离子流体中的电场诱导振荡：修正Poisson-Nernst-Planck模型的统一表述及其与关联函数分析的相关性
Electric-field-induced oscillations in ionic fluids: a unified formulation of modified Poisson-Nernst-Planck models and its relevance to correlation function analysis
AI总结：
本研究利用随机密度泛函理论建立了浓电解质原始模型的统一动力学表述，论证了Poisson-Nernst-Planck模型修正的合理性，并通过关联函数分析揭示了电场诱导的振荡同步、条纹态及转变特性。
摘要：
我们从理论上研究了作为外加电场下浓电解质原始模型的带电球电场驱动系统。首先，我们利用随机密度泛函理论（DFT），为电场驱动原始模型的随机电荷与密度动力学提供了统一表述。该随机DFT整合了平衡与动态DFT、液态理论以及场论方法的多种框架，使我们能够以统一方式论证此前针对Poisson-Nernst-Planck模型所做的各类修正的合理性。接下来，我们研究了存在静电场时该原始模型的稳态密度-密度与电荷-电荷关联函数。我们重点关注电场诱导的密度与电荷振荡出现之间的同步现象，即密度-密度与电荷-电荷关联从单调衰减到振荡衰减的转变。关联函数分析表明，系统会出现由垂直于外场的分凝带形成的条纹态。我们还预测了以下两点：（i）电场诱导的转变发生在无外加电场的常规Kirkwood转变之前；（ii）电场诱导转变处衰减长度的离子浓度依赖性，与平衡态下振荡衰减长度的模拟和理论研究中发现的欠屏蔽行为具有相似性。
英文摘要：
We theoretically investigate an electric-field-driven system of charged spheres as a primitive model of concentrated electrolytes under an applied electric field. First, we provide a unified formulation for the stochastic charge and density dynamics of the electric-field-driven primitive model using the stochastic density functional theory (DFT). The stochastic DFT integrates various frameworks of the equilibrium and dynamic DFTs, the liquid state theory, and the field-theoretic approach, which allows us to justify in a unified manner various modifications previously made for the Poisson-Nernst-Planck model. Next, we consider stationary density-density and charge-charge correlation functions of the primitive model with a static electric field. We focus on an electric-field-induced synchronization between the emergence of density and charge oscillations, or the crossover from monotonic to oscillatory decay of density-density and charge-charge correlations. The correlation function analysis demonstrates the appearance of stripe states formed by segregation bands perpendicular to the external field. We also predict the following: (i) the electric-field-induced crossover occurs prior to the conventional Kirkwood crossover without an applied electric field, and (ii) the ion concentration dependence of the decay lengths at the electric-field-induced crossovers bears a similarity to the underscreening behavior found by simulation and theoretical studies on the oscillatory decay length in equilibrium.
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