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116 records · Page 7

Ring particles - Collisional interactions and physical nature

Attention is given to the properties of, and dynamical processes affecting individual particles of Saturn's rings. Because particles tend to be gravitationally bound when located on the surfaces of larger particles, and since net tidal stresses within the particles are small, particle collisions should produce accretion in Saturn's rings. Rapid accretionary processes within the rings are counterbalanced by tidal disruption of the larger accreted aggregates, which are presently designated 'dynamic ephemeral bodies'. The coefficient of restitution is probably very low, implying that the large particles containing most of the rings' mass are in a monolayer, although the small particles responsible for most of the rings' visible cross section form a layer many particles thick. Kinematic viscosity and interparticle erosive process models should incorporate these properties.

Weidenschilling, S. J.↗

Facet-dependent dispersion and aggregation of aqueous hematite nanoparticles

Nanoparticle aggregates in solution controls surface reactivity and function. Complete dispersion often requires additive sorbents to impart a net repulsive interaction between particles. Facet engineering of nanocrystals offers an alternative approach to produce monodisperse suspensions simply based on facet-specific interaction with solvent molecules. Here, we measure the dispersion/aggregation of three morphologies of hematite (α-Fe 2 O 3 ) nanoparticles in varied aqueous solutions using ex situ electron microscopy and in situ small-angle x-ray scattering. We demonstrate a unique tendency of (104) hematite nanoparticles to maintain a monodisperse state across a wide range of solution conditions not observed with (001)- and (116)-dominated particles. Density functional theory calculations reveal an inert, densely hydrogen-bonded first water layer on the (104) facet that favors interparticle dispersion. Results validate the notion that nanoparticle dispersions can be controlled through morphology for specific solvents, which may help in the development of various nanoparticle applications that rely on their interfacial area to be highly accessible in stable suspensions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Grain dynamics in zero gravity

The dynamics of granular materials has proved difficult to model, primarily because of the complications arising from inelastic losses, friction, packing, and the effect of many grains being in contact simultaneously. One interesting limit for which it was recently possible to construct a theory is that where the grain-grain interactions are dominated by binary collisions. The kinetic model of granular systems if similar to the kinetic theory of gases, except that collisional energy losses are always present in the former and must be treated explicitly. Few granular materials on Earth are describable by this limiting model, since gravity tends to collapse the grains into a high-density state where Coulombic friction effects are dominant. The planned Space Station offers an unusual opportunity to test the kinetic grain model and to explore its predictions. Without gravity, the regime of low interparticle velocities, where an elastic description of the collision is still valid, is investigated. This will allow direct interpretation by dynamical computer simulations as well as by kinetic theory.

Werner, B. T.↗

Tuning perovskite nanocrystal superlattices for superradiance in the presence of disorder

The cooperative emission of interacting nanocrystals is an exciting topic fueled by recent reports of superfluorescence and superradiance in assemblies of perovskite nanocubes. Several studies estimated that coherent coupling is localized to a small fraction of nanocrystals (10 -7 –10 -3 ) within the assembly, raising questions about the origins of localization and ways to overcome it. In this work, we examine single-excitation superradiance by calculating radiative decays and the distribution of superradiant wave function in two-dimensional CsPbBr 3 nanocube superlattices. The calculations reveal that the energy disorder caused by size distribution and large interparticle separations reduces radiative coupling and leads to the excitation localization, with the energy disorder being the dominant factor. The single-excitation model clearly predicts that, in the pursuit of cooperative effects, having identical nanocubes in the superlattice is more important than achieving a perfect spatial order. The monolayers of large CsPbBr 3 nanocubes (L NC = 10–20 nm) are proposed as model systems for experimental tests of superradiance under conditions of non-negligible size dispersion, while small nanocubes (L NC = 5–10 nm) are preferred for realizing the Dicke state under ideal conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Fluid Physics in a Fluctuating Acceleration Environment

Our program of research aims at developing a stochastic description of the residual acceleration field onboard spacecraft (g-jitter) to describe in quantitative detail its effect on fluid motion. Our main premise is that such a statistical description is necessary in those cases in which the characteristic time scales of the process under investigation are long compared with the correlation time of g-jitter. Although a clear separation between time scales makes this approach feasible, there remain several difficulties of practical nature: (i), g-jitter time series are not statistically stationary but rather show definite dependences on factors such as active or rest crew periods; (ii), it is very difficult to extract reliably the low frequency range of the power spectrum of the acceleration field. This range controls the magnitude of diffusive processes; and (iii), models used to date are Gaussian, but there is evidence that large amplitude disturbances occur much more frequently than a Gaussian distribution would predict. The lack of stationarity does not constitute a severe limitation in practice, since the intensity of the stochastic components changes very slowly during space missions (perhaps over times of the order of hours). A separate analysis of large amplitude disturbances has not been undertaken yet, but it does not seem difficult a priori to devise models that may describe this range better than a Gaussian distribution. The effect of low frequency components, on the other hand, is more difficult to ascertain, partly due to the difficulty associated with measuring them, and partly because they may be indistinguishable from slowly changing averages. This latter effect is further complicated by the lack of statistical stationarity of the time series. Recent work has focused on the effect of stochastic modulation on the onset of oscillatory instabilities as an example of resonant interaction between the driving acceleration and normal modes of the system, and on cavity flow as an example of how an oscillatory response under periodic driving becomes diffusive if the forcing is random instead. This paper describes three different topics that illustrate behavior that is peculiar to a stochastic acceleration field. In the first case, we show that g-jitter can induce effective attractive or repulsive forces between a pair of spherical particles that are suspended in an incompressible fluid of different density provided that the momentum diffusion length is larger than the interparticle separation (as in the case in most colloidal suspensions). Second, a stochastic modulation of the control parameter in the vicinity of a pitchfork or supercritical bifurcation is known not to affect the location of the threshold. We show, however, that resonance between the modulation and linearly stable modes close to onset can lead to a shift in threshold. Finally, we discuss the classical problem of vorticity diffusion away from a plane boundary that is being vibrated along its own plane. Periodic motion with zero average vorticity production results in an exponential decay of the vorticity away from the boundary. Random vibration, on the other hand, results in power law decay away from the boundary even if vorticity production averages to zero.

Drolet, Francois↗

Dependent scattering and fractal microstructure determine the transparency of aerogel monoliths

This study reveals how dependent scattering and microstructure significantly affect electromagnetic wave propagation through aerogel monoliths, contributing to their transparency. Light scattering by particle ensembles is considered “dependent” when the scattering properties rely not only on particle size and optical constants but also on their spatial distribution, typically occurring when the average interparticle distance is small in comparison with the wavelength of incident radiation. Addressing dependent scattering requires solving Maxwell’s equations for complex heterogeneous structures, which is computationally demanding and usually limited to sample thicknesses on the same scale as the wavelength. This study combines computer-generated ambigel microstructures of fractal aggregates of polydisperse nanoparticles and the radiative transfer with reciprocal transaction method to predict the transmittance of thick ambigel slabs. Transmittance measurements of ambiently dried aerogel monoliths (ambigels) with porosities from about 50% to 90% closely matched the predicted values for their digital twins. However, ignoring dependent scattering or particle aggregation led to inaccurate predictions. This study validated the computational framework, and its findings offer insights for designing photonic metamaterials and analyzing their interactions with electromagnetic waves.

Yalcin, Refet A. (ORCID:0000000339973494)↗

Effect of Hydrophilicity and Interfacial Water Structure on Particle Attachment

Oriented attachment (OA) of nanoparticles is an important and common crystallization pathway. Efforts to isolate and quantify the interparticle forces that underlie OA have only recently been initiated and the role played by the interfacial solvent structure in the confined region between nanocrystal surfaces in enabling and controlling OA remains an open question. In this work, classical molecular dynamics (MD) simulations were performed to compute the free energy landscape of nanoparticles approaching mineral substrates in both vacuum and pure water. Periclase (MgO), muscovite (KAl 3 Si 3 O 10 (OH) 2 ), and pyrophyllite (Al 2 Si 4 O 10 (OH) 2 ) nanoparticles exposing the (100), (001), and (001) surfaces, respectively, were brought to contact with substrates exposing the same surfaces. These mineral surfaces were selected to investigate a range of hydrophilicities (periclase > muscovite > pyrophyllite). The MD simulations revealed that the interfacial water structure created free energy minima for nanoparticle approach that corresponded to integer numbers of intervening water layers. The depth of the free energy minima and the free energy barriers between minima correlated positively with the hydrophilicity of the mineral surface. While the range of solvent-mediated interactions was predicted to be short (a few intervening water layers at most for MgO), the free energy barriers were calculated to be large (fraction of an eV per nm 2 ) and the effect of misalignment diminished rapidly with the number of intervening water layers. The results help explain the formation of mesocrystals and the observed ability of nanoparticles to rotate before attachment while in a long-lived solvent-separated state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Plasmonic surface lattice resonances in nanoparticle arrays

This work reviews the literature and provides a detailed computational analysis of the optical properties of one- and two-dimensional arrays of silver and gold nanoparticles, with emphasis on surface lattice resonances (SLRs) that arise when localized plasmon resonances (LSPRs) in the nanoparticles couple to diffraction resonances that are determined by the interparticle spacing to give polariton modes in which the two types of excitations are coherently coupled. The computations are based on the coupled dipole approximation, which provides a nearly quantitative description of the extinction spectra for arrays of this type where the particles are well separated and not too large. The computations are used to determine many characteristics of SLRs associated with the lower polariton mode that is mostly photonic in nature, and we also study the upper polariton that is dominated by the LSPR response, as well as Rayleigh anomalies (RAs) that correspond to purely diffractive excitation. The calculations explore the sensitivity of these excitations to the directions of the incident wave and polarization vectors relative to the array axis, the effect of array spacing and number of particles in the array, and the effect of nanoparticle radius and background refractive indices. Details of the physical mechanisms involved in determining blue- and/or redshifts as structural parameters are varied is provided, with SLR’s being sensitive to far-field coupling, while LSPR’s can also be sensitive to near- and intermediatefield interactions that in some cases are similar to effects found in dye molecule aggregates.

77 NANOSCIENCE AND NANOTECHNOLOGY↗