Charge-Induced Polarization in Dielectric Particle Systems: A Geometry-Dependent Effect.

IF 5.7 1区 化学 Q2 CHEMISTRY, PHYSICAL
Eric B Lindgren
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引用次数: 0

Abstract

Electrostatic interactions in systems composed of finite-sized dielectric materials extend well beyond simple point-charge approximations, particularly when many-body polarization effects become significant. This study shows that asymmetries in the size or net charge of spherical particles can trigger nontrivial phenomena, including like-charge attraction and intricate force balances involving neutral species. Through a rigorous boundary-integral framework, it is substantiated that induced surface charges propagate through iterative cascades, reflecting the full many-body, nonadditive character of polarization. Significantly, a geometry-based cutoff is adopted to discriminate whether long-range interactions can be approximated by monopoles, thereby retaining near-field multipole couplings without forfeiting computational efficiency. This approach provides significant computational gains without compromising the rigor of many-body treatment, underscoring the critical interplay between geometric factors─specifically, particle size (and its associated curvature) and interparticle separation─in determining local field intensities, which often exceed conventional Coulombic predictions. The findings can illuminate pathways for understanding and designing advanced materials and self-assembled architectures in which dielectric polarization governs or contributes to emergent behavior.

介电粒子系统中的电荷诱导极化:几何相关效应。
由有限尺寸介电材料组成的系统中的静电相互作用远远超出了简单的点电荷近似,特别是当多体极化效应变得显著时。这项研究表明,球形粒子的大小或净电荷的不对称性可以引发非平凡现象,包括类电荷吸引和涉及中性物质的复杂力平衡。通过严格的边界积分框架,证明了诱导表面电荷通过迭代级联传播,反映了极化的完整多体非加性特征。值得注意的是,采用了基于几何的截止来区分远程相互作用是否可以用单极子近似,从而在不损失计算效率的情况下保留近场多极耦合。这种方法在不影响多体处理的严密性的情况下提供了显著的计算增益,强调了几何因素(特别是粒径(及其相关曲率)和粒子间分离)在确定局部场强方面的关键相互作用,而局部场强往往超过传统的库仑预测。这些发现可以照亮理解和设计先进材料和自组装结构的途径,其中介电极化控制或有助于紧急行为。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Journal of Chemical Theory and Computation
Journal of Chemical Theory and Computation 化学-物理:原子、分子和化学物理
CiteScore
9.90
自引率
16.40%
发文量
568
审稿时长
1 months
期刊介绍: The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
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