The electric double layer (EDL) has a pivotal role in screening charges on surfaces as in supercapacitor electrodes or colloidal and polymer solutions. Its structure is determined by correlations between the finite-sized ionic charge carriers of the underlying electrolyte, and, this way, these correlations affect the properties of the EDL and of applications utilizing EDLs. We study the structure of EDLs within classical density functional theory (DFT) in order to uncover whether a structural transition in the first layer of the EDL that is driven by changes in the surface potential depends on specific particle interactions or has a general footing.
View Article and Find Full Text PDFCoronavirus disease (COVID-19) is a contagious respiratory disease caused by the SARS-CoV-2 virus. The clinical phenotypes are variable, ranging from spontaneous recovery to serious illness and death. On March 2020, a global COVID-19 pandemic was declared by the World Health Organization (WHO).
View Article and Find Full Text PDFUnderscreening is a collective term for charge correlations in electrolytes decaying slower than the Debye length. Anomalous underscreening refers to phenomenology that cannot be attributed alone to steric interactions. Experiments with concentrated electrolytes and ionic fluids report anomalous underscreening, which so far has not been observed in simulation.
View Article and Find Full Text PDFScanning ion conductance microscopy (SICM) is a topographic imaging technique capable of probing biological samples in electrolyte conditions. SICM enhancements have enabled surface charge detection based on voltage-dependent signals. Here, we show how the hopping mode SICM method (HP-SICM) can be used for rapid and minimally invasive surface charge mapping.
View Article and Find Full Text PDFJ Phys Condens Matter
April 2022
The primitive model describes ions by point charges with an additional hard-core interaction. In classical density-functional theory (DFT) the mean-field electrostatic contribution can be obtained from the first order of a functional perturbation of the pair potential for an uncharged reference system of hard spheres. This mean-field electrostatic term particularly contributes at particle separations that are forbidden due to hard-core overlap.
View Article and Find Full Text PDFRecently, the reversible heat production during the electric double layer (EDL) buildup in a sodium chloride solution was measured experimentally [Janssen et al., Phys. Rev.
View Article and Find Full Text PDFElectrolytes play an important role in a plethora of applications ranging from energy storage to biomaterials. Notwithstanding this, the structure of concentrated electrolytes remains enigmatic. Many theoretical approaches attempt to model the concentrated electrolyte by introducing the idea of ion pairs, with ions either being tightly "paired" with a counter-ion or "free" to screen charge.
View Article and Find Full Text PDFSeveral modern technologies for energy storage and conversion are based on the screening of electric charge on the surface of porous electrodes by ions in an adjacent electrolyte. This so-called electric double layer (EDL) exhibits an intricate interplay with the electrolyte's temperature that was the focus of several recent studies. In one of them, Janssen et al.
View Article and Find Full Text PDFMicrobes living in biofilms, dense assemblages of cells, experience limitation for resources such as oxygen when cellular consumption outpaces diffusion. The pathogenic bacterium has strategies for coping with hypoxia that support cellular redox balancing in biofilms; these include (1) increasing access to oxygen by forming wrinkles in the biofilm surface and (2) electrochemically reducing endogenous compounds called phenazines, which can shuttle electrons to oxidants available at a distance. Phenazine-mediated extracellular electron transfer (EET) has been shown to support survival for cells in anoxic liquid cultures, but the physiological relevance of EET over a distance for biofilms has remained unconfirmed.
View Article and Find Full Text PDFWe present an approach to derive the connectivity properties of pairwise interacting n-body systems in thermal equilibrium. We formulate an integral equation that relates the pair connectedness to the distribution of nearest neighbors. For one-dimensional systems with nearest-neighbor interactions, the nearest-neighbor distribution is in turn related to the pair-correlation function g through a simple integral equation.
View Article and Find Full Text PDFThe massively parallel nature of biological information processing plays an important role due to its superiority in comparison to human-engineered computing devices. In particular, it may hold the key to overcoming the von Neumann bottleneck that limits contemporary computer architectures. Physical-model neuromorphic devices seek to replicate not only this inherent parallelism, but also aspects of its microscopic dynamics in analog circuits emulating neurons and synapses.
View Article and Find Full Text PDFNeuromorphic devices represent an attempt to mimic aspects of the brain's architecture and dynamics with the aim of replicating its hallmark functional capabilities in terms of computational power, robust learning and energy efficiency. We employ a single-chip prototype of the BrainScaleS 2 neuromorphic system to implement a proof-of-concept demonstration of reward-modulated spike-timing-dependent plasticity in a spiking network that learns to play a simplified version of the Pong video game by smooth pursuit. This system combines an electronic mixed-signal substrate for emulating neuron and synapse dynamics with an embedded digital processor for on-chip learning, which in this work also serves to simulate the virtual environment and learning agent.
View Article and Find Full Text PDFTransport processes through ion-channel proteins, protein pores, or solid-state nanopores are traditionally recorded with commercial patch-clamp amplifiers. The bandwidth of these systems is typically limited to 10 kHz by signal-to-noise-ratio (SNR) considerations associated with these measurement platforms. At high bandwidth, the input-referred current noise in these systems dominates, determined by the input-referred voltage noise of the transimpedance amplifier applied across the capacitance at the input of the amplifier.
View Article and Find Full Text PDFRecent work has pushed the noise-limited bandwidths of solid-state nanopore conductance recordings to more than 5 MHz and of ion channel conductance recordings to more than 500 kHz through the use of integrated complementary metal-oxide-semiconductor (CMOS) integrated circuits. Despite the spectral spread of the pulse-like signals that characterize these recordings when a sinusoidal basis is employed, Bessel filters are commonly used to denoise these signals to acceptable signal-to-noise ratios (SNRs) at the cost of losing many of the faster temporal features. Here, we report improvements to the SNR that can be achieved using wavelet denoising instead of Bessel filtering.
View Article and Find Full Text PDFThe decay of correlations in ionic fluids is a classical problem in soft matter physics that underpins applications ranging from controlling colloidal self-assembly to batteries and supercapacitors. The conventional wisdom, based on analyzing a solvent-free electrolyte model, suggests that all correlation functions between species decay with a common decay length in the asymptotic far field limit. Nonetheless, a solvent is present in many electrolyte systems.
View Article and Find Full Text PDFSelf-propelled Brownian particles show rich out-of-equilibrium physics, for instance, the motility-induced phase separation (MIPS). While decades of studying the structure of liquids have established a deep understanding of passive systems, not much is known about correlations in active suspensions. In this work we derive an approximate analytic theory for three-body correlations and forces in systems of active Brownian disks starting from the many-body Smoluchowski equation.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
February 2018
Single-channel recordings are widely used to explore functional properties of ion channels. Typically, such recordings are performed at bandwidths of less than 10 kHz because of signal-to-noise considerations, limiting the temporal resolution available for studying fast gating dynamics to greater than 100 µs. Here we present experimental methods that directly integrate suspended lipid bilayers with high-bandwidth, low-noise transimpedance amplifiers based on complementary metal-oxide-semiconductor (CMOS) integrated circuits (IC) technology to achieve bandwidths in excess of 500 kHz and microsecond temporal resolution.
View Article and Find Full Text PDFLipid bilayers provide many benefits for ion channel recordings, such as control of membrane composition and transport molecules. However, they suffer from high membrane capacitance limiting the bandwidth and impeding analysis of fast gating. This can be overcome by fitting the deviations of the open-channel noise from the baseline noise by extended beta distributions.
View Article and Find Full Text PDFOngoing scientific interest is aimed at the properties and structure of electric double layers (EDLs), which are crucial for capacitive energy storage, water treatment, and energy harvesting technologies like supercapacitors, desalination devices, blue engines, and thermocapacitive heat-to-current converters. A promising tool to describe their physics on a microscopic level is (classical) density functional theory (DFT), which can be applied in order to analyze pair correlations and charge ordering in the primitive model of charged hard spheres. This simple model captures the main properties of ionic liquids and solutions and it predicts many of the phenomena that occur in EDLs.
View Article and Find Full Text PDFIEEE Trans Biomed Circuits Syst
February 2017
We present results from a new approach to learning and plasticity in neuromorphic hardware systems: to enable flexibility in implementable learning mechanisms while keeping high efficiency associated with neuromorphic implementations, we combine a general-purpose processor with full-custom analog elements. This processor is operating in parallel with a fully parallel neuromorphic system consisting of an array of synapses connected to analog, continuous time neuron circuits. Novel analog correlation sensor circuits process spike events for each synapse in parallel and in real-time.
View Article and Find Full Text PDFJ Phys Condens Matter
December 2016
The slow dynamics in a glassy hard-sphere system is dominated by cage breaking events, i.e. rearrangements where a particle escapes from the cage formed by its neighboring particles.
View Article and Find Full Text PDFThe protein density in biological membranes can be extraordinarily high, but the impact of molecular crowding on the diffusion of membrane proteins has not been studied systematically in a natural system. The diversity of the membrane proteome of most cells may preclude systematic studies. African trypanosomes, however, feature a uniform surface coat that is dominated by a single type of variant surface glycoprotein (VSG).
View Article and Find Full Text PDFThe ongoing scientific interest in the properties and structure of electric double layers (EDLs) stems from their pivotal role in (super)capacitive energy storage, energy harvesting, and water treatment technologies. Classical density functional theory (DFT) is a promising framework for the study of the in- and out-of-plane structural properties of double layers. Supported by molecular dynamics simulations, we demonstrate the adequate performance of DFT for analyzing charge layering in the EDL perpendicular to the electrodes.
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