Emily Krucker-Velasquez, Martin Z. Bazant, Alfredo Alexander-Katz, James W. Swan
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引用次数: 0
Abstract
Electrolytes, chirp signals, Brownian dynamics, conductivity, Maxwell–Wagner relaxation This study investigates the dynamic response of electrolyte/macroion solutions to time-varying electric fields, which is vital for applications from water desalination to neuromorphic computing and sensor technologies. Using large-scale Brownian dynamics simulations coupled with Poisson’s equation, we examined the frequency-dependent conductivity of symmetric and binary electrolytes/nanoparticles across various concentrations. We reveal a comprehensive picture of charge transport mechanisms by employing chirp signals that excite multiple frequencies. Our results identify three distinct dynamic regimes: (1) instantaneous response at low frequencies, (2) increased lagging and imaginary conductivity at intermediate frequencies, and (3) diminished conductivity at high frequencies due to short-time ion/macroion dynamics. Significant deviations from ideal behavior at low frequencies and high concentrations are attributed to packing and many–body interactions. We propose a modified Maxwell–Wagner relaxation time that incorporates excluded volume effects, offering a more accurate time scale for the dynamic response of concentrated electrolytes/macroions. This new framework scales the frequency-dependent conductivity, revealing universal responses across different concentrations and interaction strengths.
期刊介绍:
ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.