Nanodomains and Their Temperature Dependence in a Phosphonium-Based Ionic Liquid: A Single-Molecule Tracking Study
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Opare-Addo, Jemima↗
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Influence of Kosmotrope and Chaotrope Salts on Water Structural Relaxation
The structural relaxation in water solutions of kosmotrope (structure maker) and chaotrope (structure breaker) salts, namely sodium chloride, potassium chloride, and cesium chloride, were studied through quasielastic neutron scattering measurements. We found that the collective dynamics relaxation time at the structure factor peak obtained using heavy water solutions shows a distinctively different behavior in the kosmotrope as opposed to the chaotrope solutions, increasing with the salt concentration in the former and decreasing in the latter. In both cases the trends are proportional to the concentration dependence of the relative viscosity of the solutions. Furthermore, these results indicate that kosmotropes and chaotropes influence the solution’s viscosity by impacting in opposite ways the hydrogen bond network of water, strengthening it in one case and softening it in the other.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Linear Viscoelastic Properties of Putative Cyclic Polymers Synthesized by Reversible Radical Recombination Polymerization (R3P)
Linear viscoelastic properties in both melt and solution states are reported for a series of poly(3,6-dioxa-1,8-octanedithiol) (polyDODT) made by reversible radical recombination polymerization (R 3 P) under conditions designed to produce linear (LDODT), cyclic (RDODT) and linear-cyclic mixtures (LRDODT). PolyDODT is amorphous (T g < -50 °C) and highly flexible (entanglement molecular weight M e,lin ≈ 1850 g/mol for LDODT). PolyDODT’s low T g and low M e,lin enable characterization over a wide dynamic range and a wide range of dimensionless weight-average molecular weight Z w = M w /M e,lin . Measurements at temperatures from -57 °C to 100 °C provide up to 18 deades of reduced frequency, which is necessary to characterize RDODT melts with Z w from 23 to 300. The two highest molecular weight polymers in the present RDODT series have such high M w (406k and 556k g/mol) that mass spectrometry, NMR spectroscopy, and even chemical assays for chain ends are unable to rule out up to 2 mol% linear contaminant. By studying the samples in solution (using dilution to reduce Z w ) we could compare their dynamics with those of previously established high-purity polystyrene (PS) rings (limited to Z w ≤ 13.6). RDODT solutions with Z w < 15 (concentrations <5wt% for RDODT-406k and 556k) have dynamic moduli G^* that accord with LCCC-purified PS rings in terms of the frequency dependence (including the absence of a plateau), the progression of shapes of G* as a function of Z w , and the linear scaling of their zero-shear viscosity η0 with M w . The shape of G* as a function of Z w for solutions of RDODT-406k and -556k also accord with lower M w RDODT melts (which have ≤ 1.3mol% linear contaminant). Thus, measurement of the linear viscoelastic properties of appropriate concentrations of high M w (>200k g/mol) putative cyclic polymers, in which linear chains evade spectroscopic detection, may provide an alternative means (though not fully proven) of validation of sample purity. When Z w > 15 (including all seven RDODT melts and eight of their solutions), G* has a rubbery plateau. This suggests that the onset of entanglement-like behavior in rings requires 4-5-fold greater Z w than is required for linear chains. Further, the plateau moduli of RDODT samples are indistinguishable from G N o of the corresponding LDODT (melt or matched-concentration solutions). In entangled linear polymers, the observation that G N o is independent of Z w follows from limitations on lateral fluctuations due to neighboring chains becoming independent of position along a given chain. The present results for RDODT suggest that this holds for sufficiently long endless chains, too. While the RDODT have the same G N o as entangled LDODT, when Z w > 60 the terminal relaxation, if reached at all, of RDODT extends to orders of magnitude lower frequency than an entangled linear polymer of the same Z w . Consequently, the viscosity of RDODT with Z w > 60 increases with Z w much more strongly than the 3.4-power observed for entangled linear polymers. Lastly, these novel polymers, with disulfide-linked backbone and broad relaxation time distribution may prove important in relation to biodegradable elastomers and materials with exceptional low-frequency dissipation, extending at least 12 decades below the onset of the rubbery plateau.
32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
XPCS Microrheology and Rheology of Sterically Stabilized Nanoparticle Dispersions in Aprotic Solvents
In this study, X-ray photon correlation spectroscopy (XPCS) microrheology and conventional bulk rheology were performed on silica nanoparticle dispersions associated with battery electrolyte applications to probe the properties of these specific complex materials and to explore the utility of XPCS microrheology in characterizing nanoparticle dispersions. Sterically stabilized shear-thickening electrolytes were synthesized by grafting poly(methyl methacrylate) chains onto silica nanoparticles. Coated silica dispersions containing 5–30 wt % nanoparticles dispersed in propylene carbonate were studied. In general, both XPCS microrheology and conventional rheology showed that coated silica dispersions were more viscous at higher concentrations, as expected. The complex viscosity of coated silica dispersions showed shear-thinning behavior over the frequency range probed by XPCS measurements. However, measurements using conventional mechanical rheometry yielded a shear viscosity with weak shear-thickening behavior for dispersions with the highest concentration of 30% particles. Our results indicate that there is a critical concentration needed for shear-thickening behavior, as well as appropriate particle size and surface polymer chain length, for this class of nanoparticle-based electrolytes. The results of this study can provide insights for comparing XPCS microrheology and bulk rheology for related complex fluids and whether XPCS microrheology can capture expected macroscopic rheological properties by probing small-scale particle dynamics.
36 MATERIALS SCIENCE↗
Global Simulations of Phase State and Equilibration Time Scales of Secondary Organic Aerosols with GEOS-Chem
The phase state of secondary organic aerosols (SOA) can range from liquid through amorphous semisolid to glassy solid, which is important to consider as it influences various multiphase processes including SOA formation and partitioning, multiphase chemistry, and cloud activation. In this study, we simulate the glass transition temperature and viscosity of SOA over the globe using the global chemical transport model, GEOS-Chem. The simulated spatial distributions show that SOA at the surface exist as liquid over equatorial regions and oceans, semisolid in the midlatitude continental regions, and glassy solid over lands with low relative humidity. The predicted SOA viscosities are mostly consistent with the available measurements. In the free troposphere, SOA particles are mostly predicted to be semisolid at 850 hPa and glassy solid at 500 hPa, except over tropical regions including Amazonia, where SOA are predicted to be low viscous. Phase state also exhibits seasonal variation with a higher frequency of semisolid and solid particles in winter compared to warmer seasons. We calculate equilibration time scales of SOA partitioning (τ eq ) and effective mass accommodation coefficient (α eff ), indicating that τ eq is shorter than the chemical time step of GEOS-Chem of 20 min and αeff is close to unity for most locations at the surface level, supporting the application of equilibrium SOA partitioning. However, τ eq is prolonged and α eff is lowered over drylands and most regions in the upper troposphere, suggesting that kinetically limited growth would need to be considered for these regions in future large-scale model studies.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Pore‐Scale Modeling of Carbon Dioxide and Hydrogen Transport During Geologic Gas Storage
Abstract Geologic storage of CO 2 and H 2 are climate‐positive techniques for meeting the energy transition. While similar formations could be considered for both gases, the flow dynamics could differ due to differences in their thermophysical properties. We conduct a rigorous pore‐scale study of water/CO 2 and water/H 2 systems at relevant reservoir conditions in a Bentheimer rock sample using the lattice Boltzmann method to quantify the effects of capillary, viscous, inertial, and wetting forces during gas invasion. At similar conditions, H 2 invasion is weaker compared to CO 2 due to unfavorable viscosity ratios. Increasing flow rate, however, increases the breakthrough saturation for both gas systems in the range of capillary numbers studied. At isolated conditions of flow rate, viscosity ratio, and wettability, local inertial effects are found to be critical and show consistent increase in the invaded gas saturation. The effect of inertial forces persits for both gases across all field conditions tested.
58 GEOSCIENCES↗
Thermodynamic and transport properties of two-temperature SF{sub 6} plasmas
This paper deals with thermodynamic and transport properties of SF{sub 6} plasmas in a two-temperature model for both thermal equilibrium and non-equilibrium conditions. The species composition and thermodynamic properties are numerically determined using the two-temperature Saha equation and Guldberg-Waage equation according to deviation of van de Sanden et al. Transport properties including diffusion coefficient, viscosity, thermal conductivity, and electrical conductivity are calculated with most recent collision interaction potentials by adopting Devoto's electron and heavy particle decoupling approach but expanded to the third-order approximation (second-order for viscosity) in the frame of Chapman-Enskog method. The results are computed for various values of pressures from 0.1 atm to 10 atm and ratios of the electron temperature to the heavy particle temperature from 1 to 20 with electron temperature range from 300 to 40 000 K. In the local thermodynamic equilibrium regime, results are compared with available results of previously published studies.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Spatio-temporal evolution of the L {yields} I {yields} H transition
We investigate the dynamics of the low(L) {yields} high(H) transition using a time-dependent, one dimensional (in radius) model which self-consistently describes the time evolution of zonal flows (ZFs), mean flows (MFs), poloidal spin-up, and density and pressure profiles. The model represents the physics of ZF and MF competition, turbulence suppression via E Multiplication-Sign B shearing, and poloidal flows driven by turbulence. Numerical solutions of this model show that the L{yields}H transition can occur via an intermediate phase (I-phase) which involves oscillations of profiles due to ZF and MF competition. The I-phase appears as a nonlinear transition wave originating at the edge boundary and propagates inward. Locally, I-phase exhibits the characteristics of a limit-cycle oscillation. All these observations are consistent with recent experimental results. We examine the trigger of the L{yields}H transition, by defining a ratio of the rate of energy transfer from the turbulence to the zonal flow to the rate of energy input into the turbulence. When the ratio exceeds order unity, ZF shear gains energy, and a net decay of the turbulence is possible, thus triggering the L{yields}H transition. Numerical calculations indicate that the L{yields}H transition is triggered by this peak of the normalized ZF shearing. Zonal flows act as 'reservoir,' in which to store increasing fluctuation energy without increasing transport, thus allowing the mean flow shear to increase and lock in the transition. A counterpart of the L {yields} I{yields}H transition, i.e., an L{yields}H transition without I-phase, is obtained in a fast power ramp, for which I-phase is compressed into a single burst of ZF, which triggers the transition. Effects of neutral charge exchange on the L{yields}H transition are studied by varying ZF damping and neoclassical viscosity. Results show that the predicted L{yields}H transition power increases when either ZF damping or viscosity increase, suggesting a link between recycling, ZF damping, and the L{yields}H threshold. Studies of fueling effects on the transition and pedestal structure with an emphasis on the particle pinch are reported.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Nonlinear stability of magnetic islands in a rotating helical plasma
Coexistence of the forced magnetic reconnection by a resonant magnetic perturbation (RMP) and the curvature-driven tearing mode is investigated in a helical (stellarator) plasma rotated by helical trapped particle-induced neoclassical flows. A set of Rutherford-type equations of rotating magnetic islands and a poloidal flow evolution equation is revisited. Using the model, analytical expressions of criteria of spontaneous shrinkage (self-healing) of magnetic islands and sudden growth of locked magnetic islands (penetration of RMP) are obtained, where nonlinear saturation states of islands show bifurcation structures and hysteresis characteristics. Considering radial profile of poloidal flows across magnetic islands, it is found that the self-healing is driven by neoclassical viscosity even in the absence of micro-turbulence-induced anomalous viscosity. Effects of unfavorable curvature in stellarators are found to modify the critical values. The scalings of criteria are consistent with low-{beta} experiments in the large helical device.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Effect of neutral collision and radiative heat-loss function on self-gravitational instability of viscous thermally conducting partially-ionized plasma
The problem of thermal instability and gravitational instability is investigated for a partially ionized self-gravitating plasma which has connection in astrophysical condensations. We use normal mode analysis method in this problem. The general dispersion relation is derived using linearized perturbation equations of the problem. Effects of collisions with neutrals, radiative heat-loss function, viscosity, thermal conductivity and magnetic field strength, on the instability of the system are discussed. The conditions of instability are derived for a temperature-dependent and density-dependent heat-loss function with thermal conductivity. Numerical calculations have been performed to discuss the effect of various physical parameters on the growth rate of the gravitational instability. The temperature-dependent heat-loss function, thermal conductivity, viscosity, magnetic field and neutral collision have stabilizing effect, while density-dependent heat-loss function has a destabilizing effect on the growth rate of the gravitational instability. With the help of Routh-Hurwitz's criterion, the stability of the system is discussed.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Residual turbulence from velocity shear stabilized interchange instabilities
The stabilizing effect of velocity shear on the macroscopic, broad bandwidth, ideal interchange instability is studied in linear and nonlinear regimes. A 2D dissipative magnetohydrodynamic (MHD) code is employed to simulate the system. For a given flow shear, V Prime , linear growth rates are shown to be suppressed to below the shear-free level at both the small and large wavelengths. With increasing V Prime , the unstable band in wavenumber-space shrinks so that the peak growth results for modes that correspond to relatively high wavenumbers, on the scale of the density gradient. In the nonlinear turbulent steady state, a similar turbulent spectrum obtains, and the convection cells are roughly circular. In addition, the density fluctuation level and the degree of flattening of the initial inverted density profile are found to decrease as V Prime increases; in fact, unstable modes are almost completely stabilized and the density profile reverts to laminar when V Prime is a few times the classic interchange growth rate. Moreover, the turbulent particle flux diminishes with increasing velocity shear such that all the flux is carried by the classical diffusive flux in the asymptotic limit. The simulations are compared with measurements of magnetic fluctuations from the Maryland Centrifugal Experiment, MCX, which investigated interchange modes in the presence of velocity shear. The experimental spectral data, taken in the plasma edge, are in general agreement with the numerical data obtained in higher viscosity simulations for which the level of viscosity is chosen consistent with MCX Reynolds numbers at the edge. In particular, the residual turbulence in both cases is dominated by elongated convection cells. Finally, concomitant Kelvin-Helmholtz instabilities in the system are also examined. Complete stability to interchanges is obtained only in the parameter space wherein the generalized Rayleigh inflexion theorem is satisfied.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Poloidal flow damping inside transport barriers in a tokamak
The poloidal flow in a tokamak is damped by collisions. Thus, the poloidal damping can be described by the neoclassical theory. The effective poloidal Mach number, M{sub p}, can be of the order of one or higher inside transport barriers in a tokamak. It is found that the poloidal damping rate decreases exponentially as the effective poloidal Mach number increases. The poloidal damping rate is reduced by one order of magnitude in the presence of sonic M{sub p}. We also found that the ion plasma viscosity becomes negligible compared with the electron plasma viscosity when M{sub p}>1.5. In this case, the poloidal flow is damped by electron collisions rather than ion collisions.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Viscous potential flow analysis of electrified miscible finitely conducting fluid through porous media
In this work, a viscous potential flow analysis is used to investigate capillary surface waves between two horizontal finite fluid layers. The two layers have finite conductivities and admit mass and heat transfer. A general dispersion relation is derived. The presence of finite conductivities together with the dielectric permeabilities makes the horizontal electric field play a dual role in the stability criterion. The phenomenon of negative viscosity is observed. A new growth rate parameter, depending on the kinematical viscosity of the lower fluid layer, is found and has a stabilizing effect on the unstable modes. The growth rates and neutral stability curve are given and applied to air-water interface. The effects of various parameters are discussed for the Kelvin-Helmholtz and the Rayleigh-Taylor instabilities.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Ion acoustic shock waves in plasmas with warm ions and kappa distributed electrons and positrons
The monotonic and oscillatory ion acoustic shock waves are investigated in electron-positron-ion plasmas (e-p-i) with warm ions (adiabatically heated) and nonthermal kappa distributed electrons and positrons. The dissipation effects are included in the model due to kinematic viscosity of the ions. Using reductive perturbation technique, the Kadomtsev-Petviashvili-Burgers (KPB) equation is derived containing dispersion, dissipation, and diffraction effects (due to perturbation in the transverse direction) in e-p-i plasmas. The analytical solution of KPB equation is obtained by employing tangent hyperbolic (Tanh) method. The analytical condition for the propagation of oscillatory and monotonic shock structures are also discussed in detail. The numerical results of two dimensional monotonic shock structures are obtained for graphical representation. The dependence of shock structures on positron equilibrium density, ion temperature, nonthermal spectral index kappa, and the kinematic viscosity of ions are also discussed.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Perpendicular currents and electric fields in fully and partially ionized magnetized plasma
Perpendicular currents and self-consistent electric fields in fully and partially ionized plasma in strong magnetic field are analyzed. In fully ionized plasma, the analyses are concentrated on closing of viscosity driven currents. For partially ionized plasma, it is demonstrated that the perpendicular currents could be expressed through the total pressure gradient (including the pressure gradient of neutral particles) and viscosity of neutrals. The self-consistent electric fields and corresponding E(vector sign)×B(vector sign) could be quite large, which is important for various applications, in particular, for the divertor plasma of a tokamak in the detached regime.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
The dynamical crossover in attractive colloidal systems
We study the dynamical arrest in an adhesive hard-sphere colloidal system. We examine a micellar suspension of the Pluronic-L64 surfactant in the temperature (T) and volume fraction (ϕ) phase diagram. According to mode-coupling theory (MCT), this system is characterized by a cusp-like singularity and two glassy phases: an attractive glass (AG) phase and a repulsive glass (RG) phase. The T − ϕ phase diagram of this system as confirmed by a previous series of scattering data also exhibits a Percolation Threshold (PT) line, a reentrant behavior (AG-liquid-RG), and a glass-to-glass transition. The AG phase can be generated out of the liquid phase by using T and ϕ as control parameters. We utilize viscosity and nuclear magnetic resonance (NMR) techniques. NMR data confirm all the characteristic properties of the colloidal system phase diagram and give evidence of the onset of a fractal-like percolating structure at a precise threshold. The MCT scaling laws used to study the shear viscosity as a function of ϕ and T show in both cases a fragile-to-strong liquid glass-forming dynamic crossover (FSC) located near the percolation threshold where the clustering process is fully developed. These results suggest a larger thermodynamic generality for this phenomenon, which is usually studied only as a function of the temperature. We also find that the critical values of the control parameters, coincident with the PT line, define the locus of the FSC. In the region between the FSC and the glass transition lines the system dynamics are dominated by clustering effects. We thus demonstrate that it is possible, using the conceptual framework provided by extended mode-coupling theory, to describe the way a system approaches dynamic arrest, taking into account both cage and hopping effects.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Rheology and stability kinetics of bare silicon nanoparticle inks for low-cost direct printing
Highly dispersed and stable silicon nanoparticles ink is formulated for its application in direct printing or printable electronics. These dispersions are prepared from free-standing silicon nanoparticles which are not capped with any organic ligand, making it suitable for electronic applications. Silicon nanoparticles dispersions are prepared by suspending the nanoparticles in benzonitrile or ethanol by using polypropylene glycol (PPG) as a binder. All the samples show typical shear thinning behavior while the dispersion samples show low viscosities signifying good quality dispersion. Such thinning behavior favors in fabrication of dense films with spin-coating or patterns with drop casting. The dispersion stability is monitored by turbiscan measurements showing good stability for one week. A low-cost direct printing method for dispersion samples is also demonstrated to obtain micro-sized patterns. Low electrical resistivity of resulting patterns, adjustable viscosity and good stability makes these silicon nanoparticles dispersions highly applicable for direct printing process.
36 MATERIALS SCIENCE↗
Flows and torques in Brownian ferrofluids subjected to rotating uniform magnetic fields in a cylindrical and annular geometry
Ferrofluid flow in cylindrical and annular geometries under the influence of a uniform rotating magnetic field was studied experimentally using aqueous ferrofluids consisting of low concentrations (<0.01 v/v) of cobalt ferrite nanoparticles with Brownian relaxation to test the ferrohydrodynamic equations, elucidate the existence of couple stresses, and determine the value of the spin viscosity in these fluids. An ultrasound technique was used to measure bulk velocity profiles in the spin-up (cylindrical) and annular geometries, varying the intensity and frequency of the rotating magnetic field generated by a two pole stator winding. Additionally, torque measurements in the cylindrical geometry were made. Results show rigid-body like velocity profiles in the bulk, and no dependence on the axial direction. Experimental velocity profiles were in quantitative agreement with the predictions of the spin diffusion theory, with a value of the spin viscosity of ∼10{sup −8} kg m/s, two orders of magnitude larger than the value estimated earlier for iron oxide based ferrofluids, and 12 orders of magnitude larger than estimated using dimensional arguments valid in the infinite dilution limit. These results provide further evidence of the existence of couple stresses in ferrofluids and their role in driving the spin-up flow phenomenon.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗