Field-Tunable Interactions and Frustration in Underlayer-Mediated Artificial Spin Ice.

Artificial spin ice systems have opened experimental windows into a range of model magnetic systems through the control of interactions among nanomagnet moments. This control has previously been enabled by altering the nanomagnet size and the geometry of their placement. Here we demonstrate that the interactions in artificial spin ice can be further controlled by including a soft ferromagnetic underlayer below the moments. Such a substrate also breaks the symmetry in the array when magnetized, introducing a directional component to the correlations. Using spatially resolved magneto-optical Kerr effect microscopy to image the demagnetized ground states, we show that the correlation of the demagnetized states depends on the direction of the underlayer magnetization. Further, the relative interaction strength of nearest and next-nearest neighbors varies significantly with the array geometry. We exploit this feature to induce frustration in an inherently unfrustrated square lattice geometry, demonstrating new possibilities for effective geometries in two-dimensional nanomagnetic systems.

Erratum: Guaranteed Convergence of a Regularized Kohn-Sham Iteration in Finite Dimensions [Phys. Rev. Lett. 123, 037401 (2019)].

This corrects the article DOI: 10.1103/PhysRevLett.123.037401.

Crystallites of magnetic charges in artificial spin ice.

Artificial spin ice is a class of lithographically created arrays of interacting ferromagnetic nanometre-scale islands. It was introduced to investigate many-body phenomena related to frustration and disorder in a material that could be tailored to precise specifications and imaged directly. Because of the large magnetic energy scales of these nanoscale islands, it has so far been impossible to thermally anneal artificial spin ice into desired thermodynamic ensembles; nearly all studies of artificial spin ice have either treated it as a granular material activated by alternating fields or focused on the as-grown state of the arrays. This limitation has prevented experimental investigation of novel phases that can emerge from the nominal ground states of frustrated lattices. For example, artificial kagome spin ice, in which the islands are arranged on the edges of a hexagonal net, is predicted to support states with monopolar charge order at entropies below that of the previously observed pseudo-ice manifold. Here we demonstrate a method for thermalizing artificial spin ices with square and kagome lattices by heating above the Curie temperature of the constituent material. In this manner, artificial square spin ice achieves unprecedented thermal ordering of the moments. In artificial kagome spin ice, we observe incipient crystallization of the magnetic charges embedded in pseudo-ice, with crystallites of magnetic charges whose size can be controlled by tuning the lattice constant. We find excellent agreement between experimental data and Monte Carlo simulations of emergent charge-charge interactions.

Geometrical Performance of Self-Phoretic Colloids and Microswimmers.

Within a unified formulation-encompassing self-electrophoresis, self-diffusiophoresis, and self-thermophoresis-we provide a simple integral kernel transforming the relevant surface flux to particle velocity for any spheroid with axisymmetric surface activity and uniform phoretic mobility. Appropriate scaling of the speed allows a dimensionless measure of the motion-producing performance of the motor shape and activity distribution across the surface. For bipartite designs with piecewise uniform flux over complementary surface regions, the performance is mapped out over the entire range of geometry (from discotic through spherical to rodlike shapes) and of bipartitioning, and intermediate aspect ratios that maximize performance are identified. Comparisons are made to experimental data from the literature.

Systematic Enumeration of sp(3) Nanothreads.

Slow decompression of crystalline benzene in large-volume high-pressure cells has recently achieved synthesis of a novel one-dimensional allotrope of sp(3) carbon in which stacked columns of benzene molecules rehybridize into an ordered crystal of nanothreads. The progenitor benzene molecules function as six-valent one-dimensional superatoms with multiple binding sites. Here we enumerate their hexavalent bonding geometries, recognizing that the repeat unit of interatomic connectivity ("topological unit cell") need not coincide with the crystallographic unit cell, and identify the most energetically favorable cases. A topological unit cell of one or two benzene rings with at least two bonds interconnecting each adjacent pair of rings, accommodates 50 topologically distinct nanothreads, 15 of which are within 80 meV/carbon atom of the most stable member. Optimization of aperiodic helicity reveals the most stable structures to be chiral. We generalize Euler's rules for ring counting to cover this new form of very thin one-dimensional carbon, calculated their physical properties, and propose a naming convention that can be generalized to handle nanothreads formed from other progenitor molecules.

Guiding chiral self-propellers in a periodic potential.

Ingenious suggestions continue to be made for separation of racemic mixtures according to the inert structural chirality of the constituents. Recently discovered self-motile micro- or nanoparticles express dynamical chirality, i.e., that which originates in motion, not structure. Here, we predict how dynamically chiral objects, with overdamped dynamics in a soft periodic two-dimensional potential, can display not only separation into well-defined dynamical subclasses defined by motility characteristics, but also the ability to be steered to arbitrary locations in the plane by simply changing the amplitude of the external potential. Orientational and translational diffusion produce new types of drift absent in the noise-free case. As practical implementation seems feasible with acoustic or optical fields, these phenomena can be useful for laboratory microscales manipulations, possibly including reconfigurable microfluidic circuits with complex networks of unidirectional channels.

Perpendicular magnetization and generic realization of the Ising model in artificial spin ice.

We have studied frustrated kagome arrays and unfrustrated honeycomb arrays of magnetostatically interacting single-domain ferromagnetic islands with magnetization normal to the plane. The measured pairwise spin correlations of both lattices can be reproduced by models based solely on nearest-neighbor correlations. The kagome array has qualitatively different magnetostatics but identical lattice topology to previously studied artificial spin ice systems composed of in-plane moments. The two systems show striking similarities in the development of moment pair correlations, demonstrating a universality in artificial spin ice behavior independent of specific realization in a particular material system.

Mutual information and breakdown of the Perron-Frobenius scenario in zero-temperature triangular Ising antiferromagnets on cylinders.

A nominally two-dimensional spin model wrapped onto a cylinder can profitably be viewed, especially for long cylinders, as a one-dimensional chain. Each site of such a chain is a ring of spins with a complex state space. Traditional correlation functions are inadequate for the study of correlations in such a system and need to be replaced with something like mutual information. Being induced purely by frustration, the disorder of a cylindrical zero-temperature triangular Ising antiferromagnet (TIAFM) and attendant correlations have a chance of evading the consequences of the Perron-Frobenius theorem which describes and constrains correlations in thermally disordered one-dimensional systems. Correlations in such TIAFM systems and the aforementioned evasion are studied here through a fermionic representation. For cylindrical TIAFM models with open boundary conditions, we explain and derive the following characteristics of end-to-end mutual information: period-three oscillation of the decay length, halving of the decay length compared to what Perron-Frobenius predicts on the basis of transfer matrix eigenvalues, and subexponential decay-inverse square in the length-for certain systems.

Ignoring your neighbors: moment correlations dominated by indirect or distant interactions in an ordered nanomagnet array.

We have studied the moment correlations within triangular lattice arrays of single-domain coaligned nanoscale ferromagnetic islands. Independent variation of lattice spacing along and perpendicular to the island axis tunes the magnetostatic interactions between islands through a broad range of relative strengths. For certain lattice parameters, the sign of the correlations between near-neighbor island moments is opposite to that favored by the pairwise interaction. This finding, supported by analysis of the total correlation in terms of direct and convoluted indirect contributions across multiple pairwise interactions, indicates that indirect interactions and/or those mediated by further neighbors can be tuned to be dominant, with implications for the wide range of systems composed of interacting nanomagnets.

Dynamic interactions between fast microscale rotors.

Trimetallic catalytic microrotors were fabricated by electrodeposition of cylindrical Au-Ru rods in the pores of anodic alumina membranes, dissolution of the template membrane, and then sequential vapor deposition of Cr, SiO(2), Cr, Au, and Pt on one side of each rod. This design provides two force vectors for the catalytic motor, including one perpendicular to the rod axis. The rods rotated rapidly (approximately 180 rpm) in 15% aqueous H(2)O(2) solution with minimal orbital or translational movement. The rotation was rapid enough to observe qualitatively different interactions between pairs of co- and counter-rotating rods. Counter-rotating rods were able to approach each other closely and underwent frequent tip-to-tip collisions. Co-rotating rods could approach each other only to a distance of approximately 0.9 microm. This difference is rationalized on the basis of shear forces generated by the catalytically driven rotation of the rods.

Drift-diffusion processes resulting from elimination of fast variables under inhomogeneous conditions.

The problem of eliminating fast-relaxing variables to obtain an effective diffusion process in position is solved in a uniform and straightforward way for models with velocity a function jointly of position and fast variables. A more unified view is thereby obtained of the effect of environmental inhomogeneity on the motion of a diffusing particle, in particular, whether a drift is induced, covering both passive and active particles. Infinitesimal generators (equivalently, drift-diffusion fields) for the contracted processes are worked out in detail for several models.

Carbon nanostructures as an electromechanical bicontinuum.

A two-field model provides a unifying framework for elasticity, lattice dynamics and electromechanical coupling in graphene and carbon nanotubes, describes optical phonons, nontrivial acoustic branches, strain-induced gap opening, gap-induced phonon softening, doping-induced deformations, and even the hexagonal graphenic Brillouin zone, and thus explains and extends a previously disparate accumulation of analytical and computational results.

Distinguishing advective and powered motion in self-propelled colloids.

Self-powered motion in catalytic colloidal particles provides a compelling example of active matter, i.e. systems that engage in single-particle and collective behavior far from equilibrium. The long-time, long-distance behavior of such systems is of particular interest, since it connects their individual micro-scale behavior to macro-scale phenomena. In such analyses, it is important to distinguish motion due to subtle advective effects-which also has long time scales and length scales-from long-timescale phenomena that derive from intrinsically powered motion. Here, we develop a methodology to analyze the statistical properties of the translational and rotational motions of powered colloids to distinguish, for example, active chemotaxis from passive advection by bulk flow.

Acoustic actuation of bioinspired microswimmers.

Acoustic actuation of bioinspired microswimmers is experimentally demonstrated. Microswimmers are fabricated in situ in a microchannel. Upon acoustic excitation, the flagellum of the microswimmer oscillates, which in turn generates linear or rotary movement depending on the swimmer design. The speed of these bioinspired microswimmers is tuned by adjusting the voltage amplitude applied to the acoustic transducer. Simple microfabrication and remote actuation are promising for biomedical applications.

Dynamic stabilization of Janus sphere trans-dimers.

We experimentally investigated the self-assembly of chemically active colloidal Janus spheres into dimers. The trans-dimer conformation, in which the two active sites are oriented roughly in opposite directions and the particles are osculated at their equators, becomes dominant as the hydrogen peroxide fuel concentration increases. Our observations suggest high spinning frequency combined with little translational motion is at least partially responsible for the stabilization of the trans-dimer as activity increases.

Catalytically driven colloidal patterning and transport.

We recently reported the convection and pattern formation of tracers caused by a catalytically generated electric field. The electric field arises due to the heterogeneous electrochemical reduction and oxidation of hydrogen peroxide (H2O2) on silver (Ag) and gold (Au), respectively.1 Here we describe an electrokinetic model, developed in conjunction with experiments, that explains the details of the convection and pattern formation phenomenon. The model also enables the measurement of reaction kinetic parameters that are otherwise difficult to obtain. This quantitative model serves as a platform for the modeling of other catalytic redox systems and systems with broken symmetries.

Spiral diffusion of rotating self-propellers with stochastic perturbation.

Translationally diffusive behavior arising from the combination of orientational diffusion and powered motion at microscopic scales is a known phenomenon, but the peculiarities of the evolution of expected position conditioned on initial position and orientation have been neglected. A theory is given of the spiral motion of the mean trajectory depending upon propulsion speed, angular velocity, orientational diffusion, and rate of random chirality reversal. We demonstrate the experimental accessibility of this effect using both tadpole-like and Janus sphere dimer rotating motors. Sensitivity of the mean trajectory to the kinematic parameters suggest that it may be a useful way to determine those parameters.

Acoustofluidic actuation of in situ fabricated microrotors.

We have demonstrated in situ fabricated and acoustically actuated microrotors. A polymeric microrotor with predefined oscillating sharp-edge structures is fabricated in situ by applying a patterned UV light to polymerize a photocrosslinkable polyethylene glycol solution inside a microchannel around a polydimethylsiloxane axle. To actuate the microrotors by oscillating the sharp-edge structures, we employed piezoelectric transducers which generate tunable acoustic waves. The resulting acoustic streaming flows rotate the microrotors. The rotation rate is tuned by controlling the peak-to-peak voltage applied to the transducer. A 6-arm microrotor can exceed 1200 revolutions per minute. Our technique is an integration of single-step microfabrication, instant assembly around the axle, and easy acoustic actuation for various applications in microfluidics and microelectromechanical systems (MEMS).

Self-consistent nonlocal feedback theory for electrocatalytic swimmers with heterogeneous surface chemical kinetics.

We present a self-consistent nonlocal feedback theory for the phoretic propulsion mechanisms of electrocatalytic micromotors or nanomotors. These swimmers, such as bimetallic platinum and gold rods catalyzing decomposition of hydrogen peroxide in aqueous solution, have received considerable theoretical attention. In contrast, the heterogeneous electrochemical processes with nonlocal feedback that are the actual "engines" of such motors are relatively neglected. We present a flexible approach to these processes using bias potential as a control parameter field and a locally-open-circuit reference state, carried through in detail for a spherical motor. While the phenomenological flavor makes meaningful contact with experiment easier, required inputs can also conceivably come from, e.g., Frumkin-Butler-Volmer kinetics. Previously obtained results are recovered in the weak-heterogeneity limit and improved small-basis approximations tailored to structural heterogeneity are presented. Under the assumption of weak inhomogeneity, a scaling form is deduced for motor speed as a function of fuel concentration and swimmer size. We argue that this form should be robust and demonstrate a good fit to experimental data.

Selectively manipulable acoustic-powered microswimmers.

Selective actuation of a single microswimmer from within a diverse group would be a first step toward collaborative guided action by a group of swimmers. Here we describe a new class of microswimmer that accomplishes this goal. Our swimmer design overcomes the commonly-held design paradigm that microswimmers must use non-reciprocal motion to achieve propulsion; instead, the swimmer is propelled by oscillatory motion of an air bubble trapped within the swimmer's polymer body. This oscillatory motion is driven by the application of a low-power acoustic field, which is biocompatible with biological samples and with the ambient liquid. This acoustically-powered microswimmer accomplishes controllable and rapid translational and rotational motion, even in highly viscous liquids (with viscosity 6,000 times higher than that of water). And by using a group of swimmers each with a unique bubble size (and resulting unique resonance frequencies), selective actuation of a single swimmer from among the group can be readily achieved.