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Disentangling Acid‐Base Chemistry through Blue Shifting Hydrogen Bond Contributions

The blue shifting of vibrational frequencies in hydrogen bonded molecules, as observed in aqueous environments, has been attributed to local partial charge transfer from solvation. Here, in this study, we extrapolate the blue shift model to the stronger ionic interactions between hydrogen bond acceptors associated with protonation through augmented pH levels and competitive interactions with counter ion pairing. The chemical model we utilize in this work is the aqueous pyridine‐pyridinium equilibrium to characterize the blue shifts observed in the pyridinium chloride ionic system. The observed agreement between observed experimental and calculated spectral shifts shows that the blue shifting model can be extrapolated to stronger interactions and accurately describe the nature of the hydrogen bond.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tropospheric gas composition and cloud structure of the Jovian North Equatorial Belt

Voyager IRIS observations of the NEB reveal longitudinal variability of 5-micron brightness temperatures of order 100 C. An anisotropic multiple scattering radiative transfer model is used to calculate synthetic spectra for comparison with the IRIS observations. Mie theory is used to model the spectral dependence of cloud extinction from 180 to 2300/cm. Cloud base locations within the model vary with assumed gas abundances according to thermochemical equilibrium. It is found that spatial variations in the abundance profiles of the condensible species, parahydrogen profiles and cloud optical depths can be used as tracers of the local and large-scale dynamics. The variation of cloud opacity is strongly correlated with the variation of relative humidity, which suggests that dynamic depletion of water vapor above the cloud forming level is the most plausible model to explain the spatial variation in the water profile within the NEB.

Carlson, Barbara E.↗

Airport Pricing Strategies

Conventional economic wisdom suggests that congestion pricing would be an appropriate response to cope with the growing congestion levels currently experienced at many airports. Several characteristics of aviation markets, however, may make naive congestion prices equal to the value of marginal travel delays a non-optimal response. This paper has developed a model of airport pricing that captures a number of these features. The model in particular reflects that airlines typically have market power and are engaged in oligopolistic competition at different sub-markets; that part of external travel delays that aircraft impose are internal to an operator and hence should not be accounted for in congestion tolls. We presented an analytical treatment for a simple bi-nodal symmetric network, which through the use of 'hyper-networks' would be readily applicable to dynamic problems (in discrete time) such as peak - off-peak differences, and some numerical exercises for the same symmetric network, which was only designed to illustrate the possible comparative static impacts of tolling, in addition to marginal equilibrium conditions as could be derived for the general model specification. Some main conclusions are that second-best optimal tolls are typically lower than what would be suggested by congestion costs alone and may even be negative, and that the toll as derived by Brueckner (2002) may not lead to an increase in total welfare. While Brueckner (2002) has made clear that congestion tolls on airports may be smaller than expected when congestion costs among aircraft are internal for a firm, our analysis adds to this that a further downward adjustment may be in order due to market power. The presence of market power (which causes prices to exceed marginal costs) may cause the pure congestion toll to be suboptimal, because the resulting decrease in demand is too high (the pure congestion tall does not take into account the decrease in consumer surplus). The various downward adjustments in welfare maximizing tolls may well cause the optimal values of these to be negative. Insofar as subsidization is considered unacceptable for whichever reason, our results warn that the most efficient among the non-negative tolls may actually be a zero toll; the pure congestion toll may actually decrease welfare compared to the base case. The model in this paper contains a few simplifying assumptions that may be relaxed in future work. Load factors and aircraft capacity are fixed in this model for simplicity. In a more advanced version of this model, load factors and aircraft capacity can be endogenized. This makes the derivation of the optimality conditions far more complicated, but it should be feasible in a numerical experiment. One can also add a fourth layer to the model, describing the airport's optimization problem. For example, the airport can maximize profits under a cost recovery constraint. The model then deals with interactions between four types of agents. No distinction is made between peak and off-peak traffic in this paper. Finally, the results of the numerical exercise in this paper need to be checked against an asymmetric equilibrium.

Pels, Eric↗

Thermodynamic constraints on the textural evolution of eucrite, EET 90020

Basaltic eucrites, which are possibly parts of the Vestan crust, formed as either lava flows or intrusions, and can offer insights into early crust formation. However most eucrites have experienced thermal metamorphism, which exacerbates the challenges of understanding these samples. A variety of petrogenetic models such as, partial melting of a primitive source, fractional crystallization of magmas emplaced in a primitive crust, and/or partial melting of a eucritic source coupled with melt mixing and assimilation have been proposed in order to explain observed petrologic and chemical characteristics of eucrites. EET 90020 is an unbrecciated eucrite that has experienced significant thermal metamorphism, with temperatures of metamorphic equilibration calculated to be ~840-1040°C. Its petrologic history remains contentious, in part due to differences in trace element analyses [10,17, this work], which has led to multiple metamorphic interpretations [8,10-11]. Here, we combined petrologic observations, chemical analyses, and thermodynamic modeling, to interpret micro-domain textures identified in EET 90020 and better constrain its petrologic history. Ultimately, the development of such textures is a direct result of the geologic processes operating on a young Vesta or similar asteroid. Sample description: We identified three textural domains in EET 90020 (Figure 1); (I) A coarse grain domain with granoblastic plagioclase and pyroxene, (II) a medium grain domain with curved grain boundaries between plagioclase and pyroxene, and (III) a fine grain domain dominated by tridymite that fills in interstitial space between spherical plagioclase. Major element chemistry in phases is consistent across domains. Pyroxene have distinctive high Ca lamellae (Wo40.92En28.1Fs31.0) forming from the low-Ca pigeonite host (Wo3.5En33.7Fs62.8). There are small amounts of fayalitic olivine along pyroxene/oxide grain boundaries, where pyroxenes have reacted with ilmenite/chromite clasts. Plagioclase is anorthitic (Avg ~An88), with little variation (An86-92.5). Trace element bulk rock analyses were collected via ICP-MS and individual mineral analyses with LA-ICP-MS (Figure 2). The bulk sample has an observable enrichment in light rare earth elements, with a notable depletion in Eu. Plagioclase is enriched in LREEs, depleted in HREEs, and has a positive Eu anomaly while pyroxene is enriched in HREEs with a negative Eu anomaly. Variations in trace element analyses is likely influenced by the presence of phosphates because are highly enriched in REEs and have a dramatic effect on the bulk domain compositions. Thermodynamic modeling: The software package, Perple_X, was used to calculate mineral phase equilibria over a range of conditions using a Gibbs free energy minimization approach [12]. Models used all major/minor elements except P2O5. Thermodynamic properties from [13] were used to constrain endmember phase stabilities. Activity models were used to describe mixing in phases with solid solution. Isochemical P-T phase diagrams were constructed for the bulk thin section, and the coarse, medium and fine grain domain compositions. Domain compositions were determined using microprobe analyses of phases identified in each domain and observed modal mineral abundancies. Thermodynamically stable pyroxene compositions were extracted from model results and compared to pyroxene compositions collected via EMPA, allowing us to calculate temperatures for metamorphic equilibrium. Results: Results that use the coarse domain composition (Fig. 3a) demonstrate overlap at T ~ 1020°C indicating high T equilibration. There was no overlap for the medium and fine grain domains, or the bulk composition (e.g., Fig. 3b) indicating that these are not equilibrium assemblages. These results were replicated using data from [8,20]. Discussion: The disequilibrium results from the bulk rock, fine grain and medium grain models imply that EET 90020 was modified during and/or after peak metamorphism (open system behavior). However, this is in contrast to the coarse domain where it appears as if equilibrium was maintained. We suggest that this conflict is explained by highly localized equilibrium occurring at millimeter length-scales, which has been observed in terrestrial metamorphism where aqueous fluid infiltrate [14] or melt loss occurs [15]. It is unlikely that aqueous alteration was significant in modifying the bulk composition of EET 90020, because it lacks hydrated minerals. However, the presence of melt is supported by the presence of an abundance of curved grain boundaries and spherical grains in the medium and fine grain domains This contrasts the coarse domain, where grain boundaries are angular. Given the evidence for disequilibrium in the medium and fine grain domains, it would be inappropriate to draw additional conclusions about textural evolution using thermodynamic models of those domains. However, modeling results of the coarse grain domain, where equilibrium was maintained, can provide useful insights into the geologic evolution of EET 90020. We approximate maximum metamorphic temperatures, using the Ca component in pyroxene, at ~1020°C (Fig. 4), which is consistent with previous two-pyroxene thermometry [11]. At this temperature, up to 10 vol % melt can be produced in the coarse grain domain, which is at the boundary of minimum melt needed in order to segregate and form a melt network [16]. Tridymite and plagioclase would be the first minerals to melt out during heating starting ~990°C. This is consistent with the observed melt textures formed by tridymite and plagioclase in the fine grain domain. We suggest that a partial melting model best explains the textural development of EET 90020. Upon heating, melt generated was either trapped, resulting in no net change in the localized rock composition, or migrated, resulting in disequilibrium between pyroxene and the surrounding matrix. A positive Eu anomaly in plagioclase indicates that all of the plagioclase was melted previously. This is consistent with previous studies that have suggested that EET 90020 represents a residual eucrite that experienced partial melting and subsequent melt loss [8]. We speculate that partial melting could have occurred when EET 90020 was heated in the asteroid’s lower crust or adjacent to an intrusion [7]. Future work will study other, texturally heterogeneous samples to see if EET 90020 presents a unique circumstance or whether crustal partial melting was ubiquitous on the eucrite asteroid.

Eucrites↗

Near-term tropical cyclone risk and coupled Earth system model biases

Most current climate models predict that the equatorial Pacific will evolve under greenhouse gas–induced warming to a more El Niño-like state over the next several decades, with a reduced zonal sea surface temperature gradient and weakened atmospheric Walker circulation. Yet, observations over the last 50 y show the opposite trend, toward a more La Niña-like state. Recent research provides evidence that the discrepancy cannot be dismissed as due to internal variability but rather that the models are incorrectly simulating the equatorial Pacific response to greenhouse gas warming. This implies that projections of regional tropical cyclone activity may be incorrect as well, perhaps even in the direction of change, in ways that can be understood by analogy to historical El Niño and La Niña events: North Pacific tropical cyclone projections will be too active, North Atlantic ones not active enough, for example. Other perils, including severe convective storms and droughts, will also be projected erroneously. While it can be argued that these errors are transient, such that the models’ responses to greenhouse gases may be correct in equilibrium, the transient response is relevant for climate adaptation in the next several decades. Given the urgency of understanding regional patterns of climate risk in the near term, it would be desirable to develop projections that represent a broader range of possible future tropical Pacific warming scenarios—including some in which recent historical trends continue—even if such projections cannot currently be produced using existing coupled earth system models.

Science & Technology - Other Topics↗

Single-Well Push–Pull Tracer Test Analyses to Determine Aquifer Reactive Transport Parameters at a Former Uranium Mill Site (Grand Junction, Colorado)

At a former uranium mill site where tailings have been removed, prior work has determined several potential ongoing secondary uranium sources. These include locations with uranium sorbed to organic carbon, uranium in the unsaturated zone, and uranium associated with the presence of gypsum. To better understand uranium mobility controls at the site, four single-well push–pull tests (with a drift phase) were completed with the goal of deriving aquifer flow and contaminant transport parameters for inclusion in a future sitewide reactive transport model. This goes beyond the traditional use of a constant sorption distribution coefficient (K d ) and allows for the evaluation of alternative remedial injection fluids, which can produce variable K d values. Dispersion was first removed from the resulting data to determine possible reactions before conducting reactive transport simulations. These initial analyses indicated the potential need to include cation exchange, uranium sorption, and gypsum dissolution. A reactive transport model using multiple layers to account for partially penetrating wells was completed using the PHT-USG reactive transport modeling code and calibrated using PEST. The model results quantify the hydraulic conductivity and dispersion parameters using the injected tracer concentrations. Uranium sorption, cation exchange, and gypsum dissolution parameters were quantified by comparing the simulated versus observed geochemistry. All simulations required some cation exchange and calcite equilibrium, and one simulation required gypsum dissolution to improve the model fit for calcium and sulfate. Uranium sorption parameters were not strongly influenced by the other parameter values but were highly influenced by uranium concentrations during the drift phase, with possible kinetic rate limitations. Thus, a future recommendation for such push–pull tests is to collect more geochemical data during the drift phase. The final uranium sorption parameters were within the range of values determined from prior column testing. The flow and transport parameters derived from these single-well push–pull tests will provide initial parameters for any future sitewide reactive transport model.

54 ENVIRONMENTAL SCIENCES↗

Resolving ECRH deposition broadening due to edge turbulence in DIII-D

Microwave heat pulse propagation experiments have demonstrated a correlation between millimeter-scale turbulence and deposition profile broadening of electron cyclotron (EC) waves on the DIII-D tokamak. In a set of discharges in DIII-D, a variation in edge density fluctuations on the mm-scale is associated with 40%–150% broader deposition profiles, expressed in terms of normalized minor radius, as compared with equilibrium ray tracing. The 1D power profile is determined from transport analysis of the electron temperature response to EC power modulation using perturbative analysis with a square wave power modulation at 20–70 Hz, producing a series of Fourier harmonics that are fit collectively to resolve transport. Fitting an integrated heat flux expressed in the Fourier basis of the modulation to diffusive, convective, and coupled transport terms in a linear model can resolve the broadened EC deposition width from the power perturbation to resolve a broadening in each case. The best fit degree of beam broadening observed scales approximately linearly with the Doppler backscattering measured fluctuation level in the steep gradient region. Quantifying the effect of edge fluctuation broadening on EC current drive power needs of future devices will require 3D full-wave codes that can be validated on the current generation of machines. These DIII-D experiments provide a quantitative measure of fluctuation effects and a dataset to benchmark full-wave simulations that can model and eventually predict nonlinear effects neglected by 1D equilibrium beam and ray tracing.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Modeling Climate Responses to Spectral Solar Forcing on Centennial and Decadal Time Scales

We report a series of experiments to explore clima~ responses to two types of solar spectral forcing on decadal and centennial time scales - one based on prior reconstructions, and another implied by recent observations from the SORCE (Solar Radiation and Climate Experiment) SIM (Spectral 1rradiance Monitor). We apply these forcings to the Goddard Institute for Space Studies (GISS) Global/Middle Atmosphere Model (GCMAM). that couples atmosphere with ocean, and has a model top near the mesopause, allowing us to examine the full response to the two solar forcing scenarios. We show different climate responses to the two solar forCing scenarios on decadal time scales and also trends on centennial time scales. Differences between solar maximum and solar minimum conditions are highlighted, including impacts of the time lagged reSponse of the lower atmosphere and ocean. This contrasts with studies that assume separate equilibrium conditions at solar maximum and minimum. We discuss model feedback mechanisms involved in the solar forced climate variations.

Wen, G.↗

Non-Maxwellian velocity distribution functions associated with steep temperature gradients in the solar transition region. Paper 2: The effect of non-Maxwellian electron distribution functions on ionization equilibrium calculations for carbon, nitrogen and oxygen

Non-Maxwellian electron velocity distribution functions, previously computed for Dupree's model of the solar transition region are used to calculate ionization rates for ions of carbon, nitrogen, and oxygen. Ionization equilibrium populations for these ions are then computed and compared with similar calculations assuming Maxwellian distribution functions for the electrons. The results show that the ion populations change (compared to the values computed with a Maxwellian) in some cases by several orders of magnitude depending on the ion and its temperature of formation.

Roussel-Dupre, R.↗

A Particle Representation Model for the Deformation of Homogeneous Turbulence

In simple flows, where the mean deformation rates are mild and the turbulence has time to come to equilibrium with the mean flow, the Reynolds stresses are determined by the applied strain rate. Hence in these flows, it is often adequate to use an eddy-viscosity representation. The modern family of kappa-epsilon models has been very useful in predicting near equilibrium turbulent flows, where the rms deformation rate S is small compared to the reciprocal time scale of the turbulence (epsilon/kappa). In modern engineering applications, turbulence models are quite often required to predict flows with very rapid deformations (large S kappa/epsilon). In these flows, the structure takes some time to respond and eddy viscosity models are inadequate. The response of turbulence to rapid deformations is given by rapid distortion theory (RDT). Under RDT the nonlinear effects due to turbulence-turbulence interactions are neglected in the governing equations, but even when linearized in this fashion, the governing equations are unclosed at the one-point level due to the non-locality of the pressure fluctuations.

Kassinos, S. C.↗

Thermodynamic re-modeling of the Yb-Sb system aided by first-principles calculations

Here, the thermodynamic description of the Yb-Sb binary system is developed by means of the CALculations of PHAse Diagrams (CALPHAD) method by combining experimental data in the literature and predictions from first-principles calculations based on density functional theory (DFT) in the literature and the present work. Two pseudopotentials of Yb are compared in the present DFT-based calculations with 14 and 13 f-electrons frozen in the core, i.e., 5p 6 6s 2 and 5p 6 6s 2 5 d 1 electrons as valence electrons, termed Yb_2 and Yb_3, respectively. It is shown that the phonon spectrum of the YbSb phase calculated using the Yb_3 pseudopotential does not have imaginary phonon modes and is subsequently used to predict its temperature dependent thermodynamic properties by the DFT-based quasiharmonic phonon calculations. The present thermodynamic database includes the Yb 16 Sb 11 phase in addition to five intermetallic phases that were considered in previous modeling studies, i.e., YbSb 2 , YbSb, Yb 11 Sb 10 , Yb 4 Sb 3 , and Yb 5 Sb 3 . The high temperature orthorhombic structure of the Yb 5 Sb 3 phase is not considered in the present work as it was stabilized by hydrogen. The associate solution model is used to describe the short-range ordering behavior in the liquid phase. The calculations from the present thermodynamic model show good agreement with thermochemical and phase equilibrium data from both the present work and the literature.

36 MATERIALS SCIENCE↗

Microstructural changes and mass transport in cement-based materials: A modeling approach

Highlights: • Concept to relate microstructural changes, mass transport, and chemical reactions in cement-based materials is presented. • Multi-physics modeling approach utilizing an extended version of the PNP equation and the geochemical code IPHREEQC. • Case studies indicate significant changes in mass transport properties due to alterations in the microstructure. • Microstructural changes depend on exposure and interactions between chemical reactions, pore structure, and mass transport. A generic modeling framework is presented to relate microstructural changes, i.e. changes in the pore volume distribution and phase assemblage, and mass transport in cement-based materials. The modeling framework accounts for mass transport and chemical equilibrium between ions in the pore solution and solid hydrates by means of an extended version of the Poisson-Nernst-Planck equation, in which the chemical equilibrium is solved by the external geochemical code IPHREEQC. Results of numerical studies concerning carbonation and leaching of a cement-based material indicate significant changes in mass transport properties due to chemical reactions leading to alterations in the microstructure. The resulting highly non-linear (both spatial and temporal) microstructural changes are thereby depending on the exposure and indicate that interactions between chemical reactions, pore structure changes, and mass transport have to be accounted for as a whole.

36 MATERIALS SCIENCE↗

The BEST framework for the search for the QCD critical point and the chiral magnetic effect

The Beam Energy Scan Theory (BEST) Collaboration was formed with the goal of providing a theoretical framework for analyzing data from the Beam Energy Scan (BES) program at the relativistic heavy ion collider (RHIC) at Brookhaven National Laboratory. The physics goal of the BES program is the search for a conjectured QCD critical point as well as for manifestations of the chiral magnetic effect. We describe progress that has been made over the previous five years. This includes studies of the equation of state and equilibrium susceptibilities, the development of suitable initial state models, progress in constructing a hydrodynamic framework that includes fluctuations and anomalous transport effects, as well as the development of freezeout prescriptions and hadronic transport models. Lastly, we address the challenge of integrating these components into a complete analysis framework. This document describes the collective effort of the BEST Collaboration and its collaborators around the world.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Resolving atomic transport through iron oxide under irradiation using isotopic tracers

Structural materials in nuclear environments are exposed to complex and harsh conditions, including high temperatures, corrosive solutions, and irradiation. Material stability and likewise degradation are fundamentally controlled by atomic transport mechanisms. Here, we investigate the influence of radiation-induced, non-equilibrium point defect populations on mass transport within model oxide systems using isotopic tracers and atom probe tomography. An isotopically labelled hematite (a-Fe2O3) film was synthesized with 16O- and 18O-rich layers (>30nm and 10 nm, respectively) sequentially deposited via molecular beam epitaxy. One region of the film was proton irradiated to ~0.1 dpa at 450°C, and regions outside the beam spot provided a non-irradiated control of thermal annealing only. 3D APT was used to directly visualize the elemental and O-isotopic redistribution following both thermal and combined thermal and irradiation conditions. Complementary scanning transmission electron microscopy (STEM) was also employed to study the microstructural evolution. Error function fits of the 18O-concentration profiles enabled quantification of diffusion coefficients.

isotopic tracers, diffusion, proton irradiation, h↗

Examining the Reactions of Ethanolamine’s Thermal Degradation Compounds in Carbon Capture through 1 H NMR and 13 C NMR

In amine scrubbing carbon capture, concerns about amine solvent degradation include whether it can affect the ability of the solvent to capture CO 2 . This study examines the interactions between the three most reported monoethanolamine (MEA) thermal degradation compounds namely, oxazolidine-2-one (OZD), N-(2-hydroxyethyl)-ethylenediamine (HEEDA), and N-(2- hydroxyethyl)-imidazoline-2-one (HEIA) with CO 2 in the presence and absence of MEA. We compared 1 H NMR, 13 C NMR, and heteronuclear single-quantum coherence (HSQC) NMR for neat OZD, HEEDA, and HEIA samples with CO 2 -loaded samples to observe changes in protonation and unique carbamate species formation. We found that OZD and HEIA did not directly react with CO 2 or undergo proton shifting based on our comparison of the neat OZD and HEIA samples with CO 2 -loaded spectra. However, we observed that the OZD can protonate when sparged with CO 2 in the presence of MEA, which suggests that the OZD acts as an intermediate. The NMR spectra for HEEDA indicated that HEEDA directly reacts with CO 2 at both amino groups and can protonate. In the presence of MEA, HEEDA and MEA can act like a solvent blend, resulting in multiple carbamates forming within the solvent. The neat HEIA spectrum, compared with CO 2 -loaded HEIA spectra, revealed similar results as OZD, where it does not react with CO 2 or protonate directly. However, HEIA does not protonate in the presence of MEA. These degradation compound reactions can increase the number of general equilibrium reactions during carbon capture and impact the model MEA solvent. This work helps provide a more complete picture of the reactions as the solvent degrades. Although this study examines CO 2 effects on thermal degradation products for MEA, other amines such as piperazine or 1- amino-3-propanol will degrade, and the degradation may speciate similarly with CO 2 . Furthermore, this study can impact and improve process models by assessing the degradation compounds’ reactions with CO 2 and potentially incorporating them into the model based on a neat solvent.

20 FOSSIL-FUELED POWER PLANTS↗

Observation of persistent species temperature separation in inertial confinement fusion mixtures

The injection and mixing of contaminant mass into the fuel in inertial confinement fusion (ICF) implosions is a primary factor preventing ignition. ICF experiments have recently achieved an alpha-heating regime, in which fusion self-heating is the dominant source of yield, by reducing the susceptibility of implosions to instabilities that inject this mass. We report the results of unique separated reactants implosion experiments studying pre-mixed contaminant as well as detailed high-resolution three-dimensional simulations that are in good agreement with experiments. At conditions relevant to mixing regions in high-yield implosions, we observe persistent chunks of contaminant that do not achieve thermal equilibrium with the fuel throughout the burn phase. The assumption of thermal equilibrium is made in nearly all computational ICF modeling and methods used to infer levels of contaminant from experiments. We estimate that these methods may underestimate the amount of contaminant by a factor of two or more.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Modification of the magneto-hydrodynamic equilibrium by the lower-hybrid wave driven fast electrons on the TST-2 spherical tokamak

Presence of a large population of fast particles may qualitatively modify the tokamak equilibrium from the one that can be described by standard magneto-hydrodynamics (MHD). The kinetic modification of the MHD equilibrium was studied for a lower-hybrid (LH) wave driven plasma on the TST-2 spherical tokamak. The analysis was performed using an equilibrium reconstruction method based on an extended MHD model that considers a two-component plasma of bulk MHD fluid and kinetic fast electrons. Scrape-off-layer current appeared naturally in the extended MHD analysis because of the finite electron orbit excursion from the flux surfaces. This reduced the bulk pressure contribution to the toroidal current substantially. Furthermore, the resulting poloidal flux profile was more consistent with that inferred from the Thomson scattering measurement.

extended magneto-hydrodynamics↗

Reconfigurable structure and tunable transport in synchronized active spinner materials

Ensembles of actuated colloids are excellent model systems to explore emergent out-of-equilibrium structures, complex collective dynamics, and design rules for the next generation materials. Here, we demonstrate that ferromagnetic microparticles suspended at an air-water interface and energized by an external rotating magnetic field spontaneously form dynamic ensembles of synchronized spinners in a certain range of the excitation field parameters. Each spinner generates strong hydrodynamic flows, and collective interactions of the multiple spinners promote a formation of dynamic lattices. On the basis of experiments and simulations, we reveal structural transitions from liquid to nearly crystalline states in this novel active spinner material and demonstrate that dynamic spinner lattices are reconfigurable, capable of self-healing behavior and that the transport of embedded inert cargo particles can be remotely tuned by the parameters of the external excitation field. Our findings provide insights into the behavior of active spinner materials with reconfigurable structural order and tunable functionalities.

36 MATERIALS SCIENCE↗