Microswimmers are self-propelled particles that navigate fluid environments, offering significant potential for applications in environmental pollutant decomposition, biosensing, and targeted drug delivery. Their performance relies on engineered catalytic surfaces. Gold nanoclusters (AuNCs), with atomically precise structures, tunable optical properties, and high surface area-to-volume ratio, provide a new optimal catalyst for enhancing microswimmer propulsion. Unlike bulk gold or nanoparticles, AuNCs may deliver tunable photocatalytic activity and increased catalytic specificity, making them ideal co-catalysts for hybrid microswimmers. For the first time, this study combines AuNCs with TiO2/Cr2O3 Janus microswimmers, combining the unique properties of both materials. This hybrid system capitalizes on the tuned optical properties of AuNCs and their role as co-catalysts with TiO2, driving enhanced photocatalytic performance under ultraviolet (UV) excitation. Using motion analysis, it is shown that the AuNC-microswimmers exhibit significantly greater propulsion and mean squared displacement (MSD) as compared to controls. These findings suggest that the integration of nanoclusters with semiconductor materials enables state of the art, light-switchable microswimmers. These AuNC-microswimmer systems may thus offer new opportunities for environmental catalysis and other applications, providing precise control over catalytic and motile behaviors at the microscale.

Strong chiroptical activity has been an active area of research due to potential applications in polarization control and enhanced molecular sensing. However, the creation and investigation of hybrid chiral nanostructures, consisting of multiple active materials, are relatively unexplored areas. In this work, we fabricated nanohelices with a semiconducting material, titanium dioxide, which were "decorated" with a plasmonic material, gold (Au), via physical vapor deposition. Due to the hybrid nature of the samples, we observed broadband chiroptical activity spanning from the ultraviolet through visible wavelengths, which is not observed with either material alone. Remarkably, the magnitude of the visible-wavelength chiroptical activity was found to be highly enhanced and highly sensitive to the amount of Au. This dramatic signal enhancement and high sensitivity cannot be explained by a simple algebraic addition of the optical activities of the two underlying materials and is thus expected to be a result of the plasmonic-semiconducting interface.

In this study, a direct-grown helical-shaped tungsten-oxide-based (h-WOx) selection device is presented for emerging memory applications. The selectivity in the selection devices is from 10 to 103 with a low off-current of 0.1 to 0.01 nA. In addition, the selectivity of volatile switching in the h-WOx selection devices is reconfigurable with a pseudo RESET process on the one-time negative voltage operations. The helical-shaped selection devices with the glancing angle deposition (GLAD) method show good compatibility, low power consumption, good selectivity, and good reconfigurability for next-generation memory applications.

Active colloidal microcrystallites capable of generating flow patterns around or through their porous network are introduced, which in combination with “free microspheres,” create self‐assembled active clusters with multiple moving parts. Fluid flow draws microspheres within a microcrystallite's local environment toward—and aggregate at—the edge of the microcrystallite, where the previously translational movement transitions to continuous spinning. These experiments show that the spinning frequency decreases with an increase in diameter and that when the center of mass of a spinning particle is shifted off‐center—here Janus spheres—a time‐varying angular frequency is observed. Weight‐anisotropy also leads to a particularly intriguing phenomenon, which manifests as the spontaneous realignment of the rotational axis to a preferential direction; this effect is attributed to a gravitropic self‐correcting mechanism. Thus, the dynamics of the self‐assembled active structure remains stable over long time periods, despite being subjected to significant noise, for example, Brownian forces.

The development of emerging memory technology with high density crossbar memory array is widely investigated for fulfilling the high demand on future applications, e.g. artificial intelligence, internet-of-things (IoT), edge computing, sensing with storage etc [1] – [3] . In the array, the sneak path current is a fatal problem subverting the read/write margin with the crossbar configuration, where...

The evaporation of liquid droplets containing colloids is an omnipresent natural phenomenon that has received much attention due to the fundamental effects it entails, as well as the multitudes of fields in which it can be applied. The deposition of particulates onto a solid surface during evaporation tends to form ring-like stains, which are a hallmark of the "coffee-ring effect." A wide variety of systems has already been employed to suppress or enable this effect, however, little attention has been focused on particles in restricted geometries that are driven far from equilibrium. Here, we investigate how self-propelled, "active" catalytic Janus microspheres affect the ring stains left behind during the drying of a geometrically confined suspension containing such particles. Self-propulsion results indirectly from the decomposition of hydrogen peroxide (H2O2) on the catalytically active hemispherical shell, while the diametrically opposite face is inert; this is how the system is driven out of equilibrium. The magnitude of activity can be controlled by adjusting the volume concentration of aqueous H2O2 within the suspension. This parameter strongly influences the ring-shaped microstructures obtained, especially when the concentration is sufficiently high to produce oxygen bubbles that take over the motion as opposed to auto-phoresis.

Self-propelling, light-activated colloidal particles can be actuated in water alone. Here we study the effect of adding different amounts of a gold/palladium alloy to titanium dioxide-based, active colloids. We observe a correlation between alloy-thickness and the average speed of the particles, and we discover an intermediate thickness leads to the highest activity for this system. We argue that a non-continuous thin-film of the co-catalyst improves the efficiency of water-splitting at the surface of the particles, and in-turn, the performance of "fuel-free" self-propulsion.

Reactive burn models represent a significant leap in high explosive (HE) modeling capability. The first generation of engineering models of HE detonation are called programmed burn models and they are largely based on the distance between a prescribed detonation point and each zone in a simulation. There have been many advancements to programmed burn models over the years and when the assumptions upon which they are based are met, a properly tuned programmed burn model can be highly accurate but if any of their assumptions is not met, as is the case for corner turning or weakly initiated HE burn, they will give the wrong answer. Reactive burn models represent an entirely new way of modeling HE burn. They use the local conditions of a zone – e.g. temperature, pressure or density – as calculated by a hydrocode to determine if and when the zone is going to detonate and if so, how rapidly. This difference opens up an entirely new set of capabilities for HE modeling. It makes it possible to accurately and predictively model phenomena like the effect of confinement and the formation of dead zones. Reactive burn models have seen sustained development effort at LANL for at least the last decade but several recent developments make it timely to transition reactive burn models from a research topic to a production tool. The main goal of this milestone is to facilitate and accelerate the adoption of reactive burn as a commonly available modeling option, with recommendations on the resolution that will be required and uncertainties associated with their modeling choices. To achieve this, we have performed verification, validation, and uncertainty quantification (UQ) assessments of AWSD and SURF/SURFplus in xRage and FLAG on a variety of different problems.

It is demonstrated how the strength of activation for photocatalytic, self-propelled colloids can be enhanced with a constant, uniform magnetic field. When exposed to ultraviolet light and hydrogen peroxide, the titanium dioxide-based colloids become actively propelled. Due to the iron oxide core, a uniform field oriented perpendicular to the surface where motion takes place causes the asymmetrically shaped particles to rotate, which consequently leads to an increase in activity. The field-dependent dynamics of self-propulsion is quantified, and a qualitative description of how this effect arises is proposed. Since the application of the field is easily reversible, modulating the field on-and-off serves as a de facto "switch" that controls particle behavior.

Self‐propelled colloids are primed to become scaled up, nano‐ and microscale inorganic analogues of molecular motors and machines. In order to advance toward the ambitious goal of employing such active particles to form genuine man‐made small scale machinery, a significantly diversified library of particle types, capable of a wide range of motive behaviors, must be available. Here, it is shown that the dynamics of photoactivated, self‐phoretic particles can be engineered by targeted design of metal–semiconductor heterojunctions. This effect is demonstrated with three different microswimmers consisting of an elongated semiconducting tail made from anatase titanium dioxide; all three of which would otherwise be identical absent vapor‐deposited coatings of gold at different locations on the tails. The specific location of the heterojunction determines the swimming behavior for each type. Although here only one shape and material combination is focused upon, engineering active particles with site‐specific metal–semiconductor heterojunctions is a general technique for achieving desired kinematic behavior in active colloidal matter.

Active colloids powered by self-generated, local chemical concentration gradients exhibit dynamics that are a function of the particles' morphology and material properties. These characteristics also govern how the active colloids interact with surfaces, including other particles and nearby walls. Thus, by targeted design, the dynamic behavior, on average, can be engineered, despite a lack of "external" control such as an applied magnetic field. This allows for the development of new applications and the investigation of novel effects that arise when self-propelled active colloids have complex shapes and material composition. Here, we explore some of our recent work on this topic including the dynamics and interactions of photoactivated, self-propelled colloids with such multifaceted properties. We also delve into some special cases, such as a new variety of active particle-particle interaction that we recently developed, in which direct contact between the active colloids is forbidden, and the direction of propulsion for pairs of particles is correlated. The unifying theme of the work highlighted herein is the relationship between the physical, chemical, and material properties of active colloids and their motive behavior, the understanding of which opens up a wide range of new possibilities as we move toward the ultimate goal of realizing functional, man-made micro- and nanomachinery.

We harness a synergy between morphology and the electromagnetic response of semiconducting material to engineer the chiro-optical properties of metamaterials that are active at ultraviolet (UV) wavelengths. Chiral metamaterials have recently ushered in new research directions in fundamental light-matter interactions, while simultaneously opening a range of promising photonics-based applications from polarization control to improved biosensing methods. Despite these recent advances, to date, very little attention has been focused upon engineered large UV chiro-optical activity, where naturally occurring molecular optical activity bands are most typically encountered. Here, we systematically alter the morphology of titanium dioxide nanohelices, which make up the elements of the chiral metamaterials, to investigate how the nanoparticle shape affects chiro-optical activity across the UV spectrum. When the nanoscale critical dimensions fall within a particular size range, giant chiro-optical activity is observed, which is on the order of the strongest demonstrated in the UV to date and can be tuned by slight alterations of the nanohelices' morphology.

We investigate the dynamics of structured photoactive microswimmers and show that morphology sensitively determines the swimming behavior. Particular to this study, a major portion of the light-activated particles' underlying structure is built from a photocatalytic material, made possible by dynamic physical vapor deposition (DPVD). We find that swimmers of this type exhibit unique shape-dependent autonomous swimming that is distinct from what is seen in systems with similar structural morphology but not fabricated directly from the catalyst. Notably, the direction of motion is a function of these parameters. Because the swimming behavior is strongly correlated with particle shape and material composition, DPVD allows for engineering small-scale propulsion by adjusting the fabrication parameters to match the desired performance.

Using a dynamic fabrication process, hybrid, photoactivated microswimmers made from two different semiconductors, titanium dioxide (TiO2 ) and cuprous oxide (Cu2 O) are developed, where each material occupies a distinct portion of the multiconstituent particles. Structured light-activated microswimmers made from only TiO2 or Cu2 O are observed to be driven in hydrogen peroxide and water most vigorously under UV or blue light, respectively, whereas hybrid structures made from both of these materials exhibit wavelength-dependent modes of motion due to the disparate responses of each photocatalyst. It is also found that the hybrid particles are activated in water alone, a behavior which is not observed in those made from a single semiconductor, and thus, the system may open up a new class of fuel-free photoactive colloids that take advantage of semiconductor heterojunctions. The TiO2 /Cu2 O hybrid microswimmer presented here is but an example of a broader method for inducing different modes of motion in a single light-activated particle, which is not limited to the specific geometries and materials presented in this study.

Self-phoretic colloids are emerging as critical components of programmable nano- and microscale active matter and may usher in a new area of complex, small-scale machinery. To date, most studies have focused upon active particles confined by gravity to a plane located just above a solid/liquid interface. Despite this ubiquity, little attention has been directed at how the physicochemical qualities of this interface might affect motion. Here, we show that both the chemical and physical properties of the solid, above which motion takes place, significantly influence the behavior of particles propelled by self-generated concentration gradients. More specifically, titania/silica (TiO2/SiO2) photoactive microswimmers move faster when the local osmotic flow over the stationary solid is diminished, which we demonstrate by reducing the magnitude of the surface's zeta potential or by increasing surface roughness. Our results suggest that consideration of surface properties is crucial for modeling self-phoretic active matter while simultaneously offering a new avenue for engineering the kinematic behavior of such systems.

Westudy both experimentally and theoretically the dynamics of chemically self-propelled Janus colloids moving atop a two-dimensional crystalline surface. The surface is a hexagonally close-packed monolayer of colloidal particles of the same size as the mobile one. The dynamics of the self-propelled colloid reflects the competition between hindered diffusion due to the periodic surface and enhanced diffusion due to active motion. Which contribution dominates depends on the propulsion strength, which can be systematically tuned by changing the concentration of a chemical fuel. The mean-square displacements (MSDs) obtained from the experiment exhibit enhanced diffusion at long lag times. Our experimental data are consistent with a Langevin model for the effectively two-dimensional translational motion of an active Brownian particle in a periodic potential, combining the confining effects of gravity and the crystalline surface with the free rotational diffusion of the colloid. Approximate analytical predictions are made for the MSD describing the crossover from free Brownian motion at short times to active diffusion at long times. The results are in semi-quantitative agreement with numerical results of a refined Langevin model that treats translational and rotational degrees of freedom on the same footing.

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.

Janus spheres, micron-sized silica spheres half-coated with platinum, move rectilinearly away from the platinum side in aqueous hydrogen peroxide. Upon self-assembling, these colloidal particles can form dimers with different conformations that exhibit both rectilinear and rotational modes of motion depending upon the relative orientation of each Janus sphere. At the micron length-scale, stochastic rotational Brownian dynamics is of the order of deterministic dynamics, and their coupling results in effective diffusion, in addition to passive translational diffusion. For dimers with rotary motion, the dynamic coupling leads to spiral trajectories for an ensemble average of the displacement vector.