Discharge Characteristics and Active Particle Distribution Mechanism of Ar/O2/CF4 Dielectric Barrier Discharge

We conduct a numerical study exploring the rotation of a symmetric gear driven by chiral particles in a two-dimensional box with periodic boundary conditions. The symmetric gear is submerged in a sea of chiral active particles. Surprisingly, even though the gear is perfectly symmetric, the microscopic random motion of chiral active particles can be converted into macroscopic directional rotation of the gear. (i) In the case of zero alignment interaction, the direction of rotation of the gear is determined by the chirality of active particles. Optimal parameters (the chirality, self-propelled speed, and packing traction) exist, at which the rotational speed reaches its maximum value. (ii) When considering a finite alignment interaction, alignment interactions between particles play an important role in driving the gear to rotate. The direction of rotation is dictated by the competition between the chirality of active particles and the alignment interactions between them. By tuning the system parameters, we can observe multiple rotation reversals. Our findings are relevant to understanding how the macroscopic rotation of a gear connects to the microscopic random motion of active particles.

Validation and/or calibration of distinct element method (DEM) models is usually performed by comparing element test simulation results with the corresponding stress-strain relationships observed in the laboratory [1]. However, such a validation procedure performed at the macroscopic level does not ensure capturing the microscopic particle-level motion [2]. Thus, the reliability of the DEM model may be limited to some stress paths and may not hold when the material response becomes non-uniform for example when shear bands develop. In this study, the validity of the DEM is assessed by comparing the numerical result with experimental data considering both particle-scale behavior (including particle rotations) and macroscopic stress-strain characteristics observed in shearing tests on granular media. Biaxial shearing tests were conducted on bi-disperse granular assemblies composed of around 2700 circular particles under different confining pressures. Particle-level motions were detected by a novel image analysis technique. Particle rotations are observed to be a key mechanism for the deformation of granular materials. The results from this study suggest that to properly calibrate DEM models able to capture the mechanical behavior in a more realistic way particle scale motions observed in laboratory experiments along with macroscopic response are necessary.

Mechanical and electrical pumps are conventionally used to drive fluid flow in microfluidic devices; these pumps require external power supplies, thus limiting the portability of the devices. Harnessing catalytic reactions in solution allows pumping to be shifted into the chemical realm and alleviates the need for extraneous equipment. Chemical "pumps" involve surface-bound catalytic patches that decompose dissolved reagents into the products of the reaction. The catalytic reactions thereby produce chemical gradients that in turn generate pronounced flow fields. Such chemically-generated flows can be harnessed to transport particles in the solution and regulate their self-organization into complex structures within confined chambers. The challenge, however, is determining the reactions and conditions that will yield "programmable" flows, which permit control over the structure formation. In this Account, we review our modeling efforts to design chemical pumps (and "motors") to regulate the motion and assembly of microscopic particles in solution. In the first scenario, microcapsules release reagents in a microchamber with stationary catalytic patches and thereby act as "fuel" for the microcapsules' self-sustained motion. As the reagent is consumed, the capsules aggregate into "colonies" on the catalyst-covered sites. The shape of the assembled colonies can be tailored by patterning the distribution of the catalyst on the surface. Hence, these chemical pumps can be utilized to regulate the autonomous motion and targeted delivery of microcarriers in microfluidic devices. Notably, this fundamental physicochemical mechanism could have played a role in the self-organization of early biological cells (protocells). In the second example, the catalysts are localized on mobile, active particles, which are called "motors". Reactants dispersed in the solution are decomposed at the surface of the motors and produce a convective flow that transports both the active particles and nearby passive, non-coated particles. Depending on the numbers of active and passive particles and the structure of the self-organized cluster, these assemblies can translate or spin and thus act as self-assembled "conveyor belts" or gears in the microchamber. The latter examples involve the formation of two-dimensional structures. In the final scenario, we devise a mechanism for assembling three-dimensional towerlike structures using microcapsules in solution. Here, chemicals diffusing from a central patch on a surface generate a radially directed flow along the surface toward the center. This toroidal roll of fluid lifts the capsules above the patch and draws out the cluster into a tower, whose structure can be tailored by varying the attractive capsule-capsule and capsule-surface interaction strengths. Hence, our method of flow-directed assembly can permit the growth of reconfigurable 3D structures from simple subunits. Taken together, these findings facilitate the fabrication of stand-alone microfluidic devices that autonomously perform multistage chemical reactions and assays for portable biomedical applications and act as small-scale factories to autonomously build microscale components.

To explore the coupling between a growing population of microorganisms such as E. coli and a nonuniform nutrient distribution, we formulate a minimalistic model. It consists of active Brownian particles that divide and grow at a nutrient-dependent rate following the Monod equation. The nutrient concentration obeys a diffusion equation with a consumption term and a point source. In this setting the heterogeneity in the nutrient distribution can be tuned by the diffusion coefficient. In particle-based simulations, we demonstrate that passive and weakly active particles form proliferation-induced clusters when the nutrient is localized, without relying on further mechanisms such as chemotaxis or adhesion. In contrast, strongly active particles disperse in the whole system during their lifetime and no clustering is present. The steady population is unaffected by activity or nonuniform nutrient distribution and only determined by the ratio of nutrient influx and bacterial death. However, the transient dynamics strongly depends on the nutrient distribution and activity. Passive particles in almost uniform nutrient profiles display a strong population overshoot, with clusters forming all over the system. In contrast, when slowly diffusing nutrients remain centred around the source, the bacterial population quickly approaches the steady state due to its strong coupling to the nutrient. Conversely, the population overshoot of highly active particles becomes stronger when the nutrient localisation increases. We successfully map the transient population dynamics onto a uniform model where the effect of the nonuniform nutrient and bacterial distributions are rationalized by two effective areas.

Exploring the macroscopic scale's similarities to the microscale is part and parcel of this thesis as reflected in the research question: what can we learn about the microscopic scale by studying the macroscale? Investigations of the environment in which the self-assembly takes place, and the self-assembly itself helps to answer this question. We mimicked the microscale and identified several analogue parameters. Instead of heat we use turbulence, instead of microscopic we use centimeter-sized particles. Gravity was counteracted by anupward directed water flow since its influence on macroscopic particles is considerable but has only a minor influence on microscopic particles. Likewise heat has a great influence on the microscopic scale but a minor influence on macroscopic particles. Turbulence proved to be an accurate representation for heat and was modelled as if on a microscopic scale, applying thermodynamical concepts such as Brownian motion, diffusion, kinetics and the Einstein relation. Those concepts proved suitable also on the macroscopic scale. Particle velocity is Maxwell-Boltzmann distributed and the average squared displacement is in agreement with a confined random walk. The diffusion coefficient and velocity is independent on particle size. This leads to the interpretation that the motion of a single centimeter-size sphere resembles the motion of a microscopic particle in that it conducts a random walk and Brownian motion. To visualize micro- or nanoscopic particles electron- or light-microscopy is often used. Instead of microscopes we used video cameras to record the experiments with centimeter sized particles. A swimmingpool pump and asymmetric inflow is used to create upward flow and turbulence. The asymmetric inflow causes large macroscopic swirls representing the applied heat level at the microscale. In the microscopic case the Brownian motion of particles is result of propagating heat originating at its source whereas at the macroscopic scale the vortice propagation originating in the asymmetry of flow cause the Brownian motion of large particles. Despite of those analogies between heat and turbulence the values for the disturbing energy varies considerably depending on if they were determined via single sphere diffusion (Einstein relation) and velocity (kinetic energy) or via two sphere interactions over distance. The latter case is an order of magnitude lower, approximately 6.5mJ compared to 80mJ. This suggests that the heat or turbulence energy spectra may differ with respect to its action on the particle(s). There is a directional dependency of particle velocity, diffusion and disturbing energy. The horizontal dimensions are similar but the vertical component show a stronger dependency with respect to flow asymmetry and turbulence. The directional dependency can most likely be counteracted via future technical adjustments. It can also be interpreted as a temperature gradient. Self-assembly was studied via structure formation of multiple magnetic spheres or twelve heptagonal magnetic platelets by systematic variation of turbulence and asymmetry. The multiple magnetic spheres form lines and rings and their occurance were in accordance with theory, however the absolute energies of the structures deviated from theory. For experiments with increasing number of spheres, four spheres represents a transition between lines and rings. The system proved to seak for the minimum energy structure which again makes the our macroscopic system behave similar to the microscale. Turbulence acted in a similar way as heat since almost only individual particles were observed at high turbulence whereas lines and rings formed as turbulence decreased which resembles a phase transition between a liquid and a solid or a gas and a liquid. Self-assembly of twelve centimeter-sized pentagonal platelets showed the same energy minimum seaking behavior. A complete self-assembly of the dodecahedron was not achieved. Predominantley intermediate structures with maximum contacts to each particle formed (trimer and tetramer etc.) which is the minimum energy structure. Also in this more complex case the system prove to behave similar to the microscale. The two examples of self-assembly represent on the one hand formation of simple structures (rings and lines) and on the other hand a more complex case of self-assembly (a hollow dodecahedron). The later example can be interpreted as self-assembly of geometrical construct or as a representation of self-assembly of a spherical virus. This underlines the potential of macroscopic self-assembly; it can be used in the investigation of general largely scale-independent problems or as an analogue representation in the investigations of natural occuring phenomena.

We report enhanced active particle motion in hydrogen peroxide-fueled self-diffusiophoretic active particle systems of up to 400% via addition of low concentrations of oxygen scavenging agents such as formic acid (as well as other organic acids, hydrazine, and citric acid), whereas active motion was inhibited at higher concentrations. Control experiments showed that enhanced motion was decoupled from catalytic hydrogen peroxide decomposition rate and insensitive to particle surface chemistry. Experimental results point to bulk oxygen scavenging as the cause for the enhanced active motion, representing a realization of recently predicted promotional effects of product sinks on self-diffusiophoretic motion. Diminished active motion at high oxygen scavenger concentrations was attributed to catalytic site blocking by adsorbed solute.

Combining experiments on active colloids, whose propulsion velocity can be controlled via a feedback loop, and the theory of active Brownian motion, we explore the dynamics of an overdamped active particle with a motility that depends explicitly on the particle orientation. In this case, the active particle moves faster when oriented along one direction and slower when oriented along another, leading to anisotropic translational dynamics which is coupled to the particle's rotational diffusion. We propose a basic model of active Brownian motion for orientation-dependent motility. On the basis of this model, we obtain analytical results for the mean trajectories, averaged over the Brownian noise for various initial configurations, and for the mean-square displacements including their non-Gaussian behavior. The theoretical results are found to be in good agreement with the experimental data. Orientation-dependent motility is found to induce significant anisotropy in the particle displacement, mean-square displacement, and non-Gaussian parameter even in the long-time limit. Our findings establish a methodology for engineering complex anisotropic motilities of active Brownian particles, with a potential impact in the study of the swimming behavior of microorganisms subjected to anisotropic driving fields.

This paper focuses on control of electron transports and switching of molecular devices (Mdevices). To accomplish these objectives one should control motion of charge carriers. Various phenomena and transitions, exhibited by Mdevices (microscopic systems) and microscopic particles, can be utilized only if specific effects, evolutions and events are controlled ensuring device functionality and required capabilities. Concentrating on molecular electronics, our objective is to develop sound and practical solutions. Molecular (nano) electronics is fundamentally distinct and cannot be compared to solid-state microelectroncs due to: (1) Distinct phenomena exhibited and utilized; (2) Device physics and functionality differences; (3) Distinct device-physics centered control principles and mechanisms; etc. We examine dynamics and control of microscopic charge carriers in Mdevices. In particular, for solid and fluidic Mdevices, the controlled motion of electrons, ions and molecules is studied. Applying sound device physics, we report theoretical and applied developments in analysis and control of Mdevice transitions with a primary focusing on: (i) Device physics and analysis consistency; (ii) Device physics and control coherency; (iii) Device physics and technology soundness. It is possible to control the transitions and motion of microscopic particles (charge carriers) thereby control tunneling, transport, characteristics and other evolutions exhibited by Mdevice variables (quantities of interest). The processing and memory transitions at the device level are defined by the device physics, control principles, behavior of microscopic system (device) and particles, etc. The ability to control microscopic particles means guarantying the overall device functionality. We examine the device physics and demonstrate that the device functionality, performance requirements and specified capabilities can be achieved by controlling principles. The results are validated by examining device transitions by applying quantum mechanics. We perform high-fidelity modeling and carry out heterogeneous simulations. The quantifying and qualifying studies are reported.

Directional locking occurs when a particle moving over a periodic substrate becomes constrained to travel along certain substrate symmetry directions. Such locking effects arise for colloids and superconducting vortices moving over ordered substrates when the direction of the external drive is varied. Here we study the directional locking of run-and-tumble active matter particles interacting with a periodic array of obstacles. In the absence of an external biasing force, we find that the active particle motion locks to various symmetry directions of the substrate when the run time between tumbles is large. The number of possible locking directions depends on the array density and on the relative sizes of the particles and the obstacles. For a square array of large obstacles, the active particle only locks to the x, y, and 45^{∘} directions, while for smaller obstacles, the number of locking angles increases. Each locking angle satisfies θ=arctan(p/q), where p and q are integers, and the angle of motion can be measured using the ratio of the velocities or the velocity distributions in the x and y directions. When a biasing driving force is applied, the directional locking behavior is affected by the ratio of the self-propulsion force to the biasing force. For large biasing, the behavior resembles that found for directional locking in passive systems. For large obstacles under biased driving, a trapping behavior occurs that is nonmonotonic as a function of increasing run length or increasing self-propulsion force, and the trapping diminishes when the run length is sufficiently large.

Probing surface-adsorbate interactions through active particle dynamics

The microscopic particle motions from the crystal to the disordered state of a dusty plasma with micrometer-sized silicon dioxide particle suspensions in a radio-frequency glow discharge system were studied through an optical microimaging system. Small-amplitude random motion around the lattice sites of the crystal state, relative domain motion with varying boundaries, cooperative hopping in the liquid state, and highly disordered motion with increasing radio-frequency power were observed. Chaotic states with different spatial scales under the coherent and stochastic coupling between dust particles and self-organized background plasma fluctuations were also demonstrated.

Active particles that are self-propelled by converting energy into mechanical motion represent an expanding research realm in physics and chemistry. For micrometer-sized particles moving in a liquid ("microswimmers"), most of the basic features have been described by using the model of overdamped active Brownian motion. However, for macroscopic particles or microparticles moving in a gas, inertial effects become relevant such that the dynamics is underdamped. Therefore, recently, active particles with inertia have been described by extending the active Brownian motion model to active Langevin dynamics that include inertia. In this perspective article, recent developments of active particles with inertia ("microflyers," "hoppers," or "runners") are summarized both for single particle properties and for collective effects of many particles. These include inertial delay effects between particle velocity and self-propulsion direction, tuning of the long-time self-diffusion by the moment of inertia, effects of fictitious forces in noninertial frames, and the influence of inertia on motility-induced phase separation. Possible future developments and perspectives are also proposed and discussed.

Colloidal probes immersed in an active bath have been found to behave like active particles themselves. Here, we use simulations to investigate the mechanisms behind this behavior. We find that the active motion of the colloid cannot be simply attributed to the convective motion in the bath. Instead, the boundary of the probe contributes significantly to these adopted dynamics by causing active bath particles to spontaneously accumulate at the probe. This gathering of active bath particles then pushes the probe, thus promoting its emergent active-particle-like behavior. Furthermore, we find that the dynamic properties of the probe depend on its size in a non-monotonic way, which further highlights the non-trivial interplay between probe and bath.

Anisotropic active colloidal particles in liquid crystals: A Multi-particle Collision Dynamics simulation study

To develop new techniques for reducing the effects of microscopic and macroscopic patient motion in diffusion imaging acquired with high-resolution multishot echo-planar imaging. The previously reported multiplexed sensitivity encoding (MUSE) algorithm is extended to account for macroscopic pixel misregistrations, as well as motion-induced phase errors in a technique called augmented MUSE (AMUSE). Furthermore, to obtain more accurate quantitative diffusion-tensor imaging measures in the presence of subject motion, we also account for the altered diffusion encoding among shots arising from macroscopic motion. MUSE and AMUSE were evaluated on simulated and in vivo motion-corrupted multishot diffusion data. Evaluations were made both on the resulting imaging quality and estimated diffusion tensor metrics. AMUSE was found to reduce image blurring resulting from macroscopic subject motion compared to MUSE but yielded inaccurate tensor estimations when neglecting the altered diffusion encoding. Including the altered diffusion encoding in AMUSE produced better estimations of diffusion tensors. The use of AMUSE allows for improved image quality and diffusion tensor accuracy in the presence of macroscopic subject motion during multishot diffusion imaging. These techniques should facilitate future high-resolution diffusion imaging.