Department of Physics and Astronomy, Washington State University, Pullman, WA, USA.
Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, NC, USA.
Nat Commun. 2021 May 25;12(1):3123. doi: 10.1038/s41467-021-23382-8.
Self-assembled molecular nanostructures embody an enormous potential for new technologies, therapeutics, and understanding of molecular biofunctions. Their structure and function are dependent on local environments, necessitating in-situ/operando investigations for the biggest leaps in discovery and design. However, the most advanced of such investigations involve laborious labeling methods that can disrupt behavior or are not fast enough to capture stimuli-responsive phenomena. We utilize X-rays resonant with molecular bonds to demonstrate an in-situ nanoprobe that eliminates the need for labels and enables data collection times within seconds. Our analytical spectral model quantifies the structure, molecular composition, and dynamics of a copolymer micelle drug delivery platform using resonant soft X-rays. We additionally apply this technique to a hydrocarbon sequestrating polysoap micelle and discover that the critical organic-capturing domain does not coalesce upon aggregation but retains distinct single-molecule cores. This characteristic promotes its efficiency of hydrocarbon sequestration for applications like oil spill remediation and drug delivery. Such a technique enables operando, chemically sensitive investigations of any aqueous molecular nanostructure, label-free.
自组装分子纳米结构为新技术、疗法和分子生物功能的理解提供了巨大的潜力。它们的结构和功能依赖于局部环境，因此需要原位/实时研究才能在发现和设计方面取得最大的飞跃。然而，最先进的此类研究涉及繁琐的标记方法，这些方法可能会破坏行为，或者不够快，无法捕捉到对刺激有响应的现象。我们利用与分子键共振的 X 射线，展示了一种无需标记的原位纳米探针，能够在几秒钟内完成数据收集。我们的分析光谱模型使用共振软 X 射线定量了共聚物胶束药物传递平台的结构、分子组成和动力学。我们还将该技术应用于烃类捕获聚皂胶束，并发现该胶束的关键有机捕获结构域在聚集时不会合并，而是保留了独特的单分子核心。这种特性提高了其在溢油处理和药物传递等应用中的烃类捕获效率。这种技术能够对任何水溶液分子纳米结构进行无需标记的实时、化学敏感研究。
