标题： 复合电介质中的协同界面效应：通过多尺度建模对电荷捕获调控的见解 显示英文标题

标题： Synergistic Interface Effects in Composite Dielectrics: Insights into Charge Trapping Regulation through Multiscale Modeling

摘要： 现代能源应用的快速发展推动了提高储能电介质介电强度的迫切需求，以实现更高的功率密度。界面设计是一种有前景的策略，用于调节决定介电强度的关键电荷传输过程。然而，由于缺乏对涉及基本电子过程和分子构建块特性和界面形态复杂相互作用的基本机制的深入理解，针对电荷传输的界面效应的定向开发受到限制——这些细节无法通过实验方法完全解析。在这里，我们采用一种多尺度建模方法，将电荷载体的量子特性与复杂界面的纳米和介观尺度结构细节联系起来。应用于一种经过应用验证的纤维素-油复合材料，其中油、无序区和晶体纤维素区域之间形成了界面，这种方法表明电荷被捕获在无序区域。具体而言，它揭示了这种捕获是两种调控传输的界面机制的协同效应：由于能量因素，电荷回传到油区被抑制，而由于低电子耦合，电荷前传到晶体纤维素也被抑制。通过双界面调控揭示界面效应的分子起源，为先进能源材料的发展提供了新的路径。 显示英文摘要

摘要： The rapid development of modern energy applications drives an urgent need to enhance the dielectric strength of energy storage dielectrics for higher power density. Interface design is a promising strategy to regulate the crucial charge transport process determining dielectric strength. However, the targeted exploitation of interface effects on charge transport is limited due to a lack of fundamental understanding of the underlying mechanisms involving elementary electronic processes and details of the intricate interplay of characteristics of molecular building blocks and the interfacial morphology -- details that cannot fully be resolved with experimental methods. Here we employ a multiscale modeling approach linking the quantum properties of the charge carriers with nano- and mesoscale structural details of complex interfaces. Applied to a prototypical application-proven cellulose-oil composite with interfaces formed between oil, disordered, and crystalline cellulose regions, this approach demonstrates that charges are trapped in the disordered region. Specifically, it unveils this trapping as a synergistic effect of two transport-regulating interface mechanisms: back-transfer to the oil region is suppressed by energetic factors, while forward-transfer to the crystalline cellulose is suppressed by low electronic coupling. The insight into the molecular origins of interface effects via dual-interface regulation offers new development paths for advanced energy materials.