojan co-orbital of Saturn's moon Dione. Its hemisphere features an unusual morphology consisting of broad depressions and a generally smooth surface patterned with streaks and grooves. The streaks appear to be oriented down-gradient, as are the grooves. This pattern suggests intensive mass-wasting as a dominant process on the leading hemisphere. Kilometer-scale impact craters are very sparse on the leading hemisphere other than the degraded kilometer-scale basins defining the overall satellite shape, and many small craters have a diffuse appearance suggesting ongoing mass wasting. Thus mass wasting must dominate surface-modifying processes at present. In fact, the mass wasting appears to have been sufficient in magnitude to narrow the divides between adjacent basins to narrow septa, similar, but in lower relief, to the honeycomb pattern of Hyperion. The prominent groves occur primarily near topographic divides and appear have cut into a broad, slightly lower albedo surface largely conforming to the present topography but elevated a few meters above the smooth surfaces undergoing mass wasting flow. Low ridges and albedo markings on the surface suggest surface flow of materials traveling up to several kilometers. Diffusive mass wasting produces smooth surfaces - such a pattern characterizes most of the low-lying surfaces. The grooves, however, imply that the transport process is advective at those locations where they occur, that is, erosion tends to concentrate along linear pathways separated by divides. In fact, in many places grooves have a fairly regular spacing of 125-160 meters, defining a characteristic erosional scale. Several questions are prompted by the unusual morphology of Helene: 1) What is the nature of the surface materials? 2) Are the transport processes gradual or catastrophic motion from one or a few events? 3) What mechanisms drive mass wasting and groove development? 4) Have the formative processes been active in the recent past? 5) Finally, is the surface accreting or eroding? The smooth character of the leading edge hemisphere of Helene and the dominance of mass wasting suggest that the surface is composed of fine-grained debris, probably dominated by dust-size to small gravel particles. The Lagrangian points of saturnian satellites are locations where planetesimals might have accreted to form co-orbital satellites such as and they may capture ejecta from their master moon. Published models suggest that Helene is a site of net accretion, but we find no extant explanation for the dominance of fine grain sizes for the surface (and probable subsurface) composition of Helene and the other Lagrangian satellites. Observation of the mass wasting tracks on Helene suggests the presence of well-defined streams of debris with low bordering levees that may be depositional features or remnants of the dissected higher surface. Some flows in grazing illumination appear to have a convex cross-section. This mass-flow morphology might be consistent with the occurrence of large-scale flow events, but which might have occurred through rapid emplacement or slow glacier-like creep. On the other hand, small craters appear to have been "softened" by creep-like processes, indicating ongoing mass wasting.

honeycomb pattern of Hyperion↗

DOE OSTI2016

Printing-assisted surface modifications of patterned ultrafiltration membranes

Understanding and restricting microbial surface attachment will enhance wastewater treatment with membranes. We report a maskless lithographic patterning technique for the generation of patterned polymer coatings on ultrafiltration membranes. Polyethylene glycol, zwitterionic, or negatively charged hydrophilic polymer compositions in parallel- or perpendicular-striped patterns with respect to feed flow were evaluated using wastewater. Membrane fouling was dependent on the orientation and chemical composition of the coatings. Modifications reduced alpha diversity in the attached microbial community (Shannon indices decreased from 2.63 to 1.89) which nevertheless increased with filtration time. Sphingomonas species, which condition membrane surfaces and facilitate cellular adhesion, were depleted in all modified membranes. Microbial community structure was significantly different between control, different patterns, and different chemistries. Lastly, this study broadens the tools for surface modification of membranes with polymer coatings and for understanding and optimization of antifouling surfaces.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Femtosecond laser induced tunable surface transformations on (111) Si aided by square grids diffraction

We report an extra freedom to modulate the femtosecond laser energy distribution to control the surface ablated structures through a copper-grid mask. Due to the reduced deposited pulse energy by changing the scanning speed or the pulse fluence, a sequential evolution of three distinctly different surface patterns with periodic distributions is formed, namely, striped ripple lines, ripple microdots, and surface modification. By changing the scanning speed, the number of the multiple dots in a lattice can be modulated. Moreover, by exploring the ablation process through the copper grid mask, it shows an abnormal enhanced ablation effect with strong dependence of the diffraction-aided fs laser ablated surface structures on polarization direction. The sensitivity shows a quasi-cosinusoid-function with a periodicity of π/2. Particularly, the connection process of striped ripple lines manifests a preferential formation direction with the laser polarization.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2019

Surface chemistry and composition-induced variation of laser interference-based surface treatment of Al alloys

A key limitation for the use of aluminum alloys in multi-material structural components is effective surface cleaning and texturing techniques to improve the quality of structural joints. In this study, the surface and sub-surface chemistries are investigated for a novel surface treatment method using laser interferometry produced by two beams of a pulsed Nd:YAG laser. Surfaces of AA 5128 aluminum alloy were treated using a two-beam laser interference setup, enabling the structuring of the surface at length scales much less than that of the laser beam. Periodic and patterned surface structures were created by the interference power profile through ablation of deposits and debris and melting and re-solidification of the near-surface region during laser-treatment. Chemical changes to the Al alloy surface induced by laser treatment were examined in detail in this study using both x-ray photoelectron spectroscopy (XPS) and scanning Auger microanalysis (SAM) as a function of number of interfering laser shots. XPS surface analysis indicates that this laser technique is effective at cleaning aluminum surfaces. Furthermore, SAM data indicated that there is a compositional-induced variation of Mg due to laser-interference as Mg-rich areas were found in periodic interference-structured ridges.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Enhanced resistance to decay of imprinted nanopatterns in thin films by bare nanoparticles compared to polymer-grafted nanoparticles

We extend a previous study on the influence of nanoparticles on the decay of nanoimprinted polymer film patterns to compare the effects of “bare” silica (SiO 2 ) nanoparticles and SiO 2 nanoparticles with grafted polymer layers having the same chemical composition as the polymer matrix. This method involves nanoimprinting substrate-supported polymer films using a pattern replicated from a digital versatile disc (DVD), and then annealing the patterned polymer nanocomposite films at elevated temperatures to follow the decay of the topographic surface pattern with time by atomic force microscopy imaging after quenching. We quantified the relaxation of the pattern height (“slumping”) and determined the relaxation time τ for this pattern decay process as a function of nanoparticle filler type and concentration to determine how nanoparticle additives influence relative film stability. Attractive interactions between the bare nanoparticles and the polymer matrix significantly enhance the thermal resilience of the nanopatterns to decay, compared to those of the particle brushes, wherein the particle core interactions are screened from the matrix via the brush layer. A novel aspect of this method is that it readily lends itself to in situ film relaxation measurements in a manufacturing context. We observe that the relaxation time of the pattern relaxation exhibits entropy–enthalpy compensation in the free energy parameters governing the pattern relaxation process as a function of temperature, irrespective of the NP system used, consistent with our previous experimental and computational studies.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Determining protein polarization proteome-wide using physical dissection of individual Stentor coeruleus cells

Cellular components are non-randomly arranged with respect to the shape and polarity of the whole cell. Patterning within cells can extend down to the level of individual proteins and mRNA. But how much of the proteome is actually localized with respect to cell polarity axes? Proteomics combined with cellular fractionation has shown that most proteins localize to one or more organelles but does not tell us how many proteins have a polarized localization with respect to the large-scale polarity axes of the intact cell. Genome-wide localization studies in yeast found that only a few percent of proteins have a localized position relative to the cell polarity axis defined by sites of polarized cell growth. Here, we describe an approach for analyzing protein distribution within a cell with a visibly obvious global patterning - the giant ciliate Stentor coeruleus. Ciliates, including Stentor, have highly polarized cell shapes with visible surface patterning. A Stentor cell is roughly 2mmlong, allowing a ‘‘proteomic dissection’’ in which microsurgery is used to separate cellular fragments along the anterior-posterior axis, followed by comparative proteomic analysis. In our analysis, 25% of the proteome, including signaling proteins, centrin/SFI proteins, and GAS2 orthologs, shows a polarized location along the cell’s anterior-posterior axis. We conclude that a large proportion of all proteins are polarized with respect to global cell polarity axes and that proteomic dissection provides a simple and effective approach for spatial proteomics.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2026

Optimized Tandem Catalyst Patterning for CO 2 Reduction Flow Reactors

Tandem catalysis involves two or more catalysts arranged in proximity within a single reaction vessel, with the aim of synergistically aligning the catalysts’ reaction pathways to maximize overall system performance. This study presents a proof of concept showing the integration of continuum transport modeling with design optimization in a simplified two-dimensional flow reactor setup for electrochemical CO 2 reduction. Ag catalysts provide the CO 2 ⟶ CO reaction capability, and Cu catalysts provide the CO ⟶ high-value products reaction capability. Given a set of input parameters, the optimization algorithm uses adjoint methods to modify the Ag/Cu surface patterning in order to maximize the current density toward high-value products, such as ethylene. The optimized designs yield significant performance enhancement especially at more negative applied voltages (i.e., stronger surface reactions) and for larger numbers of patterning sections. For an applied voltage of −1.7 V vs. SHE, the 12-section optimized design increases the current density toward ethylene by up to 65% compared to the unoptimized 2-section design. For the optimized cases, observed differences in the production and consumption of CO (the key intermediate species) and minimized zones of low CO reactant surface concentration on Cu sections explain the improved reactor performance.

CO2 reduction↗