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Rubinstein, Shmuel M.

Publications and source records attributed to Rubinstein, Shmuel M..

Quantitative local state of charge mapping by operando electrochemical fluorescence microscopy in porous electrodes

We introduce operando quantitative electrochemical fluorescence state of charge mapping (QEFSM), a non-invasive technique to study operating electrochemical systems along with a new design of optically transparent microfluidic redox flow cells compatible with the most demanding optical requirements. QEFSM allows quantitative mappings of the concentration of a particular oxidation state of a redox-active species within a porous electrode during its operation. In this study, we used confocal microscopy to map the fluorescence signal of the reduced form of 2,7-anthraquinone disulfonate (AQDS) in a set of multistep-chronoamperometry experiments. Calibrating these images and incorporating an analytical model of quinhydrone heterodimer formation with no free parameters, and accounting for the emission of each species involved, we determined the local molecular concentration and the state of charge (SOC) fields within a commercial porous electrode during operation. With this method, electrochemical conversion and species advection, reaction and diffusion can be monitored at heretofore unprecedented transverse and axial resolution (1 μm and 25 μm, respectively) at frame rates of 0.5 Hz, opening new routes to understanding local electrochemical processes in porous electrodes. Here, we observed pore-scale SOC inhomogeneities appearing when the fraction of electroactive species converted in a single pass through the electrode becomes large.

42 ENGINEERING↗

Seismological Stress Drops for Confined Ruptures Are Invariant to Normal Stress

Seismic moment and rupture length can be combined to infer stress drop, a key parameter for assessing earthquakes. In natural earthquakes, stress drops are largely depth-independent, which is surprising given the expected dependence of frictional stress on normal stresses and hence overburden. We have developed a transparent experimental fault that allows direct observation of thousands of slip events, with ruptures that are fully contained within the fault. Surprisingly, the observed stress drops are largely independent of both the magnitude of normal stress and its heterogeneity, capturing the independence seen in nature. However, we observe larger, normal stress-dependent stress drops when the fault area is reduced, which allows slip events to frequently reach the edge of the interface. We conclude that confined ruptures have normal stress independent stress drops, and thus the depth-independent stress drops of tectonic earthquakes may be a consequence of their confined nature.

58 GEOSCIENCES↗

A model for the fragmentation kinetics of crumpled thin sheets

As a confined thin sheet crumples, it spontaneously segments into flat facets delimited by a network of ridges. Despite the apparent disorder of this process, statistical properties of crumpled sheets exhibit striking reproducibility. Experiments have shown that the total crease length accrues logarithmically when repeatedly compacting and unfolding a sheet of paper. Here, we offer insight to this unexpected result by exploring the correspondence between crumpling and fragmentation processes. We identify a physical model for the evolution of facet area and ridge length distributions of crumpled sheets, and propose a mechanism for re-fragmentation driven by geometric frustration. This mechanism establishes a feedback loop in which the facet size distribution informs the subsequent rate of fragmentation under repeated confinement, thereby producing a new size distribution. We then demonstrate the capacity of this model to reproduce the characteristic logarithmic scaling of total crease length, thereby supplying a missing physical basis for the observed phenomenon.

42 ENGINEERING↗

Geometric frustration induces the transition between rotation and counterrotation in swirled granular media

Granular material in a swirled container exhibits a curious transition as the number of particles is increased: At low densities, the particle cluster rotates in the same direction as the swirling motion of the container, while at high densities it rotates in the opposite direction. We investigate this phenomenon experimentally and numerically using a corotating reference frame in which the system reaches a statistical steady state. In this steady state, the particles form a cluster whose translational degrees of freedom are stationary, while the individual particles constantly circulate around the cluster's center of mass, similar to a ball rolling along the wall within a rotating drum. We show that the transition to counterrotation is friction dependent. At high particle densities, frictional effects result in geometric frustration, which prevents particles from cooperatively rolling and spinning. Consequently, the particle cluster rolls like a rigid body with no-slip conditions on the container wall, which necessarily counterrotates around its own axis. Furthermore, numerical simulations verify that both wall-disk friction and disk-disk friction are critical for inducing counterrotation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Machine learning in a data-limited regime: Augmenting experiments with synthetic data uncovers order in crumpled sheets

Machine learning has gained widespread attention as a powerful tool to identify structure in complex, high-dimensional data. However, these techniques are ostensibly inapplicable for experimental systems where data are scarce or expensive to obtain. Here, we introduce a strategy to resolve this impasse by augmenting the experimental dataset with synthetically generated data of a much simpler sister system. Specifically, we study spontaneously emerging local order in crease networks of crumpled thin sheets, a paradigmatic example of spatial complexity, and show that machine learning techniques can be effective even in a data-limited regime. This is achieved by augmenting the scarce experimental dataset with inexhaustible amounts of simulated data of rigid flat-folded sheets, which are simple to simulate and share common statistical properties. This considerably improves the predictive power in a test problem of pattern completion and demonstrates the usefulness of machine learning in bench-top experiments where data are good but scarce.

97 MATHEMATICS AND COMPUTING↗

A state variable for crumpled thin sheets

Despite the apparent ease with which sheets of paper are crumpled and tossed away, crumpling dynamics are often considered a paradigm of complexity. This arises from the infinite number of configurations that disordered, crumpled sheets can take. Here we experimentally show that key aspects of axially confined crumpled Mylar sheets have a very simple description; evolution of damage in crumpling dynamics can largely be described by a single global quantity—the total length of creases. We follow the evolution of the damage network in repetitively crumpled elastoplastic sheets, and show that the dynamics are deterministic, depending only on the instantaneous state of the crease network and not on the crumpling history. We also show that this global quantity captures the crumpling dynamics of a sheet crumpled for the first time. This leads to a remarkable reduction in complexity, allowing a description of a highly disordered system by a single state parameter.

42 ENGINEERING↗