Computational modeling of degradation and recovery processes of self-healing functional materials

自修复材料因其能够修复结构损伤，从而恢复其机械稳定性和性能而在许多应用中非常有趣。对于自愈合功能材料，除了结构修复外，理想的情况下也应该恢复功能。这种材料的设计是非常具有挑战性的，可以受益于对自我修复过程和低至分子水平的功能的计算研究。在此背景下，将在这个项目中应用大量的理论和模拟方法来了解各种自修复功能材料的降解和恢复。所采用的方法涵盖了一系列相关的空间和时间尺度：从更大规模的动力学过程和结构性质(分子动力学和分子力学计算)到分子水平(量子化学和混合量子化学-分子力学计算)。调查系统的选择是与本研究单位的实验项目密切合作的。该项目的总体目标是对导致降解的基本机制进行建模和探索，从而帮助面向合成的项目确定避免降解或使材料和功能再生的可能性。特别是，将模拟光谱可观测性，如UV/VIS、拉曼或2D相关光谱，用于自愈过程的实验研究。最终，功能自修复材料的一般结构-性能关系将被揭示，这将有助于这些材料的设计。

Self-healing materials are very interesting for many applications due to their ability to repair structural damage and, thus, to regain their mechanical stability and properties. For self-healing functional materials, in addition to the structural repair, ideally the functionality should also be recovered. The design of such materials is very challenging and can benefit from computational studies of the self-healing process and of the functionality down to the molecular level. In this context, a large toolset of theoretical and simulation methods will be applied in this project to understand the degradation and recovery of various self-healing functional materials. The employed methods cover a range of relevant spatial and temporal scales: From larger-scale dynamical processes and structural properties (molecular dynamics and molecular mechanics calculations) to the molecular level (quantum chemical and hybrid quantum chemical-molecular mechanical calculations). The systems of investigation are chosen in close collaboration with the experimental projects of this research unit. The overall objective of the project is the modelling and exploring the underlying mechanisms leading to degradation, thereby aiding the synthesis-oriented projects in identifying possibilities either to avoid degradation or to regenerate the material and the functionality. In particular, spectroscopic observables will be simulated such as UV/vis, Raman or 2D-correlation spectra which are used in the experimental investigations of self-healing processes. Eventually, general structure-property relationships will be revealed for functional self-healing materials which can help aiding the design of those materials.