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Report studies elucidation and description of effect of interparticle forces on feasibility of gaseous fluidization of particles below 50 microns in diameter. Interparticle forces are determined by inclined-plane method. Study indicated that fluidizability is related to the interparticle adhesive force.
Ultrasound propagation through externally stressed, disordered granular materials was experimentally and numerically investigated. Experiments employed piezoelectric transducers to excite and detect longitudinal ultrasound waves of various frequencies traveling through randomly packed sapphire spheres subjected to uniaxial compression. The experiments featured in situ X-ray tomography and diffraction measurements of contact fabric, particle kinematics, average per-particle stress tensors, and interparticle forces. The experimentally measured packing configuration and inferred interparticle forces at different sample stresses were used to construct spring networks characterized by Hessian and damping matrices. The ultrasound responses of these network were simulated to investigate the origins of wave velocity, acoustic paths, dispersion, and attenuation. Results revealed that both packing structure and interparticle force heterogeneity played an important role in controlling wave velocity and dispersion, while packing structure alone quantitatively explained most of the observed wave attenuation. This research provides insight into time- and frequency-domain features of wave propagation in randomly packed granular materials, shedding light on the fundamental mechanisms controlling wave velocities, dispersion, and attenuation in such systems.
In the study of planetary aeolian processes the effect of gravity is not readily modeled. Gravity appears in the equations of particle motion along with the interparticle forces but the two are not separable. A wind tunnel that perimits multiphase flow experiments with wind blown particles at variable gravity was built and experiments were conducted at reduced gravity. The equations of particle motion initiation (saltation threshold) with variable gravity were experimentally verified and the interparticle force was separated. A uniquely design Carousel Wind Tunnel (CWT) allows for the long flow distance in a small sized tunnel since the test section if a continuous loop and develops the required turbulent boundary layer. A prototype model of the tunnel where only the inner drum rotates was built and tested in the KC-135 Weightless Wonder 4 zero-g aircraft. Future work includes further experiments with walnut shell in the KC-135 which sharply graded particles of widely varying median sizes including very small particles to see how interparticle force varies with particle size, and also experiments with other aeolian material.
Results are reported for wind-tunnel experiments performed to determine the threshold friction speed of particles with different densities. Experimentally determined threshold speeds are plotted as a function of particle diameter and in terms of threshold parameter vs particle friction Reynolds number. The curves are compared with those of previous experiments, and an A-B curve is plotted to show differences in threshold speed due to differences in size distributions and particle shapes. Effects of particle diameter are investigated, an expression for threshold speed is derived by considering the equilibrium forces acting on a single particle, and other approximately valid expressions are evaluated. It is shown that the assumption of universality of the A-B curve is in error at very low pressures for small particles and that only predictions which take account of both Reynolds number and effects of interparticle forces yield reasonable agreement with experimental data. Effects of nonerodible surface roughness are examined, and threshold speeds computed with allowance for this factor are compared with experimental values. Threshold friction speeds on Mars are then estimated for a surface pressure of 5 mbar, taking into account all the factors considered.
The physical and chemical properties of colloidal systems are central to both natural and synthetic processes that enable a wide range of energy and environmental applications. These properties are an emergent outcome of the structure that colloidal systems adopt in response to the interplay of electrical, van der Waals, hydration, and steric forces coupled to the inherent fluctuations of the system. Here, in this study, we review the nature of those forces and show how variations in their relative importance lead to distinct free energy landscapes and consequent dynamic behaviors, illustrated for colloidal dispersions, nanocrystal superlattices, and mesocrystlline solids formed through oriented attachment. We end by discussing the challenges to future progress arising from the need to seamless couple from molecular to particle to ensemble scales.
Superlattice structures formed by nanoparticle (NP) self-assembly have attracted increasing attention due to their potential as a novel class of nanomaterials with enhanced physicochemical properties tailored by the assembly structure. However, many key questions remain regarding the correlation between the dynamics of individual NPs and the emerging superlattice patterns. Here we investigated the self-assembly of gold NPs by employing in situ transmission electron microscopy equipped with direct detection camera capabilities, which enabled us to track the rapid motion of individual nanoparticles in real time. By calculating the contributions of Brownian, van der Waals, hydrodynamic, and steric hindrance forces, we obtained a quantitative evaluation of the competitive interactions that drive the assembly process. Such competition between forces over various separations is critical for the kinetics of cluster growth, as well as the superlattice formation. Brownian motion resulted in random particle motions to form small-sized clusters, whose growth dynamics was characterized as reaction-limited aggregation. Subsequently, at relative short-range particle separation, van der Waals force overrode the Brownian force and dominantly drove the assembly process. In the close proximity, a delicate balance between van der Waals and steric hindrance forces surprisingly led to a unique dynamic nature of the assembled superlattice. Our study provides a fundamental understanding of coupling energetics and dynamics of NPs involved in the assembly process, enabling the control and design of the structure of nanoparticle superlattices.
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Nanoparticle (NP) superlattices have attracted increasing attention due to their unique properties. However, key questions remain for predicting the nanoparticle behavior from interparticle forces, especially the role of hydration force (Fhyd) and its correlation to other forces, regarding the transient and final superlattice configurations. Here we investigated the self-assembly of Ag NPs in aqueous solution by employing in situ liquid cell transmission electron microscopy, combined with atomic force microscopy based force measurements and theoretical calculations. In spite of instantaneous Brownian motion of NPs, a correlation between velocity and van der Waals force (FvdW) on average was observed during the later self-assembly process. In the post-assembly state, a delicate balance between Fhyd and FvdW gives rise to ~ 0.6~0.9 nm separation be-tween NPs in the superlattice. Our study demonstrates pivotal roles of interparticle forces, enabling the control of the separation which is critical for tailoring the properties of superlattices.
The interplay between crystal and solvent structure, interparticle forces and ensemble particle response dynamics governs the process of crystallization by oriented attachment (OA), yet a quantitative understanding is lacking. Using as a model system ZnO, we combine in situ TEM observations of single particle and ensemble assembly dynamics with simulations of interparticle forces and responses to relate experimentally derived interparticle potentials to the underlying interactions. We show that OA is driven by forces and torques due to a combination of electrostatic ion-solvent correlations and dipolar interactions that act at separations well beyond 5 nm. Importantly, coalignment is achieved before particles reach separations at which strong attractions drive the final jump to contact. The observed barrier to attachment is negligible, while dissipative factors in the quasi-2D confinement of the TEM fluid cell lead to abnormal diffusivities with timescales for rotation much less than for translation, thus enabling OA to dominate.
Nanoparticle self-assembly plays a key role in formation of superlattices, which exhibit remarkable physical and chemical properties. However, controlling assembly remains a challenge partly due to a lack of understanding of the assembly dynamics and the difficulty in linking interfacial solution properties to interparticle forces. In this study, using liquid-cell transmission electron microscopy, self-assembly of gold nanoparticles (NPs) into superlattices in mixtures of water and ionic liquid (IL) was visualized, revealing a dual role of the IL in the assembly process. At intermediate concentrations, the IL acts as a surfactant stabilizing the particles at a well-defined equilibrium separation corresponding to the length of hydrogen bonded IL cations adsorbed onto neighboring NPs. Analysis of the interparticle forces reveals attractive long-range interactions of a van der Waals nature. At separations of 1-3 nm, interactions are dominated by attractive ion correlation and repulsive hydration forces giving rise to an energy minimum at 1.5 nm separation. The superlattice is further stabilized by hydrogen bonding, which shifts the equilibrium interparticle distance to 1.1 nm. In contrast, at higher concentrations, IL accumulates and forms a structured network in the gap between nanoparticles, where it acts as a solvent that eliminates the repulsive barrier and thus promotes particle coalescence. This solvent-surfactant duality of IL opens new opportunities for their use in directing particle assembly.
Predicting nanoparticle aggregation and attachment phenomena requires a rigorous understanding of the interplay among crystal structure, particle morphology, surface chemistry, solution conditions, and interparticle forces, yet no comprehensive picture exists. We used an integrated suite of experimental, theoretical, and simulation methods to resolve the effect of solution pH on the aggregation of boehmite nanoplatelets, a case study with important implications for the environmental management of legacy nuclear waste. Real-time observations showed that the particles attach preferentially along the (010) planes at pH 8.5 and the (101) planes at pH 11. To rationalize these results, we established the connection between key physicochemical phenomena across the relevant length scales. Starting from molecular-scale simulations of surface hydroxyl reactivity, we developed an interfacial-scale model of the corresponding electrostatic potentials, with subsequent particle-scale calculations of the resulting driving forces allowing successful prediction of the attachment modes. Finally, we scaled these phenomena to understand the collective structure at the aggregate-scale . Here, our results indicate that facet-specific differences in surface chemistry produce heterogeneous surface charge distributions that are coupled to particle anisotropy and shape-dependent hydrodynamic forces, to play a key role in controlling aggregation behavior.
The constitutive behavior of uncemented granular materials such as strength, stiffness, and localization of deformations are to a large extend derived from interparticle friction transmitted between solid particles and particle groups. Interparticle forces are highly dependent on gravitational body forces. At very low effective confining pressures, the true nature of the Mohr envelope, which defines the Mohr-Coulomb failure criterion for soils, as well as the relative contribution of each of non-frictional components to soil's shear strength cannot be evaluated in terrestrial laboratories. Because of the impossibility of eliminating gravitational body forces on earth, the weight of soil grains develops interparticle compressive stresses which mask true soil constitutive behavior even in the smallest samples of models. Therefore the microgravity environment induced by near-earth orbits of spacecraft provides unique experimental opportunities for testing theories related to the mechanical behavior of terrestrial granular materials. Such materials may include cohesionless soils, industrial powders, crushed coal, etc. This paper will describe the microgravity experiment, 'Mechanics of Granular Materials (MGM)', scheduled to be flown on Space Shuttle-MIR missions. The paper will describe the experiment's hardware, instrumentation, specimen preparation procedures, testing procedures in flight, as well as a brief summary of the post-mission analysis. It is expected that the experimental results will significantly improve the understanding of the behavior of granular materials under very low effective stress levels.
The development of structural hierarchy on various length scales during crystallization process is ubiquitous in biological systems and is also observed in synthetic nanomaterials. The driving forces for the formations of complex architectures range from local interfacial interactions, that modify interfacial speciation, local supersaturation, and nucleation barriers, to macroscopic interparticle forces. Although it is enticing to interpret the formation of hierarchical architectures as the assembly of independently nucleated building blocks, often crystallization pathways follow monomer-by-monomer addition with structural complexity arising from interfacial chemical coupling and strongly correlated fluctuation dynamics in the electric double layers. Here, the mechanism of the development of structural hierarchy through heterogeneous nucleation, coupled interfacial nucleation and assembly, and oriented attachment of independently nucleated particles is discussed. In this article, the emphasis is made on the discussion of the underlying interfacial forces and chemical coupling that drives crystallization pathways towards the formation of structural hierarchy.
The development of structural hierarchy on various length scales during the crystallization process is ubiquitous in biological systems and minerals and is common in synthetic nanomaterials. The driving forces for the formation of complex architectures range from local interfacial interactions, that modify interfacial speciation, local supersaturation, and nucleation barriers, to macroscopic interparticle forces. Although it is enticing to interpret the formation of hierarchical architectures as the assembly of independently nucleated building blocks, crystallization pathways often follow monomer-by-monomer addition with structural complexity arising from interfacial chemical coupling and strongly correlated fluctuation dynamics in the electric double layers. Here, we show that the development of structural hierarchy through heterogeneous nucleation is driven by dipolar and solvation forces. Specifically, coupled simulations and experimental studies revealed that dipole build-up along the slow growth direction can trigger twinning and the development of branched architectures. Enthalpic solvation interactions were shown to either enhance or reduce the dipole moment of the nanoparticles and, thereby, control crystal morphology and architecture. The systematic studies of chemical coupling between different solvents and undercoordinated surface atoms of the growing nanocrystals revealed the mechanism of dimensionality control and the development of structural hierarchy without ligands or structure-directing agents.
The multi-step crystallization processes involving the formation of stable building blocks that subsequently assemble into a crystal are ubiquitous in mineral formation and biomineralization and are particularly attractive in materials synthesis. Utilizing these pathways offers the approach to overcoming the restrictions on the expression of various crystal faces imposed by the interfacial energy during monomer-by-monomer growth to unlock the breadth of architectures with unique properties. Further, controlling particle-based crystallization proved challenging despite its promise due to the complex interdependence of interfacial forces and their non-linear dependence on synthesis parameters. Here, the status of the development of state-of-the-art approaches to measuring interparticle forces and predictive theoretical models of particle-based crystallization are reviewed.
The NASA HEDS Program is duly concerned for human explorers regarding the potential hazard posed by the ubiquitous dust mantle on Mars. To evaluate properties of dust that could be hazardous to humans, the MPS 2001 Lander payload will include the Mars Environmental Compatibility Assessment (MECA) experiment. This includes optical and atomic-force microscopy to evaluate soil grains for shape and size, wet chemistry to evaluate toxic substances, electrometry to evaluate triboelectric charging, and test-material palets to evaluate electrostatic and magnetic adhesion, and the hardness/abrasiveness of soil grains; these experimental subcomponents are delivered samples by the camera-equipped robotic arm of the lander which will acquire material from depths of 0.5 to 1.0 m in the soil. Data returned by MECA will be of value to both the BEDS and planetary/astrobiology communities. Dust poses a threat to human exploration because the martian system does not hydrologically or chemically remove fine particles that are being continuously generated by thermal, aeolian, and colluvial weathering, and by volcanism and impact over billions of years. The dust is extremely fine-grained, in copious quantities, ubiquitous in distribution, continually mobile, and a source of poorly-grounded static charges -- a suite of characteristics posing a particulate and electrical threat to explorers and their equipment. Dust is mobilized on global and regional scales, but probably also unpredictably and violently at local scales by dust devils. The latter might be expected in great abundance owing to near surface atmospheric instability (dust devils were detected by Pathfinder during its brief lifetime). Preliminary laboratory experiments suggest that space-suit materials subjected to windblown dust may acquire a uniform, highly adhesive dust layer that is also highly cohesive laterally owing to electrostatic forces. This layer will obscure visibility through the helmet visor, penetrate joints and fabrics, change the thermal properties of the suit, and possibly affect electronic/electrical suit functions. It is paramount that future missions address the issue of interparticle forces, and in particular, the role played by ionizing radiation in affecting these forces on Mars.
The NASA HEDS Program is duly concerned for human explorers regarding the potential hazard posed by the ubiquitous dust mantle on Mars. To evaluate properties of dust that could be hazardous to humans, the NMS 2001 Lander payload will include the Mars Environmental Compatibility Assessment (MECA) experiment. This includes optical and atomic-force microscopy to evaluate soil grains for shape and size, wet chemistry to evaluate toxic substances, electrometry to evaluate triboelectric charging, and test-material palets to evaluate electrostatic and magnetic adhesion, and the hardness/abrasiveness of soil grains; these experimental subcomponents are delivered samples by the camera-equipped robotic arm of the lander which will acquire material from depths of 0.5 to 1.0 m in the soil. Data returned by MECA will be of value to both the hEDS and planetary/astrobiology communities. Dust poses a threat to human exploration because the martian system does not hydrologically or chemically remove fine particles that are being continuously generated by thermal, aeolian, and colluvial weathering, and by volcanism and impact over billions of years. The dust is extremely fine-grained, in copious quantities, ubiquitous in distribution, continually mobile, and a source of poorly-grounded static charges -- a suite of characteristics posing a particulate and electrical threat to explorers and their equipment. Dust is mobilized on global and regional scales, but probably also unpredictably and violently at local scales by dust devils. The latter might be expected in great abundance owing to near surface atmospheric instability (dust devils were detected by Pathfinder during its brief lifetime). Preliminary laboratory experiments suggest that space-suit materials subjected to windblown dust may acquire a uniform, highly adhesive dust layer that is also highly cohesive laterally owing to electrostatic forces. This layer will obscure visibility through the helmet visor, penetrate joints and fabrics, change the thermal properties of the suit, and possibly affect electronic/electrical suit functions. It is paramount that future missions address the issue of interparticle forces, and in particular, the role played by ionizing radiation in affecting these forces on Mars.
Understanding defect healing is necessary for realizing devices based on nanoparticle-superlattices with controlled electronic and optoelectronic performance. However, key questions remain regarding nanoparticle interactions and resulting assembly dynamics and defect self-elimination. In particular, for anisotropic particles, additional degrees of freedom beyond those of spherical particles, such as rotational dynamics and toques, significantly impact phenomena. Here, in this work, we investigate nanocube (NC) superlattices by employing liquid phase transmission electron microscopy, continuum theories and molecular dynamics simulations. Analyzing interparticle forces and torques due to van der Waals, Brownian, and ligand interactions, we find that the latter dominates and that the anisotropic NC morphology introduces significant torques. In imperfect regions, unbalanced forces and torques induce NC translations and rotations that are transmitted to neighboring NCs, prompting “chain interactions” in a 2D network, which lead to defect self-elimination. This fundamental understanding will further enable design and fabrication of defect-free superlattices, as well as those with tailored defects, via assembly of anisotropic particles.