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At least 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Non-classical crystallization in soft and organic materials

Classical nucleation and crystal growth theories describe how nuclei form, become stable after reaching a critical size and then enlarge through monomer attachment. More than two decades ago, non-classical pathways have been proposed for various types of (bio)molecules and materials, which can substantially alter the crystallization kinetics and outcomes. Direct observation of non-classical crystallization of inorganic nanomaterials, including metastable structure-mediated and particle attachment-based pathways that usually occur on the nanoscale, was enabled by in situ liquid-phase electron microscopy. However, it was not until recently that the crystallization dynamics of beam-sensitive soft materials were directly imaged with sufficient spatial resolution, and a level of microstructural understanding of defects and interfaces emerged. This article provides a high-level review of the non-classical crystallization pathways discovered in soft and organic materials and a forward-looking guide for future research. We first analyse how the characteristics of soft materials affect their crystallization pathways and kinetics. We then identify technical approaches to studying the crystallization trajectories of soft materials and discuss strategies to properly select and apply them to different systems. Breakthroughs made in understanding the crystallization of small organic molecules, (bio)macromolecules, colloids and reticular framework materials are examined. Lastly, we provide an outlook on the challenges in elucidating soft material crystallization pathways and the opportunities for assisting the design and synthesis of new materials and structures.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Bridging microscopic dynamics and rheology in the yielding of charged colloidal suspensions

The yielding of soft materials is critical to many natural and industrial processes, yet experimental insights into microscopic aspects of yielding are limited. This study combines angle X-ray scattering, X-ray photon correlation spectroscopy, and in situ rheology (Rheo-SAXS-XPCS) with fast lubrication dynamics simulations to examine how interparticle interactions influence yielding in charged colloidal suspensions. By tuning attraction through salt addition, we compare repulsive and attractive systems under deformation. Repulsive suspensions yield uniformly with Andrade-like creep and minimal structural change. In contrast, attractive suspensions show complex behaviors, including shear banding, delayed yielding, and resolidification, governed by transient dynamics at shear band interfaces. These results directly link microscopic particle dynamics to macroscopic flow and demonstrate how interaction potentials control rheological behavior. This work offers a framework for designing soft materials with tailored properties for applications in coatings, food processing, drug delivery, and other technologies requiring precise mechanical control.

Molecular Dynamics Simulation↗
DOE OSTI2022

Mass Changes the Diffusion Coefficient of Particles with Ligand-Receptor Contacts in the Overdamped Limit

Inertia does not generally affect the long-time diffusion of passive overdamped particles in fluids. Yet a model starting from the Langevin equation predicts a surprising property of particles coated with ligands that bind reversibly to surface receptors: heavy particles diffuse more slowly than light ones of the same size. We show this by simulation and by deriving an analytic formula for the mass-dependent diffusion coefficient in the overdamped limit. We estimate the magnitude of this effect for a range of biophysical ligand-receptor systems, and find it is potentially observable for tailored micronscale DNA-coated colloids.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2025

Probing the Self-Assembly dynamics of cellulose nanocrystals by X-ray photon correlation spectroscopy

Charge-stabilized colloidal cellulose nanocrystals (CNCs) can self-assemble into higher-ordered chiral nematic structures by varying the volume fraction. The assembly process exhibits distinct dynamics during the isotropic to liquid crystal phase transition, which can be elucidated using X-ray photon correlation spectroscopy (XPCS). Anionic CNCs were dispersed in propylene glycol (PG) and water spanning a range of volume fractions, encompassing several phase transitions. Coupled with traditional characterization techniques, XPCS was conducted to monitor the dynamic evolution of the different phases. Additionally, simulated XPCS results were obtained using colloidal rods and compared with the experimental data, offering additional insights into the dynamic behavior of the system. The results indicate that the particle dynamics of CNCs undergo a stepped decay in three stages during the self-assembly process in PG, coinciding with the observed phases. The phase transitions are associated with a total drop of Brownian diffusion rates by four orders of magnitude, a decrease of more than a thousand times slower than expected in an ideal system of repulsive Brownian rods. Given the similarity in the phase behaviors in CNCs dispersed in PG and in water, we hypothesize that these dynamic behaviors can be extrapolated to other polar solvent environments. Importantly, these findings represent the direct measurement of CNC dynamics using XPCS, underscoring the feasibility of directly assessing the dynamic behavior of other rod-like colloidal suspensions.

36 MATERIALS SCIENCE↗
DOE OSTI2024

High Temperature, Isothermal Growth Promotes Close Packing and Thermal Stability in DNA-Engineered Colloidal Crystals

Here, we report a strategy to accelerate the synthesis and increase the crystallinity of colloidal crystals engineered with DNA. Specifically, by holding the DNA-modified Au particle building blocks above the T m of the individual nanoparticle building blocks, but slightly below the T m of the anticipated colloidal crystal during the assembly process, crystallinity is increased, and enthalpically-favored phases with high degrees of facet registration are observed. We studied the utility of this approach with systems for which the commonly adopted slow-cooling approach yielded primarily amorphous aggregates. In particular, we used it to synthesize high-volume fraction colloidal crystals from large (80 nm) anisotropic nanoparticles (cubes and rhombic dodecahedra) with short (<14 nm) DNA designed to restrict the degrees of freedom for the DNA bonds and maintain the anisotropy of the particle building block. Small-angle X-ray scattering and electron microscopy studies show that the crystalline phases synthesized via this method are more thermally stable than their corresponding aggregate phases, likely due to an increased number of DNA-DNA bonds between particles. Crystal size tunability (between 0.5 and 15 µm edge lengths) and epitaxial growth were demonstrated using this strategy by modulating the NaCl concentration in tandem with previously synthesized colloidal crystal nuclei. Taken together, this isothermal strategy provides a route to deliberately crystallize a wide variety of anisotropic colloidal materials and expands the phase space accessible to nanoparticles modified with DNA.

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↗
NASA NTRS1986

Colloidal characterization of silicon nitride and silicon carbide

The colloidal behavior of aqueous ceramic slips strongly affects the forming and sintering behavior and the ultimate mechanical strength of the final ceramic product. The colloidal behavior of these materials, which is dominated by electrical interactions between the particles, is complex due to the strong interaction of the solids with the processing fluids. A surface titration methodology, modified to account for this interaction, was developed and used to provide fundamental insights into the interfacial chemistry of these systems. Various powder pretreatment strategies were explored to differentiate between true surface chemistry and artifacts due to exposure history. The colloidal behavior of both silicon nitride and carbide is dominated by silanol groups on the powder surfaces. However, the colloid chemistry of silicon nitride is apparently influenced by an additional amine group. With the proper powder treatments, silicon nitride and carbide powder can be made to appear colloidally equivalent. The impact of these results on processing control will be discussed.

Feke, Donald L.↗
DOE OSTI2023

Arrested coarsening and large density fluctuations in driven particle mixtures in two dimensions

Abstract Using molecular dynamics simulations, we study a driven, nonadditive binary mixture of spherical particles confined to move in two dimensions and immersed in an explicit solvent consisting of point particles with purely repulsive interactions. We show that, without a drive, the mixture of spherical particles phase separates and coarsens with kinetics consistent with an Ising-like conserved dynamics. Conversely, when the drive is applied, the coarsening is arrested and the system develops large density fluctuations. We show that the drive creates domains of a characteristic size which decreases with an increasing force. Furthermore, we find that these domains are anisotropic and can be oriented either parallel or perpendicular to the drive direction. Finally, we connect our findings to existing theories of strongly-driven systems, pointing out the importance of introducing the explicit solvent particles to break the Galilean invariance of the system.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Enhancing nanoscale charged colloid crystallization near a metastable liquid binodal

Achieving predictive control over crystallization using non-classical nucleation while avoiding kinetic traps would be a step towards designing materials with new functionalities. We address these challenges by inducing the bottom-up assembly of nanocrystals into ordered arrays, or superlattices. Using electrostatics—rather than density—to tune the interactions between particles, we watch self-assembly proceed through a metastable liquid phase. Here, we systematically investigate the phase behaviour as a function of quench conditions in situ and in real time using small-angle X-ray scattering. By fitting to colloid, liquid and superlattice models, we extract the time evolution of each phase and the system phase diagram, which we find to be consistent with short-range attractive interactions. Using the predictive power of the phase diagram, we establish control of the self-assembly rate over three orders of magnitude, and we identify one- and two-step self-assembly regimes, with only the latter implicating the metastable liquid as an intermediate. The presence of the metastable liquid increases the superlattice formation rate relative to the equivalent one-step pathway, and the superlattice order increases with the rate, revealing a generalizable kinetic strategy for promoting and enhancing ordered assembly.

Tanner, Christian P. N. [University of California,↗
NASA NTRS2004

Compact Microscope Imaging System With Intelligent Controls Improved

The Compact Microscope Imaging System (CMIS) with intelligent controls is a diagnostic microscope analysis tool with intelligent controls for use in space, industrial, medical, and security applications. This compact miniature microscope, which can perform tasks usually reserved for conventional microscopes, has unique advantages in the fields of microscopy, biomedical research, inline process inspection, and space science. Its unique approach integrates a machine vision technique with an instrumentation and control technique that provides intelligence via the use of adaptive neural networks. The CMIS system was developed at the NASA Glenn Research Center specifically for interface detection used for colloid hard spheres experiments; biological cell detection for patch clamping, cell movement, and tracking; and detection of anode and cathode defects for laboratory samples using microscope technology.

McDowell, Mark↗
DOE OSTI2023

Colloidal superionic conductors

Nanoparticles with highly asymmetric sizes and charges that self-assemble into crystals via electrostatics may exhibit behaviors reminiscent of those of metals or superionic materials. Here, we use coarse-grained molecular simulations with underdamped Langevin dynamics to explore how a binary charged colloidal crystal reacts to an external electric field. As the field strength increases, we find transitions from insulator (ionic state), to superionic (conductive state), to laning, to complete melting (liquid state). In the superionic state, the resistivity decreases with increasing temperature, which is contrary to metals, yet the increment decreases as the electric field becomes stronger. Additionally, we verify that the dissipation of the system and the fluctuation of charge currents obey recently developed thermodynamic uncertainty relation. Our results describe charge transport mechanisms in colloidal superionic conductors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1996

Momentum Transfer Studies and Studies of Linear and Nonlinear Optical Properties of Metal Colloids and Semiconductor Quantum Dots

Phase 1 of this work involved design work on a momentum transfer device. The progress on design and testing will be presented. Phase 2 involved the systematic study of the MPD thruster for dual uses. Though it was designed as a thruster for space vehicles, the characteristics of the plasma make it an excellent candidate for industrial applications. This project sought to characterize the system for use in materials processing and characterization. The surface modification on ZnCdTe, CdTe, and ZnTe will be presented. Phase 3 involved metal colloids and semiconductor quantum dots. One aspect of this project involves a collaborative effort with the Solid State Division of ORNL. The thrust behind this research is to develop ion implantation for synthesizing novel materials (quantum dots wires and wells, and metal colloids) for applications in all optical switching devices, up conversion, and the synthesis of novel refractory materials. The ions of interest are Au, Ag, Cd, Se, In, P, Sb, Ga, and As. The specific materials of interest are: CdSe, CdTe, InAs, GaAs, InP, GaP, InSb, GaSb, and InGaAs. A second aspect of this research program involves using porous glass (25-200 A) for fabricating materials of finite size. The results of some of this work will also be reported.

Collins, W. E.↗
NASA NTRS2003

18-Degree-of-Freedom Controller Design for the ST7 Disturbance Reduction System

This paper presents the overall design and analysis process of the spacecraft controller being developed at NASA's Goddard Space Flight Center to close the loop between the GRS and the micro-newton colloidal thrusters. The essential dynamics of the ST7-DRS are captured in a simulation including eighteen rigid-body dynamic degrees of freedom: three translations and three rotations for the spacecraft and for each test mass. The ST7 DRS comprises three control systems: the attitude control system (ACS) to maintain a sun-pointing attitude; the drag free control (DFC) to center the spacecraft about the test masses; and the test mass suspension control. This paper summarizes the control design and analysis of the ST7-DRS 18-DOF model, and is an extension of previous analyses employing a 7-DOF planar model of ST-7.

Markley, F. L.↗
DOE OSTI2022

Kibble-Zurek mechanism for nonequilibrium phase transitions in driven systems with quenched disorder

Abstract We show that the Kibble-Zurek mechanism applies to nonequilibrium phase transitions found in driven assemblies of superconducting vortices and colloids moving over quenched disorder where a transition occurs from a plastic disordered flowing state to a moving anisotropic crystal. We measure the density of topological defects as a function of quench rate through the nonequilibrium phase transition, and find that on the ordered side of the transition, the topological defect density ρ d scales as a power law, $${\rho }_{{{{{{{{\rm{d}}}}}}}}}\propto 1/{t}_{{{{{{{{\rm{q}}}}}}}}}^{\beta }$$ ρ d ∝ 1 / t q β , where t q is the quench time duration, consistent with the Kibble-Zurek mechanism. We show that scaling with the same exponent holds for varied strengths of quenched disorder and that the exponents fall in the directed percolation universality class. Our results suggest that the Kibble-Zurek mechanism can be applied to the broader class of systems that exhibit absorbing phase transitions.

97 MATHEMATICS AND COMPUTING↗
NASA NTRS2000

Diffusing Wave Spectroscopy Used to Study Foams

The white appearance of familiar objects such as clouds, snow, milk, or foam is due to the random scattering of light by the sample. As we all know, pure water is clear and easily passes a beam of light. However, tiny water droplets, such as those in a cloud, scatter light because the air and water droplet have different indexes of refraction. When many droplets, or scattering sites, are present, the incident light is scattered in random directions and the sample takes on a milky white appearance. In a glass of milk, the scattering is due to small colloidal particles. The white appearance of shaving cream, or foam, is due to the scattering of light at the water-bubble interface. Diffusing wave spectroscopy (DWS) is a laser light-scattering technique used to noninvasively probe the particle dynamics in systems that strongly scatter light. The technique takes advantage of the diffuse nature of light, which is reflected or transmitted from samples such as foams, dense colloidal suspensions (such as paint and milk), emulsions, liquid crystals, sandpiles, and even biological tissues.

Zimmerli, Gregory A.↗
DOE OSTI2022

The nanocaterpillar's random walk: diffusion with ligand–receptor contacts

Particles with ligand–receptor contacts bind and unbind fluctuating “legs” to surfaces, whose fluctuations cause the particle to diffuse. Quantifying the diffusion of such “nanoscale caterpillars” is a challenge, since binding events often occur on very short time and length scales. Here, in this work, we derive an analytical formula, validated by simulations, for the long time translational diffusion coefficient of an overdamped nanocaterpillar, under a range of modeling assumptions. We demonstrate that the effective diffusion coefficient, which depends on the microscopic parameters governing the legs, can be orders of magnitude smaller than the background diffusion coefficient. Furthermore it varies rapidly with temperature, and reproduces the striking variations seen in existing data and our own measurements of the diffusion of DNA-coated colloids. Our model gives insight into the mechanism of motion, and allows us to ask: when does a nanocaterpillar prefer to move by sliding, where one leg is always linked to the surface, and when does it prefer to move by hopping, which requires all legs to unbind simultaneously? We compare a range of systems (viruses, molecular motors, white blood cells, protein cargos in the nuclear pore complex, bacteria such as Escherichia coli, and DNA-coated colloids) and present guidelines to control the mode of motion for materials design.

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

Unveiling Structural Heterogeneity and Imbalance of Gold Decahedral Nanoparticles using Four-dimensional Scanning Transmission Electron Microscopy

Multi-twinned structures have been observed in technologically important crystal systems, for example diamond cubic and face-centered cubic (FCC) lattices, that include materials such as diamond, silicon, a wide range of noble metals, and their nanoscale counterparts. Beyond atomic building blocks, the special arrangements also occur in the self-assembly of nanoparticles (NP) and μm-sized colloidal particles and occupy parts of their phase diagrams. Spanning a wide range of length scales, the universality of the structures arises when the systems attempt to achieve multitwinned structures by overcoming geometric misfits during minimizing surface energies with entirely {111} or close-packing facets. While it is fundamental to understand how strain is sustained upon twinned structures and symmetry breaking, the knowledge will be paramount in practical aspects such as guiding and controlling the thin film growth, anisotropic NP growth, and self-assembly of NPs. Au decahedral (Dh) NP, as the most prevalent multi-twinned model system, fits five tetrahedral motifs into a circle by sharing an axis resulting in a geometric misfit angle of 7.35°, or a disclination with power of -7.35°. Postulating how Au FCC lattice adopts the misfit, theoretical models have been developed to address the underlying lattice symmetry and inhomogeneous strain distribution separately. Yet, experimental reports regarding the former have been limited due to the relatively large X-ray beam sizes that do not fit the sizes of NPs. On the other hand, though the latter has been widely adapted in the thermodynamics of small (<10 nm) multi-twinned nanoparticles, previous literature has shown that, at edge length of 17 nm, the theory’s is invalidated by shear strain that is observed in a defect-free Au Dh NP by high-resolution transmission electron microscopy (HR-TEM) imaging. Though the advancement of aberrationcorrected scanning transmission electron microscopy (AC-STEM) imaging and ab initio calculation techniques brings new opportunities, along with challenges in complicated image analysis and limitation in particle size (usually below 10 nm), the gap between nanoscale and mesoscale has never been extended to gain insight from atomic system with straightforward interaction potentials.

4D-STEM↗