State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (i-ChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen 361005, China.
Sci Adv. 2023 Nov 24;9(47):eadh8362. doi: 10.1126/sciadv.adh8362. Epub 2023 Nov 22.
Despite great advances in protein structure analysis, label-free and ultrasensitive methods to obtain the natural and dynamic three-dimensional (3D) structures are still urgently needed. Surface-enhanced Raman spectroscopy (SERS) can be a good candidate, whereas the complexity originated from the interactions between the protein and the gradient surface electric field makes it extremely challenging to determine the protein structure. Here, we propose a deciphering strategy for accurate determination of 3D protein structure from experimental SERS spectra in seconds by simply summing SERS spectra of isolated amino acids in electric fields of different strength with their orientations in protein. The 3D protein structure can be reconstructed by comparing the experimental spectra obtained in a well-defined gap-mode SERS configuration with the simulated spectra. The gradient electric field endows SERS with a unique advantage to section biomolecules with atomic precision, which makes SERS a competent tool for monitoring biomolecular events under physiological conditions.
尽管在蛋白质结构分析方面取得了重大进展，但仍然迫切需要能够无标记且超灵敏地获取天然和动态三维（3D）结构的方法。表面增强拉曼光谱（SERS）可以作为一种很好的候选方法，然而，由于蛋白质与梯度表面电场之间的相互作用所产生的复杂性，使得确定蛋白质结构极具挑战性。在这里，我们提出了一种通过简单地将不同强度电场中分离氨基酸的 SERS 光谱与其在蛋白质中的取向相加，从实验 SERS 光谱中在几秒钟内准确确定 3D 蛋白质结构的破译策略。通过将在明确定义的间隙模式 SERS 配置中获得的实验光谱与模拟光谱进行比较，可以重建 3D 蛋白质结构。梯度电场赋予 SERS 以原子精度对生物分子进行切片的独特优势，这使得 SERS 成为在生理条件下监测生物分子事件的有力工具。
