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Results for “colloidal templating”

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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53 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Synthesis of Core@Shell Cu-Ni@Pt-Cu Nano-Octahedra and Their Improved MOR Activity

Fabrication of 3d metal-based core@shell nanocatalysts with engineered Pt-surfaces provides an effective approach for improving the catalytic performance. The challenges in such preparation include shape control of the 3d metallic cores and thickness control of the Pt-based shells. Herein, we report a colloidal seed-mediated method to prepare octahedral CuNi@Pt-Cu core@shell nanocrystals using CuNi octahedral cores as the template. By precisely controlling the synthesis conditions including the deposition rate and diffusion rate of the shell-formation through tuning the capping ligand, reaction temperature, and heating rate, uniform Pt-based shells can be achieved with a thickness of < 1 nm. Furthermore, the resultant carbon-supported CuNi@Pt-Cu core@shell nano-octahedra showed superior activity in electrochemical methanol oxidation reaction (MOR) compared with the commercial Pt/C catalysts and carbon-supported CuNi@Pt-Cu nano-polyhedron counterparts, demonstrating that both the lattice strain and shape effects arising from the as-prepared CuNi@Pt-Cu octahedral nanocatalysts play a crucial role in MOR performance.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Building superlattices from individual nanoparticles via template-confined DNA-mediated assembly

DNA programmable assembly has been combined with top-down lithography to construct superlattices of discrete, reconfigurable nanoparticle architectures on a gold surface over large areas. Specifically, the assembly of individual colloidal plasmonic nanoparticles with different shapes and sizes is controlled by oligonucleotides containing “locked” nucleic acids and confined environments provided by polymer pores to yield oriented architectures that feature tunable arrangements and independently controllable distances at both nanometer- and micrometer-length scales. These structures, which would be difficult to construct by other common assembly methods, provide a platform to systematically study and control light-matter interactions in nanoparticle-based optical materials. The generality and potential of this approach are explored by identifying a broadband absorber with a solvent polarity response that allows dynamic tuning of visible light absorption.

36 MATERIALS SCIENCE↗
DOE OSTI2021

The diversity of three-dimensional photonic crystals

Many butterflies, birds, beetles, and chameleons owe their spectacular colors to the microscopic patterns within their wings, feathers, or skin. When these patterns, or photonic crystals, result in the omnidirectional reflection of commensurate wavelengths of light, it is due to a complete photonic band gap (PBG). The number of natural crystal structures known to have a PBG is relatively small, and those within the even smaller subset of notoriety, including diamond and inverse opal, have proven difficult to synthesize. Here, we report more than 150,000 photonic band calculations for thousands of natural crystal templates from which we predict 351 photonic crystal templates – including nearly 300 previously-unreported structures – that can potentially be realized for a multitude of applications and length scales, including several in the visible range via colloidal self-assembly. With this large variety of 3D photonic crystals, we also revisit and discuss oft-used primary design heuristics for PBG materials.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Colloidal plasmonic DNA-origami with photo-switchable chirality in liquid crystals

Photo-responsive nanomaterials hold great promise for realizing information processing devices, micro-machines and biosensors. Scalable assembly of such materials using mesostructured liquids such as liquid crystals remains a challenge due to the poor compatibility of nanostructures and the host medium. Here we demonstrate a new type of colloidal dispersion of plasmonic DNA-origami with photo-switchable chirality in cellulose nanofiber-based liquid crystals. The composite material inherits properties of DNA-origami plasmonic nanostructures, so that the composite’s chirality can be erased by ultraviolet light and recovered by visible light. Here, the cellulose nanofibers provide a liquid crystalline host with weak optical birefringence, which barely affects the polarization of the incident light, so that the response is dominated by circular dichroism of uniformly dispersed plasmonic nanostructures. Our approach may serve as a new platform for scalable assembling DNA origami-templated nanomaterials.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2018

Highly Stable, Ultrasmall Polymer-Grafted Nanobins (usPGNs) with Stimuli-Responsive Capability

In this work, highly stable and stimuli/pH-responsive ultrasmall polymer-grafted nanobins (usPGNs) have been developed by grafting a small amount (10 mol %) of short (4.3 kDa) cholesterol-terminated poly(acrylic acid) (Chol-PAA) into an ultrasmall unilamellar vesicle (uSUV). The usPGNs are stable against fusion and aggregation over several weeks, exhibiting over 10-fold enhanced cargo retention in biologically relevant media at pH 7.4 in comparison with the parent uSUV template. Coarse-grained molecular dynamics (CGMD) simulations confirm that the presence of the cholesterol moiety can greatly stabilize the lipid bilayer. They also show extended PAA chain conformations that can be interpreted as causing repulsion between colloidal particles, thus stabilizing them against fusion. Notably, CGMD predicted a clustering of the Chol-PAA chains on the lipid bilayer under acidic conditions due to intra- and interchain hydrogen bonding, leading to the destabilization of local membrane areas. This explains the experimental observation that usPGNs can be triggered to release a significant amount of cargo upon acidification to pH 5. These developments put the lipid-bilayer-embedded Chol-PAA in stark contrast with traditional poly(acrylic acid) systems where the molar mass (M n ) of the polymer chains must exceed 16.5 kDa to achieve stimuli-responsive changes in conformation. They also distinguish the small usPGNs from the much-larger polymer-caged nanobin platform where the Chol-PAA chains must be covalently cross-linked to engender stimuli-responsive behaviors.

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

Compact quantum dot surface modification to enable emergent behaviors in quantum dot-DNA composites

Quantum dot (QD) biological imaging and sensing applications often require surface modification with single-stranded deoxyribonucleic acid (ssDNA) oligonucleotides. Furthermore, ssDNA conjugation can be leveraged for precision QD templating via higher-order DNA nanostructures to exploit emergent behaviors in photonic applications. Use of ssDNA-QDs across these platforms requires compact, controlled conjugation that engenders QD stability over a wide pH range and in solutions of high ionic strength. However, cur-rent ssDNA-QD conjugation approaches suffer from limitations, such as the requirement for thick coatings, low control over ssDNA labeling density, requirement of large amounts of ssDNA, or low colloidal or photostability, restraining implementation in many applications. Here, we combine thin, multidentate, phytochelatin-3 (PC3) QD passivation techniques with strain-promoted copper-free alkyne-azide click chemistry to yield functional ssDNA-QDs with high stability. This process was broadly applicable across QD sizes (i.e.,λ em = 540, 560, 600 nm), ssDNA lengths (i.e., 10–16 base pairs, bps), and sequences (poly thymine, mixed bps). The resulting compacts sDNA-QDs displayed a fluorescence quenching efficiency of up to 89% by hybridization with complementary ssDNA-AuNPs. Further-more, ssDNA-QDs were successfully incorporated with higher-order DNA origami nanostructure templates. Finally, this approach, combining PC3 passivation with click chemistry, generates ssDNA-PC3-QDs that enable emergent QD properties in DNA-based devices and applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Directing the far-from-equilibrium assembly of nanoparticles in confined liquid crystals by hydrodynamic fields

The assembly of nematic colloids relies on long-range elastic interactions that can be manipulated through external stimuli. Confinement and the presence of a hydrodynamic field alter the defect structures and the energetic interactions between the particles. Here, the assembly landscape of nanoparticles embedded in a nematic liquid crystal confined in a nanochannel under a pressure-driven flow is determined. The dynamics of the liquid crystal tensor alignment field is determined through a Poisson-Bracket framework, namely the Stark–Lubensky equations, coupled with the zero-Reynolds momentum equations and the liquid crystal Landau-de Gennes free energy functional. A second order semi-implicit time integration and a three-dimensional Galerkin finite element method are used to resolve flow and nematic fields under several conditions. In general, the zero Reynolds flow displaces the defects around the particles in the upstream direction and renders the surface anchoring ineffective when the flow strength dominates over the nematic elasticity. More importantly, the potential of mean force for particle assembly is non-monotonic independent of surface anchoring. Our results show that the confinement length scale determines the repulsion/attraction transition between colloids, while the flow strength modifies the static defect structure surrounding the particles and determines the magnitude of the energetic barrier for successful assembly. In the attractive regime, the particles move at different rates through the nematic until one particle eventually catches up with the other. This process occurs against or along the direction of flow depending on the flow strength. Ultimately, these results provide a template for engineering and controlling the transport and assembly of nanoparticles under far-from equilibrium conditions in anisotropic media.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Lattice-scale variations in viscosity are correlated with solution structure at mineral-water interfaces

At solid-liquid interfaces, the viscosity increases markedly from the bulk due to the collective interactions of ions and water molecules, influencing phenomena relevant to nanofluidics, colloidal dynamics, and electrochemistry. Here, in this study, we investigated dissipative forces at the boehmite-water interface using 3D atomic force microscopy. We observed an increase in interfacial solution viscosity, η, by 10-100-fold as the nanoprobe approached the surface in normal direction, with up to four oscillatory features showing average peaks of η/η bulk = 44-71. Moreover, the viscosity showed sub-nanometer variations within 0.5 nm from the interface, templated by the underlying crystal lattice and correlated with the interfacial solution structure. Beyond a near-wall region of approximately 1.2 nm, the dissipative response was comparable to that in bulk solution. Molecular dynamics simulations, along with statistical mechanical analyses, provided details on hydrodynamic structures near the interface. Specifically, the lattice-dependent dissipative responses are correlated with extensive hydrogen bonding by interfacial water molecules, which increased friction, particularly along the [001] direction. These results demonstrate how solution viscosity at mineral-water interfaces is anisotropic and correlated with the local solution structure, providing insights into the dynamics of nanocrystal attachment.

Viscosity↗
DOE OSTI2018

DNA-Mediated Size-Selective Nanoparticle Assembly for Multiplexed Surface Encoding

Multiplexed surface encoding is achieved by positioning two different sizes of gold nanocubes on gold surfaces with precisely defined locations for each particle via template-confined, DNA-mediated nanoparticle assembly. As a proof-of-concept demonstration, cubes with 86 and 63 nm edge lengths are assembled into arrangements that physically and spectrally encrypt two sets of patterns in the same location. These patterns can be decrypted by mapping the absorption intensity of the substrate at $λ$ = 773 and 687 nm, respectively. This multiplexed encoding platform dramatically increases the sophistication and density of codes that can be written using colloidal nanoparticles, which may enable high-security, high-resolution encoding applications.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Structure Prediction of Ionic Epitaxial Interfaces with Ogre Demonstrated for Colloidal Heterostructures of Lead Halide Perovskites

Colloidal epitaxial heterostructures are nanoparticles composed of two different materials connected at an interface, which can exhibit properties different from those of their individual components. Combining dissimilar materials offers exciting opportunities to create a wide variety of functional heterostructures. However, assessing structural compatibility–the main prerequisite for epitaxial growth–is challenging when pairing complex materials with different lattice parameters and crystal structures. This complicates both the selection of target heterostructures for synthesis and the assignment of interface models when new heterostructures are obtained. Here, we demonstrate Ogre as a powerful tool to accelerate the design and characterization of colloidal heterostructures. To this end, we implemented developments tailored for the high-efficiency prediction of epitaxial interfaces between ionic/polar materials, which encompass most colloidal semiconductors. These include the use of pre-screening candidate models based on charge balance at the interface and the use of a classical potential for fast energy evaluations, with parameters automatically calculated based on the input bulk structures. These developments are validated for perovskite-based CsPbBr 3 /Pb 4 S 3 Br 2 heterostructures, where Ogre produces interface models in excellent agreement with density functional theory and experiments. Furthermore, we use Ogre to rationalize the templating effect of CsPbCl 3 on the growth of lead sulfochlorides, where perovskite seeds induce the formation of Pb 4 S 3 Cl 2 rather than Pb 3 S 2 Cl 2 due to better epitaxial compatibility. Finally, combining Ogre simulations with experimental data enables us to unravel the structure and composition of the hitherto unsolved CsPbBr 3 /Bi x Pb y S z interface, and to assign a structure to several other reported metal halide- and oxide-based interfaces. The Ogre package is available on GitHub or via the OgreInterface desktop application, available for Windows, Linux, and Mac.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2009

NASA Tech Briefs, December 2009

Topics include: A Deep Space Network Portable Radio Science Receiver; Detecting Phase Boundaries in Hard-Sphere Suspensions; Low-Complexity Lossless and Near-Lossless Data Compression Technique for Multispectral Imagery; Very-Long-Distance Remote Hearing and Vibrometry; Using GPS to Detect Imminent Tsunamis; Stream Flow Prediction by Remote Sensing and Genetic Programming; Pilotless Frame Synchronization Using LDPC Code Constraints; Radiometer on a Chip; Measuring Luminescence Lifetime With Help of a DSP; Modulation Based on Probability Density Functions; Ku Telemetry Modulator for Suborbital Vehicles; Photonic Links for High-Performance Arraying of Antennas; Reconfigurable, Bi-Directional Flexfet Level Shifter for Low-Power, Rad-Hard Integration; Hardware-Efficient Monitoring of I/O Signals; Video System for Viewing From a Remote or Windowless Cockpit; Spacesuit Data Display and Management System; IEEE 1394 Hub With Fault Containment; Compact, Miniature MMIC Receiver Modules for an MMIC Array Spectrograph; Waveguide Transition for Submillimeter-Wave MMICs; Magnetic-Field-Tunable Superconducting Rectifier; Bonded Invar Clip Removal Using Foil Heaters; Fabricating Radial Groove Gratings Using Projection Photolithography; Gratings Fabricated on Flat Surfaces and Reproduced on Non-Flat Substrates; Method for Measuring the Volume-Scattering Function of Water; Method of Heating a Foam-Based Catalyst Bed; Small Deflection Energy Analyzer for Energy and Angular Distributions; Polymeric Bladder for Storing Liquid Oxygen; Pyrotechnic Simulator/Stray-Voltage Detector; Inventions Utilizing Microfluidics and Colloidal Particles; RuO2 Thermometer for Ultra-Low Temperatures; Ultra-Compact, High-Resolution LADAR System for 3D Imaging; Dual-Channel Multi-Purpose Telescope; Objective Lens Optimized for Wavefront Delivery, Pupil Imaging, and Pupil Ghosting; CMOS Camera Array With Onboard Memory; Quickly Approximating the Distance Between Two Objects; Processing Images of Craters for Spacecraft Navigation; Adaptive Morphological Feature-Based Object Classifier for a Color Imaging System; Rover Slip Validation and Prediction Algorithm; Safety and Quality Training Simulator; Supply-Chain Optimization Template; Algorithm for Computing Particle/Surface Interactions; Cryogenic Pupil Alignment Test Architecture for Aberrated Pupil Images; and Thermal Transport Model for Heat Sink Design.

Source record↗
DOE OSTI2025

Confinement-Driven Segregation Enables Glassy Polymer Hybrid Materials Featuring Disordered Hyperuniformity and Integrated Self-Healing

The blending of glassy copolymer-brush modified colloids with a viscoelastic linear copolymer featuring intrinsic self-healing enabled disordered hyperuniform hybrid materials that combined mechanical robustness with structural color, processability, environmental stability, and the ability to recover structure and properties after incurring physical damage via ‘integrated self-healing’. Symmetric linear n-butyl acrylate/methyl methacrylate (BA/MMA) were co-assembled with asymmetric glassy BA/MMA statistical copolymer brush (silica) particles. ‘Confinement-driven segregation’ resulted in a microphase-separated morphology in which the linear copolymer resided within the interstitial regions of a rigid (∼1 GPa) copolymer brush particle template with disordered hyperuniform microstructure. Diffusion of the self-healing copolymer additive into damage regions drove the recovery after damage, along with the restoration of structural color due to the materials hyperuniform microstructure. The synergistic action of intrinsic and extrinsic healing mechanisms could provide a versatile platform for the bottom-up fabrication of multifunctional hybrid materials with increased damage resistance and functional longevity.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Nanoparticle Superlattices through Template-Encoded DNA Dendrimers

The chemical interactions that lead to the emergence of hierarchical structures are often highly complex and difficult to program. In this paper, the synthesis of a series of superlattices based upon 30 different structurally reconfigurable DNA dendrimers is reported, each of which presents a well-defined number of single-stranded oligonucleotides (i.e., sticky ends) on its surface. Such building blocks assemble with complementary DNA-functionalized gold nanoparticles (AuNPs) to yield five distinct crystal structures, depending upon choice of dendrimer and defined by phase symmetry. These DNA dendrimers can associate to form micelle-dendrimers, whereby the extent of association can be modulated based upon surfactant concentration and dendrimer length to produce a low-symmetry Ti5Ga4-type phase that has yet to be reported in the field of colloidal crystal engineering. Taken together, colloidal crystals that feature three different types of particle bonding interactions.template-dendron, dendrimer-dendrimer, and DNA-modified AuNP-dendrimer.are reported, illustrating how sequence-defined recognition and dynamic association can be combined to yield complex hierarchical materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Harnessing emergent multiple scattering resonances in a photonic glass structure for photoelectrochemical energy conversion

Light trapping nanostructures are often necessary to improve carrier collection yields in semiconductor photoelectrodes with intrinsically poor electron transport. Photonic crystal templates can generate tailorable light trapping via periodic and precise nanostructure, though this is not a scalable strategy for photoelectrochemical (PEC) applications. It is therefore critical to identify alternative mechanisms for light trapping that tolerate disorder. Light trapping in disordered media is generated by the diffusive transport caused by multiple scattering. In some cases, multiple scattering can generate resonances that resemble those observed in photonic crystals. While resonant multiple scattering is a disorder tolerant light trapping mechanism, it is unclear if the effect is sufficiently adaptable, or even useful, for PEC applications. Here, we describe a photonic omission glass, a nanostructure that can controllably induce resonances in multiple scattering transport. We characterized the emergence of these resonances after coating a disordered SiO 2 colloidal structure with a layer of TiO 2 , which functions both as dielectric contrast and as a light absorbing semiconductor. We show in finite element simulations and spectroscopic characterization that the resonant multiple scattering effect improves light trapping near the interface between the structure and the bulk electrolyte. This effect, coupled with the increased electrochemically active surface area, results in a hierarchically structured TiO 2 photoanode with orders of magnitude higher photocurrents compared to an equivalent planar photoanode for PEC reactions such as alkaline water oxidation. We show that controlling this resonant multiple scattering effect can be advantageous for improving PEC energy conversion in disordered photoelectrodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Crystallization of binary nanocrystal superlattices and the relevance of short-range attraction

The synthesis of binary nanocrystal superlattices (BNSLs) enables the targeted integration of orthogonal physical properties, such as photoluminescence and magnetism, into a single superstructure, unlocking a vast design space for multifunctional materials. However, the formation mechanism of BNSLs remains poorly understood, restricting the prediction of the structure and properties of superlattices. Here we use a combination of in situ scattering and molecular simulation to elucidate the self-assembly of two common BNSLs (AlB 2 and NaZn 13 ) through emulsion templating. Our self-assembly experiments reveal that no intermediate structures precede the formation of the final binary phases, indicating that their formation proceeds through classical nucleation. Using simulations, we find that, despite the formation of AlB 2 and NaZn 13 typically being attributed to entropy, their self-assembly is most consistent with the nanocrystals possessing short-range interparticle attraction, which we find can accelerate nucleation kinetics in BNSLs. Here, we also find homogeneous, classical nucleation in simulations, corroborating our experiments. These results establish a robust correspondence between experiment and theory, paving the way towards prediction of BNSLs.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Confined Growth of DNA-Assembled Superlattice Films

Here, we study the assembly of DNA-functionalized nanocubes under lateral confinement in microscale square trenches on a DNA-functionalized substrate. Microfocus small-angle X-ray scattering (SAXS) and scanning electron microscopy (SEM) are used to characterize the superlattices (SLs). The results indicate that nanocubes form simple-cubic SLs with square-prism morphology and a (100) out-of-plane orientation to maximize DNA bonding. In-plane, SLs align with the template, exposing their {100} side facets, and the degree of alignment depends on trench size. Interestingly, the distribution of in-plane orientations determined from SAXS and SEM do not agree, indicating that the internal and external structures of the SLs differ. To understand this discrepancy, X-ray ptychography is employed to image the internal structures of the SLs, revealing that SLs which appear to be single-crystalline in SEM may have subsurface grain boundaries, depending on trench size. SEM reveals that the SLs grow via nucleation and growth of randomly oriented domains, which then coalesce; this mechanism explains the observed dependence of alignment and defect structure on size. Interestingly, crystallization occurs via an unusual growth mode, whereby continuous SL layers grow on top of several misoriented islands. Overall, this work elucidates the effect of lateral confinement on the crystallization of DNA-functionalized nanoparticles and shows how X-ray ptychography can be used to gain insight into nanoparticle crystallization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗