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At least 667 records · Page 37
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Femtosecond laser pulse driven melting in gold nanorod aqueous colloidal suspension: Identification of a transition from stretched to exponential kinetics

Many potential industrial, medical, and environmental applications of metal nanorods rely on the physics and resultant kinetics and dynamics of the interaction of these particles with light. We report a surprising kinetics transition in the global melting of femtosecond laser-driven gold nanorod aqueous colloidal suspension. At low laser intensity, the melting exhibits a stretched exponential kinetics, which abruptly transforms into a compressed exponential kinetics when the laser intensity is raised. It is found the relative formation and reduction rate of intermediate shapes play a key role in the transition. Supported by both molecular dynamics simulations and a kinetic model, the behavior is traced back to the persistent heterogeneous nature of the shape dependence of the energy uptake, dissipation and melting of individual nanoparticles. These results could have significant implications for various applications such as water purification and electrolytes for energy storage that involve heat transport between metal nanorod ensembles and surrounding solvents.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2026

Single-Particle Insights Into the Electronic Structure and Enhanced Stability of CsPbBr 3 /FAPbBr 3 Core/Crown Nanoplatelets at the Nanometer Scale

Colloidal perovskite nanoplatelets (NPLs), despite their exceptional optoelectronic properties, face significant challenges due to their intrinsic instability and trap-assisted non-radiative recombination. Although many studies employing surface engineering, such as selecting ligands or coating to passivate defects, have demonstrated improved optoelectronic properties, these enhancements are typically inferred from bulk-ensemble measurements; the effects at the single-particle level remain elusive. Here, we conduct single-particle-level studies using scanning tunneling spectroscopy (STS) on a unique core–crown system, CsPbBr 3 @FAPbBr 3 NPLs, where the lateral surfaces of the CsPbBr 3 core are coated with an FAPbBr 3 crown. Experimental density-of-states (DOS) analysis reveals a 47% reduction in deep-trap states in core-crown NPLs compared to core-only NPLs, consistent with nearly two-fold enhancements in photoluminescence quantum yields. Progressive I–V sweep measurements demonstrate superior electrical stability in core-crown NPLs, preserving band structure with minimal degradation, while core-only NPLs exhibit rapid bandgap shrinkage and trap formation. Density functional theory (DFT) calculations indicate that FA incorporation distorts Pb octahedral lattice, widening the bandgap. This study elucidates how surface engineering modulates charge localization, passivates defects, and enhances stability at the single-particle level. Moreover, by uncovering bias-induced trap states in single unpassivated NPLs, this study establishes a precise, robust approach for characterizing emerging perovskite nanocrystals.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2019

Instantons, colloids and convergence of the 1/N expansion for the homogeneous electron gas

We investigate non-perturbative corrections to the large N expansion of the homogeneous electron gas. These are associated with instanton solutions to the effective action of the plasmon field. We show that, although the large field behavior of that action dominates the quadratic bare Coulomb term, there are no solutions at large field, and consequently none at large density. We argue that solutions would exist at low density if the large N theory had a Wigner crystal (WC) phase. However, we argue that this is not the case. Together with the implied convergence of the large N expansion, this implies that the homogeneous electron gas with N component spins and a Coulomb interaction scaling like 1∕N can only have a WC phase below a curve in the plane of N and density, which asymptotes to zero density at infinite N. We argue that for systems with a semi-classical expansion for order parameter dynamics, and a first order quantum transition between fluid and crystal phases, there are instantons associated with the decays of meta-stable fluid and crystal phases in the appropriate regions of the phase diagram. We argue that the crystal will decay into one or more colloidal or bubble phases (Kivelson and Spivak, 2006) rather than directly into the fluid. It is possible that the bubble phases remain stable all the way to the density where the crystal solution disappears. The bubbles of fluid will expand as the density is raised and gradually convert the system into a fluid filled with chunks of crystal. The transition to a translationally invariant phase is likely to be second order. Unfortunately, the HEG does not have a crystal phase at large N, where these semi-classical ideas could be examined in detail. We suggest that the evidence for negative dielectric function at intermediate densities for N=2 is an indicator of this second order transition. While the infinite N limit does not have a negative dielectric function at any density, it is possible that the closed large N equation for the plasmon two point function, derived in Banks (2018) might capture at least the qualitative features of the second order transition.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Colloidal Three-Dimensional Covalent Organic Frameworks and Their Application as Porous Liquids

Developing solid porous materials into free-flowing liquids with permanent porosity is a promising strategy for overcoming certain limitations of conventional sorbent materials employed in gas storage and separation applications. The ability to control the pore size and chemical functionalities of organic frameworks gives these particular nanoporous materials distinct advantages over other small cage-like molecules or hollow particles that have been developed into porous liquids. Here, we describe the synthesis of a 3D imine-linked colloidal covalent organic framework (COF)-based porous liquid, designed for efficient size-exclusion of solvent, as well as for long-term stability. By tethering ionic liquids to the colloid surface, the colloids can be dried, purified, and resuspended in a variety of solvents without irreversible aggregation typically observed of COF colloids. Colloid size could be controlled between 50 and 400 nm, with surface areas as high as 800 m2/g. The 3D intertwining morphology of the colloids had pore sizes ranging from 5 to 14 Å, allowing them to efficiently sizeexclude bulky ionic liquids. The COF colloids were stable towards flocculation in an ionic liquid for > 1 year. Permanent porosity was confirmed with a combination of 19F NMR measurements and gas sorption techniques. CO2 and CH4 uptake in these porous liquids increased more than 10 and 20-fold, respectively, over non-porous, neat ionic liquid control samples. The work not only advances the state of COF-based colloid science but also represents a practical advance towards developing more robust, tunable framework-based porous liquid materials for a host of gas storage and separation applications.

Mow, Rachel E.↗
DOE OSTI2014

Growth of arrays of oriented epitaxial platinum nanoparticles with controlled size and shape by natural colloidal lithography

Here, we developed a method for production of arrays of platinum nanocrystals of controlled size and shape using templates from ordered silica bead monolayers. Silica beads with nominal sizes of 150 and 450 nm were self-assembl into monolayers over strontium titanate single crystal substrates. The monolayers were used as shadow masks for platinum metal deposition on the substrate using the three-step evaporation technique. Produced arrays of epitaxial platinum islands were transformed into nanocrystals by annealing in a quartz tube in nitrogen flow. The shape of particles is determined by the substrate crystallography, while the size of the particles and their spacing are controlled by the size of the silica beads in the mono- layer mask. As a proof of concept, arrays of platinum nanocrystals of cubooctahedral shape were prepared on (100) strontium titanate substrates. We also characterized the nanocrystal arrays by atomic force microscopy, scanning electron microscopy, and synchrotron X-ray diffraction techniques.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Origin of Broad Emission Spectra in InP Quantum Dots: Contributions from Structural and Electronic Disorder

The ensemble emission spectra of colloidal InP quantum dots are broader than achievable spectra of cadmium- and lead-based quantum dots, despite similar single-particle line widths and significant efforts invested in the improvement of synthetic protocols. Here, we seek to explain the origin of persistently broad ensemble emission spectra of colloidal InP quantum dots by investigating the nature of the electronic states responsible for luminescence. We identify a correlation between red-shifted emission spectra and anomalous broadening of the excitation spectra of luminescent InP colloids, suggesting a trap-associated emission pathway in highly emissive core shell quantum dots. Time-resolved pump probe experiments find that s are largely untrapped on photoluminescence relevant time scales pointing to emission from recombination of localized holes with free electrons. Two-dimensional electronic spectroscopy on InP quantum dots reveals multiple emissive states and increased electron phonon coupling associated with hole localization. These localized hole states near the valence band edge are hypothesized to arise from incomplete surface passivation and structural disorder associated with lattice defects. We confirm the presence and effect of lattice disorder by X-ray absorption spectroscopy and Raman scattering measurements. Participation of localized electronic states that are associated with various classes of lattice defects gives rise to phonon-coupled defect related emission. These findings explain the origins of the persistently broad emission spectra of colloidal InP quantum dots and suggest future strategies to narrow ensemble emission lines comparable to what is observed for cadmium-based materials.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Shape-Controlled Narrow-Gap SnTe Nanostructures: From Nanocubes to Nanorods and Nanowires

The rational design and synthesis of narrow-gap colloidal semiconductor nanocrystals (NCs) is an important step toward the next generation of solution-processable photovoltaics, photodetectors, and thermoelectric devices. SnTe NCs are particularly attractive as a Pb-free alternative to NCs of narrow-gap lead chalcogenides. Previous synthetic efforts on SnTe NCs have focused on spherical nanoparticles. Here we report new strategies for synthesis of SnTe NCs with shapes tunable from highly monodisperse nanocubes, to nanorods (NRs) with variable aspect ratios, and finally to long, straight nanowires (NWs). Reaction at high temperature quickly forms thermodynamically favored nanocubes, but low temperatures lead to elongated particles. Transmission electron microscopy studies of reaction products at various stages of the synthesis reveal that the growth and shape-focusing of monodisperse SnTe nanocubes likely involves interparticle ripening, while directional growth of NRs and NWs may be initiated by particle dimerization via oriented attachment.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Spontaneous liquid crystal and ferromagnetic ordering of colloidal magnetic nanoplates

Ferrofluids are familiar as colloidal suspensions of ferromagnetic nanoparticles in aqueous or organic solvents. The dispersed particles are randomly oriented but their moments become aligned if a magnetic field is applied, producing a variety of exotic and useful magnetomechanical effects. A longstanding interest and challenge has been to make such suspensions macroscopically ferromagnetic, that is having uniform magnetic alignment in the absence of a field. Here we report a fluid suspension of magnetic nanoplates that spontaneously aligns into an equilibrium nematic liquid crystal phase that is also macroscopically ferromagnetic. We find Its zero-field magnetization produces distinctive magnetic self-interaction effects, including liquid crystal textures of fluid block domains arranged in closed flux loops, and makes this phase highly sensitive, with it dramatically changing shape even in the Earth’s magnetic field.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2026

Two-dimensional non-equilibrium melting of charged colloids

Thermodynamic two-dimensional melting has been extensively studied in experiments and simulations, and is well predicted by theory. For systems in equilibrium, this transition is well described by the Kosterlitz–Thouless–Halperin–Nelson–Young theory, where melting is directly linked to the unbinding of topological defects. For driven, non-equilibrium melting and other non-equilibrium phase transitions, the picture is less clear. Here, in this work, we study the two-dimensional melting of a crystal of charged colloids. By randomly replacing some charged colloids with magnetic colloids, we can melt our system by rotating a fraction of the particles to create non-equilibrium, hydrodynamic random flows and local stresses. We can also melt it thermally by changing the particle number density. We find that an effective temperature approach cannot explain the results of our driven system. Rather, in both experiments and simulations, we observe that plotting the hexatic order parameter and the hexatic correlation’s exponent versus the density of disclinations and dislocations, respectively, yields universal curves. This implies that in our systems, two-dimensional melting depends directly on the density of topological defects and is independent of whether thermal or non-equilibrium forces generate them.

critical phenomena↗
DOE OSTI2016

Emergent ultra–long-range interactions between active particles in hybrid active–inactive systems

Significance Particle–particle interactions determine the state of a system. Control over the range and magnitude of such interactions is critical for science and technology. Here, we show that active particles experience an emergent ultra–long-range attractive interaction in the presence of a passive medium. The range and magnitude of this interaction are controlled by the elasticity of the medium and the activity of the particles. For the conditions studied here, we have found the range to be as large as 20 particle diameters, which is much larger than the typical interaction range between colloids. This interaction may open up new routes of control between active objects in passive environments and help us to understand the emergent interactions in nonequilibrium (biological) systems.

Steimel, Joshua P.↗
DOE OSTI2020

Directional locking effects for active matter particles coupled to a periodic substate

Directional locking occurs when a particle moving over a periodic substrate becomes constrained to travel along certain substrate symmetry directions. Such locking effects arise for colloids and superconducting vortices moving over ordered substrates when the direction of the external drive is varied. Here we study the directional locking of run-and-tumble active matter particles interacting with a periodic array of obstacles. In the absence of an external biasing force, we find that the active particle motion locks to various symmetry directions of the substrate when the run time between tumbles is large. The number of possible locking directions depends on the array density and on the relative sizes of the particles and the obstacles. For a square array of large obstacles, the active particle only locks to the x, y, and 45° directions, while for smaller obstacles, the number of locking angles increases. Each locking angle satisfies θ = arctan (p/q) , where p and q are integers, and the angle of motion can be measured using the ratio of the velocities or the velocity distributions in the x and y directions. When a biasing driving force is applied, the directional locking behavior is affected by the ratio of the self-propulsion force to the biasing force. For large biasing, the behavior resembles that found for directional locking in passive systems. For large obstacles under biased driving, a trapping behavior occurs that is nonmonotonic as a function of increasing run length or increasing self-propulsion force, and the trapping diminishes when the run length is sufficiently large.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Possibilities of surface-sensitive X-ray methods for studying the molecular mechanisms of interaction of nanoparticles with model membranes

The processes of structural rearrangement in a model membrane, i.e., an arachic acid monolayer formed on a colloidal solution of cerium dioxide or magnetite, are studied in situ in real time by the methods of X-ray standing waves and 2D diffraction. It is shown that the character of the interaction of nanoparticles with the monolayer is determined by their nature and sizes and depends on the conditions of nanoparticle synthesis. In particular, the structure formation in the monolayer–particle system is greatly affected by the stabilizer (citric acid), which is introduced into the colloidal solution during synthesis.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1997

Crystalline Colloidal Arrays in Polymer Matrices

Crystalline Colloidal Arrays (CCA, also known as colloidal crystals), composed of aqueous or nonaqueous dispersions of self-assembled nanosized polymer colloidal spheres, are emerging toward the development of advanced optical devices for technological applications. The spontaneous self assembly of polymer spheres in a dielectric medium results from the electrostatic repulsive interaction between particles of uniform size and charge distribution. In a way similar to atomic crystals that diffract X-rays, CCA dispersions in thin quartz cells selectively and efficiently Bragg diffract the incident visible light. The reason for this diffraction is because the lattice (body or face centered cubic) spacing is on the order of the wavelength of visible light. Unlike the atomic crystals that diffract a fixed wavelength, colloidal crystals in principle, depending on the particle size, particle number and charge density, can diffract W, Vis or IR light. Therefore, the CCA dispersions can be used as laser filters. Besides, the diffraction intensity depends on the refractive index mismatch between polymer spheres and dielectric medium; therefore, it is possible to modulate incident light intensities by manipulating the index of either the spheres or the medium. Our interest in CCA is in the fabrication of all-optical devices such as optical switches, limiters, and spatial light modulators for optical signal processing. The two major requirements from a materials standpoint are the incorporation of suitable nonlinear optical materials (NLO) into polymer spheres which will allow us to alter the refractive index of the spheres by intense laser radiation, and preparation of solid CCA filters which can resist laser damage. The fabrication of solid composite filters not only has the advantage that the films are easier to handle, but also the arrays in solid films are more robust than in liquid media. In this paper, we report the photopolymerization process used to trap CCA in polymer matrices, the factors which affect the optical diffraction qualities of resulting polymer films, and methods to improve the efficiencies of solid optical filters. Before this, we also present the experimental demonstration, of controlling the optical diffraction intensities from aqueous CCA dispersions by varying the temperature, which establishes the feasibility of fabricating all-optical switching devices with nonlinear periodic array structures.

Sunkara, Hari B.↗
NASA NTRS2001

Visualization of Microbial Biomarkers by Scanning Electron Microscopy

We are developing tools to link the biochemical structure of selected biomarkers with putative biogenic structures observed in mineralized samples. The detection of evidence of life on Mars and other planets will rely on methods that can discriminate compounds formed exclusively by living organisms. While biogenic compounds, such as amino acids and nucleotides have been discovered in extraterrestrial sources, such as meteorites and comets, their formation can be explained by abiotic means. The formation of cellular structures, or more elaborate organic molecules, such as complex lipids, proteins or nucleic acids, however, is strongly correlated to the presence of even the most primitive life processes. Recent evidence lends support to the hypothesis that life may have once existed on Mars. Carbonate globules and ppm concentrations of polycyclic aromatic hydrocarbons (PAHs) have been described in ALH84001, a meteorite originating from Mars ejecta captured by Earth over 13,000 years ago. The localized high concentration of PAHs that follow an increasing gradient from the intact fusion crust towards the interior corresponds to microgram quantities of hydrocarbon. Even though ALH84001 and other similar meteorites have withstood the forces capable of ejecting rock through Mars' escape velocity, upon entering Earth's atmosphere, their core temperatures are likely not to have been raised significantly, as evidenced by the survival of remanent magnetic signatures. Ideal biomarkers of ancient or modern biological life would include molecules that are (or were) pervasive and highly resistant to degradation. Also, requisite methods of detection should be simple, extremely sensitive and broadly inclusive (NASA SP-530). Lipopolysaccharide (LPS), peptidoglycan or pseudopeptidoglycan and beta-glucan are microbial cell wall components which together cover the entire microbial spectrum of eubacteria, archea and fungi. They are all remarkably resistant to thermal degradation. Fortunately, many antimicrobial defense systems of higher organisms require sensitive detection to combat microbial pathogens. We employ here the primitive immune system of the evolutionarily ancient horseshoe crab, Limulus polyphemus. This species relies on multi-enzyme signal amplification detection of cell wall molecules and they can be applied to the development of useful detectors of life. An extension of this work includes the visualization of microbial signatures by labeling LAL components with chromogenic or electron dense markers. The protein Limulus Anti-LPS Factor (LALF) has an extremely high affinity for LPS. By coupling LALF binding with colloidal gold labels we demonstrate a correlation of the structures visible by electron microscopy with biochemical evidence of microbial cell wall materials. Pure silica particles were mixed with cultures of E. coli (10(exp 6) cfu/mL). Samples were washed sequentially with buffered saline, LALF, antibody to LALF and finally colloidal gold-labeled Protein A. Negative controls were not exposed to E. coli but received identical treatment otherwise. Samples were coated with carbon and imaged on a JEOL JSM-840 scanning electron microscope with LaB6 source in the back scatter mode with the JEOL annular back scatter detector. 20 nm-scale black spots in this contrast-reversed image originate from electrons back-scattered by gold atoms. Negative controls did not give any signal. Future work will expand application of this technique to soil simulants and mineralized rock samples.

Wainwright, Norman R.↗
DOE OSTI2015

Pair mobility functions for rigid spheres in concentrated colloidal dispersions: Force, torque, translation, and rotation

The formulation of detailed models for the dynamics of condensed soft matter including colloidal suspensions and other complex fluids requires accurate description of the physical forces between microstructural constituents. In dilute suspensions, pair-level interactions are sufficient to capture hydrodynamic, interparticle, and thermodynamic forces. In dense suspensions, many-body interactions must be considered. Prior analytical approaches to capturing such interactions such as mean-field approaches replace detailed interactions with averaged approximations. However, long-range coupling and effects of concentration on local structure, which may play an important role in, e.g., phase transitions, are smeared out in such approaches. An alternative to such approximations is the detailed modeling of hydrodynamic interactions utilizing precise couplings between moments of the hydrodynamic traction on a suspended particle and the motion of that or other suspended particles. For two isolated spheres, a set of these functions was calculated by Jeffrey and Onishi [J. Fluid Mech. 139, 261–290 (1984)] and Jeffrey [J. Phys. Fluids 4, 16–29 (1992)]. Along with pioneering work by Batchelor, these are the touchstone for low-Reynolds-number hydrodynamic interactions and have been applied directly in the solution of many important problems related to the dynamics of dilute colloidal dispersions [G. K. Batchelor and J. T. Green, J. Fluid Mech. 56, 375–400 (1972) and G. K. Batchelor, J. Fluid Mech. 74, 1–29 (1976)]. Toward extension of these functions to concentrated systems, here we present a new stochastic sampling technique to rapidly calculate an analogous set of mobility functions describing the hydrodynamic interactions between two hard spheres immersed in a suspension of arbitrary concentration, utilizing accelerated Stokesian dynamics simulations. These mobility functions provide precise, radially dependent couplings of hydrodynamic force and torque to particle translation and rotation, for arbitrary colloid volume fraction ϕ. The pair mobilities (describing entrainment of one particle by the disturbance flow created by another) decay slowly with separation distance: as 1/r, for volume fractions 0.05 ≤ ϕ ≤ 0.5. For the relative mobility, we find an initially rapid growth as a pair separates, followed by a slow, 1/r growth. Up to ϕ ≤ 0.4, the relative mobility does not reached the far-field value even beyond separations of many particle sizes. In the case of ϕ = 0.5, the far-field asymptote is reached but only at a separation of eight radii and after a slow 1/r growth. At these higher concentrations, the coefficients also reveal liquid-like structural effects on pair mobility at close separations. These results confirm that long-range many-body hydrodynamic interactions are an essential part of the dynamics of concentrated systems and that care must be taken when applying renormalization schemes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Scaling of Shear Rheology of Concentrated Charged Colloidal Suspensions across Glass Transition

Electrostatic interparticle interactions are a key component in controlling and designing rheological characteristics of concentrated charged colloidal suspensions. Herein, we investigate electroviscous effects on shear rheology using highly charged silica particles. By fixing the volume fraction but varying the salinity, the system undergoes a glass transition as evidenced by the evolution of the yield stress and zero-shear viscosity. We show that the steady shear viscosities obey a critical scaling relation that scales the flow curves into a super- and a sub-critical branch with glass transition salinity serving as the bifurcation point; we also demonstrate an isoviscosity scaling that collapses all isoviscosity lines into a single master curve that exhibits no singularity. Based on each scaling relation, in conjunction with common modeling equations, the quantitative relationships between the shear viscosity, stress, and salinity are established. This study demonstrates a new framework to model the steady shear rheology of concentrated charged colloids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Crystals of Janus colloids at various interaction ranges

We investigate the effect of interaction range on the phase behaviour of Janus particles with a Kern-Frenkel potential. Specifically, we study interaction ranges Δ = 0.1σ, 0.3σ, 0.4σ, 0.5σ with σ the particle diameter, and use variable box shape simulations to predict crystal structures. We found that changing the interaction range beyond 0.2σ drastically increases the variety of possible crystal structures. In addition to close-packed structures, we find body-centered tetragonal and AA-stacked hexagonal crystals, as well as several lamellar crystals. For long interaction ranges and low temperatures, we also observe an extremely large number of metastable structures which compete with the thermodynamically stable ones. These competing structures hinder the detection of the lowest-energy crystal structures, and are also likely to interfere with the spontaneous formation of the ground-state structure. Finally, we determine the gas-liquid coexistence curves for several interaction ranges, and observe that these are metastable with respect to crystallization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗