Combinatorial-Entropy-Driven Aggregation in DNA-Grafted Nanoparticles
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99 GENERAL AND MISCELLANEOUS↗
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Leveraging Hydration Forces for Size-Specific Nanoparticle Enrichment with a Redox-Responsive Silica-Binding Elastin-Like Polypeptide
Elastin-like polypeptides (ELPs) are low-complexity proteins that coacervate above a characteristic lower critical solution temperature (LCST). While the thermoresponsiveness of ELPs has been widely exploited in the biomedical and biomaterials fields, their ability to mediate nanoparticle assembly below their transition temperature remains largely unexplored. Here, we show that unmodified ELPs induce the reversible flocculation of silica nanoparticles (SiNPs) by forming backbone hydrogen bonds with surface silanols. Interparticle bridging is modulated by ELP length and concentration and by the presence of N- and C-terminal anchoring groups such as a cysteine residue and a Car9 silica-binding peptide. Using a redox-responsive fusion protein consisting of disulfide-bonded ELP domains terminated by Car9 segments, we stabilize 20 nm SiNPs under oxidizing conditions while triggering particle flocculation upon addition of reductant. We find that SiNP sedimentation under reducing conditions exhibits a sharp dependency on particle size that arises from the curvature-dependent structure of surface silanols. While the isolated silanols of SiNPs smaller than 30 nm are efficiently engaged by the ELP domains of Car9-anchored proteins, repulsion forces associated with the presence of a layer of molecular water together with increased electrostatic repulsion preclude efficient engagement of H-bonded silanols displayed on the surface of SiNPs larger than 60 nm. We harness these findings to selectively enrich SiNPs based on size and expand the concept to titania (TiO2) by demonstrating that rutile nanoparticles can be stabilized or sedimented with solid-binding ELPs by adjusting the solution pH to promote or discourage the formation of a hydration layer. These strategies should prove broadly useful for the separation of other oxides and their polymorphs and provide a tunable strategy for nanoparticle assembly and bioinspired colloidal design.
ELP↗
Mesoscale fractal whey protein particles derived from microscale linear-shaped protein assemblies (Part 1): Manufacturing method and particle characteristics
Whey protein isolates (WPI) are widely used in processed foods for their versatile functional properties. Modifying the structural properties of proteins by assembling them into mesoscale or microscale particles may improve their functionality and broaden their applications. This study aims to manufacture and characterize mesoscale whey protein particles (WPP) derived from WPI. Two types of WPP, WPP1 (0.05 mL/min) and WPP2 (0.25 mL/min), were prepared through a multistep approach involving liquid antisolvent (LAS) precipitation, heat treatment, and microfluidization. Liquid antisolvent precipitation was performed by injecting a 20% (wt/vol) WPI dispersion (pH 7) into an ethanol-glycerol mixture (75:25, vol/vol) under laminar flow, followed by heat treatment at 80°C for 20 min as a particle hardening step. This process produced stable fiber- and ribbon-shaped whey protein assemblies (WPA), which served as precursors to WPP. Subsequent microfluidization (150 MPa, 6 passages) reduced the size of WPA, yielding mesoscale WPP with irregular morphologies and a more uniform size distribution, as revealed by microscopy and dynamic light scattering. ζ-Potential and fluorescence labeling indicated higher surface charge and surface hydrophobicity of WPP compared with untreated WPI. The WPP showed internal mass fractal and surface fractal structures at larger length scales, analyzed using small-angle X-ray scattering. Fourier transform infrared spectroscopy demonstrated an increased fraction of intermolecular β-sheets in WPP, suggesting that hydrogen bonding contributed to their formation. Gel electrophoresis confirmed that disulfide bonds served as the primary cross-links stabilizing the WPP structure. Furthermore, turbidity measurements showed that WPP exhibited superior colloidal phase stability compared with untreated WPI and maintained high colloidal stability under both acidic and neutral pH conditions.
Antisolvent precipitation↗
Inverse design of equilibrium cluster fluids applied to a physically informed model
Inverse design strategies have proven highly useful for the discovery of interaction potentials that prompt self-assembly of a variety of interesting structures. However, often the optimized particle interactions do not have a direct relationship to experimental systems. In this work, we show that Relative Entropy minimization is able to discover physically meaningful parameter sets for a model interaction built from depletion attraction and electrostatic repulsion that yield self-assembly of size-specific clusters. Here, we then explore the sensitivity of the optimized interaction potentials with respect to deviations in the underlying physical quantities, showing that clustering behavior is largely preserved even as the optimized parameters are perturbed.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Rational Design of Hierarchically Open-Porous Spherical Hybrid Architectures for Lithium Ion Batteries
Controlling the internal microstructure and overall morphology of building blocks used to form hybrid materials is crucial for the realization of deterministically designed architectures with desirable properties. Here, we demonstrate an integrative spray-frozen (SF) assembly for forming hierarchically structured open-porous microspheres (hpMSs) composed of Fe 3 O 4 and reduced graphene oxide (rGO). The SF process drives the formation of a radially-aligned microstructure within the sprayed colloidal droplets and also controls the overall microsphere morphology. The Fe 3 O 4 /rGO hpMSs contain interconnected open-pores and spherical morphology, which, when used as a lithium-ion battery anode, enables then to provide gravimetric and volumetric capacities of 1069.7 mAh g -1 and 686.7 mAh cm -3 , much greater than those of samples with similar composition and different morphologies. The hpMSs have good rate and cycling performances, retaining 78.5% from 100 to 1000 mA g -1 and 74.6% over 300 cycles. Using in-situ synchrotron x-ray absorption spectroscopy, the reaction pathway and phase evolution of the hpMSs are monitored observing the very small domain size and highly disordered nature of Fe x O y . Here, the reduced capacity fading relative to other conversion systems is due to the good electrical contact between the pulverized Fe x O y particles and rGO, the overall structural integrity of the hpMSs, and interconnected openporosity.
25 ENERGY STORAGE↗
Effect of Minerals on the Removal of Uranium (VI) in the Presence of Humic Acid and Colloidal Silica - 19406
Uranium is one of the key contaminants of concern in groundwater as a result of past nuclear processing activities at the Department of Energy (DOE) facilities such as the Savannah River Site (SRS) in Aiken, South Carolina. SRS was one of the major nuclear processing facilities during the Cold War where plutonium was produced. Beginning with the implementation of the environmental cleanup program in 1981, SRS has become a hazardous waste management facility responsible for the storage and remediation of contaminated soil and groundwater from radionuclides. Approximately 1.8 billion gallons of acidic waste containing radionuclides and dissolved heavy metals was disposed in the F/H Area seepage basins. This led to the unintentional creation of highly contaminated groundwater plumes, consisting of radionuclides with an acidic pH between 3 and 5.5. The acidity of the plumes contributed to the mobility of several constituents of concern (COC) such as tritium ({sup 3}H), uranium-238 ({sup 238}U), iodine-129 ({sup 129}I), and strontium-90 ({sup 90}Sr) for the F-Area plume and {sup 3}H, {sup 90}Sr and mercury for the H-Area plume. This investigation will focus on uranium in the oxidation state +6 (U(VI)), which is a key contaminant of concern in the groundwater plume of the FArea. Initially, the pump-treat-reinject system was implemented from 1997 to 2003 to remove contaminants from polluted groundwater. Downgrade groundwater within the system would be pumped to the water treatment facility and re-injected upgrade within the aquifer. The effectiveness and sustainability of this process diminished over time. Therefore, it was discontinued and replaced with a funnel-and-gate process in 2004. This new process injects sodium hydroxide directly into the gates of the F-Area groundwater to effectively raise pH levels. By raising the pH of the groundwater, a treatment zone is created by reversing the acidic nature of the contaminated sediments and producing a negative net charge on the surface of sediment particles. As a result, the adsorption of cationic contaminants is expected to be enhanced. So far, this process has resulted in a decrease of {sup 90}Sr and {sup 238}U concentrations, though the concentration of iodine has been unaffected by this treatment. The solution used for the injections contains a high carbonate alkalinity in order to overcome the surface acidic conditions and natural partitions in the groundwater system. To maintain the neutral pH in the treatment zone, systematic injections are required. The continuous use of high concentrations of a carbonate solution to raise pH could re-mobilize uranium previously adsorbed within the treatment zone, though this has not been observed in the monitoring data. Humic substances (HS) are major components of soil organic matter. HS are polyfunctional organic macromolecules formed by the chemo-microbiological decomposition of biomass or dead organic matter. These substances are usually divided into three main fractions: humin (insoluble at all pH values), humic acid (soluble at pH greater than 3.5), and fulvic acid (soluble at all pH values). Humic acid carries a large number of functional groups such as aromatic rings, carboxyl groups, phenols, aliphatic chains, etc. Humic acid is an important ion exchange and metal complexing ligand with a high complexation capacity. The ability of humic acid to chemically bind to metals influences in their migration behavior and fate in natural systems. Various studies have suggested that the retention of U(VI) via sorption in the presence of humic acid is a complex process. For instance, humic acid can form an organic coating at the surface of minerals, which can enhance the sequestration of metals. Ivanov et al. (2012) studied the sorption of U(VI) sorption onto bentonite in the presence and absence of humic acid. The study found that uranium sorption in the presence of humic acid was enhanced at low pH (below 3.8) while at moderate pH (3.8 and 6.5) uranium sorption was reduced compared to the absence of humic acid. At high pH (7 and 9), uranium sorption was reduced for both the presence and absence of humic acid. Also, Krepelova et al. (2007) not only found that U(VI) sorption onto kaolinite was influenced by pH, U(VI) concentration, the presence of inorganic carbon species, and humic acid but also that U(VI) preferred to be adsorbed onto kaolinite as a uranyl-humate complex. This investigation analyzed the mechanisms of the synergetic interactions of humic acid and colloidal silica on the removal of uranium in the presence of pure minerals such as quartz, kaolinite and goethite which are characteristic of the F/H area. (authors)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
How Robust are Semiconductor Nanorods? Investigating the Stability and Chemical Decomposition Pathways of Photoactive Nanocrystals
Anisotropic II–VI semiconductor nanostructures are important photoactive materials for various energy conversion and optical applications. However, aside from the many available surface chemistry studies and from their ubiquitous photodegradation under continuous illumination, the general chemical reactivity and thermal stability (phase and shape transformations) of these materials are poorly understood. Using CdSe and CdS nanorods as model systems, we have investigated the behavior of II–VI semiconductor nanorods against various conditions of extreme chemical and physical stress (acids, bases, oxidants, reductants, and heat). CdSe nanorods react rapidly with acids, becoming oxidized to Se or SeO2. In contrast, CdSe nanorods remain mostly unreactive when treated with bases or strong oxidants, although bases do partially etch the tips of the nanorods (along their axis). Roasting (heating in air) of CdSe nanorods results in rock-salt CdO, but neither CdSe nor CdO is easily reduced by hydrogen (H2). Another reductant, n-BuLi, reduces CdSe nanorods to metallic Cd. Variable temperature X-ray diffraction experiments show that axial annealing and selective axial melting of the nanorods precede particle coalescence. Furthermore, thermal analysis shows that the axial melting of II–VI nanorods is a ligand-dependent process. In agreement with chemical reactivity and thermal stability observations, silica-coating experiments show that the sharpest (most curved) II–VI surfaces are most active against heterogeneous nucleation of a silica shell. These results provide valuable insights into the fate and possible ways to enhance the stability and improve the use of II–VI semiconductor nanostructures in the fields of optics, magnetism, and energy conversion.
36 MATERIALS SCIENCE↗
Binary Diamondoid Building Blocks for Molecular Gels
Adamantane is a type of diamondoid molecules that has a cage or globular shape with a diameter of 6.34 ± 0.04 Å.8 Anisotropic interactions between these truly nanoscopic particles can be induced through the derivatization of the diamondoid cage. Here we explore the gelation of paired systems of adamantane where attractions are introduced through van der Waals forces and hydrogen bonding. Gels are produced through the mixing of 1-adamantanecarboxylic acid (A1C) and 1-adamantylamine (A1N). Upon mixing dimethyl sulfoxide solutions of these molecules at vanishing concentrations, these diamondoid molecules rapidly precipitate. A space-filling gel of the resulting aggregates is observed at approximately 3% by weight. These resulting gels have elastic moduli of 10 2 –10 4 Pa in the 3–7 wt % concentration range. At a 1:1 mol ratio of 1-adamantanecarboxylic acid (A1C) and 1-adamantylamine (A1N), the gel’s elastic modulus and yield stress increase as volume fractions Φ x and Φ y with x ≈ 4.2 and y ≈ 3.5. Here, the dependencies of moduli and yield stress on the volume fraction display characteristics of colloidal gels. Transmission electron microscope (TEM) images indicate that the gels are formed from a network of interwoven and branched fibers which are composed of ~30 nm crystallites that have undergone oriented aggregation to form fibers.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Electrophoretic deposition improves catalytic performance of Co 3 O 4 nanoparticles for oxygen reduction/oxygen evolution reactions
The effects of nanoparticle deposition on the catalytic activity of Co 3 O 4 nanoparticles for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) are evaluated for two deposition methods: dropcasting and electrophoretic deposition (EPD). In this work it is found that the EPD catalyst films demonstrate better catalytic activity per unit mass than do the dropcast films, as defined by diffusion-limited current, by approximately 27% for ORR and 25% for OER. When accounting for different loading levels, the absolute activities of these catalysts are superior to those of other reported Co 3 O 4 colloidal nanoparticulate catalysts without conductive additives, showing that this material has excellent intrinsic activity for future optimization. Inspection of the electrode kinetics shows that EPD catalysts have more favorable characteristics as exhibited by their smaller Tafel slope (96 mV per decade for EPD versus 109 mV per decade for dropcast films). We analyze this enhancement by determining the metal oxide surface area for each catalyst film using a novel sequential metal deposition technique starting with electrodeposition of Ag followed by Pb underpotential deposition (UPD). Through UPD experiments we find, surprisingly, that EPD films have a smaller surface area than the dropcast films. We conclude that EPD films are more active per unit surface area. When accounting for surface area and mass, the EPD catalyst outperforms dropcast by a factor of 2.5 for ORR and 2.6 for OER. We anticipate that morphological differences in the EPD films relative to the dropcast ones, such as particle coverage and electrical conductivity, are responsible for this behavior. Such a result has important implications for future studies on the structure of EPD-manufactured nanoparticulate thin films and on the mechanisms for performance enhancement in such catalysts.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Green synthesis and characterization of nontoxic L-methionine capped silver and gold nanoparticles
The simple green method for synthesis of stable L-Methionine (L-Met) capped silver (Ag@LM NPs) and gold (Au@LM NPs) nanoparticles (NPs) without adding any additional reduction agent or stabilizer was developed. Colloidal dispersions were characterized by UV–Vis spectrophotometry. The size and spherical shape of NPs were evaluated by transmission electron microscopy. Their surface covering was confirmed by atomic force microscopy, Fourier transform infrared spectroscopy, dynamic light scattering, and zeta potential measurements. Density functional theory calculations pointed that the preferential adsorption mode of L-Met on both Ag and Au surfaces was a vertical binding geometry via –NH2 group, while horizontal binding mode via [sbnd]S[sbnd] and –NH2 groups is also possible. The genotoxicity (evaluated by the micronucleus assay) of NPs, as well as their effects on some oxidative stress parameters (catalase activity, malondialdehyde level), were assessed in vitro using human peripheral blood cells as a model system. The influence of NPs on the morphology of lymphocyte cells studied using atomic force microscopy revealed that the membrane of cells remained unaffected after the treatment with NPs. When considering the effects of NPs on catalase activity and malondialdehyde level, neither particle type promoted oxidative stress. However, the treatment of lymphocytes with Ag@LM NPs induced a concentration-dependent enhancement of the micronuclei incidence and suppression of the cell proliferation while Au@LM NPs promoted cell proliferation, with no significant effects on micronuclei formation. The Ag@LM NPs were more prone to induce DNA damage than Au@LM NPs, which makes the latter type more suitable for further studies in nano-medicine. © 2019.
60 APPLIED LIFE SCIENCES↗
Regulating phase behavior of nanoparticle assemblies through engineering of DNA-mediated isotropic interactions
Self-assembly of isotropically interacting particles into desired crystal structures could allow for creating designed functional materials via simple synthetic means. However, the ability to use isotropic particles to assemble different crystal types remains challenging, especially for generating low-coordinated crystal structures. Here, we demonstrate that isotropic pairwise interparticle interactions can be rationally tuned through the design of DNA shells in a range that allows transition from common, high-coordinated FCC-CuAu and BCC-CsCl lattices, to more exotic symmetries for spherical particles such as the SC-NaCl lattice and to low-coordinated crystal structures (i.e., cubic diamond, open honeycomb). The combination of computational and experimental approaches reveals such a design strategy using DNA-functionalized nanoparticles and successfully demonstrates the realization of BCC-CsCl, SC-NaCl, and a weakly ordered cubic diamond phase. The study reveals the phase behavior of isotropic nanoparticles for DNA–shell tunable interaction, which, due to the ease of synthesis is promising for the practical realization of non-close-packed lattices.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Anticipating gelation and vitrification with medium amplitude parallel superposition (MAPS) rheology and artificial neural networks
Abstract Anticipating qualitative changes in the rheological response of complex fluids (e.g., a gelation or vitrification transition) is an important capability for processing operations that utilize such materials in real-world environments. One class of complex fluids that exhibits distinct rheological states are soft glassy materials such as colloidal gels and clay dispersions, which can be well characterized by the soft glassy rheology (SGR) model. We first solve the model equations for the time-dependent, weakly nonlinear response of the SGR model. With this analytical solution, we show that the weak nonlinearities measured via medium amplitude parallel superposition (MAPS) rheology can be used to anticipate the rheological aging transitions in the linear response of soft glassy materials. This is a rheological version of a technique called structural health monitoring used widely in civil and aerospace engineering. We design and train artificial neural networks (ANNs) that are capable of quickly inferring the parameters of the SGR model from the results of sequential MAPS experiments. The combination of these data-rich experiments and machine learning tools to provide a surrogate for computationally expensive viscoelastic constitutive equations allows for rapid experimental characterization of the rheological state of soft glassy materials. We apply this technique to an aging dispersion of Laponite ® clay particles approaching the gel point and demonstrate that a trained ANN can provide real-time detection of transitions in the nonlinear response well in advance of incipient changes in the linear viscoelastic response of the system.
Lennon, Kyle R. (ORCID:0000000212515461)↗
Single-crystal-like NiO colloidal nanocrystal-aggregated microspheres with mesoporous structure: Synthesis and enhanced electrochemistry, photocatalysis and water treatment properties
A new microwave-assisted hydrothermal synthetic route based on the self-assembly and subsequently controlled thermal decomposition process is proposed to fabricate nickel oxide colloidal nanocrystal aggregated microspheres (CNAMs) with mesoporous structure. XRD, EDS, SEM, TEM. FTIR, and N{sub 2} adsorption and desorption isotherm techniques are employed for morphology and structure characterizations. The as-prepared nickel oxide CNAMs, which has a high surface area (234 m{sup 2}/g) with narrow pore distribution at around 3.25 nm, are composed of numerous hexagonal mesoporous nanocrystals of approximately 50–60 nm in size, and present a single-crystal-like characteristic. The experimental results also demonstrated that the CNAMs showed outstanding performance in electrochemistry, photocatalysis and waste water treatment due to their special hierarchical and mesoporous structure, presenting the promising candidate for catalysis and catalysis support materials. - Graphical abstract: CNAMs with mesoporous structure synthesized via a simple microwave-assisted hydrothermal method was applied in electrochemistry and catalysis and exhibited enhanced performance. Display Omitted - Highlights: • CNAMs with mesoporous structure are achieved via a simple microwave-assisted hydrothermal method. • Morphology, structure and pore distribution of sample particles is specifically controlled. • The samples show enhanced properties in electrochemistry and catalysis due to hierarchical structure.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Moving beyond the Solvent-Tip Approximation to Determine Site-Specific Variations of Interfacial Water Structure through 3D Force Microscopy
Although interfacial solution structure impacts environmental, biological, and technological phenomena, including colloidal stability, protein assembly, heterogeneous nucleation, and water desalination, its molecular details remain poorly understood. Here, we visualize the three-dimensional (3D) hydration structure at the boehmite(010)-water interface using fast force mapping (FFM). Using a self-consistent scheme to decouple long-range tip-sample interactions from short-range solvation forces, we obtain the solution structure with lattice resolution. The results are benchmarked against molecular dynamics simulations that explicitly include the effects of the tip with different levels of approximation and systematically account for tip size, chemistry, and confinement effects. We find four laterally structured water layers within 1 nm of the surface, with the highest water densities at sites adjacent to hydroxyl groups. The key features beyond the first two layers can only be predicted using a full-scale simulation of the boehmite-water-silica system. Our findings further reveal a complex relationship between site-specific chemistry, water density, and long-range particle interactions; and present important advances toward quantitative data interpretation in 3D FFM.
36 MATERIALS SCIENCE↗
Comparative Evaluation of U.S. Brand and Generic Intravenous Sodium Ferric Gluconate Complex in Sucrose Injection: Physicochemical Characterization
The objective of this study was to evaluate physicochemical equivalence between brand (i.e., Ferrlecit) and generic sodium ferric gluconate (SFG) in sucrose injection by conducting a series of comparative in vitro characterizations using advanced analytical techniques. The elemental iron and carbon content, thermal properties, viscosity, particle size, zeta potential, sedimentation coefficient, and molecular weight were determined. There was no noticeable difference between brand and generic SFG in sucrose injection for the above physical parameters evaluated, except for the sedimentation coefficient determined by sedimentation velocity analytical ultracentrifugation (SV-AUC) and molecular weight by asymmetric field flow fractionation-multi-angle light scattering (AFFF-MALS). In addition, brand and generic SFG complex products showed comparable molecular weight distributions when determined by gel permeation chromatography (GPC). The observed minor differences between brand and generic SFG, such as sedimentation coefficient, do not impact their biological activities in separate studies of in vitro cellular uptake and rat biodistribution. Coupled with the ongoing clinical study comparing the labile iron level in healthy volunteers, the FDA-funded post-market studies intended to illustrate comprehensive surveillance efforts ensuring safety and efficacy profiles of generic SFG complex in sucrose injection, and also to shed new light on the approval standards on generic parenteral iron colloidal products.
60 APPLIED LIFE SCIENCES↗
Ultrahigh Hot Carrier Transient Photocurrent in Nanocrystal Arrays by Auger Recombination
Here, we show that a new mechanism for carrier transport in solution-processed colloidal semiconductor nanocrystal arrays exists at high excitation intensity on ultrafast time scales and allows for facile intrinsic transport between as-prepared nanocrystals over long distances. By combining a high speed photoconductive switch with an ultrafast laser excitation in a sub-40 ps photoconductor, we observed transient photocurrents with peak densities of 3 × 10 4 – 10 6 mA/ cm 2 in self-assembled PbSe nanocrystals capped with long native oleic acid ligands. The ratio between the transient photocurrent peak and the steady-state dark current is 10 orders of magnitude. The transient mobility at the peak current is estimated to range between 0.5–17.5 cm 2 /(V s) for the various nanocrystal sizes studied, which is 6 to 9 orders of magnitude higher than the dark current steady-state mobility in PbSe, CdSe, and CdTe nanocrystals capped with native ligands. The results are analyzed using a kinetic model which attributes the ultrahigh transient photocurrent to multiple photogenerated excitons undergoing on-particle Auger recombination, followed by rapid tunneling at high energies. This mechanism is demonstrated for a wide range of PbSe nanocrystals sizes (diameters from 2.7 to 7.1 nm) and experimental parameters. Our observations indicate that native ligand-capped nanocrystal arrays are promising for optoelectronics applications wherein multiple carriers are photoinjected to interband states.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Emergence of Lanes and Turbulent-like Motion in Active Spinner Fluid
Assemblies of self-rotating particles are gaining interest as a novel realization of active matter with unique collective behaviors such as edge currents and non-trivial dynamic states. Here, we develop a continuum model for a system of fluid-embedded spinners by coarse-graining the equations of motion of the discrete particles. We apply the model to explore mixtures of clockwise and counterclockwise rotating spinners. We find that the dynamics is sensitive to fluid inertia: in the inertialess system, after transient turbulent-like motion the spinners segregate and form steady traffic lanes. At small but finite Reynolds number instead, the turbulent-like motion persists and the system exhibits a chirality breaking transition leading to a single rotation sense state. Our results shed light on the dynamic behavior of non-equilibrium materials exemplified by active spinners.
36 MATERIALS SCIENCE↗
Programmable chiral states in flocks of active magnetic rollers
Inspired by nature, active matter exemplified by self-organization of motile units into macroscopic structures holds great promise for advanced tunable materials capable of flocking, shape-shifting, and self-healing. Active particles driven by external fields have repeatedly demonstrated potential for complex self-organization and collective behavior, yet how to guide the direction of their collective motion largely remains unexplored. Here, we report a system of microscopic ferromagnetic rollers driven by an alternating magnetic field that demonstrates programmable control of the direction of a self-organized coherent vortical motion (i.e., chirality). Facilitated by a droplet confinement, the rollers get synchronized and display either right- or left-handed spontaneous vortical motion, such that their moving direction determines the vortex chirality. Here, we reveal that one can remotely command a flock of magnetic rollers to switch or maintain its chiral state by modulating a phase shift of the sinusoidal magnetic field powering the active rollers. Building on our findings, we realize a self-assembled remotely controlled micro-pump architecture capable of switching the fluid transport direction on demand. Our studies may stimulate new design strategies for directed transport and flocking robotics at the microscale based on active colloids.
36 MATERIALS SCIENCE↗