Nature Communications ( IF 14.7 ) Pub Date : 2022-12-02 , DOI: 10.1038/s41467-022-35271-9 Shuzhen Yan 1 , Kaiming Hu 2 , Shuai Chen 1 , Tiantian Li 1 , Wenming Zhang 2 , Jie Yin 1 , Xuesong Jiang 1
Stress relaxation in reconfigurable supramolecular polymer networks is strongly related to intermolecular behavior. However, the relationship between molecular motion and macroscopic mechanics is usually vague, and the visualization of internal stress reflecting precise regulation of molecules remains challenging. Here, we present a strategy for visualizing photo-driven stress relaxation induced by infinitesimal perturbations in the intermolecular exchange reaction via reprogrammable wrinkle patterns. The supramolecular films exhibit visible changes in microscopic wrinkle topography through ultraviolet (UV)-induced dynamic disulfide exchange reaction. In accordance with the trans-scale theoretical models, which quantitatively evaluate the chemical-dependent mechanical stresses in the supramolecular network, the unexposed disordered wrinkles evolved into highly oriented patterns and underwent subsequent mutations after thermal treatment. The stress-sensitive wrinkle macro-patterns can be repetitively written/erased through network topology rearrangement using different stimuli. This strategy provides an approach for visualizing and understanding the molecular behavior from dynamic chemistry to mechanical changes, and directly programming wrinkle patterns with regulated structures.
中文翻译:
动态起皱可视化的可重构二硫化物交联超分子膜中的光诱导应力松弛
可重构超分子聚合物网络中的应力松弛与分子间行为密切相关。然而,分子运动与宏观力学之间的关系通常是模糊的,反映分子精确调控的内应力可视化仍然具有挑战性。在这里,我们提出了一种策略,用于通过可重新编程的皱纹模式可视化由分子间交换反应中的无穷小扰动引起的光驱动应力松弛。通过紫外线 (UV) 诱导的动态二硫化物交换反应,超分子薄膜在微观皱纹形貌中表现出明显的变化。根据跨尺度理论模型,定量评估超分子网络中化学相关的机械应力,未暴露的无序皱纹演变成高度定向的图案,并在热处理后发生后续突变。压力敏感的皱纹宏观模式可以通过使用不同刺激的网络拓扑重排来重复写入/擦除。该策略提供了一种方法,用于可视化和理解从动态化学到机械变化的分子行为,并直接对具有调节结构的皱纹模式进行编程。