原子间相互作用对无序大分子结构和动力学影响的中子散射研究  

The influence of interatomic interaction on the structure and dynamics of disordered macromolecules:a neutron scattering study

作　　者：韩泽华 左太森[1,2] 马长利 李雨晴 程贺 Zehua Han;Taisen Zuo;Changli Ma;Yuqing Li;He Cheng(China Spallation Neutron Source,Institute of High Energy Physics,Chinese Academy of Sciences,Dongguan 523800,China;Spallation Neutron Source Science Center,Guangdong 523800,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院高能物理研究所,中国散裂中子源,东莞523800 [2]散裂中子源科学中心,东莞523800 [3]中国科学院大学,北京100049

出　　处：《中国科学：化学》2023年第4期678-692,共15页SCIENTIA SINICA Chimica

基　　金：国家自然科学基金(编号:22273046,U1932161)资助项目。

摘　　要：不同单体在原子尺度的相互作用使得不同大分子体系在微观、介观的多尺度复杂结构及动力学行为有明显差异,从而进一步影响了体系的宏观性质.联用中子散射和计算机模拟,利用相同分子量和分子量分布的氘代大分子与氢化大分子具有相同分子结构、不同中子衬度,以及中子散射和计算机模拟宽广的时间、空间观察尺度,我们可以得到无序大分子体系最可几全原子结构,进而分析其从原子到纳米的多尺度空间结构,与从皮秒到微秒的多模式动力学行为的成因.近年来,我们使用该方法,从小分子到大分子的稀溶液、溶胀体系,从大分子熔体到玻璃态,成功分析了原子间相互作用对不同空间尺度结构和跨时间运动模式动力学行为的影响.本文介绍了这些典型的例子,希望将该方法推广到更广阔的研究领域,把大分子原子结构的多样性与多尺度的复杂结构和动力学有机地联系起来.The interactions between different monomers at the atomic scale make the microscopic and mesoscopic multi-scale structures and dynamics behaviors of different macromolecules obviously different,and they further influence their macroscopic properties.We can use the combination of neutron scattering and computer simulations to observe a wide range of time and space scales,and find out their relations.Deuterated macromolecule has the same structure,dynamics,and different neutron contrast with its hydrogenated counterpart,when they have the same molecular weight and molecular weight distributions.Based on that,neutron scattering and computer simulations can reveal the most probable all-atom structures of disordered macromolecules,and further analyze the origin of multi-scale spatial structures from atoms to nanometers,and the dynamics from pico-seconds to micro-seconds.In recent years,we have successfully used this method in different systems,i.e.,from disordered small molecules and macromolecular solutions to its swelling states,from macromolecular melt to its glass state.We find out the relations between their atomic interactions and their multiscale structures and dynamics.In this review,we introduce our typical works,and hope to generalize this method to a broader research field,linking the diversity of atomic structures with multi-scale structures and dynamics.

关 键 词：无序大分子中子全散射 准弹性中子散射 计算机模拟 全原子结构 多尺度结构和动力学 

分 类 号：O641.3[理学—物理化学] O643.1[理学—化学]