多位点聚合物吸附的首达时间态分辨积分

中文摘要 AI 辅助

理解多位点聚合物吸附的界面结构对于功能纳米材料的合理设计至关重要。然而，通过一个、两个或多个锚点连接的链的分布一直无法通过实验和常规模拟获得。实验通常测量系综平均值，如总吸附质量，而分子动力学模拟仅限于比相关吸附过程短得多的时间尺度。为了应对这一挑战，我们引入了首达时间态分辨积分（SR-IFS）方法。该方法将层内构象调整的快速动力学与外部链交换的慢动力学解耦，从而能够定量预测多位点吸附层内附着状态（$p_1$、$p_2$、$p_3$）的时间依赖性分布。以三臂星形聚合物为模型系统，我们展示了界面态分布从最初的三点附着占主导演变为长时间尺度上更异质的混合物，并且平衡分布可以通过调节单体结合能系统地调控。SR-IFS方法提供了访问这种态分辨信息的途径，为微观动力学与宏观界面性质之间建立了联系。

英文摘要

Understanding the interfacial structure of multi-site polymer adsorption is critical for the rational design of functional nanomaterials. However, the distribution of chains attached via one, two, or more anchor points has remained inaccessible to experiments and conventional simulations. Experiments typically measure ensemble averages such as total adsorbed mass, while molecular dynamics simulations are limited to timescales far shorter than the relevant adsorption processes. To address this challenge, we introduce the State-Resolved Integral of First-Passage Times (SR-IFS) method. This approach decouples fast intra-layer conformational adjustments from the slow kinetics of external chain exchange, enabling quantitative prediction of the time-dependent distribution of attachment states ($p_1$, $p_2$, $p_3$) within a multi-site adsorbed layer. Using 3-arm star-like polymers as a model system, we show that the interfacial state distribution evolves from an initial prevalence of three-point attachments to a more heterogeneous mixture over long time scales, and that the equilibrium distribution can be systematically tuned by adjusting the monomer binding energy. The SR-IFS method provides access to this state-resolved information, offering a connection between microscopic kinetics and macroscopic interfacial properties.

发表机构

• Southeast University（东南大学）

机构由 AI 辅助整理，请以论文原文为准。